Articles | Volume 21, issue 3
https://doi.org/10.5194/acp-21-2067-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-2067-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Feb 2021
Research article |
| 11 Feb 2021
| 11 Feb 2021
High-resolution hybrid inversion of IASI ammonia columns to constrain US ammonia emissions using the CMAQ adjoint model
Yilin Chen
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
Huizhong Shen
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
Jennifer Kaiser
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
School of Earth and Atmospheric Sciences, Georgia Institute of
Technology, Atlanta, GA 30332, United States
Yongtao Hu
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
Shannon L. Capps
Department of Civil, Architectural, and Environmental Engineering,
Drexel University, Philadelphia, PA 19104, United States
Shunliu Zhao
Department of Civil and Environmental Engineering, Carleton
University, Ottawa, Ontario K1S5B6, Canada
Amir Hakami
Department of Civil and Environmental Engineering, Carleton
University, Ottawa, Ontario K1S5B6, Canada
Jhih-Shyang Shih
Resources for the Future, Washington, D.C. 20036, USA
Gertrude K. Pavur
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
Matthew D. Turner
SAIC, Stennis Space Center, MS 39529, USA
Daven K. Henze
Mechanical Engineering Department, University of Colorado, Boulder, CO
80309, USA
Jaroslav Resler
Institute of Computer Science of the Czech Academy of Sciences,
Prague, 182 07, Czech Republic
Athanasios Nenes
Institute for Chemical Engineering Sciences, Foundation for Research
and Technology Hellas, Patras, 26504, Greece
School of Architecture, Civil & Environmental Engineering, Ecole
polytechnique fédérale de Lausanne, 1015, Lausanne, Switzerland
Sergey L. Napelenok
Atmospheric & Environmental Systems Modeling Division, U.S. EPA,
Research Triangle Park, NC 27711, USA
Jesse O. Bash
Atmospheric & Environmental Systems Modeling Division, U.S. EPA,
Research Triangle Park, NC 27711, USA
Kathleen M. Fahey
Atmospheric & Environmental Systems Modeling Division, U.S. EPA,
Research Triangle Park, NC 27711, USA
Gregory R. Carmichael
Department of Chemical and Biochemical Engineering, University of
Iowa, Iowa City, IA 52242, USA
Tianfeng Chai
NOAA Air Resources Laboratory (ARL), Cooperative Institute for
Satellites Earth System Studies (CISESS), University of Maryland, College
Park, MD 20740, USA
Lieven Clarisse
Université libre de Bruxelles (ULB), Spectroscopy, Quantum
Chemistry and Atmospheric Remote Sensing (SQUARES), Brussels, Belgium
Pierre-François Coheur
Université libre de Bruxelles (ULB), Spectroscopy, Quantum
Chemistry and Atmospheric Remote Sensing (SQUARES), Brussels, Belgium
Martin Van Damme
Université libre de Bruxelles (ULB), Spectroscopy, Quantum
Chemistry and Atmospheric Remote Sensing (SQUARES), Brussels, Belgium
School of Civil and Environmental Engineering, Georgia Institute of
Technology, Atlanta, GA 30332, United States
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Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
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In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Jaroslav Resler, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, and Igor Ezau
EGUsphere, https://doi.org/10.5194/egusphere-2024-1222, https://doi.org/10.5194/egusphere-2024-1222, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We implemented an observation campaign focused on street-level air quality and vertical meteorological profile measurement in Prague using low-cost sensors and remote sensing devices. Low-cost sensors have undergone long-term field testing, own data correction and drift evaluation procedures. A high level of NO2 pollution was confirmed due to the traffic load in streets, peaks of aerosol pollution appeared more under inversion conditions. The data will be further used for PALM model validation.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
EGUsphere, https://doi.org/10.5194/egusphere-2024-1579, https://doi.org/10.5194/egusphere-2024-1579, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This study investigates the impact of dust on the global radiative effect of nitrate aerosols. The results indicate both positive and negative regional shortwave and longwave radiative effects due to aerosol-radiation interactions and cloud adjustments. The global average net REari and REaci of nitrate aerosols are -0.11 and +0.17 W/m², respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O. T. Pye
EGUsphere, https://doi.org/10.5194/egusphere-2024-1680, https://doi.org/10.5194/egusphere-2024-1680, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Here, we develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry representation, we then estimate the cancer risk in the contiguous US from exposure to ambient formaldehyde and estimate 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Monica Crippa, Diego Guizzardi, Federico Pagani, Marcello Schiavina, Michele Melchiorri, Enrico Pisoni, Francesco Graziosi, Marilena Muntean, Joachim Maes, Lewis Dijkstra, Martin Van Damme, Lieven Clarisse, and Pierre Coheur
Earth Syst. Sci. Data, 16, 2811–2830, https://doi.org/10.5194/essd-16-2811-2024, https://doi.org/10.5194/essd-16-2811-2024, 2024
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Knowing where emissions occur is essential for planning effective emission reduction measures and atmospheric modelling. Disaggregating national emissions over high-resolution grids requires spatial proxies that contain information on the location of different emission sources. This work incorporates state-of-the-art spatial information to improve the spatial representation of global emissions with the Emissions Database for Global Atmospheric Research (EDGAR).
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O’Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
EGUsphere, https://doi.org/10.5194/egusphere-2024-1485, https://doi.org/10.5194/egusphere-2024-1485, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Prescribed burning is an important method for managing ecosystems and preventing wildfires, however, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in two different years, we characterize the emissions and evolution up to 8 hours of PM2.5 mass, BC, and BrC in smoke from burning of forested lands in the southeastern US.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
EGUsphere, https://doi.org/10.5194/egusphere-2024-1401, https://doi.org/10.5194/egusphere-2024-1401, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US, and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to enable explaining the weaker hourly variation in NO2 columns than at the surface.
Jean-Paul Vernier, Thomas J. Aubry, Claudia Timmreck, Anja Schmidt, Lieven Clarisse, Fred Prata, Nicolas Theys, Andrew T. Prata, Graham Mann, Hyundeok Choi, Simon Carn, Richard Rigby, Susan C. Loughlin, and John A. Stevenson
Atmos. Chem. Phys., 24, 5765–5782, https://doi.org/10.5194/acp-24-5765-2024, https://doi.org/10.5194/acp-24-5765-2024, 2024
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The 2019 Raikoke eruption (Kamchatka, Russia) generated one of the largest emissions of particles and gases into the stratosphere since the 1991 Mt. Pinatubo eruption. The Volcano Response (VolRes) initiative, an international effort, provided a platform for the community to share information about this eruption and assess its climate impact. The eruption led to a minor global surface cooling of 0.02 °C in 2020 which is negligible relative to warming induced by human greenhouse gas emissions.
Michal Belda, Nina Benešová, Jaroslav Resler, Peter Huszár, Ondřej Vlček, Pavel Krč, Jan Karlický, Pavel Juruš, and Kryštof Eben
Geosci. Model Dev., 17, 3867–3878, https://doi.org/10.5194/gmd-17-3867-2024, https://doi.org/10.5194/gmd-17-3867-2024, 2024
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For modeling atmospheric chemistry, it is necessary to provide data on emissions of pollutants. These can come from various sources and in various forms, and preprocessing of the data to be ingestible by chemistry models can be quite challenging. We developed the FUME processor to use a database layer that internally transforms all input data into a rigid structure, facilitating further processing to allow for emission processing from the continental to the street scale.
Jaroslav Resler, Petra Bauerová, Michal Belda, Martin Bureš, Kryštof Eben, Vladimír Fuka, Jan Geletič, Radek Jareš, Jan Karel, Josef Keder, Pavel Krč, William Patiño, Jelena Radović, Hynek Řezníček, Matthias Sühring, Adriana Šindelářová, and Ondřej Vlček
EGUsphere, https://doi.org/10.5194/egusphere-2024-1231, https://doi.org/10.5194/egusphere-2024-1231, 2024
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Detailed modeling of urban air quality in stable conditions represents a challenge. This study shows sensitivity of the LES model to meteorological boundary conditions and selected model parameters in a real urban environment in strongly stable conditions. The results show the crucial role of the precise boundary conditions for the comparability of the results with observations as well as the strongly increased sensitivity of the model to studied processes during such stable conditions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
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This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Bruno Franco, Lieven Clarisse, Nicolas Theys, Juliette Hadji-Lazaro, Cathy Clerbaux, and Pierre Coheur
Atmos. Chem. Phys., 24, 4973–5007, https://doi.org/10.5194/acp-24-4973-2024, https://doi.org/10.5194/acp-24-4973-2024, 2024
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Using IASI global infrared measurements, we retrieve nitrous acid (HONO) in fire plumes from space. We detect large enhancements of pyrogenic HONO worldwide, especially from intense wildfires at Northern Hemisphere mid- and high latitudes. Predominance of IASI nighttime over daytime measurements sheds light on HONO's extended lifetime and secondary formation during long-range transport in smoke plumes. Our findings deepen the understanding of atmospheric HONO, crucial for air quality assessment.
Marios Chatziparaschos, Stelios Myriokefalitakis, Nikos Kalivitis, Nikos Daskalakis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Mihalis Vrekoussis, and Maria Kanakidou
EGUsphere, https://doi.org/10.5194/egusphere-2024-952, https://doi.org/10.5194/egusphere-2024-952, 2024
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We show distinct seasonal and geographical patterns in the contributions of mineral dust, marine and terrestrial biological particles to ice-nucleating particles (INP) concentrations that lead to atmospheric ice formation, a major source of uncertainty in climate predictions. Bioaerosols are the major source of INP at high temperatures, while mineral dust influences the global INP population at lower temperatures. These particles can satisfactorily reproduce INP in a climate model.
Jelena Radović, Michal Belda, Jaroslav Resler, Kryštof Eben, Martin Bureš, Jan Geletič, Pavel Krč, Hynek Řezníček, and Vladimír Fuka
Geosci. Model Dev., 17, 2901–2927, https://doi.org/10.5194/gmd-17-2901-2024, https://doi.org/10.5194/gmd-17-2901-2024, 2024
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Boundary conditions are of crucial importance for numerical model (e.g., PALM) validation studies and have a large influence on the model results, especially when studying the atmosphere of real, complex, and densely built urban environments. Our experiments with different driving conditions for the large-eddy simulation model PALM show its strong dependency on boundary conditions, which is important for the proper separation of errors coming from the boundary conditions and the model itself.
Manu Anna Thomas, Klaus Wyser, Shiyu Wang, Marios Chatziparaschos, Paraskevi Georgakaki, Montserrat Costa-Surós, Maria Gonçalves Ageitos, Maria Kanakidou, Carlos Pérez García-Pando, Athanasios Nenes, Twan van Noije, Philippe Le Sager, and Abhay Devasthale
EGUsphere, https://doi.org/10.5194/egusphere-2024-248, https://doi.org/10.5194/egusphere-2024-248, 2024
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Aerosol-cloud interactions occur at a range of spatio-temporal scales. While evaluating recent developments in EC-Earth3-AerChem model, this study aims to understand the extent to which Twomey effect manifests itself at larger scales. We report a reduction in the warm bias over the Southern Ocean due to model improvements. While we do see footprints of Twomey effect at larger scales, the negative relationship between cloud droplet number and liquid water drives the shortwave radiative effect.
Asher P. Mouat, Zelda A. Siegel, and Jennifer Kaiser
Atmos. Meas. Tech., 17, 1979–1994, https://doi.org/10.5194/amt-17-1979-2024, https://doi.org/10.5194/amt-17-1979-2024, 2024
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Three fast-measurement formaldehyde monitors were deployed at two field sites in Atlanta, GA, over 1 year. Four different zeroing methods were tested to develop an optimal field setup as well as procedures for instrument calibration. Observations agreed well after calibration but were much higher compared to the TO-11A monitoring method, which is the golden standard. Historical HCHO concentrations were compared with measurements in this work, showing a 22 % reduction in midday HCHO since 1999.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
EGUsphere, https://doi.org/10.5194/egusphere-2024-737, https://doi.org/10.5194/egusphere-2024-737, 2024
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PM1 chemical characterization and PMF source apportionment on the combined organic and inorganic fraction took place at the high-altitude (HAC)2 station. Cloud presence was found to reduce PM1 concentrations, affecting sulphate more than organics. Interstitial aerosol was richer in low hygroscopic organics and acidic inorganics, compared to activated. Higher relative abundance of eBC compared to the other components was revealed for FT conditions compared to PBL.
Romanos Foskinis, Ghislain Motos, Maria I. Gini, Olga Zografou, Kunfeng Gao, Stergios Vratolis, Konstantinos Granakis, Ville Vakkari, Kalliopi Violaki, Andreas Aktypis, Christos Kaltsonoudis, Zongbo Shi, Mika Komppula, Spyros N. Pandis, Konstantinos Eleftheriadis, Alexandros Papayannis, and Athanasios Nenes
EGUsphere, https://doi.org/10.5194/egusphere-2024-490, https://doi.org/10.5194/egusphere-2024-490, 2024
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Analysis of modeling, in-situ & remote sensing reveal the microphysical state of orographic clouds & their response to aerosol from the boundary layer & free troposphere. We should that this cloud responses to aerosol is robust, as predicted supersaturation and cloud droplet number levels agree with those determined from in-cloud measurements. The ability to determine if clouds are velocity- or aerosol-limited allow for novel model constraints and remote sensing products.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
EGUsphere, https://doi.org/10.5194/egusphere-2024-554, https://doi.org/10.5194/egusphere-2024-554, 2024
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Chemical transport model simulations are combined with ozone observations to estimate the bias in ozone attributable to US anthropogenic sources as well as several individual sources of US background ozone: natural sources, non-US anthropogenic sources, and stratospheric ozone. Results indicate a positive bias correlated with US anthropogenic emissions during summer in the eastern US and a negative bias correlated with stratospheric ozone during spring.
Kunfeng Gao, Franziska Vogel, Romanos Foskinis, Stergios Vratolis, Maria I. Gini, Konstantinos Granakis, Anne-Claire Billault-Roux, Paraskevi Georgakaki, Olga Zografou, Prodromos Fetfatzis, Alexis Berne, Alexandros Papagiannis, Konstantinos Eleftheridadis, Ottmar Möhler, and Athanasios Nenes
EGUsphere, https://doi.org/10.5194/egusphere-2024-511, https://doi.org/10.5194/egusphere-2024-511, 2024
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Ice nucleating particle concentrations (INPs) are required for correct predictions of clouds & precipitation in a changing climate and is poorly constrained in climate models. We unravel airmass & source contributions to INPs in the E.Mediterranean & find that biological particles are important regardless of origin (continental/marine – even during Saharan dust events). The parameterizations developed exhibit superior performance & enable models to consider biological particle effects on INPs.
Min Huang, Gregory R. Carmichael, James H. Crawford, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
EGUsphere, https://doi.org/10.5194/egusphere-2024-484, https://doi.org/10.5194/egusphere-2024-484, 2024
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This study uses model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutants’ budgets in this area as local emissions go down.
Alexandros Milousis, Alexandra P. Tsimpidi, Holger Tost, Spyros N. Pandis, Athanasios Nenes, Astrid Kiendler-Scharr, and Vlassis A. Karydis
Geosci. Model Dev., 17, 1111–1131, https://doi.org/10.5194/gmd-17-1111-2024, https://doi.org/10.5194/gmd-17-1111-2024, 2024
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This study aims to evaluate the newly developed ISORROPIA-lite aerosol thermodynamic module within the EMAC model and explore discrepancies in global atmospheric simulations of aerosol composition and acidity by utilizing different aerosol phase states. Even though local differences were found in regions where the RH ranged from 20 % to 60 %, on a global scale the results are similar. Therefore, ISORROPIA-lite can be a reliable and computationally effective alternative to ISORROPIA II in EMAC.
Jiachen Liu, Eric Chen, and Shannon L. Capps
Geosci. Model Dev., 17, 567–585, https://doi.org/10.5194/gmd-17-567-2024, https://doi.org/10.5194/gmd-17-567-2024, 2024
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Air pollution harms human life and ecosystems, but its sources are complex. Scientists and policy makers use air pollution models to advance knowledge and inform control strategies. We implemented a recently developed numeral system to relate any set of model inputs, like pollutant emissions from a given activity, to all model outputs, like concentrations of pollutants harming human health. This approach will be straightforward to update when scientists discover new processes in the atmosphere.
Irene Constantina Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-233, https://doi.org/10.5194/gmd-2023-233, 2024
Revised manuscript accepted for GMD
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Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Hyerim Kim, Xi Chen, Jun Wang, Zhendong Lu, Meng Zhou, Gregory Carmichael, Sang Seo Park, and Jhoon Kim
EGUsphere, https://doi.org/10.5194/egusphere-2023-3115, https://doi.org/10.5194/egusphere-2023-3115, 2024
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We compare aerosol layer height (ALH) derived from satellite platforms (GEMS, EPIC, TROPOMI). Validation against CALIOP shows high correlation for EPIC and TROPOMI (R > 0.7, overestimation ~0.8 km), while GEMS displays minimal bias (0.1 km) with a lower correlation (R = 0.64). Categorizing GEMS ALH with UVAI ≥ 3 improves agreement. GEMS exhibits a narrower ALH range and lower mean value than TROPOMI and EPIC. Diurnal variation of EPIC and GEMS ALH aligns with the boundary layer development.
Camille Viatte, Nadir Guendouz, Clarisse Dufaux, Arjan Hensen, Daan Swart, Martin Van Damme, Lieven Clarisse, Pierre Coheur, and Cathy Clerbaux
Atmos. Chem. Phys., 23, 15253–15267, https://doi.org/10.5194/acp-23-15253-2023, https://doi.org/10.5194/acp-23-15253-2023, 2023
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Ammonia (NH3) is an important air pollutant which, as a precursor of fine particulate matter, raises public health concerns. Models have difficulty predicting events of pollution associated with NH3 since ground-based observations of this gas are still relatively sparse and difficult to implement. We present the first relatively long (2.5 years) and continuous record of hourly NH3 concentrations in Paris to determine its temporal variabilities at different scales to unravel emission sources.
Jiemei Liu, Jesper Heile Christensen, Zhuyun Ye, Shikui Dong, Camilla Geels, Jørgen Brandt, Athanasios Nenes, Yuan Yuan, and Ulas Im
EGUsphere, https://doi.org/10.5194/egusphere-2023-2615, https://doi.org/10.5194/egusphere-2023-2615, 2023
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In this study, China was chosen as an example to conduct a quantitative analysis using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from WRF weather forecast model. It found that meteorological conditions and emission inventories contributed 46 % (65 %) and 54 % (35 %) to the variations in PM2.5 concentrations (OP), respectively, highlighting secondary aerosol formation and biomass burning as the primary contributors to PM2.5 and OP levels.
Ghislain Motos, Gabriel Freitas, Paraskevi Georgakaki, Jörg Wieder, Guangyu Li, Wenche Aas, Chris Lunder, Radovan Krejci, Julie Thérèse Pasquier, Jan Henneberger, Robert Oscar David, Christoph Ritter, Claudia Mohr, Paul Zieger, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13941–13956, https://doi.org/10.5194/acp-23-13941-2023, https://doi.org/10.5194/acp-23-13941-2023, 2023
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Low-altitude clouds play a key role in regulating the climate of the Arctic, a region that suffers from climate change more than any other on the planet. We gathered meteorological and aerosol physical and chemical data over a year and utilized them for a parameterization that help us unravel the factors driving and limiting the efficiency of cloud droplet formation. We then linked this information to the sources of aerosol found during each season and to processes of cloud glaciation.
Calvin Howes, Pablo E. Saide, Hugh Coe, Amie Dobracki, Steffen Freitag, Jim M. Haywood, Steven G. Howell, Siddhant Gupta, Janek Uin, Mary Kacarab, Chongai Kuang, L. Ruby Leung, Athanasios Nenes, Greg M. McFarquhar, James Podolske, Jens Redemann, Arthur J. Sedlacek, Kenneth L. Thornhill, Jenny P. S. Wong, Robert Wood, Huihui Wu, Yang Zhang, Jianhao Zhang, and Paquita Zuidema
Atmos. Chem. Phys., 23, 13911–13940, https://doi.org/10.5194/acp-23-13911-2023, https://doi.org/10.5194/acp-23-13911-2023, 2023
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To better understand smoke properties and its interactions with clouds, we compare the WRF-CAM5 model with observations from ORACLES, CLARIFY, and LASIC field campaigns in the southeastern Atlantic in August 2017. The model transports and mixes smoke well but does not fully capture some important processes. These include smoke chemical and physical aging over 4–12 days, smoke removal by rain, sulfate particle formation, aerosol activation into cloud droplets, and boundary layer turbulence.
Stylianos Kakavas, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 13555–13564, https://doi.org/10.5194/acp-23-13555-2023, https://doi.org/10.5194/acp-23-13555-2023, 2023
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Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out 1-year aerosol simulations over the continental US. We show that such organic water impacts can increase dry PM1 levels by up to 2 μg m-3 when RH levels and PM1 concentrations are high.
Lieven Clarisse, Bruno Franco, Martin Van Damme, Tommaso Di Gioacchino, Juliette Hadji-Lazaro, Simon Whitburn, Lara Noppen, Daniel Hurtmans, Cathy Clerbaux, and Pierre Coheur
Atmos. Meas. Tech., 16, 5009–5028, https://doi.org/10.5194/amt-16-5009-2023, https://doi.org/10.5194/amt-16-5009-2023, 2023
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Ammonia is an important atmospheric pollutant. This article presents version 4 of the algorithm which retrieves ammonia abundances from the infrared measurements of the satellite sounder IASI. A measurement operator is introduced that can emulate the measurements (so-called averaging kernels) and measurement uncertainty is better characterized. Several other changes to the product itself are also documented, most of which improve the temporal consistency of the 2007–2022 IASI NH3 dataset.
Rui Wang, Da Pan, Xuehui Guo, Kang Sun, Lieven Clarisse, Martin Van Damme, Pierre-François Coheur, Cathy Clerbaux, Melissa Puchalski, and Mark A. Zondlo
Atmos. Chem. Phys., 23, 13217–13234, https://doi.org/10.5194/acp-23-13217-2023, https://doi.org/10.5194/acp-23-13217-2023, 2023
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Ammonia (NH3) is a key precursor for fine particulate matter (PM2.5) and a primary form of reactive nitrogen, yet it has sparse ground measurements. We perform the first comprehensive comparison between ground observations and satellite retrievals in the US, demonstrating that satellite NH3 data can help fill spatial gaps in the current ground monitoring networks. Trend analyses using both datasets highlight increasing NH3 trends across the US, including the NH3 hotspots and urban areas.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Rimal Abeed, Camille Viatte, William C. Porter, Nikolaos Evangeliou, Cathy Clerbaux, Lieven Clarisse, Martin Van Damme, Pierre-François Coheur, and Sarah Safieddine
Atmos. Chem. Phys., 23, 12505–12523, https://doi.org/10.5194/acp-23-12505-2023, https://doi.org/10.5194/acp-23-12505-2023, 2023
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Ammonia emissions from agricultural activities will inevitably increase with the rise in population. We use a variety of datasets (satellite, reanalysis, and model simulation) to calculate the first regional map of ammonia emission potential during the start of the growing season in Europe. We then apply our developed method using a climate model to show the effect of the temperature increase on future ammonia columns under two possible climate scenarios.
Guangyu Li, Elise K. Wilbourn, Zezhen Cheng, Jörg Wieder, Allison Fagerson, Jan Henneberger, Ghislain Motos, Rita Traversi, Sarah D. Brooks, Mauro Mazzola, Swarup China, Athanasios Nenes, Ulrike Lohmann, Naruki Hiranuma, and Zamin A. Kanji
Atmos. Chem. Phys., 23, 10489–10516, https://doi.org/10.5194/acp-23-10489-2023, https://doi.org/10.5194/acp-23-10489-2023, 2023
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In this work, we present results from an Arctic field campaign (NASCENT) in Ny-Ålesund, Svalbard, on the abundance, variability, physicochemical properties, and potential sources of ice-nucleating particles (INPs) relevant for mixed-phase cloud formation. This work improves the data coverage of Arctic INPs and aerosol properties, allowing for the validation of models predicting cloud microphysical and radiative properties of mixed-phase clouds in the rapidly warming Arctic.
Anne-Claire Billault-Roux, Paraskevi Georgakaki, Josué Gehring, Louis Jaffeux, Alfons Schwarzenboeck, Pierre Coutris, Athanasios Nenes, and Alexis Berne
Atmos. Chem. Phys., 23, 10207–10234, https://doi.org/10.5194/acp-23-10207-2023, https://doi.org/10.5194/acp-23-10207-2023, 2023
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Secondary ice production plays a key role in clouds and precipitation. In this study, we analyze radar measurements from a snowfall event in the Jura Mountains. Complex signatures are observed, which reveal that ice crystals were formed through various processes. An analysis of multi-sensor data suggests that distinct ice multiplication processes were taking place. Both the methods used and the insights gained through this case study contribute to a better understanding of snowfall microphysics.
Mária Lbadaoui-Darvas, Ari Laaksonen, and Athanasios Nenes
Atmos. Chem. Phys., 23, 10057–10074, https://doi.org/10.5194/acp-23-10057-2023, https://doi.org/10.5194/acp-23-10057-2023, 2023
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Heterogeneous ice nucleation is the main ice formation mechanism in clouds. The mechanism of different freezing modes is to date unknown, which results in large model biases. Experiments do not allow for direct observation of ice nucleation at its native resolution. This work uses first principles molecular simulations to determine the mechanism of the least-understood ice nucleation mode and link it to adsorption through a novel modeling framework that unites ice and droplet formation.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Zhao-Cheng Zeng, Lu Lee, Chengli Qi, Lieven Clarisse, and Martin Van Damme
Atmos. Meas. Tech., 16, 3693–3713, https://doi.org/10.5194/amt-16-3693-2023, https://doi.org/10.5194/amt-16-3693-2023, 2023
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This study presents an NH3 retrieval algorithm based on the optimal estimation method for the Geostationary Interferometric Infrared Sounder (GIIRS) on board China’s FengYun-4B satellite (FY-4B/GIIRS). Retrieval results demonstrate the capability of FY-4B/GIIRS in capturing the diurnal NH3 changes in East Asia. This operational geostationary observation by FY-4B/GIIRS represents an important advancement over the twice-per-day observations provided by current low-Earth-orbit (LEO) instruments.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
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A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
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Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Qian Shu, Sergey L. Napelenok, William T. Hutzell, Kirk R. Baker, Barron H. Henderson, Benjamin N. Murphy, and Christian Hogrefe
Geosci. Model Dev., 16, 2303–2322, https://doi.org/10.5194/gmd-16-2303-2023, https://doi.org/10.5194/gmd-16-2303-2023, 2023
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Source attribution methods are generally used to determine culpability of precursor emission sources to ambient pollutant concentrations. However, source attribution of secondarily formed pollutants such as ozone and its precursors cannot be explicitly measured, making evaluation of source apportionment methods challenging. In this study, multiple apportionment approach comparisons show common features but still reveal wide variations in predicted sector contribution and species dependency.
Adrien Vu Van, Anne Boynard, Pascal Prunet, Dominique Jolivet, Olivier Lezeaux, Patrice Henry, Claude Camy-Peyret, Lieven Clarisse, Bruno Franco, Pierre-François Coheur, and Cathy Clerbaux
Atmos. Meas. Tech., 16, 2107–2127, https://doi.org/10.5194/amt-16-2107-2023, https://doi.org/10.5194/amt-16-2107-2023, 2023
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With its near-real-time observations and good horizontal coverage, the Infrared Atmospheric Sounding Interferometer (IASI) instrument can contribute to the monitoring systems for a systematic and continuous detection of exceptional atmospheric events such as fires, anthropogenic pollution episodes, volcanic eruptions, or industrial releases. In this paper, a new approach is described for the detection and characterization of unexpected events in terms of trace gases using IASI radiance spectra.
Emily D. Lenhardt, Lan Gao, Jens Redemann, Feng Xu, Sharon P. Burton, Brian Cairns, Ian Chang, Richard A. Ferrare, Chris A. Hostetler, Pablo E. Saide, Calvin Howes, Yohei Shinozuka, Snorre Stamnes, Mary Kacarab, Amie Dobracki, Jenny Wong, Steffen Freitag, and Athanasios Nenes
Atmos. Meas. Tech., 16, 2037–2054, https://doi.org/10.5194/amt-16-2037-2023, https://doi.org/10.5194/amt-16-2037-2023, 2023
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Small atmospheric particles, such as smoke from wildfires or pollutants from human activities, impact cloud properties, and clouds have a strong influence on climate. To better understand the distributions of these particles, we develop relationships to derive their concentrations from remote sensing measurements from an instrument called a lidar. Our method is reliable for smoke particles, and similar steps can be taken to develop relationships for other particle types.
Ian Chang, Lan Gao, Connor J. Flynn, Yohei Shinozuka, Sarah J. Doherty, Michael S. Diamond, Karla M. Longo, Gonzalo A. Ferrada, Gregory R. Carmichael, Patricia Castellanos, Arlindo M. da Silva, Pablo E. Saide, Calvin Howes, Zhixin Xue, Marc Mallet, Ravi Govindaraju, Qiaoqiao Wang, Yafang Cheng, Yan Feng, Sharon P. Burton, Richard A. Ferrare, Samuel E. LeBlanc, Meloë S. Kacenelenbogen, Kristina Pistone, Michal Segal-Rozenhaimer, Kerry G. Meyer, Ju-Mee Ryoo, Leonhard Pfister, Adeyemi A. Adebiyi, Robert Wood, Paquita Zuidema, Sundar A. Christopher, and Jens Redemann
Atmos. Chem. Phys., 23, 4283–4309, https://doi.org/10.5194/acp-23-4283-2023, https://doi.org/10.5194/acp-23-4283-2023, 2023
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Abundant aerosols are present above low-level liquid clouds over the southeastern Atlantic during late austral spring. The model simulation differences in the proportion of aerosol residing in the planetary boundary layer and in the free troposphere can greatly affect the regional aerosol radiative effects. This study examines the aerosol loading and fractional aerosol loading in the free troposphere among various models and evaluates them against measurements from the NASA ORACLES campaign.
Forwood Wiser, Bryan K. Place, Siddhartha Sen, Havala O. T. Pye, Benjamin Yang, Daniel M. Westervelt, Daven K. Henze, Arlene M. Fiore, and V. Faye McNeill
Geosci. Model Dev., 16, 1801–1821, https://doi.org/10.5194/gmd-16-1801-2023, https://doi.org/10.5194/gmd-16-1801-2023, 2023
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We developed a reduced model of atmospheric isoprene oxidation, AMORE-Isoprene 1.0. It was created using a new Automated Model Reduction (AMORE) method designed to simplify complex chemical mechanisms with minimal manual adjustments to the output. AMORE-Isoprene 1.0 has improved accuracy and similar size to other reduced isoprene mechanisms. When included in the CRACMM mechanism, it improved the accuracy of EPA’s CMAQ model predictions for the northeastern USA compared to observations.
Xueying Yu, Dylan B. Millet, Daven K. Henze, Alexander J. Turner, Alba Lorente Delgado, A. Anthony Bloom, and Jianxiong Sheng
Atmos. Chem. Phys., 23, 3325–3346, https://doi.org/10.5194/acp-23-3325-2023, https://doi.org/10.5194/acp-23-3325-2023, 2023
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We combine satellite measurements with a novel downscaling method to map global methane emissions at 0.1°×0.1° resolution. These fine-scale emission estimates reveal unreported emission hotspots and shed light on the roles of agriculture, wetlands, and fossil fuels for regional methane budgets. The satellite-derived emissions point in particular to missing fossil fuel emissions in the Middle East and to a large emission underestimate in South Asia that appears to be tied to monsoon rainfall.
John T. Walker, Xi Chen, Zhiyong Wu, Donna Schwede, Ryan Daly, Aleksandra Djurkovic, A. Christopher Oishi, Eric Edgerton, Jesse Bash, Jennifer Knoepp, Melissa Puchalski, John Iiames, and Chelcy F. Miniat
Biogeosciences, 20, 971–995, https://doi.org/10.5194/bg-20-971-2023, https://doi.org/10.5194/bg-20-971-2023, 2023
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Better estimates of atmospheric nitrogen (N) deposition are needed to accurately assess ecosystem risk and impacts from deposition of nutrients and acidity. Using measurements and modeling, we estimate total N deposition of 6.7 kg N ha−1 yr−1 at a forest site in the southern Appalachian Mountains, a region sensitive to atmospheric deposition. Reductions in deposition of reduced forms of N (ammonia and ammonium) will be needed to meet the lowest estimates of N critical loads for the region.
Peng Wang, Ruhan Zhang, Shida Sun, Meng Gao, Bo Zheng, Dan Zhang, Yanli Zhang, Gregory R. Carmichael, and Hongliang Zhang
Atmos. Chem. Phys., 23, 2983–2996, https://doi.org/10.5194/acp-23-2983-2023, https://doi.org/10.5194/acp-23-2983-2023, 2023
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In China, the number of vehicles has jumped significantly in the last decade. This caused severe traffic congestion and aggravated air pollution. In this study, we developed a new temporal allocation approach to quantify the impacts of traffic congestion. We found that traffic congestion worsens air quality and the health burden across China, especially in the urban clusters. More effective and comprehensive vehicle emission control policies should be implemented to improve air quality in China.
Maureen Beaudor, Nicolas Vuichard, Juliette Lathière, Nikolaos Evangeliou, Martin Van Damme, Lieven Clarisse, and Didier Hauglustaine
Geosci. Model Dev., 16, 1053–1081, https://doi.org/10.5194/gmd-16-1053-2023, https://doi.org/10.5194/gmd-16-1053-2023, 2023
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Ammonia mainly comes from the agricultural sector, and its volatilization relies on environmental variables. Our approach aims at benefiting from an Earth system model framework to estimate it. By doing so, we represent a consistent spatial distribution of the emissions' response to environmental changes.
We greatly improved the seasonal cycle of emissions compared with previous work. In addition, our model includes natural soil emissions (that are rarely represented in modeling approaches).
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
James D. East, Barron H. Henderson, Sergey L. Napelenok, Shannon N. Koplitz, Golam Sarwar, Robert Gilliam, Allen Lenzen, Daniel Q. Tong, R. Bradley Pierce, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 22, 15981–16001, https://doi.org/10.5194/acp-22-15981-2022, https://doi.org/10.5194/acp-22-15981-2022, 2022
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We present a framework that uses a computer model of air quality, along with air pollution data from satellite instruments, to estimate emissions of nitrogen oxides (NOx) across the Northern Hemisphere. The framework, which advances current methods to infer emissions from satellite observations, provides observationally constrained NOx estimates, including in regions of the world where emissions are highly uncertain, and can improve simulations of air pollutants relevant for health and policy.
Benjamin Sapper, Daven Henze, Manjula Canagaratna, and Harald Stark
EGUsphere, https://doi.org/10.5194/egusphere-2022-1221, https://doi.org/10.5194/egusphere-2022-1221, 2022
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Positive Matrix Factorization (PMF) has been used by atmospheric scientists to extract underlying factors present in large datasets. This paper presents a new technique for weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretative factors and solution diagnostics from an atmospheric chemistry dataset.
Ziqi Gao, Yifeng Wang, Petros Vasilakos, Cesunica E. Ivey, Khanh Do, and Armistead G. Russell
Geosci. Model Dev., 15, 9015–9029, https://doi.org/10.5194/gmd-15-9015-2022, https://doi.org/10.5194/gmd-15-9015-2022, 2022
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While the national ambient air quality standard of ozone is based on the 3-year average of the fourth highest 8 h maximum (MDA8) ozone concentrations, these predicted extreme values using numerical methods are always biased low. We built four computational models (GAM, MARS, random forest and SVR) to predict the fourth highest MDA8 ozone in Southern California using precursor emissions, meteorology and climatological patterns. All models presented acceptable performance, with GAM being the best.
Xun Li, Momei Qin, Lin Li, Kangjia Gong, Huizhong Shen, Jingyi Li, and Jianlin Hu
Atmos. Chem. Phys., 22, 14799–14811, https://doi.org/10.5194/acp-22-14799-2022, https://doi.org/10.5194/acp-22-14799-2022, 2022
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Photochemical indicators have been widely used to predict O3–NOx–VOC sensitivity with given thresholds. Here we assessed the effectiveness of four indicators with a case study in the Yangtze River Delta, China. The overall performance was good, while some indicators showed inconsistencies with the O3 isopleths. The methodology used to determine the thresholds may produce uncertainties. These results would improve our understanding of the use of photochemical indicators in policy implications.
Simon Whitburn, Lieven Clarisse, Marc Crapeau, Thomas August, Tim Hultberg, Pierre François Coheur, and Cathy Clerbaux
Atmos. Meas. Tech., 15, 6653–6668, https://doi.org/10.5194/amt-15-6653-2022, https://doi.org/10.5194/amt-15-6653-2022, 2022
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With more than 15 years of measurements, the IASI radiance dataset is becoming a reference climate data record. Its exploitation for satellite applications requires an accurate and unbiased detection of cloud scenes. Here, we present a new cloud detection algorithm for IASI that is both sensitive and consistent over time. It is based on the use of a neural network, relying on IASI radiance information only and taking as a reference the last version of the operational IASI L2 cloud product.
Gonzalo A. Ferrada, Meng Zhou, Jun Wang, Alexei Lyapustin, Yujie Wang, Saulo R. Freitas, and Gregory R. Carmichael
Geosci. Model Dev., 15, 8085–8109, https://doi.org/10.5194/gmd-15-8085-2022, https://doi.org/10.5194/gmd-15-8085-2022, 2022
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The smoke from fires is composed of different compounds that interact with the atmosphere and can create poor air-quality episodes. Here, we present a new fire inventory based on satellite observations from the Visible Infrared Imaging Radiometer Suite (VIIRS). We named this inventory the VIIRS-based Fire Emission Inventory (VFEI). Advantages of VFEI are its high resolution (~500 m) and that it provides information for many species. VFEI is publicly available and has provided data since 2012.
Beatriz Herrera, Alejandro Bezanilla, Thomas Blumenstock, Enrico Dammers, Frank Hase, Lieven Clarisse, Adolfo Magaldi, Claudia Rivera, Wolfgang Stremme, Kimberly Strong, Camille Viatte, Martin Van Damme, and Michel Grutter
Atmos. Chem. Phys., 22, 14119–14132, https://doi.org/10.5194/acp-22-14119-2022, https://doi.org/10.5194/acp-22-14119-2022, 2022
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This work investigates atmospheric ammonia (NH3), a key trace gas with consequences for the environment and human health, in Mexico City. The results from the ground-based and satellite instruments show the variability and spatial distribution of NH3 over this region. NH3 in Mexico City has been increasing for the past 10 years and most of its sources are urban. This work contributes to a better understanding of NH3 sources and variability in urban and remote areas.
Alice Crawford, Tianfeng Chai, Binyu Wang, Allison Ring, Barbara Stunder, Christopher P. Loughner, Michael Pavolonis, and Justin Sieglaff
Atmos. Chem. Phys., 22, 13967–13996, https://doi.org/10.5194/acp-22-13967-2022, https://doi.org/10.5194/acp-22-13967-2022, 2022
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This study describes the development of a workflow which produces probabilistic and quantitative forecasts of volcanic ash in the atmosphere. The workflow includes methods of incorporating satellite observations of the ash cloud into a modeling framework as well as verification statistics that can be used to guide further model development and provide information for risk-based approaches to flight planning.
Fan Wang, Gregory R. Carmichael, Jing Wang, Bin Chen, Bo Huang, Yuguo Li, Yuanjian Yang, and Meng Gao
Atmos. Chem. Phys., 22, 13341–13353, https://doi.org/10.5194/acp-22-13341-2022, https://doi.org/10.5194/acp-22-13341-2022, 2022
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Unprecedented urbanization in China has led to serious urban heat island (UHI) issues, exerting intense heat stress on urban residents. We find diverse influences of aerosol pollution on urban heat island intensity (UHII) under different circulations. Our results also highlight the role of black carbon in aggravating UHI, especially during nighttime. It could thus be targeted for cooperative management of heat islands and aerosol pollution.
Camille Viatte, Rimal Abeed, Shoma Yamanouchi, William C. Porter, Sarah Safieddine, Martin Van Damme, Lieven Clarisse, Beatriz Herrera, Michel Grutter, Pierre-Francois Coheur, Kimberly Strong, and Cathy Clerbaux
Atmos. Chem. Phys., 22, 12907–12922, https://doi.org/10.5194/acp-22-12907-2022, https://doi.org/10.5194/acp-22-12907-2022, 2022
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Large cities can experience high levels of fine particulate matter (PM2.5) pollution linked to ammonia (NH3) mainly emitted from agricultural activities. Using a combination of PM2.5 and NH3 measurements from in situ instruments, satellite infrared spectrometers, and atmospheric model simulations, we have demonstrated the role of NH3 and meteorological conditions on pollution events occurring over Paris, Toronto, and Mexico City.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys., 22, 12749–12767, https://doi.org/10.5194/acp-22-12749-2022, https://doi.org/10.5194/acp-22-12749-2022, 2022
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We assess Community Multiscale Air Quality (CMAQ) model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement–model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US; we find increasing amounts of reduced nitrogen to the total nitrogen budget.
Asher P. Mouat, Clare Paton-Walsh, Jack B. Simmons, Jhonathan Ramirez-Gamboa, David W. T. Griffith, and Jennifer Kaiser
Atmos. Chem. Phys., 22, 11033–11047, https://doi.org/10.5194/acp-22-11033-2022, https://doi.org/10.5194/acp-22-11033-2022, 2022
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We examine emissions of volatile organic compounds from 2020 wildfires in forested regions of Australia (AU). We find that biomass burning in temperate regions of the US and AU emit similar species in similar proportion, both in natural and lab settings. This suggests studies of wildfires in one region may be used to help improve air quality models in other parts of the world. We observe time series of ozone and nitrogen dioxide. Last, we look at which compounds contribute most to OH reactivity.
Catherine Wespes, Gaetane Ronsmans, Lieven Clarisse, Susan Solomon, Daniel Hurtmans, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Chem. Phys., 22, 10993–11007, https://doi.org/10.5194/acp-22-10993-2022, https://doi.org/10.5194/acp-22-10993-2022, 2022
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The first 10-year data record (2008–2017) of HNO3 total columns measured by the IASI-A/MetOp infrared sounder is exploited to monitor the relationship between the temperature decrease and the HNO3 loss observed each year in the Antarctic stratosphere during the polar night. We verify the recurrence of specific regimes in the cycle of IASI HNO3 and identify the day and the 50 hPa temperature (
drop temperature) corresponding to the onset of denitrification in Antarctic winter for each year.
Nicolas Theys, Christophe Lerot, Hugues Brenot, Jeroen van Gent, Isabelle De Smedt, Lieven Clarisse, Mike Burton, Matthew Varnam, Catherine Hayer, Benjamin Esse, and Michel Van Roozendael
Atmos. Meas. Tech., 15, 4801–4817, https://doi.org/10.5194/amt-15-4801-2022, https://doi.org/10.5194/amt-15-4801-2022, 2022
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Sulfur dioxide plume height after a volcanic eruption is an important piece of information for many different scientific studies and applications. Satellite UV retrievals are useful in this respect, but available algorithms have shown so far limited sensitivity to SO2 height. Here we present a new technique to improve the retrieval of SO2 plume height for SO2 columns as low as 5 DU. We demonstrate the algorithm using TROPOMI measurements and compare with other height estimates.
Zhenqi Luo, Yuzhong Zhang, Wei Chen, Martin Van Damme, Pierre-François Coheur, and Lieven Clarisse
Atmos. Chem. Phys., 22, 10375–10388, https://doi.org/10.5194/acp-22-10375-2022, https://doi.org/10.5194/acp-22-10375-2022, 2022
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We quantify global ammonia (NH3) emissions over the period from 2008 to 2018 using an improved fast top-down method that incorporates Infrared Atmospheric
Sounding Interferometer (IASI) satellite observations and GEOS-Chem atmospheric chemical simulations. The top-down analysis finds a global total NH3 emission that is 30 % higher than the bottom-up estimate, largely reconciling a large discrepancy of more than a factor of 2 found in previous top-down studies using the same satellite data.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanasios Nenes, Arthur Sedlacek III, Hugh Coe, Jens Redemann, Paquita Zuidema, Steven Howell, and James Haywood
Atmos. Chem. Phys., 22, 9389–9412, https://doi.org/10.5194/acp-22-9389-2022, https://doi.org/10.5194/acp-22-9389-2022, 2022
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Transmission electron microscopy was used to analyze aged African smoke particles and how the smoke interacts with the marine atmosphere. We found that the volatility of organic aerosol increases with biomass burning plume age, that black carbon is often mixed with potassium salts and that the marine atmosphere can incorporate Na and Cl into smoke particles. Marine salts are more processed when mixed with smoke plumes, and there are interesting Cl-rich yet Na-absent marine particles.
Lu Zhang, Michal Segal-Rozenhaimer, Haochi Che, Caroline Dang, Arthur J. Sedlacek III, Ernie R. Lewis, Amie Dobracki, Jenny P. S. Wong, Paola Formenti, Steven G. Howell, and Athanasios Nenes
Atmos. Chem. Phys., 22, 9199–9213, https://doi.org/10.5194/acp-22-9199-2022, https://doi.org/10.5194/acp-22-9199-2022, 2022
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Widespread biomass burning (BB) events occur annually in Africa and contribute ~ 1 / 3 of global BB emissions, which contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantifies the BrC absorption of aged BB particles and highlights the potential presence of absorbing iron oxides in this climatically important region.
Bo Li, Cheng Liu, Qihou Hu, Mingzhai Sun, Chengxin Zhang, Shulin Zhang, Yizhi Zhu, Ting Liu, Yike Guo, Gregory R. Carmichael, and Meng Gao
EGUsphere, https://doi.org/10.5194/egusphere-2022-578, https://doi.org/10.5194/egusphere-2022-578, 2022
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Ambient particles have an important impact on human health, meteorology and climate change. By building a deep spatiotemporal neural network model we have overcome the long-standing limitations and get the full time and space coverage ground PM2.5 concentrations. We open the neural network black box data model by using sensitivity analysis and visualization techniques. This research will help improve health effects studies, climate effects of aerosols, and air quality prediction.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Chenhong Zhou, Fan Wang, Yike Guo, Cheng Liu, Dongsheng Ji, Yuesi Wang, Xiaobin Xu, Xiao Lu, Yan Wang, Gregory Carmichael, and Meng Gao
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-187, https://doi.org/10.5194/essd-2022-187, 2022
Manuscript not accepted for further review
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We develop an eXtreme Gradient Boosting (XGBoost) model integrating high-resolution meteorological data, satellite retrievals of trace gases, etc. to provide reconstructed daily ground-level O3 over 2005–2021 in China. It can facilitate climatological, ecological, and health research. The dataset is freely available at Zenodo (https://zenodo.org/record/6507706#.Yo8hKujP13g; Zhou, 2022).
Maria-Elissavet Koukouli, Konstantinos Michailidis, Pascal Hedelt, Isabelle A. Taylor, Antje Inness, Lieven Clarisse, Dimitris Balis, Dmitry Efremenko, Diego Loyola, Roy G. Grainger, and Christian Retscher
Atmos. Chem. Phys., 22, 5665–5683, https://doi.org/10.5194/acp-22-5665-2022, https://doi.org/10.5194/acp-22-5665-2022, 2022
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Volcanic eruptions eject large amounts of ash and trace gases into the atmosphere. The use of space-borne instruments enables the global monitoring of volcanic SO2 emissions in an economical and risk-free manner. The main aim of this paper is to present its extensive verification, accomplished within the ESA S5P+I: SO2LH project, over major recent volcanic eruptions, against collocated space-borne measurements, as well as assess its impact on the forecasts provided by CAMS.
Ranjeet S. Sokhi, Nicolas Moussiopoulos, Alexander Baklanov, John Bartzis, Isabelle Coll, Sandro Finardi, Rainer Friedrich, Camilla Geels, Tiia Grönholm, Tomas Halenka, Matthias Ketzel, Androniki Maragkidou, Volker Matthias, Jana Moldanova, Leonidas Ntziachristos, Klaus Schäfer, Peter Suppan, George Tsegas, Greg Carmichael, Vicente Franco, Steve Hanna, Jukka-Pekka Jalkanen, Guus J. M. Velders, and Jaakko Kukkonen
Atmos. Chem. Phys., 22, 4615–4703, https://doi.org/10.5194/acp-22-4615-2022, https://doi.org/10.5194/acp-22-4615-2022, 2022
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This review of air quality research focuses on developments over the past decade. The article considers current and future challenges that are important from air quality research and policy perspectives and highlights emerging prominent gaps of knowledge. The review also examines how air pollution management needs to adapt to new challenges and makes recommendations to guide the direction for future air quality research within the wider community and to provide support for policy.
Stelios Myriokefalitakis, Elisa Bergas-Massó, María Gonçalves-Ageitos, Carlos Pérez García-Pando, Twan van Noije, Philippe Le Sager, Akinori Ito, Eleni Athanasopoulou, Athanasios Nenes, Maria Kanakidou, Maarten C. Krol, and Evangelos Gerasopoulos
Geosci. Model Dev., 15, 3079–3120, https://doi.org/10.5194/gmd-15-3079-2022, https://doi.org/10.5194/gmd-15-3079-2022, 2022
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We here describe the implementation of atmospheric multiphase processes in the EC-Earth Earth system model. We provide global budgets of oxalate, sulfate, and iron-containing aerosols, along with an analysis of the links among atmospheric composition, aqueous-phase processes, and aerosol dissolution, supported by comparison to observations. This work is a first step towards an interactive calculation of the deposition of bioavailable atmospheric iron coupled to the model’s ocean component.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Marie Bouillon, Sarah Safieddine, Simon Whitburn, Lieven Clarisse, Filipe Aires, Victor Pellet, Olivier Lezeaux, Noëlle A. Scott, Marie Doutriaux-Boucher, and Cathy Clerbaux
Atmos. Meas. Tech., 15, 1779–1793, https://doi.org/10.5194/amt-15-1779-2022, https://doi.org/10.5194/amt-15-1779-2022, 2022
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The IASI instruments have been observing Earth since 2007. We use a neural network to retrieve atmospheric temperatures. This new temperature data record is validated against other datasets and shows good agreement. We use this new dataset to compute trends over the 2008–2020 period. We found a warming of the troposphere, more important at the poles. In the stratosphere, we found that temperatures decrease everywhere except at the South Pole. The cooling is more pronounced at the South pole.
Paraskevi Georgakaki, Georgia Sotiropoulou, Étienne Vignon, Anne-Claire Billault-Roux, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 22, 1965–1988, https://doi.org/10.5194/acp-22-1965-2022, https://doi.org/10.5194/acp-22-1965-2022, 2022
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The modelling study focuses on the importance of ice multiplication processes in orographic mixed-phase clouds, which is one of the least understood cloud types in the climate system. We show that the consideration of ice seeding and secondary ice production through ice–ice collisional breakup is essential for correct predictions of precipitation in mountainous terrain, with important implications for radiation processes.
Mohamed H. Salim, Sebastian Schubert, Jaroslav Resler, Pavel Krč, Björn Maronga, Farah Kanani-Sühring, Matthias Sühring, and Christoph Schneider
Geosci. Model Dev., 15, 145–171, https://doi.org/10.5194/gmd-15-145-2022, https://doi.org/10.5194/gmd-15-145-2022, 2022
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Radiative transfer processes are the main energy transport mechanism in urban areas which influence the surface energy budget and drive local convection. We show here the importance of each process to help modellers decide on how much detail they should include in their models to parameterize radiative transfer in urban areas. We showed how the flow field may change in response to these processes and the essential processes needed to assure acceptable quality of the numerical simulations.
Sarah J. Doherty, Pablo E. Saide, Paquita Zuidema, Yohei Shinozuka, Gonzalo A. Ferrada, Hamish Gordon, Marc Mallet, Kerry Meyer, David Painemal, Steven G. Howell, Steffen Freitag, Amie Dobracki, James R. Podolske, Sharon P. Burton, Richard A. Ferrare, Calvin Howes, Pierre Nabat, Gregory R. Carmichael, Arlindo da Silva, Kristina Pistone, Ian Chang, Lan Gao, Robert Wood, and Jens Redemann
Atmos. Chem. Phys., 22, 1–46, https://doi.org/10.5194/acp-22-1-2022, https://doi.org/10.5194/acp-22-1-2022, 2022
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Between July and October, biomass burning smoke is advected over the southeastern Atlantic Ocean, leading to climate forcing. Model calculations of forcing by this plume vary significantly in both magnitude and sign. This paper compares aerosol and cloud properties observed during three NASA ORACLES field campaigns to the same in four models. It quantifies modeled biases in properties key to aerosol direct radiative forcing and evaluates how these biases propagate to biases in forcing.
Xueying Yu, Dylan B. Millet, and Daven K. Henze
Geosci. Model Dev., 14, 7775–7793, https://doi.org/10.5194/gmd-14-7775-2021, https://doi.org/10.5194/gmd-14-7775-2021, 2021
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We conduct observing system simulation experiments to test how well inverse analyses of high-resolution satellite data from sensors such as TROPOMI can quantify methane emissions. Inversions can improve monthly flux estimates at 25 km even with a spatially biased prior or model transport errors, but results are strongly degraded when both are present. We further evaluate a set of alternate formalisms to overcome limitations of the widely used scale factor approach that arise for missing sources.
Irini Tsiodra, Georgios Grivas, Kalliopi Tavernaraki, Aikaterini Bougiatioti, Maria Apostolaki, Despina Paraskevopoulou, Alexandra Gogou, Constantine Parinos, Konstantina Oikonomou, Maria Tsagkaraki, Pavlos Zarmpas, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 21, 17865–17883, https://doi.org/10.5194/acp-21-17865-2021, https://doi.org/10.5194/acp-21-17865-2021, 2021
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We analyze observations from year-long measurements at Athens, Greece. Nighttime wintertime PAH levels are 4 times higher than daytime, and wintertime values are 15 times higher than summertime. Biomass burning aerosol during wintertime pollution events is responsible for these significant wintertime enhancements and accounts for 43 % of the population exposure to PAH carcinogenic risk. Biomass burning poses additional health risks beyond those associated with the high PM levels that develop.
Mária Lbadaoui-Darvas, Satoshi Takahama, and Athanasios Nenes
Atmos. Chem. Phys., 21, 17687–17714, https://doi.org/10.5194/acp-21-17687-2021, https://doi.org/10.5194/acp-21-17687-2021, 2021
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Aerosol–cloud interactions constitute the most uncertain contribution to climate change. The uptake kinetics of water by aerosol is a central process of cloud droplet formation, yet its molecular-scale mechanism is unknown. We use molecular simulations to study this process for phase-separated organic particles. Our results explain the increased cloud condensation activity of such particles and can be generalized over various compositions, thus possibly serving as a basis for future models.
Nicolas Theys, Vitali Fioletov, Can Li, Isabelle De Smedt, Christophe Lerot, Chris McLinden, Nickolay Krotkov, Debora Griffin, Lieven Clarisse, Pascal Hedelt, Diego Loyola, Thomas Wagner, Vinod Kumar, Antje Innes, Roberto Ribas, François Hendrick, Jonas Vlietinck, Hugues Brenot, and Michel Van Roozendael
Atmos. Chem. Phys., 21, 16727–16744, https://doi.org/10.5194/acp-21-16727-2021, https://doi.org/10.5194/acp-21-16727-2021, 2021
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We present a new algorithm to retrieve sulfur dioxide from space UV measurements. We apply the technique to high-resolution TROPOMI measurements and demonstrate the high sensitivity of the approach to weak SO2 emissions worldwide with an unprecedented limit of detection of 8 kt yr−1. This result has broad implications for atmospheric science studies dealing with improving emission inventories and identifying and quantifying missing sources, in the context of air quality and climate.
Jonathan E. Hickman, Niels Andela, Enrico Dammers, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Courtney A. Di Vittorio, Money Ossohou, Corinne Galy-Lacaux, Kostas Tsigaridis, and Susanne E. Bauer
Atmos. Chem. Phys., 21, 16277–16291, https://doi.org/10.5194/acp-21-16277-2021, https://doi.org/10.5194/acp-21-16277-2021, 2021
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Ammonia (NH3) gas emitted from soils and biomass burning contributes to particulate air pollution. We used satellite observations of the atmosphere over Africa to show that declines in NH3 concentrations over South Sudan's Sudd wetland in 2008–2017 are related to variation in wetland extent. We also find NH3 concentrations increased in West Africa as a result of biomass burning and increased in the Lake Victoria region, likely due to agricultural expansion and intensification.
Siqi Ma, Daniel Tong, Lok Lamsal, Julian Wang, Xuelei Zhang, Youhua Tang, Rick Saylor, Tianfeng Chai, Pius Lee, Patrick Campbell, Barry Baker, Shobha Kondragunta, Laura Judd, Timothy A. Berkoff, Scott J. Janz, and Ivanka Stajner
Atmos. Chem. Phys., 21, 16531–16553, https://doi.org/10.5194/acp-21-16531-2021, https://doi.org/10.5194/acp-21-16531-2021, 2021
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Predicting high ozone gets more challenging as urban emissions decrease. How can different techniques be used to foretell the quality of air to better protect human health? We tested four techniques with the CMAQ model against observations during a field campaign over New York City. The new system proves to better predict the magnitude and timing of high ozone. These approaches can be extended to other regions to improve the predictability of high-O3 episodes in contemporary urban environments.
Hugues Brenot, Nicolas Theys, Lieven Clarisse, Jeroen van Gent, Daniel R. Hurtmans, Sophie Vandenbussche, Nikolaos Papagiannopoulos, Lucia Mona, Timo Virtanen, Andreas Uppstu, Mikhail Sofiev, Luca Bugliaro, Margarita Vázquez-Navarro, Pascal Hedelt, Michelle Maree Parks, Sara Barsotti, Mauro Coltelli, William Moreland, Simona Scollo, Giuseppe Salerno, Delia Arnold-Arias, Marcus Hirtl, Tuomas Peltonen, Juhani Lahtinen, Klaus Sievers, Florian Lipok, Rolf Rüfenacht, Alexander Haefele, Maxime Hervo, Saskia Wagenaar, Wim Som de Cerff, Jos de Laat, Arnoud Apituley, Piet Stammes, Quentin Laffineur, Andy Delcloo, Robertson Lennart, Carl-Herbert Rokitansky, Arturo Vargas, Markus Kerschbaum, Christian Resch, Raimund Zopp, Matthieu Plu, Vincent-Henri Peuch, Michel Van Roozendael, and Gerhard Wotawa
Nat. Hazards Earth Syst. Sci., 21, 3367–3405, https://doi.org/10.5194/nhess-21-3367-2021, https://doi.org/10.5194/nhess-21-3367-2021, 2021
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The purpose of the EUNADICS-AV (European Natural Airborne Disaster Information and Coordination System for Aviation) prototype early warning system (EWS) is to develop the combined use of harmonised data products from satellite, ground-based and in situ instruments to produce alerts of airborne hazards (volcanic, dust, smoke and radionuclide clouds), satisfying the requirement of aviation air traffic management (ATM) stakeholders (https://cordis.europa.eu/project/id/723986).
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Xinxin Ye, Pargoal Arab, Ravan Ahmadov, Eric James, Georg A. Grell, Bradley Pierce, Aditya Kumar, Paul Makar, Jack Chen, Didier Davignon, Greg R. Carmichael, Gonzalo Ferrada, Jeff McQueen, Jianping Huang, Rajesh Kumar, Louisa Emmons, Farren L. Herron-Thorpe, Mark Parrington, Richard Engelen, Vincent-Henri Peuch, Arlindo da Silva, Amber Soja, Emily Gargulinski, Elizabeth Wiggins, Johnathan W. Hair, Marta Fenn, Taylor Shingler, Shobha Kondragunta, Alexei Lyapustin, Yujie Wang, Brent Holben, David M. Giles, and Pablo E. Saide
Atmos. Chem. Phys., 21, 14427–14469, https://doi.org/10.5194/acp-21-14427-2021, https://doi.org/10.5194/acp-21-14427-2021, 2021
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Wildfire smoke has crucial impacts on air quality, while uncertainties in the numerical forecasts remain significant. We present an evaluation of 12 real-time forecasting systems. Comparison of predicted smoke emissions suggests a large spread in magnitudes, with temporal patterns deviating from satellite detections. The performance for AOD and surface PM2.5 and their discrepancies highlighted the role of accurately represented spatiotemporal emission profiles in improving smoke forecasts.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Geosci. Model Dev., 14, 5751–5768, https://doi.org/10.5194/gmd-14-5751-2021, https://doi.org/10.5194/gmd-14-5751-2021, 2021
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The Community Multiscale Air Quality (CMAQ) modeling system extended for hemispheric-scale applications (H-CMAQ) incorporated the satellite-constrained degassing SO2 emissions from 50 volcanos across the Northern Hemisphere. The impact on tropospheric sulfate aerosol (SO42−) is assessed for 2010. Although the considered volcanic emissions occurred at or below the middle of free troposphere (500 hPa), SO42− enhancements of more than 10 % were detected up to the top of free troposphere (250 hPa).
Andreas Tilgner, Thomas Schaefer, Becky Alexander, Mary Barth, Jeffrey L. Collett Jr., Kathleen M. Fahey, Athanasios Nenes, Havala O. T. Pye, Hartmut Herrmann, and V. Faye McNeill
Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, https://doi.org/10.5194/acp-21-13483-2021, 2021
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Feedbacks of acidity and atmospheric multiphase chemistry in deliquesced particles and clouds are crucial for the tropospheric composition, depositions, climate, and human health. This review synthesizes the current scientific knowledge on these feedbacks using both inorganic and organic aqueous-phase chemistry. Finally, this review outlines atmospheric implications and highlights the need for future investigations with respect to reducing emissions of key acid precursors in a changing world.
Jaroslav Resler, Kryštof Eben, Jan Geletič, Pavel Krč, Martin Rosecký, Matthias Sühring, Michal Belda, Vladimír Fuka, Tomáš Halenka, Peter Huszár, Jan Karlický, Nina Benešová, Jana Ďoubalová, Kateřina Honzáková, Josef Keder, Šárka Nápravníková, and Ondřej Vlček
Geosci. Model Dev., 14, 4797–4842, https://doi.org/10.5194/gmd-14-4797-2021, https://doi.org/10.5194/gmd-14-4797-2021, 2021
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We describe validation of the PALM model v6.0 against measurements collected during two observational campaigns in Dejvice, Prague. The study focuses on the evaluation of the newly developed or improved radiative and energy balance modules in PALM related to urban modelling. In addition to the energy-related quantities, it also evaluates air flow and air quality under street canyon conditions.
Meng Gao, Yang Yang, Hong Liao, Bin Zhu, Yuxuan Zhang, Zirui Liu, Xiao Lu, Chen Wang, Qiming Zhou, Yuesi Wang, Qiang Zhang, Gregory R. Carmichael, and Jianlin Hu
Atmos. Chem. Phys., 21, 11405–11421, https://doi.org/10.5194/acp-21-11405-2021, https://doi.org/10.5194/acp-21-11405-2021, 2021
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Light absorption and radiative forcing of black carbon (BC) is influenced by both BC itself and its interactions with other aerosol chemical compositions. In this study, we used the online coupled WRF-Chem model to examine how emission control measures during the Asian-Pacific Economic Cooperation (APEC) conference affect the mixing state and light absorption of BC and the associated implications for BC-PBL interactions.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Simon Rosanka, Bruno Franco, Lieven Clarisse, Pierre-François Coheur, Andrea Pozzer, Andreas Wahner, and Domenico Taraborrelli
Atmos. Chem. Phys., 21, 11257–11288, https://doi.org/10.5194/acp-21-11257-2021, https://doi.org/10.5194/acp-21-11257-2021, 2021
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The strong El Niño in 2015 led to a particular dry season in Indonesia and favoured severe peatland fires. The smouldering conditions of these fires and the high carbon content of peat resulted in high volatile organic compound (VOC) emissions. By using a comprehensive atmospheric model, we show that these emissions have a significant impact on the tropospheric composition and oxidation capacity. These emissions are transported into to the lower stratosphere, resulting in a depletion of ozone.
Min Huang, James H. Crawford, Joshua P. DiGangi, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Xiwu Zhan
Atmos. Chem. Phys., 21, 11013–11040, https://doi.org/10.5194/acp-21-11013-2021, https://doi.org/10.5194/acp-21-11013-2021, 2021
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This study evaluates the impact of satellite soil moisture data assimilation on modeled weather and ozone fields at various altitudes above the southeastern US during the summer. It emphasizes the importance of soil moisture in the understanding of surface ozone pollution and upper tropospheric chemistry, as well as air pollutants’ source–receptor relationships between the US and its downwind areas.
Michal Belda, Jaroslav Resler, Jan Geletič, Pavel Krč, Björn Maronga, Matthias Sühring, Mona Kurppa, Farah Kanani-Sühring, Vladimír Fuka, Kryštof Eben, Nina Benešová, and Mikko Auvinen
Geosci. Model Dev., 14, 4443–4464, https://doi.org/10.5194/gmd-14-4443-2021, https://doi.org/10.5194/gmd-14-4443-2021, 2021
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The analysis summarizes how sensitive the modelling of urban environment is to changes in physical parameters describing the city (e.g. reflectivity of surfaces) and to several heat island mitigation scenarios in a city quarter in Prague, Czech Republic. We used the large-eddy simulation modelling system PALM 6.0. Surface parameters connected to radiation show the highest sensitivity in this configuration. For heat island mitigation, urban vegetation is shown to be the most effective measure.
Paraskevi Georgakaki, Aikaterini Bougiatioti, Jörg Wieder, Claudia Mignani, Fabiola Ramelli, Zamin A. Kanji, Jan Henneberger, Maxime Hervo, Alexis Berne, Ulrike Lohmann, and Athanasios Nenes
Atmos. Chem. Phys., 21, 10993–11012, https://doi.org/10.5194/acp-21-10993-2021, https://doi.org/10.5194/acp-21-10993-2021, 2021
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Aerosol and cloud observations coupled with a droplet activation parameterization was used to investigate the aerosol–cloud droplet link in alpine mixed-phase clouds. Predicted droplet number, Nd, agrees with observations and never exceeds a characteristic “limiting droplet number”, Ndlim, which depends solely on σw. Nd becomes velocity limited when it is within 50 % of Ndlim. Identifying when dynamical changes control Nd variability is central for understanding aerosol–cloud interactions.
Georgia Sotiropoulou, Luisa Ickes, Athanasios Nenes, and Annica M. L. Ekman
Atmos. Chem. Phys., 21, 9741–9760, https://doi.org/10.5194/acp-21-9741-2021, https://doi.org/10.5194/acp-21-9741-2021, 2021
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Mixed-phase clouds are a large source of uncertainty in projections of the Arctic climate. This is partly due to the poor representation of the cloud ice formation processes. Implementing a parameterization for ice multiplication due to mechanical breakup upon collision of two ice particles in a high-resolution model improves cloud ice phase representation; however, cloud liquid remains overestimated.
Kristina Pistone, Paquita Zuidema, Robert Wood, Michael Diamond, Arlindo M. da Silva, Gonzalo Ferrada, Pablo E. Saide, Rei Ueyama, Ju-Mee Ryoo, Leonhard Pfister, James Podolske, David Noone, Ryan Bennett, Eric Stith, Gregory Carmichael, Jens Redemann, Connor Flynn, Samuel LeBlanc, Michal Segal-Rozenhaimer, and Yohei Shinozuka
Atmos. Chem. Phys., 21, 9643–9668, https://doi.org/10.5194/acp-21-9643-2021, https://doi.org/10.5194/acp-21-9643-2021, 2021
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Using aircraft-based measurements off the Atlantic coast of Africa, we found the springtime smoke plume was strongly correlated with the amount of water vapor in the atmosphere (more smoke indicated more humidity). We see the same general feature in satellite-assimilated and free-running models. Our analysis suggests this relationship is not caused by the burning but originates due to coincident continental meteorology plus fires. This air is transported over the ocean without further mixing.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Syuichi Itahashi, Baozhu Ge, Keiichi Sato, Zhe Wang, Junichi Kurokawa, Jiani Tan, Kan Huang, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 21, 8709–8734, https://doi.org/10.5194/acp-21-8709-2021, https://doi.org/10.5194/acp-21-8709-2021, 2021
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This study presents the detailed analysis of acid deposition over southeast Asia based on the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Simulated wet deposition is evaluated with observation data from the Acid Deposition Monitoring Network in East Asia (EANET). The difficulties of models to capture observations are related to the model performance on precipitation. The precipitation-adjusted approach was applied, and the distribution of wet deposition was successfully revised.
Na Zhao, Xinyi Dong, Kan Huang, Joshua S. Fu, Marianne Tronstad Lund, Kengo Sudo, Daven Henze, Tom Kucsera, Yun Fat Lam, Mian Chin, and Simone Tilmes
Atmos. Chem. Phys., 21, 8637–8654, https://doi.org/10.5194/acp-21-8637-2021, https://doi.org/10.5194/acp-21-8637-2021, 2021
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Black carbon acts as a strong climate forcer, especially in vulnerable pristine regions such as the Arctic. This work utilizes ensemble modeling results from the task force Hemispheric Transport of Air Pollution Phase 2 to investigate the responses of Arctic black carbon and surface temperature to various source emission reductions. East Asia contributed the most to Arctic black carbon. The response of Arctic temperature to black carbon was substantially more sensitive than the global average.
Benjamin N. Murphy, Christopher G. Nolte, Fahim Sidi, Jesse O. Bash, K. Wyat Appel, Carey Jang, Daiwen Kang, James Kelly, Rohit Mathur, Sergey Napelenok, George Pouliot, and Havala O. T. Pye
Geosci. Model Dev., 14, 3407–3420, https://doi.org/10.5194/gmd-14-3407-2021, https://doi.org/10.5194/gmd-14-3407-2021, 2021
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The algorithms for applying air pollution emission rates in the Community Multiscale Air Quality (CMAQ) model have been improved to better support users and developers. The new features accommodate emissions perturbation studies that are typical in atmospheric research and output a wealth of metadata for each model run so assumptions can be verified and documented. The new approach dramatically enhances the transparency and functionality of this critical aspect of atmospheric modeling.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, T. Nash Skipper, and Armistead G. Russell
Atmos. Chem. Phys., 21, 8341–8356, https://doi.org/10.5194/acp-21-8341-2021, https://doi.org/10.5194/acp-21-8341-2021, 2021
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Extended ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosols in China are significantly less acidic than those in the United States, with pH values 1–2 units higher. Higher aerosol mass concentrations and the abundance of ammonia and ammonium in China, compared to the United States, are leading causes of the pH difference between these two countries.
Pavel Krč, Jaroslav Resler, Matthias Sühring, Sebastian Schubert, Mohamed H. Salim, and Vladimír Fuka
Geosci. Model Dev., 14, 3095–3120, https://doi.org/10.5194/gmd-14-3095-2021, https://doi.org/10.5194/gmd-14-3095-2021, 2021
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The adverse effects of an urban environment, e.g. heat stress and air pollution, pose a risk to health and well-being. Precise modelling of the urban climate is crucial to mitigate these effects. Conventional atmospheric models are inadequate for modelling the complex structures of the urban environment; in particular, they lack a 3-D model of radiation and its interaction with surfaces and the plant canopy. The new RTM simulates these processes within the PALM-4U urban climate model.
K. Wyat Appel, Jesse O. Bash, Kathleen M. Fahey, Kristen M. Foley, Robert C. Gilliam, Christian Hogrefe, William T. Hutzell, Daiwen Kang, Rohit Mathur, Benjamin N. Murphy, Sergey L. Napelenok, Christopher G. Nolte, Jonathan E. Pleim, George A. Pouliot, Havala O. T. Pye, Limei Ran, Shawn J. Roselle, Golam Sarwar, Donna B. Schwede, Fahim I. Sidi, Tanya L. Spero, and David C. Wong
Geosci. Model Dev., 14, 2867–2897, https://doi.org/10.5194/gmd-14-2867-2021, https://doi.org/10.5194/gmd-14-2867-2021, 2021
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This paper details the scientific updates in the recently released CMAQ version 5.3 (and v5.3.1) and also includes operational and diagnostic evaluations of CMAQv5.3.1 against observations and the previous version of the CMAQ (v5.2.1). This work was done to improve the underlying science in CMAQ. This article is used to inform the CMAQ modeling community of the updates to the modeling system and the expected change in model performance from these updates (versus the previous model version).
Yunhua Chang, Yan-Lin Zhang, Sawaeng Kawichai, Qian Wang, Martin Van Damme, Lieven Clarisse, Tippawan Prapamontol, and Moritz F. Lehmann
Atmos. Chem. Phys., 21, 7187–7198, https://doi.org/10.5194/acp-21-7187-2021, https://doi.org/10.5194/acp-21-7187-2021, 2021
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In this study, we integrated satellite constraints on atmospheric NH3 levels and fire intensity, discrete NH3 concentration measurement, and N isotopic analysis of NH3 in order to assess the regional-scale contribution of biomass burning to ambient atmospheric NH3 in the heartland of Southeast Asia. The combined approach provides a valuable cross-validation framework for source apportioning of NH3 in the lower atmosphere and will thus help to ameliorate predictions of biomass burning emissions.
Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
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NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes atmospheric CO2 globally. We use a multiple regression and inverse model to quantify the relationships between OCO-2 and environmental drivers within individual years for 2015–2018 and within seven global biomes. Our results point to limitations of current space-based observations for inferring environmental relationships but also indicate the potential to inform key relationships that are very uncertain in process-based models.
Karn Vohra, Eloise A. Marais, Shannen Suckra, Louisa Kramer, William J. Bloss, Ravi Sahu, Abhishek Gaur, Sachchida N. Tripathi, Martin Van Damme, Lieven Clarisse, and Pierre-F. Coheur
Atmos. Chem. Phys., 21, 6275–6296, https://doi.org/10.5194/acp-21-6275-2021, https://doi.org/10.5194/acp-21-6275-2021, 2021
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We find satellite observations of atmospheric composition generally reproduce variability in surface air pollution, so we use their long record to estimate air quality trends in major UK and Indian cities. Our trend analysis shows that pollutants targeted with air quality policies have not declined in Delhi and Kanpur but have in London and Birmingham, with the exception of a recent and dramatic increase in reactive volatile organics in London. Unregulated ammonia has increased only in Delhi.
Pooja V. Pawar, Sachin D. Ghude, Chinmay Jena, Andrea Móring, Mark A. Sutton, Santosh Kulkarni, Deen Mani Lal, Divya Surendran, Martin Van Damme, Lieven Clarisse, Pierre-François Coheur, Xuejun Liu, Gaurav Govardhan, Wen Xu, Jize Jiang, and Tapan Kumar Adhya
Atmos. Chem. Phys., 21, 6389–6409, https://doi.org/10.5194/acp-21-6389-2021, https://doi.org/10.5194/acp-21-6389-2021, 2021
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In this study, simulations of atmospheric ammonia (NH3) with MOZART-4 and HTAP-v2 are compared with satellite (IASI) and ground-based measurements to understand the spatial and temporal variability of NH3 over two emission hotspot regions of Asia, the IGP and the NCP. Our simulations indicate that the formation of ammonium aerosols is quicker over the NCP than the IGP, leading to smaller NH3 columns over the higher NH3-emitting NCP compared to the IGP region for comparable emissions.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Nikolaos Evangeliou, Yves Balkanski, Sabine Eckhardt, Anne Cozic, Martin Van Damme, Pierre-François Coheur, Lieven Clarisse, Mark W. Shephard, Karen E. Cady-Pereira, and Didier Hauglustaine
Atmos. Chem. Phys., 21, 4431–4451, https://doi.org/10.5194/acp-21-4431-2021, https://doi.org/10.5194/acp-21-4431-2021, 2021
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Ammonia, a substance that has played a key role in sustaining life, has been increasing in the atmosphere, affecting climate and humans. Understanding the reasons for this increase is important for the beneficial use of ammonia. The evolution of satellite products gives us the opportunity to calculate ammonia emissions easier. We calculated global ammonia emissions over the last 10 years, incorporated them into a chemistry model and recorded notable improvement in reproducing observations.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Jianjun Li, Huangjian Wu, Qizhong Wu, Huansheng Chen, Lili Zhu, Wei Wang, Bing Liu, Qian Wang, Duohong Chen, Yuepeng Pan, Tao Song, Fei Li, Haitao Zheng, Guanglin Jia, Miaomiao Lu, Lin Wu, and Gregory R. Carmichael
Earth Syst. Sci. Data, 13, 529–570, https://doi.org/10.5194/essd-13-529-2021, https://doi.org/10.5194/essd-13-529-2021, 2021
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China's air pollution has changed substantially since 2013. Here we have developed a 6-year-long high-resolution air quality reanalysis dataset over China from 2013 to 2018 to illustrate such changes and to provide a basic dataset for relevant studies. Surface fields of PM2.5, PM10, SO2, NO2, CO, and O3 concentrations are provided, and the evaluation results indicate that the reanalysis dataset has excellent performance in reproducing the magnitude and variation of air pollution in China.
Shoma Yamanouchi, Camille Viatte, Kimberly Strong, Erik Lutsch, Dylan B. A. Jones, Cathy Clerbaux, Martin Van Damme, Lieven Clarisse, and Pierre-Francois Coheur
Atmos. Meas. Tech., 14, 905–921, https://doi.org/10.5194/amt-14-905-2021, https://doi.org/10.5194/amt-14-905-2021, 2021
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Ammonia (NH3) is a major source of pollution in the air. As such, there have been increasing efforts to measure the atmospheric abundance of NH3 and its spatial and temporal variability. In this study, long-term measurements of NH3 over Toronto, Canada, derived from multiscale datasets are examined. These NH3 datasets were compared to each other and to a model to better understand NH3 variability and to assess model performance.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Pierre-Yves Tournigand, Valeria Cigala, Elzbieta Lasota, Mohammed Hammouti, Lieven Clarisse, Hugues Brenot, Fred Prata, Gottfried Kirchengast, Andrea K. Steiner, and Riccardo Biondi
Earth Syst. Sci. Data, 12, 3139–3159, https://doi.org/10.5194/essd-12-3139-2020, https://doi.org/10.5194/essd-12-3139-2020, 2020
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The detection and monitoring of volcanic clouds are important for aviation management, climate and weather forecasts. We present in this paper the first comprehensive archive collecting spatial and temporal information about volcanic clouds generated by the 11 largest eruptions of this century. We provide a complete set of state-of-the-art data allowing the development and testing of new algorithms contributing to improve the accuracy of the estimation of fundamental volcanic cloud parameters.
Liqiang Wang, Shaocai Yu, Pengfei Li, Xue Chen, Zhen Li, Yibo Zhang, Mengying Li, Khalid Mehmood, Weiping Liu, Tianfeng Chai, Yannian Zhu, Daniel Rosenfeld, and John H. Seinfeld
Atmos. Chem. Phys., 20, 14787–14800, https://doi.org/10.5194/acp-20-14787-2020, https://doi.org/10.5194/acp-20-14787-2020, 2020
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The Chinese government has made major strides in curbing anthropogenic emissions. In this study, we constrain a state-of-the-art CTM by a reliable data assimilation method with extensive chemical and meteorological observations. This comprehensive technical design provides a crucial advance in isolating the influences of emission changes and meteorological perturbations over the Yangtze River Delta (YRD) from 2016 to 2019, thus establishing the first map of the PM2.5 mitigation across the YRD.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Audrey Fortems-Cheiney, Gaëlle Dufour, Karine Dufossé, Florian Couvidat, Jean-Marc Gilliot, Guillaume Siour, Matthias Beekmann, Gilles Foret, Frederik Meleux, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Cathy Clerbaux, and Sophie Génermont
Atmos. Chem. Phys., 20, 13481–13495, https://doi.org/10.5194/acp-20-13481-2020, https://doi.org/10.5194/acp-20-13481-2020, 2020
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Studies have suggested the importance of ammonia emissions on pollution particle formation over Europe, whose main atmospheric source is agriculture. In this study, we performed an inter-comparison of two alternative inventories, both with a reference inventory, that quantify the French ammonia emissions during spring 2011. Over regions with large mineral fertilizer use, like over northeastern France, NH3 emissions are probably considerably underestimated by the reference inventory.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys., 20, 13109–13130, https://doi.org/10.5194/acp-20-13109-2020, https://doi.org/10.5194/acp-20-13109-2020, 2020
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We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Yohei Shinozuka, Pablo E. Saide, Gonzalo A. Ferrada, Sharon P. Burton, Richard Ferrare, Sarah J. Doherty, Hamish Gordon, Karla Longo, Marc Mallet, Yan Feng, Qiaoqiao Wang, Yafang Cheng, Amie Dobracki, Steffen Freitag, Steven G. Howell, Samuel LeBlanc, Connor Flynn, Michal Segal-Rosenhaimer, Kristina Pistone, James R. Podolske, Eric J. Stith, Joseph Ryan Bennett, Gregory R. Carmichael, Arlindo da Silva, Ravi Govindaraju, Ruby Leung, Yang Zhang, Leonhard Pfister, Ju-Mee Ryoo, Jens Redemann, Robert Wood, and Paquita Zuidema
Atmos. Chem. Phys., 20, 11491–11526, https://doi.org/10.5194/acp-20-11491-2020, https://doi.org/10.5194/acp-20-11491-2020, 2020
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In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016.
Hyun Cheol Kim, Tianfeng Chai, Ariel Stein, and Shobha Kondragunta
Atmos. Chem. Phys., 20, 10259–10277, https://doi.org/10.5194/acp-20-10259-2020, https://doi.org/10.5194/acp-20-10259-2020, 2020
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Smoke forecasts have been challenged by high uncertainty in fire emission estimates. We develop an inverse modeling system, the HYSPLIT-based Emissions Inverse Modeling System for wildfires, that estimates wildfire emissions from the transport and dispersion of smoke plumes as measured by satellite observations. Using NOAA HYSPLIT and GOES Aerosol/Smoke Product (GASP), the system resolves smoke source strength as a function of time and vertical level and outperforms current operational system.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Solène Turquety, Laurent Menut, Guillaume Siour, Sylvain Mailler, Juliette Hadji-Lazaro, Maya George, Cathy Clerbaux, Daniel Hurtmans, and Pierre-François Coheur
Geosci. Model Dev., 13, 2981–3009, https://doi.org/10.5194/gmd-13-2981-2020, https://doi.org/10.5194/gmd-13-2981-2020, 2020
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Biomass burning emissions are a major source of trace gases and aerosols that need to be accounted for in air quality assessment and forecasting. The APIFLAME model presented in this paper allows the calculation of these emissions based on merged satellite observations at hourly time steps and kilometer scales. Implementing emissions in a chemistry transport model allows realistic simulations of fire plumes as illustrated for wildfires in Portugal in August 2016 using the CHIMERE model.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Jiani Tan, Joshua S. Fu, Gregory R. Carmichael, Syuichi Itahashi, Zhining Tao, Kan Huang, Xinyi Dong, Kazuyo Yamaji, Tatsuya Nagashima, Xuemei Wang, Yiming Liu, Hyo-Jung Lee, Chuan-Yao Lin, Baozhu Ge, Mizuo Kajino, Jia Zhu, Meigen Zhang, Hong Liao, and Zifa Wang
Atmos. Chem. Phys., 20, 7393–7410, https://doi.org/10.5194/acp-20-7393-2020, https://doi.org/10.5194/acp-20-7393-2020, 2020
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This study evaluated the performance of 12 chemical transport models from MICS-Asia III for predicting the particulate matter (PM) over East Asia. Four model processes were investigated as the possible reasons for model bias with measurements and the factors causing inconsistent predictions of PM from different models: (1) model inputs, (2) gas–particle conversion, (3) dust emission modules and (4) removal mechanisms (wet and dry depositions). The influence of each process was discussed.
Matthew J. Cooper, Randall V. Martin, Daven K. Henze, and Dylan B. A. Jones
Atmos. Chem. Phys., 20, 7231–7241, https://doi.org/10.5194/acp-20-7231-2020, https://doi.org/10.5194/acp-20-7231-2020, 2020
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Comparisons between satellite-retrieved and model-simulated NO2 columns are affected by differences between the model vertical profile and the assumed profile used in the retrieval process. We examine how such differences impact NOx emission estimates from satellite observations. Larger differences between the simulated and assumed profile shape correspond to larger emission errors. This reveals the importance of using consistent profile information when comparing satellite columns to models.
Yi Wang, Jun Wang, Xiaoguang Xu, Daven K. Henze, Zhen Qu, and Kai Yang
Atmos. Chem. Phys., 20, 6631–6650, https://doi.org/10.5194/acp-20-6631-2020, https://doi.org/10.5194/acp-20-6631-2020, 2020
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The use of OMPS satellite observations to inverse-model SO2 and NO2 emissions is presented through the GEOS-Chem adjoint modeling framework. The work is illustrated over China. The robustness of the results is studied through separate and joint inversions of SO2 and NO2 and the consideration of NH3 uncertainty. Independent validation is performed with OMI SO2 and NO2 data. It is shown that simultaneous inversion of NO2 and SO2 from OMPS provides an effective way to rapidly update emissions.
Yi Wang, Jun Wang, Meng Zhou, Daven K. Henze, Cui Ge, and Wei Wang
Atmos. Chem. Phys., 20, 6651–6670, https://doi.org/10.5194/acp-20-6651-2020, https://doi.org/10.5194/acp-20-6651-2020, 2020
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We developed four different methods to downscale SO2 and NO2 emissions derived from OMPS satellite observations (in Part 1) for regional air quality modeling at a spatial resolution that is finer than satellite observations. The VIIRS (city lights), TROPOMI, and OMI satellite data as well as surface data are used to evaluate the model. The method of using the top-down emissions from the past month for the air quality forecast in the present month is also shown to have practical merit.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Sojin Lee, Chul Han Song, Kyung Man Han, Daven K. Henze, Kyunghwa Lee, Jinhyeok Yu, Jung-Hun Woo, Jia Jung, Yunsoo Choi, Pablo E. Saide, and Gregory R. Carmichael
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2020-116, https://doi.org/10.5194/gmd-2020-116, 2020
Revised manuscript not accepted
Dong Gao, Krystal J. Godri Pollitt, James A. Mulholland, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 20, 5197–5210, https://doi.org/10.5194/acp-20-5197-2020, https://doi.org/10.5194/acp-20-5197-2020, 2020
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This study provides a direct intercomparison between two assays for quantifying oxidative potential (OP) of ambient particles: the synthetic respiratory-tract-lining fluid (RTLF) assay and the dithiothreitol (DTT) assay. The results suggest that the DTT assay and the ascorbic acid depletion in RTLF are associated with organic species, transition metal ions, and antagonistic interactions between species. The glutathione depletion in RTLF is strongly dependent on water-soluble copper.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Syuichi Itahashi, Rohit Mathur, Christian Hogrefe, Sergey L. Napelenok, and Yang Zhang
Atmos. Chem. Phys., 20, 3397–3413, https://doi.org/10.5194/acp-20-3397-2020, https://doi.org/10.5194/acp-20-3397-2020, 2020
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The state-of-the-science Community Multiscale Air Quality model extended for hemispheric applications (H-CMAQ) is used to model the trans-Pacific transport which has been recognized as a potential source of air pollutants over the US. In Part 2, the higher-order decoupled direct method (HDDM) is applied to investigate the emission impacts from east Asia and the US during April 2010. Furthermore, changes in trans-Pacific transport caused by the recent emissions are examined.
Björn Maronga, Sabine Banzhaf, Cornelia Burmeister, Thomas Esch, Renate Forkel, Dominik Fröhlich, Vladimir Fuka, Katrin Frieda Gehrke, Jan Geletič, Sebastian Giersch, Tobias Gronemeier, Günter Groß, Wieke Heldens, Antti Hellsten, Fabian Hoffmann, Atsushi Inagaki, Eckhard Kadasch, Farah Kanani-Sühring, Klaus Ketelsen, Basit Ali Khan, Christoph Knigge, Helge Knoop, Pavel Krč, Mona Kurppa, Halim Maamari, Andreas Matzarakis, Matthias Mauder, Matthias Pallasch, Dirk Pavlik, Jens Pfafferott, Jaroslav Resler, Sascha Rissmann, Emmanuele Russo, Mohamed Salim, Michael Schrempf, Johannes Schwenkel, Gunther Seckmeyer, Sebastian Schubert, Matthias Sühring, Robert von Tils, Lukas Vollmer, Simon Ward, Björn Witha, Hauke Wurps, Julian Zeidler, and Siegfried Raasch
Geosci. Model Dev., 13, 1335–1372, https://doi.org/10.5194/gmd-13-1335-2020, https://doi.org/10.5194/gmd-13-1335-2020, 2020
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In this paper, we describe the PALM model system 6.0. PALM is a Fortran-based turbulence-resolving code and has been applied for studying a variety of atmospheric and oceanic boundary layers for about 20 years. The model is optimized for use on massively parallel computer architectures. During the last years, PALM has been significantly improved and now offers a variety of new components that are especially designed to simulate the urban atmosphere at building-resolving resolution.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Wei Wang, Cheng Liu, Lieven Clarisse, Martin Van Damme, Pierre-François Coheur, Yu Xie, Changgong Shan, Qihou Hu, Huifang Zhang, Youwen Sun, Hao Yin, and Nicholas Jones
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2020-39, https://doi.org/10.5194/amt-2020-39, 2020
Revised manuscript not accepted
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Ground-based FTIR observations are used to obtain the total columns and vertical profiles of atmospheric NH3 at a measurement site in Hefei, China. The spatial distribution, temporal variation, seasonal trend, and emission sources of NH3 are analyzed. FTIR observations captured the seasonal cycle of NH3. The IASI data are in broad agreement with our FTIR data. This is the first time that ground-based FTIR remote sensing of NH3 columns and comparison with satellite data are reported in China.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
Syuichi Itahashi, Baozhu Ge, Keiichi Sato, Joshua S. Fu, Xuemei Wang, Kazuyo Yamaji, Tatsuya Nagashima, Jie Li, Mizuo Kajino, Hong Liao, Meigen Zhang, Zhe Wang, Meng Li, Junichi Kurokawa, Gregory R. Carmichael, and Zifa Wang
Atmos. Chem. Phys., 20, 2667–2693, https://doi.org/10.5194/acp-20-2667-2020, https://doi.org/10.5194/acp-20-2667-2020, 2020
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This study gives an overview of acid deposition from the Model Inter-Comparison Study for Asia (MICS-Asia) phase III. Wet deposition simulated by a total of nine models is evaluated with observation data from the Acid Deposition Monitoring Network in East Asia (EANET). The total deposition maps comparing to emissions over Asia are presented. To seek a way to improve the model performance, ensemble approaches and the precipitation-adjusted method are discussed.
Zhining Tao, Mian Chin, Meng Gao, Tom Kucsera, Dongchul Kim, Huisheng Bian, Jun-ichi Kurokawa, Yuesi Wang, Zirui Liu, Gregory R. Carmichael, Zifa Wang, and Hajime Akimoto
Atmos. Chem. Phys., 20, 2319–2339, https://doi.org/10.5194/acp-20-2319-2020, https://doi.org/10.5194/acp-20-2319-2020, 2020
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One goal of the Model Inter-Comparison Study for Asia (MICS-Asia) Phase III is to identify strengths and weaknesses of current air quality models to provide insights into reducing uncertainties. This study identified that a 15 km grid would be the optimal horizontal resolution in terms of performance and resource usage to capture average and extreme air quality over East Asia and is thus suggested for use in future MICS-Asia modeling activities if the investigation domain remains the same.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Camille Viatte, Tianze Wang, Martin Van Damme, Enrico Dammers, Frederik Meleux, Lieven Clarisse, Mark W. Shephard, Simon Whitburn, Pierre François Coheur, Karen E. Cady-Pereira, and Cathy Clerbaux
Atmos. Chem. Phys., 20, 577–596, https://doi.org/10.5194/acp-20-577-2020, https://doi.org/10.5194/acp-20-577-2020, 2020
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We study concentrations and spatiotemporal variabilities of atmospheric NH3 from the agricultural sector to gain insights on its effects on the Paris megacity air quality using satellite data from IASI and CrIS.
We evaluate the regional CHIMERE model capacity to reproduce NH3 and particulate matter (PM2.5) concentrations and variabilities in the domain of study.
We quantify the main meteorological parameters driving the optimal conditions involved in the PM2.5 formation from NH3 in Paris.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Cheng Chen, Oleg Dubovik, Daven K. Henze, Mian Chin, Tatyana Lapyonok, Gregory L. Schuster, Fabrice Ducos, David Fuertes, Pavel Litvinov, Lei Li, Anton Lopatin, Qiaoyun Hu, and Benjamin Torres
Atmos. Chem. Phys., 19, 14585–14606, https://doi.org/10.5194/acp-19-14585-2019, https://doi.org/10.5194/acp-19-14585-2019, 2019
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Global BC, OC and DD aerosol emissions are inverted from POLDER/PARASOL observations for the year 2010 based on the GEOS-Chem inverse modeling framework. The retrieved emissions are 18.4 Tg yr−1 BC, 109.9 Tg yr−1 OC and 731.6 Tg yr−1 DD, which indicate an increase of 166.7 % for BC and 184.0 % for OC, while a decrease of 42.4 % for DD with respect to GEOS-Chem a priori emission inventories is seen. Global annul mean AOD and AAOD resulting from retrieved emissions are 0.119 and 0.0071 at 550 nm.
Marie Boichu, Olivier Favez, Véronique Riffault, Jean-Eudes Petit, Yunjiang Zhang, Colette Brogniez, Jean Sciare, Isabelle Chiapello, Lieven Clarisse, Shouwen Zhang, Nathalie Pujol-Söhne, Emmanuel Tison, Hervé Delbarre, and Philippe Goloub
Atmos. Chem. Phys., 19, 14253–14287, https://doi.org/10.5194/acp-19-14253-2019, https://doi.org/10.5194/acp-19-14253-2019, 2019
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This study, benefiting especially from recently developed mass spectrometry observations of aerosols, highlights unknown properties of volcanic sulfates in the troposphere. It shows their specific chemical fingerprint, distinct from those of freshly emitted industrial sulfates and background aerosols. We also demonstrate the large-scale persistence of the volcanic sulfate pollution over weeks. Hence, these results cast light on the impact of tropospheric eruptions on air quality and climate.
Catherine Wespes, Daniel Hurtmans, Simon Chabrillat, Gaétane Ronsmans, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Chem. Phys., 19, 14031–14056, https://doi.org/10.5194/acp-19-14031-2019, https://doi.org/10.5194/acp-19-14031-2019, 2019
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This paper highlights the global fingerprint of recent changes in O3 in both the middle–upper and lower stratosphere from the first 10 years of the IASI/Metop-A satellite measurements. The results present the first detection of a significant O3 recovery at middle–high latitudes in winter–spring in the stratosphere as well as in the total column from one single dataset. They also show a speeding up in the recovery at high southern latitudes contrasting with a decline at northern mid-latitudes.
Sajeev Philip, Matthew S. Johnson, Christopher Potter, Vanessa Genovesse, David F. Baker, Katherine D. Haynes, Daven K. Henze, Junjie Liu, and Benjamin Poulter
Atmos. Chem. Phys., 19, 13267–13287, https://doi.org/10.5194/acp-19-13267-2019, https://doi.org/10.5194/acp-19-13267-2019, 2019
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This research was conducted to quantify the impact of different prior global biosphere models on the estimate of terrestrial CO2 fluxes when assimilating Orbiting Carbon Observatory-2 (OCO-2) satellite observations. To determine the prior model impact, we apply observing system simulation experiments (OSSEs). Even with the substantial spatiotemporal coverage of OCO-2 data, residual differences in posterior CO2 flux estimates remain due to the choice of prior flux mean and uncertainties.
Pascal Hedelt, Dmitry S. Efremenko, Diego G. Loyola, Robert Spurr, and Lieven Clarisse
Atmos. Meas. Tech., 12, 5503–5517, https://doi.org/10.5194/amt-12-5503-2019, https://doi.org/10.5194/amt-12-5503-2019, 2019
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Sulfur dioxide (SO2) emitted during volcanic eruptions poses not only a major threat to local populations, air quality, and aviation but also has an impact on the climate. The satellite-based detection of the SO2 plume is easy; however, it requires exact knowledge of the SO2 layer height. This paper presents a new method for the extremely fast and accurate determination of the layer height, which is essential in volcanic plume forecasts and the exact determination of the SO2 density.
Lieven Clarisse, Martin Van Damme, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Meas. Tech., 12, 5457–5473, https://doi.org/10.5194/amt-12-5457-2019, https://doi.org/10.5194/amt-12-5457-2019, 2019
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An imaging technique called superresolution is applied to IASI satellite measurements of atmospheric ammonia (NH3). Taking into account wind fields, this technique reveals NH3 emission sources much better than previously possible. We present a new global NH3 point-source catalog consisting of more than 500 localized and categorized point sources related to agriculture and five different types of industry.
Enrico Dammers, Chris A. McLinden, Debora Griffin, Mark W. Shephard, Shelley Van Der Graaf, Erik Lutsch, Martijn Schaap, Yonatan Gainairu-Matz, Vitali Fioletov, Martin Van Damme, Simon Whitburn, Lieven Clarisse, Karen Cady-Pereira, Cathy Clerbaux, Pierre Francois Coheur, and Jan Willem Erisman
Atmos. Chem. Phys., 19, 12261–12293, https://doi.org/10.5194/acp-19-12261-2019, https://doi.org/10.5194/acp-19-12261-2019, 2019
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Ammonia is an essential molecule in the environment, but at its current levels it is unsustainable. However, the emissions are highly uncertain. We explore the use of satellites to estimate the ammonia lifetime and emissions around point sources to help improve the budget. The same method applied to different satellite instruments shows consistent results. Comparison to the emission inventories shows that those are underestimating emissions of point sources by on average a factor of 2.5.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Sarah Safieddine, Ana Claudia Parracho, Maya George, Filipe Aires, Victor Pellet, Lieven Clarisse, Simon Whitburn, Olivier Lezeaux, Jean-Noel Thepaut, Hans Hersbach, Gabor Radnoti, Frank Goettsche, Maria Martin, Marie Doutriaux Boucher, Dorothee Coppens, Thomas August, and Cathy Clerbaux
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2019-185, https://doi.org/10.5194/amt-2019-185, 2019
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Skin temperature is one of the essential climate variables (ECVs), and is relevant for the current and future understanding of our climate. This work presents a method to retrieve skin temperature from the thermal infrared sounder IASI that provides a global observation of Earth’s surface and atmosphere twice a day. With this method, the first consistent long-term [2007-present] skin temperature record from IASI can be constructed.
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Mathieu Lachatre, Audrey Fortems-Cheiney, Gilles Foret, Guillaume Siour, Gaëlle Dufour, Lieven Clarisse, Cathy Clerbaux, Pierre-François Coheur, Martin Van Damme, and Matthias Beekmann
Atmos. Chem. Phys., 19, 6701–6716, https://doi.org/10.5194/acp-19-6701-2019, https://doi.org/10.5194/acp-19-6701-2019, 2019
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It has been observed from satellite-based instruments that ammonia levels strongly increased between 2011 and 2015. We have used the CHIMERE CTM to understand what could explain such an increase. We first focused on meteorological condition variations, and it has been concluded that meteorology did not explain ammonia evolution. Then, we focused on SO2 and NOx emission evolution rates to evaluate their influences on ammonia. It appears that theses decreases were the main explanation.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
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Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
María Teresa Pay, Gotzon Gangoiti, Marc Guevara, Sergey Napelenok, Xavier Querol, Oriol Jorba, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 19, 5467–5494, https://doi.org/10.5194/acp-19-5467-2019, https://doi.org/10.5194/acp-19-5467-2019, 2019
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The poor diagnostic of the O3 issue over southwestern Europe prevents authorities from implementing effective mitigation plans. This work is a pioneer in identifying that imported O3 is the largest input to the ground-level O3 concentration in the Iberian Peninsula, which is largely explained by vertical mixing. This study also proves that anthropogenic emissions control the severe O3 peaks during stagnant conditions. Ad hoc local actions should complement national/European strategies.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Matthew Russell, Amir Hakami, Paul A. Makar, Ayodeji Akingunola, Junhua Zhang, Michael D. Moran, and Qiong Zheng
Atmos. Chem. Phys., 19, 4393–4417, https://doi.org/10.5194/acp-19-4393-2019, https://doi.org/10.5194/acp-19-4393-2019, 2019
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High-resolution air-quality forecast modeling results are compared for two different grid spacings for the Environment and Climate Change Canada GEM-MACH model. While the higher-resolution simulations have worse formal error scores, we show that the higher-resolution model nevertheless has the ability to better resolve plume maxima and has better performance when the evaluation occurs using new scoring metrics which operate on an equal-representative-area basis.
Quazi Z. Rasool, Jesse O. Bash, and Daniel S. Cohan
Geosci. Model Dev., 12, 849–878, https://doi.org/10.5194/gmd-12-849-2019, https://doi.org/10.5194/gmd-12-849-2019, 2019
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Soils have been overlooked as a source of reactive nitrogen (N) emissions that are pronounced in the summer ozone season (growing season) and increasingly important as fertilizer use grows, while fossil fuel combustion sources of N decline. Mechanistic process models of soil N emissions are used in Earth science and soil biogeochemical modeling on a site scale. This work mechanistically models soil N emissions for the first time on a regional scale to better understand their air quality impacts.
Daniel L. Goldberg, Pablo E. Saide, Lok N. Lamsal, Benjamin de Foy, Zifeng Lu, Jung-Hun Woo, Younha Kim, Jinseok Kim, Meng Gao, Gregory Carmichael, and David G. Streets
Atmos. Chem. Phys., 19, 1801–1818, https://doi.org/10.5194/acp-19-1801-2019, https://doi.org/10.5194/acp-19-1801-2019, 2019
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Using satellite data, we are able to estimate the emissions of NOx (NOx=NO+NO2), a toxic group of air pollutants, in the Seoul metropolitan area. We first develop an enhanced satellite product that better observes NO2 in urban regions. Using this new product, we derive NOx emissions to be twice as large as the emissions reported by the South Korean government. The implication is that the measures taken to reduce NOx emissions in South Korea have not been as effective as regulators have thought.
Negin Sobhani, Sarika Kulkarni, and Gregory R. Carmichael
Atmos. Chem. Phys., 18, 18123–18148, https://doi.org/10.5194/acp-18-18123-2018, https://doi.org/10.5194/acp-18-18123-2018, 2018
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This study presents a detailed analysis of regional and sectoral sources of black carbon (BC), sulfate (SO4), and PM2.5 over the Arctic. We find that anthropogenic emissions from Europe and China are the major contributors (~ 46 % and ~ 25 %) to the Arctic surface BC annually. Emissions from the residential sector within Europe and China are the primary contributors (~ 25 % and ~ 14 %) to Arctic surface BC. Additionally, the contribution of each source region varied significantly by altitude and season.
Kang Sun, Lei Zhu, Karen Cady-Pereira, Christopher Chan Miller, Kelly Chance, Lieven Clarisse, Pierre-François Coheur, Gonzalo González Abad, Guanyu Huang, Xiong Liu, Martin Van Damme, Kai Yang, and Mark Zondlo
Atmos. Meas. Tech., 11, 6679–6701, https://doi.org/10.5194/amt-11-6679-2018, https://doi.org/10.5194/amt-11-6679-2018, 2018
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An agile, physics-based approach is developed to oversample irregular satellite observations to a high-resolution common grid. Instead of assuming each sounding as a point or a polygon as in previous methods, the proposed physical oversampling represents soundings as distributions of sensitivity on the ground. This sensitivity distribution can be determined by the spatial response function of each satellite sensor, parameterized as generalized 2-D super Gaussian functions.
Tianfeng Chai, Ariel Stein, and Fong Ngan
Geosci. Model Dev., 11, 5135–5148, https://doi.org/10.5194/gmd-11-5135-2018, https://doi.org/10.5194/gmd-11-5135-2018, 2018
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While model predictions depend on release parameters, model uncertainties in inverse modeling should also vary with the source terms. In this paper, model uncertainties that will change with the source terms are introduced in a weak-constraint inverse modeling system. Tests using HYSPLIT model and CAPTEX observations show that adding such model uncertainty terms improves release rate estimates. A cost function normalization scheme introduced to avoid spurious solutions proves to be effective.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Maryam Abdi-Oskouei, Gabriele Pfister, Frank Flocke, Negin Sobhani, Pablo Saide, Alan Fried, Dirk Richter, Petter Weibring, James Walega, and Gregory Carmichael
Atmos. Chem. Phys., 18, 16863–16883, https://doi.org/10.5194/acp-18-16863-2018, https://doi.org/10.5194/acp-18-16863-2018, 2018
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This study presents a quantification of model uncertainties due to configurations and errors in the emission inventories. The analysis includes performing simulations with different configurations and comparisons with airborne and ground-based observations with a focus on capturing transport and emissions from the oil and gas sector. The presented results reflect the challenges that one may face when attempting to improve emission inventories by contrasting measured with modeled concentrations.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Elizabeth M. Lennartson, Jun Wang, Juping Gu, Lorena Castro Garcia, Cui Ge, Meng Gao, Myungje Choi, Pablo E. Saide, Gregory R. Carmichael, Jhoon Kim, and Scott J. Janz
Atmos. Chem. Phys., 18, 15125–15144, https://doi.org/10.5194/acp-18-15125-2018, https://doi.org/10.5194/acp-18-15125-2018, 2018
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This paper is among the first to study the diurnal variations of AOD, PM2.5, and their relationships in South Korea. We show that the PM2.5–AOD relationship has strong diurnal variations, and, hence, using AOD data retrieved from geostationary satellite can improve the monitoring of surface PM2.5 air quality on a daily basis as well as constrain the diurnal variation of aerosol emission.
Hansen Cao, Tzung-May Fu, Lin Zhang, Daven K. Henze, Christopher Chan Miller, Christophe Lerot, Gonzalo González Abad, Isabelle De Smedt, Qiang Zhang, Michel van Roozendael, François Hendrick, Kelly Chance, Jie Li, Junyu Zheng, and Yuanhong Zhao
Atmos. Chem. Phys., 18, 15017–15046, https://doi.org/10.5194/acp-18-15017-2018, https://doi.org/10.5194/acp-18-15017-2018, 2018
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Our top-down estimates for annual total Chinese NMVOC emissions was 30.7 to 49.5 Tg y−1, including 16.4 to 23.6 Tg y−1 from anthropogenic sources, 12.2 to 22.8 Tg y−1 from biogenic sources, and 2.08 to 3.13 Tg y−1 from biomass burning. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. The glyoxal and formaldehyde constraints helped distinguish the NMVOC species from different sources.
Yuqiang Zhang, J. Jason West, Rohit Mathur, Jia Xing, Christian Hogrefe, Shawn J. Roselle, Jesse O. Bash, Jonathan E. Pleim, Chuen-Meei Gan, and David C. Wong
Atmos. Chem. Phys., 18, 15003–15016, https://doi.org/10.5194/acp-18-15003-2018, https://doi.org/10.5194/acp-18-15003-2018, 2018
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Here we use a fine-resolution (36 km) self-consistent 21-year air quality simulation from 1990 to 2010, a health impact function, and annual county-level population and baseline mortality rate estimates to estimate annual mortality burdens from PM2.5 and O3 in the US, and also the contributions to the trends. We found that the PM2.5-related mortality burden has steadily decreased by 53 %, while the O3-related mortality burden has increased by 13 %, with larger inter-annual variabilities.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Jan Eiof Jonson, Michael Schulz, Louisa Emmons, Johannes Flemming, Daven Henze, Kengo Sudo, Marianne Tronstad Lund, Meiyun Lin, Anna Benedictow, Brigitte Koffi, Frank Dentener, Terry Keating, Rigel Kivi, and Yanko Davila
Atmos. Chem. Phys., 18, 13655–13672, https://doi.org/10.5194/acp-18-13655-2018, https://doi.org/10.5194/acp-18-13655-2018, 2018
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Focusing on Europe, this HTAP 2 study computes ozone in several global models when reducing anthropogenic emissions by 20 % in different world regions. The differences in model results are explored
by use of a novel stepwise approach combining a tracer, CO and ozone. For ozone the contributions from the rest of the world are larger than from Europe, with the largest contributions from North America and eastern Asia. Contributions do, however, depend on the choice of ozone metric.
Anne Boynard, Daniel Hurtmans, Katerina Garane, Florence Goutail, Juliette Hadji-Lazaro, Maria Elissavet Koukouli, Catherine Wespes, Corinne Vigouroux, Arno Keppens, Jean-Pierre Pommereau, Andrea Pazmino, Dimitris Balis, Diego Loyola, Pieter Valks, Ralf Sussmann, Dan Smale, Pierre-François Coheur, and Cathy Clerbaux
Atmos. Meas. Tech., 11, 5125–5152, https://doi.org/10.5194/amt-11-5125-2018, https://doi.org/10.5194/amt-11-5125-2018, 2018
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In this paper, we perform a comprehensive validation of the IASI/Metop ozone data using independent observations (satellite, ground-based and ozonesonde). The quality of the IASI total and tropospheric ozone columns in terms of bias and long-term stability is generally good. Compared with ozonesonde data, IASI overestimates (underestimates) the ozone abundance in the stratosphere (troposphere). A negative drift in tropospheric ozone is observed, which is not well understood at this point.
Christoph Brühl, Jennifer Schallock, Klaus Klingmüller, Charles Robert, Christine Bingen, Lieven Clarisse, Andreas Heckel, Peter North, and Landon Rieger
Atmos. Chem. Phys., 18, 12845–12857, https://doi.org/10.5194/acp-18-12845-2018, https://doi.org/10.5194/acp-18-12845-2018, 2018
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Use of multi-instrument satellite data is important to get consistent simulations of aerosol radiative forcing by a complex chemistry climate model, here with a main focus on the lower stratosphere. The satellite data at different wavelengths together with the patterns in the simulated size distribution point to a significant contribution from moist mineral dust lifted to the tropopause region by the Asian summer monsoon.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Cheng Chen, Oleg Dubovik, Daven K. Henze, Tatyana Lapyonak, Mian Chin, Fabrice Ducos, Pavel Litvinov, Xin Huang, and Lei Li
Atmos. Chem. Phys., 18, 12551–12580, https://doi.org/10.5194/acp-18-12551-2018, https://doi.org/10.5194/acp-18-12551-2018, 2018
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This paper introduces a method to use satellite-observed spectral AOD and AAOD to derive three types of aerosol emission sources simultaneously based on inverse modelling at a high spatial and temporal resolution. This study shows it is possible to estimate aerosol emissions and improve the atmospheric aerosol simulation using detailed aerosol optical and microphysical information from satellite observations.
Hongyu Guo, Rene Otjes, Patrick Schlag, Astrid Kiendler-Scharr, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, https://doi.org/10.5194/acp-18-12241-2018, 2018
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Reduction in ammonia has been proposed as a way to lower fine particle mass and improve air quality, but gas-phase ammonia is linked to agricultural productivity. We assess the feasibility of ammonia control at a variety of locations through an aerosol thermodynamic analysis. We show that aerosol response to ammonia control is highly nonlinear and only becomes effective when ambient particle pH drops below approximately 3. Particle pH is a relevant aerosol air quality parameter.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Ciao-Kai Liang, J. Jason West, Raquel A. Silva, Huisheng Bian, Mian Chin, Yanko Davila, Frank J. Dentener, Louisa Emmons, Johannes Flemming, Gerd Folberth, Daven Henze, Ulas Im, Jan Eiof Jonson, Terry J. Keating, Tom Kucsera, Allen Lenzen, Meiyun Lin, Marianne Tronstad Lund, Xiaohua Pan, Rokjin J. Park, R. Bradley Pierce, Takashi Sekiya, Kengo Sudo, and Toshihiko Takemura
Atmos. Chem. Phys., 18, 10497–10520, https://doi.org/10.5194/acp-18-10497-2018, https://doi.org/10.5194/acp-18-10497-2018, 2018
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Emissions from one continent affect air quality and health elsewhere. Here we quantify the effects of intercontinental PM2.5 and ozone transport on human health using a new multi-model ensemble, evaluating the health effects of emissions from six world regions and three emission source sectors. Emissions from one region have significant health impacts outside of that source region; similarly, foreign emissions contribute significantly to air-pollution-related deaths in several world regions.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Yuqiang Zhang, Rohit Mathur, Jesse O. Bash, Christian Hogrefe, Jia Xing, and Shawn J. Roselle
Atmos. Chem. Phys., 18, 9091–9106, https://doi.org/10.5194/acp-18-9091-2018, https://doi.org/10.5194/acp-18-9091-2018, 2018
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For this study, we evaluated the WRF–CMAQ coupled model's ability to simulate the long-term trends of wet deposition of nitrogen and sulfur from 1990 to 2010 by comparing the model results with long-term observation datasets in the US. The model generally underestimates the wet deposition of both nitrogen and sulfur but captured well the decreasing trends for the deposition. Then we estimated the deposition budget in the US, including wet deposition and dry deposition from model simulations.
Arno Keppens, Jean-Christopher Lambert, José Granville, Daan Hubert, Tijl Verhoelst, Steven Compernolle, Barry Latter, Brian Kerridge, Richard Siddans, Anne Boynard, Juliette Hadji-Lazaro, Cathy Clerbaux, Catherine Wespes, Daniel R. Hurtmans, Pierre-François Coheur, Jacob C. A. van Peet, Ronald J van der A, Katerina Garane, Maria Elissavet Koukouli, Dimitris S. Balis, Andy Delcloo, Rigel Kivi, Réné Stübi, Sophie Godin-Beekmann, Michel Van Roozendael, and Claus Zehner
Atmos. Meas. Tech., 11, 3769–3800, https://doi.org/10.5194/amt-11-3769-2018, https://doi.org/10.5194/amt-11-3769-2018, 2018
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This work, performed at the Royal Belgian Institute for Space Aeronomy and the second in a series of four Ozone_cci papers, reports for the first time on data content studies, information content studies, and comparisons with co-located ground-based reference observations for all 13 nadir ozone profile data products that are part of the Climate Research Data Package (CRDP) on atmospheric ozone of the European Space Agency's Climate Change Initiative.
Stefano Galmarini, Ioannis Kioutsioukis, Efisio Solazzo, Ummugulsum Alyuz, Alessandra Balzarini, Roberto Bellasio, Anna M. K. Benedictow, Roberto Bianconi, Johannes Bieser, Joergen Brandt, Jesper H. Christensen, Augustin Colette, Gabriele Curci, Yanko Davila, Xinyi Dong, Johannes Flemming, Xavier Francis, Andrea Fraser, Joshua Fu, Daven K. Henze, Christian Hogrefe, Ulas Im, Marta Garcia Vivanco, Pedro Jiménez-Guerrero, Jan Eiof Jonson, Nutthida Kitwiroon, Astrid Manders, Rohit Mathur, Laura Palacios-Peña, Guido Pirovano, Luca Pozzoli, Marie Prank, Martin Schultz, Rajeet S. Sokhi, Kengo Sudo, Paolo Tuccella, Toshihiko Takemura, Takashi Sekiya, and Alper Unal
Atmos. Chem. Phys., 18, 8727–8744, https://doi.org/10.5194/acp-18-8727-2018, https://doi.org/10.5194/acp-18-8727-2018, 2018
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An ensemble of model results relating to ozone concentrations in Europe in 2010 has been produced and studied. The novelty consists in the fact that the ensemble is made of results of models working at two different scales (regional and global), therefore contributing in detail two different parts of the atmospheric spectrum. The ensemble defined as a hybrid has been studied in detail and shown to bring additional value to the assessment of air quality.
Catherine Wespes, Daniel Hurtmans, Cathy Clerbaux, Anne Boynard, and Pierre-François Coheur
Atmos. Chem. Phys., 18, 6867–6885, https://doi.org/10.5194/acp-18-6867-2018, https://doi.org/10.5194/acp-18-6867-2018, 2018
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Jennifer Kaiser, Daniel J. Jacob, Lei Zhu, Katherine R. Travis, Jenny A. Fisher, Gonzalo González Abad, Lin Zhang, Xuesong Zhang, Alan Fried, John D. Crounse, Jason M. St. Clair, and Armin Wisthaler
Atmos. Chem. Phys., 18, 5483–5497, https://doi.org/10.5194/acp-18-5483-2018, https://doi.org/10.5194/acp-18-5483-2018, 2018
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Isoprene emissions from vegetation have a large effect on atmospheric chemistry and air quality. Here we use the adjoint of GEOS-Chem in an inversion of OMI formaldehyde observations to produce top-down estimates of isoprene emissions in the southeast US during the summer of 2013. We find that MEGAN v2.1 is biased high on average by 40 %. Our downward correction of isoprene emissions leads to a small reduction in modeled surface O3 and decreases the contribution of isoprene to organic aerosol.
Gaétane Ronsmans, Catherine Wespes, Daniel Hurtmans, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Chem. Phys., 18, 4403–4423, https://doi.org/10.5194/acp-18-4403-2018, https://doi.org/10.5194/acp-18-4403-2018, 2018
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The paper aims at understanding the variability of nitric acid (HNO3) in the stratosphere; 9-year time series of IASI measurements are analysed and, for the first time for HNO3, fitted with regression models in order to identify the factors at play. It was found that the annual variability is the main driver and that the polar stratospheric clouds influence greatly HNO3 variability at polar latitudes. The results show the potential of such analyses to better understand the polar processes.
Kira Sadighi, Evan Coffey, Andrea Polidori, Brandon Feenstra, Qin Lv, Daven K. Henze, and Michael Hannigan
Atmos. Meas. Tech., 11, 1777–1792, https://doi.org/10.5194/amt-11-1777-2018, https://doi.org/10.5194/amt-11-1777-2018, 2018
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Ground-level ozone has negative human health impacts. In the summer of 2015, 13 low-cost sensor monitors were deployed to several neighborhoods around Riverside, California. There were significant spatial differences between monitors. This is important because it means that ozone in certain places may be higher than what EPA monitors report for an area, which is pertinent for residents of those communities. This research helps inform the limitations and advantages of low-cost sensor networks.
Thibaut Lurton, Fabrice Jégou, Gwenaël Berthet, Jean-Baptiste Renard, Lieven Clarisse, Anja Schmidt, Colette Brogniez, and Tjarda J. Roberts
Atmos. Chem. Phys., 18, 3223–3247, https://doi.org/10.5194/acp-18-3223-2018, https://doi.org/10.5194/acp-18-3223-2018, 2018
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We quantify the chemical and microphysical effects of volcanic SO2 and HCl from the June 2009 Sarychev Peak eruption using a comprehensive aerosol–chemistry model combined with in situ measurements and satellite retrievals. Our results suggest that previous studies underestimated the eruption's atmospheric and climatic impact, mainly because previous model-to-satellite comparisons had to make assumptions about the aerosol size distribution and were based on biased satellite retrievals of AOD.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Havala O. T. Pye, Andreas Zuend, Juliane L. Fry, Gabriel Isaacman-VanWertz, Shannon L. Capps, K. Wyat Appel, Hosein Foroutan, Lu Xu, Nga L. Ng, and Allen H. Goldstein
Atmos. Chem. Phys., 18, 357–370, https://doi.org/10.5194/acp-18-357-2018, https://doi.org/10.5194/acp-18-357-2018, 2018
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Thermodynamic modeling revealed that some but not all measurements of ammonium-to-sulfate ratios are consistent with theory. The measurement diversity likely explains the previously reported range of results regarding the suitability of thermodynamic modeling. Despite particles being predominantly phase separated, organic–inorganic interactions resulted in increased aerosol pH and partitioning towards the particle phase for highly oxygenated organic compounds compared to traditional methods.
Lin Zhang, Youfan Chen, Yuanhong Zhao, Daven K. Henze, Liye Zhu, Yu Song, Fabien Paulot, Xuejun Liu, Yuepeng Pan, Yi Lin, and Binxiang Huang
Atmos. Chem. Phys., 18, 339–355, https://doi.org/10.5194/acp-18-339-2018, https://doi.org/10.5194/acp-18-339-2018, 2018
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Substantial differences exist in current estimates of agricultural ammonia emissions in China, hindering understanding of their environmental consequences. This study applies both bottom-up and top-down methods to better quantify agricultural ammonia sources in China using observations from satellite and surface networks interpreted by a chemical transport model. Our estimate of annual Chinese anthropogenic ammonia emission is 11.7 tg (teragram) for 2008 with a strong seasonality peak in summer.
Youhua Tang, Mariusz Pagowski, Tianfeng Chai, Li Pan, Pius Lee, Barry Baker, Rajesh Kumar, Luca Delle Monache, Daniel Tong, and Hyun-Cheol Kim
Geosci. Model Dev., 10, 4743–4758, https://doi.org/10.5194/gmd-10-4743-2017, https://doi.org/10.5194/gmd-10-4743-2017, 2017
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In order to evaluate the data assimilation tools for regional real-time PM2.5 forecasts, we applied a 3D-Var assimilation tool to adjust the aerosol initial condition by assimilating satellite-retrieved aerosol optical depth and surface PM2.5 observations for a regional air quality model, which is compared to another assimilation method, optimal interpolation. We discuss the pros and cons of these two assimilation methods based on the comparison of their 1-month four-cycles-per-day runs.
Nelson Bègue, Damien Vignelles, Gwenaël Berthet, Thierry Portafaix, Guillaume Payen, Fabrice Jégou, Hassan Benchérif, Julien Jumelet, Jean-Paul Vernier, Thibaut Lurton, Jean-Baptiste Renard, Lieven Clarisse, Vincent Duverger, Françoise Posny, Jean-Marc Metzger, and Sophie Godin-Beekmann
Atmos. Chem. Phys., 17, 15019–15036, https://doi.org/10.5194/acp-17-15019-2017, https://doi.org/10.5194/acp-17-15019-2017, 2017
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The space–time evolutions of the Calbuco plume are investigated by combining satellite, in situ aerosol counting and lidar observations, and a numerical model. All the data at Reunion Island reveal a twofold increase in the amount of aerosol with respect to the values observed before the eruption. The dynamic context has favored the spread of the plume exclusively in the Southern Hemisphere. This study highlights the role played by dynamical barriers in the transport of atmospheric species.
Martin Van Damme, Simon Whitburn, Lieven Clarisse, Cathy Clerbaux, Daniel Hurtmans, and Pierre-François Coheur
Atmos. Meas. Tech., 10, 4905–4914, https://doi.org/10.5194/amt-10-4905-2017, https://doi.org/10.5194/amt-10-4905-2017, 2017
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This paper presents an improved version (v2.1) of the neural-network-based algorithm for retrieving atmospheric ammonia (NH3) columns from IASI satellite observations. Two datasets using different input data for the retrieval are described: one is based on the operationally provided EUMETSAT Level 2 (ANNI-NH3-v2.1), and the other uses the ECMWF ERA-Interim data (ANNI-NH3-v2.1R-I). Analyses illustrate well that the (meteorological) input data can have a large impact on the retrieved NH3 columns.
Simon Whitburn, Martin Van Damme, Lieven Clarisse, Daniel Hurtmans, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Chem. Phys., 17, 12239–12252, https://doi.org/10.5194/acp-17-12239-2017, https://doi.org/10.5194/acp-17-12239-2017, 2017
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Vegetation fires are a major source of NH3 in the atmosphere. A key parameter for the calculation of their emissions, which are still uncertain, is the NH3 enhancement ratio relative to carbon monoxide (CO), ERNH3 / CO. Here we derive new ERNH3 / CO ratios for large tropical regions from the measurements of IASI. We find important variability between and within the studied biomes, as well as interannual variability. This highlights the need for the development of dynamic ERNH3 / CO ratios.
Jun-Wei Xu, Randall V. Martin, Andrew Morrow, Sangeeta Sharma, Lin Huang, W. Richard Leaitch, Julia Burkart, Hannes Schulz, Marco Zanatta, Megan D. Willis, Daven K. Henze, Colin J. Lee, Andreas B. Herber, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 11971–11989, https://doi.org/10.5194/acp-17-11971-2017, https://doi.org/10.5194/acp-17-11971-2017, 2017
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We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem model and its adjoint to attribute the sources of Arctic BC. Anthropogenic emissions in eastern and southern Asia make the largest contribution to Arctic BC. Gas flaring emissions from oilfields in western Siberia and from the Tarim oilfield in western China could have striking impacts on Arctic BC loadings.
Matthieu Pommier, Cathy Clerbaux, and Pierre-Francois Coheur
Atmos. Chem. Phys., 17, 11089–11105, https://doi.org/10.5194/acp-17-11089-2017, https://doi.org/10.5194/acp-17-11089-2017, 2017
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A new estimation of enhancement ratios relative to CO for HCOOH over seven biomass burning regions is proposed. Fire-affected HCOOH and CO total columns are defined by combining the total columns from IASI, geographic location of the fires from the Moderate Resolution Imaging Spectroradiometer (MODIS), and surface wind speed field from the European Centre for Medium-Range Weather Forecasts (ECMWF). An additional classification of the enhancement ratios by type of fuel burned is also provided.
Valentin Duflot, Jean-Luc Baray, Guillaume Payen, Nicolas Marquestaut, Francoise Posny, Jean-Marc Metzger, Bavo Langerock, Corinne Vigouroux, Juliette Hadji-Lazaro, Thierry Portafaix, Martine De Mazière, Pierre-Francois Coheur, Cathy Clerbaux, and Jean-Pierre Cammas
Atmos. Meas. Tech., 10, 3359–3373, https://doi.org/10.5194/amt-10-3359-2017, https://doi.org/10.5194/amt-10-3359-2017, 2017
Min Huang, Gregory R. Carmichael, James H. Crawford, Armin Wisthaler, Xiwu Zhan, Christopher R. Hain, Pius Lee, and Alex B. Guenther
Geosci. Model Dev., 10, 3085–3104, https://doi.org/10.5194/gmd-10-3085-2017, https://doi.org/10.5194/gmd-10-3085-2017, 2017
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Various sensitivity simulations during two airborne campaigns were performed to assess the impact of different initialization methods and model resolutions on NUWRF-modeled weather states, heat fluxes, and the follow-on MEGAN isoprene emission calculations. Proper land initialization is shown to be important to the coupled weather modeling and the follow-on emission modeling, which is also critical to accurately representing other processes in air quality modeling and data assimilation.
Ling Qi, Qinbin Li, Daven K. Henze, Hsien-Liang Tseng, and Cenlin He
Atmos. Chem. Phys., 17, 9697–9716, https://doi.org/10.5194/acp-17-9697-2017, https://doi.org/10.5194/acp-17-9697-2017, 2017
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We find that Asian anthropogenic sources are the largest contributors (~ 40 %) to surface BC in spring in the Arctic, inconsistent with previous studies which repeatedly identified sources of surface BC as anthropogenic emissions from Europe and Russia. It takes 12–17 days for Asian anthropogenic emissions to be transported to the Arctic surface. Additionally, a large fraction (40–65 %) of Asian contribution is in the form of chronic pollution on 1- to 2-month timescales.
Jean-Lionel Lacour, Cyrille Flamant, Camille Risi, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Chem. Phys., 17, 9645–9663, https://doi.org/10.5194/acp-17-9645-2017, https://doi.org/10.5194/acp-17-9645-2017, 2017
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We present temporal and spatial δD distributions derived from IASI obtained above the North Atlantic in the vicinity of West Africa. We show that the seasonality of δD in the North Atlantic is closely associated with the influence of the Saharan heat low (SHL). We provide an interpretation of the temporal and spatial variations in δD and show that the interactions between the large-scale subsidence, the ITCZ, and the SHL can be disentangled thanks to the added information contained in δD.
Enrico Dammers, Mark W. Shephard, Mathias Palm, Karen Cady-Pereira, Shannon Capps, Erik Lutsch, Kim Strong, James W. Hannigan, Ivan Ortega, Geoffrey C. Toon, Wolfgang Stremme, Michel Grutter, Nicholas Jones, Dan Smale, Jacob Siemons, Kevin Hrpcek, Denis Tremblay, Martijn Schaap, Justus Notholt, and Jan Willem Erisman
Atmos. Meas. Tech., 10, 2645–2667, https://doi.org/10.5194/amt-10-2645-2017, https://doi.org/10.5194/amt-10-2645-2017, 2017
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Presented here is the validation of the CrIS fast physical retrieval (CFPR) NH3 column and profile measurements using ground-based Fourier transform infrared (FTIR) observations. The overall FTIR and CrIS total columns have a positive correlation of r = 0.77 (N = 218) with very little bias (a slope of 1.02). Furthermore, we find that CrIS and FTIR profile comparison differences are mostly within the range of the estimated retrieval uncertainties, with differences in the range of ~ 20 to 40 %.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363, https://doi.org/10.5194/gmd-10-2333-2017, https://doi.org/10.5194/gmd-10-2333-2017, 2017
Jonathan J. Guerrette and Daven K. Henze
Atmos. Chem. Phys., 17, 7605–7633, https://doi.org/10.5194/acp-17-7605-2017, https://doi.org/10.5194/acp-17-7605-2017, 2017
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This work describes the implementation and application of a new advanced tool, WRFDA-Chem, for top-down constraints of regional atmospheric chemical emissions. Aircraft and surface observations of black carbon are traced to anthropogenic and biomass burning sources in California during ARCTAS-CARB. The information content of the observations is quantified through variance reduction and degrees of freedom of signal, which can be used to assess observing strategies and emission inventories.
Zhe Jiang, Helen Worden, John R. Worden, Daven K. Henze, Dylan B. A. Jones, Avelino F. Arellano, Emily V. Fischer, Liye Zhu, Kazuyuki Miyazaki, K. Folkert Boersma, and Vivienne H. Payne
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-382, https://doi.org/10.5194/acp-2017-382, 2017
Preprint withdrawn
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We investigated the variation of US tropospheric NO2 in the past decade. We demonstrated significant divergence between the time variation in tropospheric NO2 columns from OMI retrievals and surface measurements. Our analysis suggests limited contributions from local effects such as fossil fuel emissions, lightning, or instrument artifacts, and indicates possible important contributions from long-range transport of Asian emissions that are modulated by ENSO.
Yi Li, Tammy M. Thompson, Martin Van Damme, Xi Chen, Katherine B. Benedict, Yixing Shao, Derek Day, Alexandra Boris, Amy P. Sullivan, Jay Ham, Simon Whitburn, Lieven Clarisse, Pierre-François Coheur, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 17, 6197–6213, https://doi.org/10.5194/acp-17-6197-2017, https://doi.org/10.5194/acp-17-6197-2017, 2017
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-96, https://doi.org/10.5194/gmd-2017-96, 2017
Revised manuscript not accepted
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Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Min Huang, Gregory R. Carmichael, R. Bradley Pierce, Duseong S. Jo, Rokjin J. Park, Johannes Flemming, Louisa K. Emmons, Kevin W. Bowman, Daven K. Henze, Yanko Davila, Kengo Sudo, Jan Eiof Jonson, Marianne Tronstad Lund, Greet Janssens-Maenhout, Frank J. Dentener, Terry J. Keating, Hilke Oetjen, and Vivienne H. Payne
Atmos. Chem. Phys., 17, 5721–5750, https://doi.org/10.5194/acp-17-5721-2017, https://doi.org/10.5194/acp-17-5721-2017, 2017
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In support of the HTAP phase 2 experiment, we conducted a number of regional-scale Sulfur Transport and dEposition Model base and sensitivity simulations over North America during May–June 2010. The STEM chemical boundary conditions were downscaled from three (GEOS-Chem, RAQMS, and ECMWF C-IFS) global chemical transport models' simulations. Analyses were performed on large spatial–temporal scales relative to HTAP1 and also on subcontinental and event scales including the use of satellite data.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
K. Wyat Appel, Sergey L. Napelenok, Kristen M. Foley, Havala O. T. Pye, Christian Hogrefe, Deborah J. Luecken, Jesse O. Bash, Shawn J. Roselle, Jonathan E. Pleim, Hosein Foroutan, William T. Hutzell, George A. Pouliot, Golam Sarwar, Kathleen M. Fahey, Brett Gantt, Robert C. Gilliam, Nicholas K. Heath, Daiwen Kang, Rohit Mathur, Donna B. Schwede, Tanya L. Spero, David C. Wong, and Jeffrey O. Young
Geosci. Model Dev., 10, 1703–1732, https://doi.org/10.5194/gmd-10-1703-2017, https://doi.org/10.5194/gmd-10-1703-2017, 2017
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The Community Multiscale Air Quality (CMAQ) model is a comprehensive multipollutant air quality modeling system. The CMAQ model is used extensively throughout the world to simulate air pollutants for many purposes, including regulatory and air quality forecasting applications. This work describes the scientific updates made to the latest version of the CMAQ modeling system (CMAQv5.1) and presents an evaluation of the new model against observations and results from the previous model version.
Kathleen M. Fahey, Annmarie G. Carlton, Havala O. T. Pye, Jaemeen Baek, William T. Hutzell, Charles O. Stanier, Kirk R. Baker, K. Wyat Appel, Mohammed Jaoui, and John H. Offenberg
Geosci. Model Dev., 10, 1587–1605, https://doi.org/10.5194/gmd-10-1587-2017, https://doi.org/10.5194/gmd-10-1587-2017, 2017
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Chemical transport models (CTMs) are a crucial tool in understanding links between emissions, air quality, and climate. Only a simple description of cloud chemistry has been implemented in many of these; however, clouds play a major role in the physicochemical processing of atmospheric species. In CMAQ, EPA’s widely used CTM, the cloud code is limited to the treatment of simple chemistry. We update CMAQ clouds to consider additional chemistry and then examine regional impacts of these updates.
Zhe Jiang, John R. Worden, Helen Worden, Merritt Deeter, Dylan B. A. Jones, Avelino F. Arellano, and Daven K. Henze
Atmos. Chem. Phys., 17, 4565–4583, https://doi.org/10.5194/acp-17-4565-2017, https://doi.org/10.5194/acp-17-4565-2017, 2017
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We constrain the long-term variation in global CO emissions for 2001–2015. Our results confirm that the decreasing trend of tropospheric CO in the Northern Hemisphere is due to decreasing CO emissions from anthropogenic and biomass burning sources. In particular, we find decreasing CO emissions from the United States and China in the past 15 years, unchanged anthropogenic CO emissions from Europe since 2008, and likely a positive trend from India and southeast Asia.
Tianfeng Chai, Alice Crawford, Barbara Stunder, Michael J. Pavolonis, Roland Draxler, and Ariel Stein
Atmos. Chem. Phys., 17, 2865–2879, https://doi.org/10.5194/acp-17-2865-2017, https://doi.org/10.5194/acp-17-2865-2017, 2017
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An inverse system based on the HYSPLIT dispersion model has been built to estimate volcanic ash source strengths, vertical distribution, and temporal variations. Using MODIS retrievals from the 2008 Kasatochi volcanic ash clouds, three options for matching model results to satellite mass loadings are tested. They all show decent skill. It is also found that simultaneously assimilating observations at different times produces better hindcasts than only assimilating the most recent observations.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543, https://doi.org/10.5194/bg-13-6519-2016, https://doi.org/10.5194/bg-13-6519-2016, 2016
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The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
Amelia F. Longo, David J. Vine, Laura E. King, Michelle Oakes, Rodney J. Weber, Lewis Gregory Huey, Armistead G. Russell, and Ellery D. Ingall
Atmos. Chem. Phys., 16, 13389–13398, https://doi.org/10.5194/acp-16-13389-2016, https://doi.org/10.5194/acp-16-13389-2016, 2016
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New synchrotron-based techniques were applied to characterize the oxidation state and composition of sulfur in ambient aerosol and emission sources. Individual particles were found to contain surprisingly high levels of elemental sulfur, a form of sulfur found in only one of the emission sources analyzed. We also show metal sulfates as a key component of urban aerosols. These metal sulfate phases are highly soluble and are indicative of acidic processes transforming metals in the environment.
Zeli Tan, Qianlai Zhuang, Daven K. Henze, Christian Frankenberg, Ed Dlugokencky, Colm Sweeney, Alexander J. Turner, Motoki Sasakawa, and Toshinobu Machida
Atmos. Chem. Phys., 16, 12649–12666, https://doi.org/10.5194/acp-16-12649-2016, https://doi.org/10.5194/acp-16-12649-2016, 2016
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Methane emissions from the pan-Arctic could be important in understanding the global carbon cycle but are still poorly constrained to date. This study demonstrated that satellite retrievals can be used to reduce the uncertainty of the estimates of these emissions. We also provided additional evidence for the existence of large methane emissions from pan-Arctic lakes in the Siberian yedoma permafrost region. We found that biogeochemical models should be improved for better estimates.
Luke D. Schiferl, Colette L. Heald, Martin Van Damme, Lieven Clarisse, Cathy Clerbaux, Pierre-François Coheur, John B. Nowak, J. Andrew Neuman, Scott C. Herndon, Joseph R. Roscioli, and Scott J. Eilerman
Atmos. Chem. Phys., 16, 12305–12328, https://doi.org/10.5194/acp-16-12305-2016, https://doi.org/10.5194/acp-16-12305-2016, 2016
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This study combines new observations and a simulation to assess the interannual variability of atmospheric ammonia concentrations over the United States. The model generally underrepresents the observed variability. Nearly two-thirds of the simulated variability is caused by meteorology, twice that caused by regulations on fossil fuel combustion emissions. Adding ammonia emissions variability does not substantially improve the simulation and has little impact on summer particle concentrations.
Gaétane Ronsmans, Bavo Langerock, Catherine Wespes, James W. Hannigan, Frank Hase, Tobias Kerzenmacher, Emmanuel Mahieu, Matthias Schneider, Dan Smale, Daniel Hurtmans, Martine De Mazière, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Meas. Tech., 9, 4783–4801, https://doi.org/10.5194/amt-9-4783-2016, https://doi.org/10.5194/amt-9-4783-2016, 2016
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HNO3 concentrations are obtained from the IASI instrument and the data set is characterized for the first time in terms of vertical profiles, averaging kernels and error profiles. A validation is also conducted through a comparison with ground-based FTIR measurements, with good results. The data set is then used to analyse HNO3 spatial and temporal variability for the year 2011. The latitudinal gradient and the large seasonal variability in polar regions are well represented with IASI data.
Quazi Z. Rasool, Rui Zhang, Benjamin Lash, Daniel S. Cohan, Ellen J. Cooter, Jesse O. Bash, and Lok N. Lamsal
Geosci. Model Dev., 9, 3177–3197, https://doi.org/10.5194/gmd-9-3177-2016, https://doi.org/10.5194/gmd-9-3177-2016, 2016
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This study updates the representation of soil NO emissions in a regional air quality model. The implementation enhances the representation of biome types and dynamic fertilizer use. Previous modeling of soil NO in CMAQ had tended to under-estimate emissions and misrepresent their response to soil conditions and meteorology. We evaluate results against satellite observations of NO2, and quantify the impacts of the new parameterization on simulations of ozone and particulate matter.
Anne Boynard, Daniel Hurtmans, Mariliza E. Koukouli, Florence Goutail, Jérôme Bureau, Sarah Safieddine, Christophe Lerot, Juliette Hadji-Lazaro, Catherine Wespes, Jean-Pierre Pommereau, Andrea Pazmino, Irene Zyrichidou, Dimitris Balis, Alain Barbe, Semen N. Mikhailenko, Diego Loyola, Pieter Valks, Michel Van Roozendael, Pierre-François Coheur, and Cathy Clerbaux
Atmos. Meas. Tech., 9, 4327–4353, https://doi.org/10.5194/amt-9-4327-2016, https://doi.org/10.5194/amt-9-4327-2016, 2016
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Seven years of O3 observations retrieved from IASI/MetOp satellite instruments are validated with independent data (UV satellite and ground-based data along with ozonesonde profiles). Overall IASI overestimates the total ozone columns (TOC) by 2–7 % depending on the latitude. The assessment of an updated version of the IASI O3 retrieval sofware shows a correction of ~ 4 % in the IASI TOC product, bringing the overall global bias with UV ground-based and satellite data to ~ 1–2 % on average.
Marie Boichu, Isabelle Chiapello, Colette Brogniez, Jean-Christophe Péré, Francois Thieuleux, Benjamin Torres, Luc Blarel, Augustin Mortier, Thierry Podvin, Philippe Goloub, Nathalie Söhne, Lieven Clarisse, Sophie Bauduin, François Hendrick, Nicolas Theys, Michel Van Roozendael, and Didier Tanré
Atmos. Chem. Phys., 16, 10831–10845, https://doi.org/10.5194/acp-16-10831-2016, https://doi.org/10.5194/acp-16-10831-2016, 2016
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Bárðarbunga eruption emitted huge amounts of sulfur into the lower troposphere causing an unprecedented air pollution in the modern era. A wealth of remote sensing and in situ data allows us to jointly analyse the dynamics of volcanic SO2 and sulfate aerosols. Based on this panel of observations, success and challenges in simulating such volcanogenic long-range pollution events are exposed, focusing on the boundary layer dynamics.
Sarah Safieddine, Anne Boynard, Nan Hao, Fuxiang Huang, Lili Wang, Dongsheng Ji, Brice Barret, Sachin D. Ghude, Pierre-François Coheur, Daniel Hurtmans, and Cathy Clerbaux
Atmos. Chem. Phys., 16, 10489–10500, https://doi.org/10.5194/acp-16-10489-2016, https://doi.org/10.5194/acp-16-10489-2016, 2016
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The Asian Summer Monsoon has implication on the weather and climate system as well as pollutants concentration over the monsoon regions leading to effects on the global air quality. Our results, combining satellite, aircraft and ground station data, show that tropospheric ozone, decrease during the period May–August over East and South Asia due to the Monsoon. The magnitude of this drop depends largely on meteorology and geographic location.
Enrico Dammers, Mathias Palm, Martin Van Damme, Corinne Vigouroux, Dan Smale, Stephanie Conway, Geoffrey C. Toon, Nicholas Jones, Eric Nussbaumer, Thorsten Warneke, Christof Petri, Lieven Clarisse, Cathy Clerbaux, Christian Hermans, Erik Lutsch, Kim Strong, James W. Hannigan, Hideaki Nakajima, Isamu Morino, Beatriz Herrera, Wolfgang Stremme, Michel Grutter, Martijn Schaap, Roy J. Wichink Kruit, Justus Notholt, Pierre-F. Coheur, and Jan Willem Erisman
Atmos. Chem. Phys., 16, 10351–10368, https://doi.org/10.5194/acp-16-10351-2016, https://doi.org/10.5194/acp-16-10351-2016, 2016
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Atmospheric ammonia (NH3) measured by the IASI satellite instrument is compared to observations from ground-based FTIR instruments. The seasonal cycles of NH3 in both datasets are consistent for most sites. Correlations are found to be high at sites with considerable NH3 levels, whereas correlations are lower at sites with low NH3 levels close to the detection limit of the IASI instrument. The study's results further indicate that the IASI-NH3 product performs better than earlier estimates.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Matthieu Pommier, Cathy Clerbaux, Pierre-François Coheur, Emmanuel Mahieu, Jean-François Müller, Clare Paton-Walsh, Trissevgeni Stavrakou, and Corinne Vigouroux
Atmos. Chem. Phys., 16, 8963–8981, https://doi.org/10.5194/acp-16-8963-2016, https://doi.org/10.5194/acp-16-8963-2016, 2016
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This work presents for the first time 7 years of formic acid (HCOOH) measurements recorded by the satellite instrument, IASI. The comparison of the data set with ground-based FTIR measurements and a CTM shows the interannual and the seasonal variation are well captured. Global distributions are provided, highlighting the long-range transport of tropospheric HCOOH over the oceans and the detection of source regions e.g. over India, USA, and Africa.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Jesse O. Bash, Kirk R. Baker, and Melinda R. Beaver
Geosci. Model Dev., 9, 2191–2207, https://doi.org/10.5194/gmd-9-2191-2016, https://doi.org/10.5194/gmd-9-2191-2016, 2016
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Biogenic volatile organic compounds (BVOCs) participate in reactions that can lead to secondarily formed ozone and particulate matter impacting air quality and climate and are important inputs for atmospheric models. BVOC emissions are sensitive to the vegetation species and leaf temperature. Here, we have improved the vegetation data and modeled leaf temperature of the Biogenic Emission Inventory System model. Updated algorithms improved model evaluation against observations in California.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Zhe Jiang, Kazuyuki Miyazaki, John R. Worden, Jane J. Liu, Dylan B. A. Jones, and Daven K. Henze
Atmos. Chem. Phys., 16, 6537–6546, https://doi.org/10.5194/acp-16-6537-2016, https://doi.org/10.5194/acp-16-6537-2016, 2016
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We quantify the impacts of anthropogenic and natural sources on free tropospheric ozone over the Middle East, using the adjoint of the GEOS-Chem model with updated NOx emissions estimates from an ensemble Kalman filter. We show that the global total contribution of lightning NOx on free tropospheric O3 over the Middle East is about 2 times larger than that from global anthropogenic sources. The summertime free tropospheric O3 enhancement is primarily due to Asian NOx emissions.
Nicolas Bousserez, Daven K. Henze, Brigitte Rooney, Andre Perkins, Kevin J. Wecht, Alexander J. Turner, Vijay Natraj, and John R. Worden
Atmos. Chem. Phys., 16, 6175–6190, https://doi.org/10.5194/acp-16-6175-2016, https://doi.org/10.5194/acp-16-6175-2016, 2016
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This work provides new insight into the observational constraints provided by current low-Earth orbit (LEO) and future potential geostationary (GEO) satellite missions on methane emissions in North America. Using efficient numerical tools, the information content (error reductions, spatial resolution of the constraints) of methane inversions using different instrument configurations (TIR, SWIR and multi-spectral) was estimated at model grid-scale resolution (0.5° × 0.7°).
Catherine Wespes, Daniel Hurtmans, Louisa K. Emmons, Sarah Safieddine, Cathy Clerbaux, David P. Edwards, and Pierre-François Coheur
Atmos. Chem. Phys., 16, 5721–5743, https://doi.org/10.5194/acp-16-5721-2016, https://doi.org/10.5194/acp-16-5721-2016, 2016
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In this paper, we assess how daily ozone measurements from the Infrared Atmospheric Sounding Interferometer (IASI/MetOp) can contribute to the analyses of the processes driving O3 variability in the troposphere and the stratosphere with a set of parameterized geophysical variables, and we demonstrate the added value of IASI exceptional frequency sampling for monitoring medium- to long-term changes in global ozone concentrations in the future.
Dimitris Balis, Maria-Elissavet Koukouli, Nikolaos Siomos, Spyridon Dimopoulos, Lucia Mona, Gelsomina Pappalardo, Franco Marenco, Lieven Clarisse, Lucy J. Ventress, Elisa Carboni, Roy G. Grainger, Ping Wang, Gijsbert Tilstra, Ronald van der A, Nicolas Theys, and Claus Zehner
Atmos. Chem. Phys., 16, 5705–5720, https://doi.org/10.5194/acp-16-5705-2016, https://doi.org/10.5194/acp-16-5705-2016, 2016
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The ESA-funded SACS-2 and SMASH projects developed and improved dedicated satellite-derived ash plume and sulfur dioxide level assessments. These estimates were validated using ground-based and aircraft lidar measurements. The validation results are promising for most satellite products and are within the estimated uncertainties of each of the comparative data sets. The IASI data show a better consistency concerning the ash optical depth and ash layer height.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Ting Fang, Vishal Verma, Josephine T. Bates, Joseph Abrams, Mitchel Klein, Matthew J. Strickland, Stefanie E. Sarnat, Howard H. Chang, James A. Mulholland, Paige E. Tolbert, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 16, 3865–3879, https://doi.org/10.5194/acp-16-3865-2016, https://doi.org/10.5194/acp-16-3865-2016, 2016
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Ascorbic acid (AA) and Dithiothreitol (DTT) assay measures of water-soluble PM2.5 oxidative potential (OP) are compared in terms of spatiotemporal trends, chemical selectivity, sources, and health impacts based on an epidemiological study with backcast estimated OP. Both assays point to metals from brake/tire wear, but only the DTT assay also identifies organics from combustion. DTT is associated with emergency department visits for asthma/wheeze and congestive heart failure, whereas AA is not.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462, https://doi.org/10.5194/acp-16-3449-2016, https://doi.org/10.5194/acp-16-3449-2016, 2016
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Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
S. E. Pusede, K. C. Duffey, A. A. Shusterman, A. Saleh, J. L. Laughner, P. J. Wooldridge, Q. Zhang, C. L. Parworth, H. Kim, S. L. Capps, L. C. Valin, C. D. Cappa, A. Fried, J. Walega, J. B. Nowak, A. J. Weinheimer, R. M. Hoff, T. A. Berkoff, A. J. Beyersdorf, J. Olson, J. H. Crawford, and R. C. Cohen
Atmos. Chem. Phys., 16, 2575–2596, https://doi.org/10.5194/acp-16-2575-2016, https://doi.org/10.5194/acp-16-2575-2016, 2016
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
Sophie Bauduin, Lieven Clarisse, Juliette Hadji-Lazaro, Nicolas Theys, Cathy Clerbaux, and Pierre-François Coheur
Atmos. Meas. Tech., 9, 721–740, https://doi.org/10.5194/amt-9-721-2016, https://doi.org/10.5194/amt-9-721-2016, 2016
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The paper presents the development of a new retrieval scheme to infer near-surface sulfur dioxide (SO2) concentrations at a global scale from the Infrared Atmospheric Sounding Interferometer (IASI). It demonstrates the capability of such an instrument to globally monitor anthropogenic SO2 pollution in the case of favourable geophysical conditions, especially high thermal contrast and low humidity.
Karoline K. Johnson, Michael H. Bergin, Armistead G. Russell, and Gayle S. W. Hagler
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2015-331, https://doi.org/10.5194/amt-2015-331, 2016
Revised manuscript not accepted
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Low-cost air quality sensors were evaluated in Atlanta, GA, in Hyderabad, India and also in lab experiments. Freeway emissions were also quantified in Atlanta. The performance of these sensors were evaluated against current measurement instruments. Results show potential usefulness for these sensors in polluted areas. The ability to inexpensively measure air pollution will enable researches, citizens, and policy makers to make informed decisions to reduce health impacts from air pollution.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
H.-M. Lee, F. Paulot, D. K. Henze, K. Travis, D. J. Jacob, L. H. Pardo, and B. A. Schichtel
Atmos. Chem. Phys., 16, 525–540, https://doi.org/10.5194/acp-16-525-2016, https://doi.org/10.5194/acp-16-525-2016, 2016
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Sources of nitrogen deposition (Ndep) in Federal Class I areas in the US are investigated, identifying unique features in contributions from different species, sectors and locations. Ndep in many parks is impacted by emissions several hundred km away; the role of oxidized vs reduced sources varies regionally. Emissions reductions in the western US most effectively reduce the extent of areas in critical load exceedance, while reductions in the east most effectively reduce exceedance magnitudes.
M. W. Shephard, C. A. McLinden, K. E. Cady-Pereira, M. Luo, S. G. Moussa, A. Leithead, J. Liggio, R. M. Staebler, A. Akingunola, P. Makar, P. Lehr, J. Zhang, D. K. Henze, D. B. Millet, J. O. Bash, L. Zhu, K. C. Wells, S. L. Capps, S. Chaliyakunnel, M. Gordon, K. Hayden, J. R. Brook, M. Wolde, and S.-M. Li
Atmos. Meas. Tech., 8, 5189–5211, https://doi.org/10.5194/amt-8-5189-2015, https://doi.org/10.5194/amt-8-5189-2015, 2015
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This study provides direct validations of Tropospheric Emission Spectrometer (TES) satellite retrieved profiles against coincident aircraft profiles of carbon monoxide, ammonia, methanol, and formic acid, all of which are of interest for air quality. The comparisons are performed over the Canadian oil sands region during an intensive field campaign in support of the Joint Canada-Alberta Implementation Plan for the Oil Sands Monitoring (JOSM). Initial model evaluations are also provided.
S. Doniki, D. Hurtmans, L. Clarisse, C. Clerbaux, H. M. Worden, K. W. Bowman, and P.-F. Coheur
Atmos. Chem. Phys., 15, 12971–12987, https://doi.org/10.5194/acp-15-12971-2015, https://doi.org/10.5194/acp-15-12971-2015, 2015
L. Zhu, D. Henze, J. Bash, G.-R. Jeong, K. Cady-Pereira, M. Shephard, M. Luo, F. Paulot, and S. Capps
Atmos. Chem. Phys., 15, 12823–12843, https://doi.org/10.5194/acp-15-12823-2015, https://doi.org/10.5194/acp-15-12823-2015, 2015
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We implement new diurnal variation scheme for ammonia livestock emissions and bidirectional exchange scheme and its adjoint in the GEOS-Chem global chemical transport model. Updated diurnal variability improves modeled-to-hourly in situ measurements comparison. The ammonium soil pool in the bidirectional exchange model largely extends the ammonia lifetime in the atmosphere. Large model biases remain as livestock emissions are still underestimated.
B. Gantt, J. T. Kelly, and J. O. Bash
Geosci. Model Dev., 8, 3733–3746, https://doi.org/10.5194/gmd-8-3733-2015, https://doi.org/10.5194/gmd-8-3733-2015, 2015
E. Dammers, C. Vigouroux, M. Palm, E. Mahieu, T. Warneke, D. Smale, B. Langerock, B. Franco, M. Van Damme, M. Schaap, J. Notholt, and J. W. Erisman
Atmos. Chem. Phys., 15, 12789–12803, https://doi.org/10.5194/acp-15-12789-2015, https://doi.org/10.5194/acp-15-12789-2015, 2015
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We present a new retrieval method for ammonia (NH3) concentrations and total columns from ground-based Fourier transform infrared (FTIR) observations. Observations from Bremen, Lauder, Réunion and Jungfraujoch are used to show the capabilities of the new retrieval. The developed retrieval provides a new way of obtaining time-resolved measurements and will be useful for understanding the dynamics of ammonia concentrations in the atmosphere and for satellite and model validation.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
T. Stavrakou, J.-F. Müller, M. Bauwens, I. De Smedt, M. Van Roozendael, M. De Mazière, C. Vigouroux, F. Hendrick, M. George, C. Clerbaux, P.-F. Coheur, and A. Guenther
Atmos. Chem. Phys., 15, 11861–11884, https://doi.org/10.5194/acp-15-11861-2015, https://doi.org/10.5194/acp-15-11861-2015, 2015
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Formaldehyde columns from two space sensors, GOME-2 and OMI, constrain by inverse modeling the global emissions of HCHO precursors in 2010. The resulting biogenic and pyrogenic fluxes from both optimizations show a very good degree of consistency. The isoprene fluxes are reduced globally by ca. 10%, and emissions from fires decrease by ca. 35%, compared to the prior. Anthropogenic emissions are weakly constrained except over China. Sensitivity inversions show robustness of the inferred fluxes.
F. Deng, D. B. A. Jones, T. W. Walker, M. Keller, K. W. Bowman, D. K. Henze, R. Nassar, E. A. Kort, S. C. Wofsy, K. A. Walker, A. E. Bourassa, and D. A. Degenstein
Atmos. Chem. Phys., 15, 11773–11788, https://doi.org/10.5194/acp-15-11773-2015, https://doi.org/10.5194/acp-15-11773-2015, 2015
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The upper troposphere and lower stratosphere (UTLS) is characterized by strong gradients in the distribution of long-lived tracers, which are sensitive to discrepancies in transport in models. We found that our model overestimates CO2 in the polar UTLS through comparison of modeled CO2 with aircraft observations. We then corrected the modeled CO2 and quantified the impact of the correction on the flux estimates using an atmospheric model together with atmospheric CO2 measured from a satellite.
M. George, C. Clerbaux, I. Bouarar, P.-F. Coheur, M. N. Deeter, D. P. Edwards, G. Francis, J. C. Gille, J. Hadji-Lazaro, D. Hurtmans, A. Inness, D. Mao, and H. M. Worden
Atmos. Meas. Tech., 8, 4313–4328, https://doi.org/10.5194/amt-8-4313-2015, https://doi.org/10.5194/amt-8-4313-2015, 2015
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
Y. Zhao, L. Zhang, Y. Pan, Y. Wang, F. Paulot, and D. K. Henze
Atmos. Chem. Phys., 15, 10905–10924, https://doi.org/10.5194/acp-15-10905-2015, https://doi.org/10.5194/acp-15-10905-2015, 2015
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Rapid Asian industrialization has led to increased atmospheric nitrogen deposition downwind. This work analyzes the sources and processes controlling atmospheric nitrogen deposition to the northwestern Pacific. Both nitrogen emissions and meteorology, largely controlled by the East Asian Monsoon, determine the seasonality of nitrogen deposition. Ascribing deposition over the marginal seas to nitrogen sources from different regions and sectors shows important contribution from fertilizer use.
P. D. Hamer, K. W. Bowman, D. K. Henze, J.-L. Attié, and V. Marécal
Atmos. Chem. Phys., 15, 10645–10667, https://doi.org/10.5194/acp-15-10645-2015, https://doi.org/10.5194/acp-15-10645-2015, 2015
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Using a simplified air quality forecasting model, we explore how characteristics of air quality observations affect our ability to understand and predict ozone air pollution. We show that the photochemical conditions can strongly influence the observing priorities for ozone prediction, such as which species are observed and how well, when, and how frequently. High-freqency observations of ozone, NOx and HCHO in combination during the morning and afternoon are particularly advantageous.
V. Duflot, C. Wespes, L. Clarisse, D. Hurtmans, Y. Ngadi, N. Jones, C. Paton-Walsh, J. Hadji-Lazaro, C. Vigouroux, M. De Mazière, J.-M. Metzger, E. Mahieu, C. Servais, F. Hase, M. Schneider, C. Clerbaux, and P.-F. Coheur
Atmos. Chem. Phys., 15, 10509–10527, https://doi.org/10.5194/acp-15-10509-2015, https://doi.org/10.5194/acp-15-10509-2015, 2015
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We present global distributions of acetylene (C2H2) and hydrogen cyanide (HCN) total
columns derived from the Infrared Atmospheric Sounding Interferometer (IASI). C2H2 and HCN are ubiquitous atmospheric trace gases with medium tropospheric lifetime, which are frequently used as indicators of combustion sources and as tracers for atmospheric transport and chemistry. We show that there is an overall agreement between ground-based and space measurements, as well as model simulations.
L. Zhang, D. K. Henze, G. A. Grell, G. R. Carmichael, N. Bousserez, Q. Zhang, O. Torres, C. Ahn, Z. Lu, J. Cao, and Y. Mao
Atmos. Chem. Phys., 15, 10281–10308, https://doi.org/10.5194/acp-15-10281-2015, https://doi.org/10.5194/acp-15-10281-2015, 2015
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We attempt to reduce uncertainties in BC emissions and improve BC model simulations by developing top-down, spatially resolved, estimates of BC emissions through assimilation of OMI observations of aerosol absorption optical depth (AAOD) with the GEOS-Chem model and its adjoint for April and October of 2006. Despite the limitations and uncertainties, using OMI AAOD to constrain BC sources we are able to improve model representation of BC distributions, particularly over China.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
G. Baldassarre, L. Pozzoli, C. C. Schmidt, A. Unal, T. Kindap, W. P. Menzel, S. Whitburn, P.-F. Coheur, A. Kavgaci, and J. W. Kaiser
Atmos. Chem. Phys., 15, 8539–8558, https://doi.org/10.5194/acp-15-8539-2015, https://doi.org/10.5194/acp-15-8539-2015, 2015
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We investigate the quality of fire emission estimates derived from SEVIRI FRP for air quality simulations with the Community Multiscale Air Quality (CMAQ) model, by comparing them with available MODIS FRP-based ones.
We demonstrate that geostationary observations allow for refining biomass burning emissions, which can subsequently be used in regional scale air quality models in order to improve the prediction of chemical composition of the atmosphere in presence of large fire episodes.
M. Boichu, L. Clarisse, J.-C. Péré, H. Herbin, P. Goloub, F. Thieuleux, F. Ducos, C. Clerbaux, and D. Tanré
Atmos. Chem. Phys., 15, 8381–8400, https://doi.org/10.5194/acp-15-8381-2015, https://doi.org/10.5194/acp-15-8381-2015, 2015
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IASI spaceborne imagery is used to reconstruct temporal variations of flux and altitude of volcanic emissions via an inversion procedure. Ground-based UV measurements underestimate the SO2 flux by 1 order of magnitude due to ash-induced plume opacity. Assimilation of SO2 altitude, retrieved directly from IASI, should render the inversion scheme independent of the wind shear prerequisite. CALIOP LiDAR observations support the coexistence of SO2 and sulfate aerosols in the volcanic cloud.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
C. E. Ivey, H. A. Holmes, Y. T. Hu, J. A. Mulholland, and A. G. Russell
Geosci. Model Dev., 8, 2153–2165, https://doi.org/10.5194/gmd-8-2153-2015, https://doi.org/10.5194/gmd-8-2153-2015, 2015
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An integral part of air quality management is knowledge of the impact of pollutant sources on ambient concentrations of particulate matter (PM). This work presents a novel spatiotemporal source apportionment method that generates source impacts for the continental USA. Key sources presented include fossil fuel combustion, biomass burning, dust, sea salt, as well as agricultural activities, biogenics, and aircraft.
Y. H. Mao, Q. B. Li, D. K. Henze, Z. Jiang, D. B. A. Jones, M. Kopacz, C. He, L. Qi, M. Gao, W.-M. Hao, and K.-N. Liou
Atmos. Chem. Phys., 15, 7685–7702, https://doi.org/10.5194/acp-15-7685-2015, https://doi.org/10.5194/acp-15-7685-2015, 2015
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604, https://doi.org/10.5194/acp-15-7585-2015, https://doi.org/10.5194/acp-15-7585-2015, 2015
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992, https://doi.org/10.5194/bg-12-3973-2015, https://doi.org/10.5194/bg-12-3973-2015, 2015
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The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
J. J. Guerrette and D. K. Henze
Geosci. Model Dev., 8, 1857–1876, https://doi.org/10.5194/gmd-8-1857-2015, https://doi.org/10.5194/gmd-8-1857-2015, 2015
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WRFPLUS-Chem is a coupled meteorology-chemistry adjoint and tangent linear model, with applications in sensitivity analysis and four-dimensional variational data assimilation. The linearized models are verified against finite difference approximations from the nonlinear forward model, WRF-Chem. A new checkpointing scheme enables data assimilation beyond 6h. New capabilities are demonstrated in an emission sensitivity study.
Z. Jiang, D. B. A. Jones, J. Worden, H. M. Worden, D. K. Henze, and Y. X. Wang
Atmos. Chem. Phys., 15, 6801–6814, https://doi.org/10.5194/acp-15-6801-2015, https://doi.org/10.5194/acp-15-6801-2015, 2015
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We present a high-resolution (0.5 x 0.667) regional CO inversion over North America in the period of June 2004–May 2005, using a combination of GEOS-Chem model and MOPITT CO observations. With optimized lateral boundary conditions, we show that regional inversion analyses can reduce the sensitivity of the CO source estimates to errors in long-range transport and in the distributions of the hydroxyl radical (OH), and consequently, provide better quantification on regional CO source estimates.
X. Fu, S. X. Wang, L. M. Ran, J. E. Pleim, E. Cooter, J. O. Bash, V. Benson, and J. M. Hao
Atmos. Chem. Phys., 15, 6637–6649, https://doi.org/10.5194/acp-15-6637-2015, https://doi.org/10.5194/acp-15-6637-2015, 2015
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In this study, we estimate, for the first time, the NH3 emission from the agricultural fertilizer application in China online using the bi-directional CMAQ model coupled to an agro-ecosystem model. Compared with previous researches, this method considers more influencing factors, such as meteorological fields, soil and the fertilizer application, and provides improved NH3 emission with higher spatial and temporal resolution.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
M. Van Damme, L. Clarisse, E. Dammers, X. Liu, J. B. Nowak, C. Clerbaux, C. R. Flechard, C. Galy-Lacaux, W. Xu, J. A. Neuman, Y. S. Tang, M. A. Sutton, J. W. Erisman, and P. F. Coheur
Atmos. Meas. Tech., 8, 1575–1591, https://doi.org/10.5194/amt-8-1575-2015, https://doi.org/10.5194/amt-8-1575-2015, 2015
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In this study, comprehensive ground-based data sets (Europe, China, Africa and United States) are used to evaluate NH3 measurements from IASI. Global yearly and regional monthly comparisons show fair agreement, while hourly measurements are used to investigate the limitations of direct comparisons. In addition, dense airborne measurements are explored and show the highest correlation coefficients in this study. Finally, the urgent need for independent NH3 column measurements is discussed.
J.-L. Lacour, L. Clarisse, J. Worden, M. Schneider, S. Barthlott, F. Hase, C. Risi, C. Clerbaux, D. Hurtmans, and P.-F. Coheur
Atmos. Meas. Tech., 8, 1447–1466, https://doi.org/10.5194/amt-8-1447-2015, https://doi.org/10.5194/amt-8-1447-2015, 2015
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This paper describes a cross-validation study of tropospheric δD (HDO/H2O ratio) profiles retrieved from IASI spectra (retrieval performed at ULB). We document how these profiles compare to profiles derived from TES/AURA sounder and from three ground-based FTIRs of the NDACC network (produced within the MUSICA project). We show that empirical differences are in agreement with the theoretical expected differences which are dominated by IASI observational and the smoothing error components.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
Z. Jiang, D. B. A. Jones, H. M. Worden, and D. K. Henze
Atmos. Chem. Phys., 15, 1521–1537, https://doi.org/10.5194/acp-15-1521-2015, https://doi.org/10.5194/acp-15-1521-2015, 2015
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Using MOPITT (version 5) tropospheric profile and surface layer retrievals, we constrain global CO emissions in the period of June 2004 – May 2005. The inversions suggest a reduction in CO emission in the tropics and an increase in emissions at middle and high latitudes. The results demonstrate that the use of the surface layer retrievals from MOPITT can significantly mitigate the potential impacts of model bias in OH and long-range transport on CO emission estimates.
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
R. H. F. Kwok, K. R. Baker, S. L. Napelenok, and G. S. Tonnesen
Geosci. Model Dev., 8, 99–114, https://doi.org/10.5194/gmd-8-99-2015, https://doi.org/10.5194/gmd-8-99-2015, 2015
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The implementation and application of the Integrated Source Apportionment Method (ISAM) for O3 and its precursors for the Community Multiscale Air Quality (CMAQ) model are described. CMAQ-ISAM is a hybrid of source apportionment and source sensitivity in that O3 production is attributed to precursor sources based on the O3 formation regime. CMAQ-ISAM offers a source attribution tool for the purposes of quantifying and understanding sources and impacts of regional air pollution.
Z. Jiang, J. R. Worden, D. B. A. Jones, J.-T. Lin, W. W. Verstraeten, and D. K. Henze
Atmos. Chem. Phys., 15, 99–112, https://doi.org/10.5194/acp-15-99-2015, https://doi.org/10.5194/acp-15-99-2015, 2015
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We use satellite measurements of O3, CO and NO2 from TES, MOPITT and OMI to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia. Using the adjoint of GEOS-Chem, we found that Chinese emissions have the largest influence on the free tropospheric O3. The contributions from lightning NOx in summer and India and southeastern Asia emissions in winter are sizable, comparable with Chinese emissions.
C. Crevoisier, C. Clerbaux, V. Guidard, T. Phulpin, R. Armante, B. Barret, C. Camy-Peyret, J.-P. Chaboureau, P.-F. Coheur, L. Crépeau, G. Dufour, L. Labonnote, L. Lavanant, J. Hadji-Lazaro, H. Herbin, N. Jacquinet-Husson, S. Payan, E. Péquignot, C. Pierangelo, P. Sellitto, and C. Stubenrauch
Atmos. Meas. Tech., 7, 4367–4385, https://doi.org/10.5194/amt-7-4367-2014, https://doi.org/10.5194/amt-7-4367-2014, 2014
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
A. Laeng, U. Grabowski, T. von Clarmann, G. Stiller, N. Glatthor, M. Höpfner, S. Kellmann, M. Kiefer, A. Linden, S. Lossow, V. Sofieva, I. Petropavlovskikh, D. Hubert, T. Bathgate, P. Bernath, C. D. Boone, C. Clerbaux, P. Coheur, R. Damadeo, D. Degenstein, S. Frith, L. Froidevaux, J. Gille, K. Hoppel, M. McHugh, Y. Kasai, J. Lumpe, N. Rahpoe, G. Toon, T. Sano, M. Suzuki, J. Tamminen, J. Urban, K. Walker, M. Weber, and J. Zawodny
Atmos. Meas. Tech., 7, 3971–3987, https://doi.org/10.5194/amt-7-3971-2014, https://doi.org/10.5194/amt-7-3971-2014, 2014
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357, https://doi.org/10.5194/gmd-7-2345-2014, https://doi.org/10.5194/gmd-7-2345-2014, 2014
S. Safieddine, A. Boynard, P.-F. Coheur, D. Hurtmans, G. Pfister, B. Quennehen, J. L. Thomas, J.-C. Raut, K. S. Law, Z. Klimont, J. Hadji-Lazaro, M. George, and C. Clerbaux
Atmos. Chem. Phys., 14, 10119–10131, https://doi.org/10.5194/acp-14-10119-2014, https://doi.org/10.5194/acp-14-10119-2014, 2014
Q. Zhu, Q. Zhuang, D. Henze, K. Bowman, M. Chen, Y. Liu, Y. He, H. Matsueda, T. Machida, Y. Sawa, and W. Oechel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-22587-2014, https://doi.org/10.5194/acpd-14-22587-2014, 2014
Revised manuscript not accepted
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497, https://doi.org/10.5194/acp-14-7485-2014, https://doi.org/10.5194/acp-14-7485-2014, 2014
Z. Shen, J. Liu, L. W. Horowitz, D. K. Henze, S. Fan, Levy II H., D. L. Mauzerall, J.-T. Lin, and S. Tao
Atmos. Chem. Phys., 14, 6315–6327, https://doi.org/10.5194/acp-14-6315-2014, https://doi.org/10.5194/acp-14-6315-2014, 2014
Y. Hu, S. Balachandran, J. E. Pachon, J. Baek, C. Ivey, H. Holmes, M. T. Odman, J. A. Mulholland, and A. G. Russell
Atmos. Chem. Phys., 14, 5415–5431, https://doi.org/10.5194/acp-14-5415-2014, https://doi.org/10.5194/acp-14-5415-2014, 2014
M. Pommier, J.-L. Lacour, C. Risi, F. M. Bréon, C. Clerbaux, P.-F. Coheur, K. Gribanov, D. Hurtmans, J. Jouzel, and V. Zakharov
Atmos. Meas. Tech., 7, 1581–1595, https://doi.org/10.5194/amt-7-1581-2014, https://doi.org/10.5194/amt-7-1581-2014, 2014
J. Kaiser, X. Li, R. Tillmann, I. Acir, F. Holland, F. Rohrer, R. Wegener, and F. N. Keutsch
Atmos. Meas. Tech., 7, 1571–1580, https://doi.org/10.5194/amt-7-1571-2014, https://doi.org/10.5194/amt-7-1571-2014, 2014
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215, https://doi.org/10.5194/acp-14-5205-2014, https://doi.org/10.5194/acp-14-5205-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
H. Brenot, N. Theys, L. Clarisse, J. van Geffen, J. van Gent, M. Van Roozendael, R. van der A, D. Hurtmans, P.-F. Coheur, C. Clerbaux, P. Valks, P. Hedelt, F. Prata, O. Rasson, K. Sievers, and C. Zehner
Nat. Hazards Earth Syst. Sci., 14, 1099–1123, https://doi.org/10.5194/nhess-14-1099-2014, https://doi.org/10.5194/nhess-14-1099-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, https://doi.org/10.5194/acp-14-4809-2014, 2014
F. Deng, D. B. A. Jones, D. K. Henze, N. Bousserez, K. W. Bowman, J. B. Fisher, R. Nassar, C. O'Dell, D. Wunch, P. O. Wennberg, E. A. Kort, S. C. Wofsy, T. Blumenstock, N. M. Deutscher, D. W. T. Griffith, F. Hase, P. Heikkinen, V. Sherlock, K. Strong, R. Sussmann, and T. Warneke
Atmos. Chem. Phys., 14, 3703–3727, https://doi.org/10.5194/acp-14-3703-2014, https://doi.org/10.5194/acp-14-3703-2014, 2014
L. Clarisse, P.-F. Coheur, N. Theys, D. Hurtmans, and C. Clerbaux
Atmos. Chem. Phys., 14, 3095–3111, https://doi.org/10.5194/acp-14-3095-2014, https://doi.org/10.5194/acp-14-3095-2014, 2014
M. Van Damme, L. Clarisse, C. L. Heald, D. Hurtmans, Y. Ngadi, C. Clerbaux, A. J. Dolman, J. W. Erisman, and P. F. Coheur
Atmos. Chem. Phys., 14, 2905–2922, https://doi.org/10.5194/acp-14-2905-2014, https://doi.org/10.5194/acp-14-2905-2014, 2014
K. C. Wells, D. B. Millet, K. E. Cady-Pereira, M. W. Shephard, D. K. Henze, N. Bousserez, E. C. Apel, J. de Gouw, C. Warneke, and H. B. Singh
Atmos. Chem. Phys., 14, 2555–2570, https://doi.org/10.5194/acp-14-2555-2014, https://doi.org/10.5194/acp-14-2555-2014, 2014
B. H. Henderson, F. Akhtar, H. O. T. Pye, S. L. Napelenok, and W. T. Hutzell
Geosci. Model Dev., 7, 339–360, https://doi.org/10.5194/gmd-7-339-2014, https://doi.org/10.5194/gmd-7-339-2014, 2014
B. S. Meland, X. Xu, D. K. Henze, and J. Wang
Atmos. Meas. Tech., 6, 3441–3457, https://doi.org/10.5194/amt-6-3441-2013, https://doi.org/10.5194/amt-6-3441-2013, 2013
T. Chai, H.-C. Kim, P. Lee, D. Tong, L. Pan, Y. Tang, J. Huang, J. McQueen, M. Tsidulko, and I. Stajner
Geosci. Model Dev., 6, 1831–1850, https://doi.org/10.5194/gmd-6-1831-2013, https://doi.org/10.5194/gmd-6-1831-2013, 2013
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445, https://doi.org/10.5194/gmd-6-1429-2013, https://doi.org/10.5194/gmd-6-1429-2013, 2013
M. Boichu, L. Menut, D. Khvorostyanov, L. Clarisse, C. Clerbaux, S. Turquety, and P.-F. Coheur
Atmos. Chem. Phys., 13, 8569–8584, https://doi.org/10.5194/acp-13-8569-2013, https://doi.org/10.5194/acp-13-8569-2013, 2013
F. Jégou, G. Berthet, C. Brogniez, J.-B. Renard, P. François, J. M. Haywood, A. Jones, Q. Bourgeois, T. Lurton, F. Auriol, S. Godin-Beekmann, C. Guimbaud, G. Krysztofiak, B. Gaubicher, M. Chartier, L. Clarisse, C. Clerbaux, J. Y. Balois, C. Verwaerde, and D. Daugeron
Atmos. Chem. Phys., 13, 6533–6552, https://doi.org/10.5194/acp-13-6533-2013, https://doi.org/10.5194/acp-13-6533-2013, 2013
K. W. Appel, G. A. Pouliot, H. Simon, G. Sarwar, H. O. T. Pye, S. L. Napelenok, F. Akhtar, and S. J. Roselle
Geosci. Model Dev., 6, 883–899, https://doi.org/10.5194/gmd-6-883-2013, https://doi.org/10.5194/gmd-6-883-2013, 2013
N. Theys, R. Campion, L. Clarisse, H. Brenot, J. van Gent, B. Dils, S. Corradini, L. Merucci, P.-F. Coheur, M. Van Roozendael, D. Hurtmans, C. Clerbaux, S. Tait, and F. Ferrucci
Atmos. Chem. Phys., 13, 5945–5968, https://doi.org/10.5194/acp-13-5945-2013, https://doi.org/10.5194/acp-13-5945-2013, 2013
R. Wang, S. Tao, P. Ciais, H. Z. Shen, Y. Huang, H. Chen, G. F. Shen, B. Wang, W. Li, Y. Y. Zhang, Y. Lu, D. Zhu, Y. C. Chen, X. P. Liu, W. T. Wang, X. L. Wang, W. X. Liu, B. G. Li, and S. L. Piao
Atmos. Chem. Phys., 13, 5189–5203, https://doi.org/10.5194/acp-13-5189-2013, https://doi.org/10.5194/acp-13-5189-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
K. A. Tereszchuk, G. González Abad, C. Clerbaux, J. Hadji-Lazaro, D. Hurtmans, P.-F. Coheur, and P. F. Bernath
Atmos. Chem. Phys., 13, 4529–4541, https://doi.org/10.5194/acp-13-4529-2013, https://doi.org/10.5194/acp-13-4529-2013, 2013
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251, https://doi.org/10.5194/acp-13-4235-2013, https://doi.org/10.5194/acp-13-4235-2013, 2013
A. Inness, F. Baier, A. Benedetti, I. Bouarar, S. Chabrillat, H. Clark, C. Clerbaux, P. Coheur, R. J. Engelen, Q. Errera, J. Flemming, M. George, C. Granier, J. Hadji-Lazaro, V. Huijnen, D. Hurtmans, L. Jones, J. W. Kaiser, J. Kapsomenakis, K. Lefever, J. Leitão, M. Razinger, A. Richter, M. G. Schultz, A. J. Simmons, M. Suttie, O. Stein, J.-N. Thépaut, V. Thouret, M. Vrekoussis, C. Zerefos, and the MACC team
Atmos. Chem. Phys., 13, 4073–4109, https://doi.org/10.5194/acp-13-4073-2013, https://doi.org/10.5194/acp-13-4073-2013, 2013
Y. R'Honi, L. Clarisse, C. Clerbaux, D. Hurtmans, V. Duflot, S. Turquety, Y. Ngadi, and P.-F. Coheur
Atmos. Chem. Phys., 13, 4171–4181, https://doi.org/10.5194/acp-13-4171-2013, https://doi.org/10.5194/acp-13-4171-2013, 2013
V. Duflot, D. Hurtmans, L. Clarisse, Y. R'honi, C. Vigouroux, M. De Mazière, E. Mahieu, C. Servais, C. Clerbaux, and P.-F. Coheur
Atmos. Meas. Tech., 6, 917–925, https://doi.org/10.5194/amt-6-917-2013, https://doi.org/10.5194/amt-6-917-2013, 2013
J. O. Bash, E. J. Cooter, R. L. Dennis, J. T. Walker, and J. E. Pleim
Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, https://doi.org/10.5194/bg-10-1635-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
J. Gazeaux, C. Clerbaux, M. George, J. Hadji-Lazaro, J. Kuttippurath, P.-F. Coheur, D. Hurtmans, T. Deshler, M. Kovilakam, P. Campbell, V. Guidard, F. Rabier, and J.-N. Thépaut
Atmos. Meas. Tech., 6, 613–620, https://doi.org/10.5194/amt-6-613-2013, https://doi.org/10.5194/amt-6-613-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
L. Clarisse, P.-F. Coheur, F. Prata, J. Hadji-Lazaro, D. Hurtmans, and C. Clerbaux
Atmos. Chem. Phys., 13, 2195–2221, https://doi.org/10.5194/acp-13-2195-2013, https://doi.org/10.5194/acp-13-2195-2013, 2013
J. T. Walker, M. R. Jones, J. O. Bash, L. Myles, T. Meyers, D. Schwede, J. Herrick, E. Nemitz, and W. Robarge
Biogeosciences, 10, 981–998, https://doi.org/10.5194/bg-10-981-2013, https://doi.org/10.5194/bg-10-981-2013, 2013
H. M. Worden, M. N. Deeter, C. Frankenberg, M. George, F. Nichitiu, J. Worden, I. Aben, K. W. Bowman, C. Clerbaux, P. F. Coheur, A. T. J. de Laat, R. Detweiler, J. R. Drummond, D. P. Edwards, J. C. Gille, D. Hurtmans, M. Luo, S. Martínez-Alonso, S. Massie, G. Pfister, and J. X. Warner
Atmos. Chem. Phys., 13, 837–850, https://doi.org/10.5194/acp-13-837-2013, https://doi.org/10.5194/acp-13-837-2013, 2013
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
M. Huang, G. R. Carmichael, T. Chai, R. B. Pierce, S. J. Oltmans, D. A. Jaffe, K. W. Bowman, A. Kaduwela, C. Cai, S. N. Spak, A. J. Weinheimer, L. G. Huey, and G. S. Diskin
Atmos. Chem. Phys., 13, 359–391, https://doi.org/10.5194/acp-13-359-2013, https://doi.org/10.5194/acp-13-359-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Spatiotemporal Source Apportionment of Ozone Pollution over the Greater Bay Area
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Estimation of Canada’s methane emissions: inverse modelling analysis using the ECCC measurement network
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
Potential of 14C-based versus ∆CO-based ∆ffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Satellite quantification of methane emissions and oil–gas methane intensities from individual countries in the Middle East and North Africa: implications for climate action
Coupled mesoscale–microscale modeling of air quality in a polluted city using WRF-LES-Chem
Impact of aerosol optics on vertical distribution of ozone in autumn over Yangtze River Delta
A view of the European carbon flux landscape through the lens of the ICOS atmospheric observation network
Technical note: The CAMS greenhouse gas reanalysis from 2003 to 2020
Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models
Impacts of urbanization on air quality and the related health risks in a city with complex terrain
Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data
Development and application of a multi-scale modeling framework for urban high-resolution NO2 pollution mapping
Towards monitoring the CO2 source–sink distribution over India via inverse modelling: quantifying the fine-scale spatiotemporal variability in the atmospheric CO2 mole fraction
Methane emissions from China: a high-resolution inversion of TROPOMI satellite observations
Estimated regional CO2 flux and uncertainty based on an ensemble of atmospheric CO2 inversions
Assessing the representativity of NH3 measurements influenced by boundary-layer dynamics and the turbulent dispersion of a nearby emission source
Analysis of CO2, CH4, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations
Technical note: Interpretation of field observations of point-source methane plume using observation-driven large-eddy simulations
Quantifying fossil fuel methane emissions using observations of atmospheric ethane and an uncertain emission ratio
The impact of peripheral circulation characteristics of typhoon on sustained ozone episodes over the Pearl River Delta region, China
Updated Global Fuel Exploitation Inventory (GFEI) for methane emissions from the oil, gas, and coal sectors: evaluation with inversions of atmospheric methane observations
High-resolution mapping of regional traffic emissions using land-use machine learning models
Land use and anthropogenic heat modulate ozone by meteorology: a perspective from the Yangtze River Delta region
Four years of global carbon cycle observed from the Orbiting Carbon Observatory 2 (OCO-2) version 9 and in situ data and comparison to OCO-2 version 7
Data assimilation of CrIS NH3 satellite observations for improving spatiotemporal NH3 distributions in LOTOS-EUROS
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
EGUsphere, https://doi.org/10.5194/egusphere-2023-3140, https://doi.org/10.5194/egusphere-2023-3140, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation of major spatiotemporal contributors to the O3 pollution under the influence of typhoons and sub-tropical high-pressure. Through the temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
EGUsphere, https://doi.org/10.5194/egusphere-2023-2550, https://doi.org/10.5194/egusphere-2023-2550, 2023
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Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface Greenhouse Gas measurements. The estimated decadal emissions show no significant trend, but the uncertainty is reduced over time as more measurements became available. We find notable features in the CH4 emissions, such as a positive correlation with surface air temperature in summer. The measurement network across Canada could monitor future CH4 emission changes and compliance for climate mitigation goals.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Fabian Manuel Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1239, https://doi.org/10.5194/egusphere-2023-1239, 2023
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates versus continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of the ffCO2 emissions in an urban region with an inverse modelling framework. We find that the CO-based ffCO2 estimates allow to reconstruct robust seasonal cycles, which show the distinct Covid-19 drawdown in 2020 and can be used to validate emission inventories.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Jianing Dai, Cathy Wing Yi Li, Pablo Lichtig, Roy Chun-Wang Tsang, Chun-Ho Liu, Tao Wang, and Guy Pierre Brasseur
Atmos. Chem. Phys., 23, 5905–5927, https://doi.org/10.5194/acp-23-5905-2023, https://doi.org/10.5194/acp-23-5905-2023, 2023
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Air quality in urban areas is difficult to simulate in coarse-resolution models. This work exploits the WRF (Weather Research and Forecasting) model coupled with a large-eddy simulation (LES) component and online chemistry to perform high-resolution (33.3 m) simulations of air quality in a large city. The evaluation of the simulations with observations shows that increased model resolution improves the representation of the chemical species near the pollution sources.
Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu
Atmos. Chem. Phys., 23, 5177–5190, https://doi.org/10.5194/acp-23-5177-2023, https://doi.org/10.5194/acp-23-5177-2023, 2023
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We analyze ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction, and upper-level photolysis enhancement under different underlying surface and pollution conditions. Thus, ozone decreases within the entire boundary layer during the daytime, and the decrease is the least in aerosol external mixing states compared to internal and core shell mixing states.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
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In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
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We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Chenchao Zhan, Min Xie, Hua Lu, Bojun Liu, Zheng Wu, Tijian Wang, Bingliang Zhuang, Mengmeng Li, and Shu Li
Atmos. Chem. Phys., 23, 771–788, https://doi.org/10.5194/acp-23-771-2023, https://doi.org/10.5194/acp-23-771-2023, 2023
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With the development of urbanization, urban land use and anthropogenic
emissions increase, affecting urban air quality and, in turn, the health risks associated with air pollutants. In this study, we systematically evaluate the impacts of urbanization on air quality and the corresponding health risks in a highly urbanized city with severe air pollution and complex terrain. This work focuses on the health risks caused by urbanization and can provide valuable insight for air pollution strategies.
Hélène Peiro, Sean Crowell, and Berrien Moore III
Atmos. Chem. Phys., 22, 15817–15849, https://doi.org/10.5194/acp-22-15817-2022, https://doi.org/10.5194/acp-22-15817-2022, 2022
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CO data can provide a powerful constraint on fire fluxes, supporting more accurate estimation of biospheric CO2 fluxes. We converted CO fire flux into CO2 fire prior, which is then used to adjust CO2 respiration. We applied this to two other fire flux products. CO2 inversions constrained by satellites or in situ data are then performed. Results show larger variations among the data assimilated than across the priors, but tropical flux from in situ inversions is sensitive to priors.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
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This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Vishnu Thilakan, Dhanyalekshmi Pillai, Christoph Gerbig, Michal Galkowski, Aparnna Ravi, and Thara Anna Mathew
Atmos. Chem. Phys., 22, 15287–15312, https://doi.org/10.5194/acp-22-15287-2022, https://doi.org/10.5194/acp-22-15287-2022, 2022
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This paper demonstrates how we can use atmospheric observations to improve the CO2 flux estimates in India. This is achieved by improving the representation of terrain, mesoscale transport, and flux variations. We quantify the impact of the unresolved variations in the current models on optimally estimated fluxes via inverse modelling and quantify the associated flux uncertainty. We illustrate how a parameterization scheme captures this variability in the coarse models.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Naveen Chandra, Prabir K. Patra, Yousuke Niwa, Akihiko Ito, Yosuke Iida, Daisuke Goto, Shinji Morimoto, Masayuki Kondo, Masayuki Takigawa, Tomohiro Hajima, and Michio Watanabe
Atmos. Chem. Phys., 22, 9215–9243, https://doi.org/10.5194/acp-22-9215-2022, https://doi.org/10.5194/acp-22-9215-2022, 2022
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This paper is intended to accomplish two goals: (1) quantify mean and uncertainty in non-fossil-fuel CO2 fluxes estimated by inverse modeling and (2) provide in-depth analyses of regional CO2 fluxes in support of emission mitigation policymaking. CO2 flux variability and trends are discussed concerning natural climate variability and human disturbances using multiple lines of evidence.
Ruben B. Schulte, Margreet C. van Zanten, Bart J. H. van Stratum, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 22, 8241–8257, https://doi.org/10.5194/acp-22-8241-2022, https://doi.org/10.5194/acp-22-8241-2022, 2022
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We present a fine-scale simulation framework, utilizing large-eddy simulations, to assess NH3 measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source. The minimum required distance from an emission source differs for concentration and flux measurements, from 0.5–3.0 km and 0.75–4.5 km, respectively. The simulation framework presented here proves to be a powerful and versatile tool for future NH3 research at high spatio-temporal resolutions.
Sieglinde Callewaert, Jérôme Brioude, Bavo Langerock, Valentin Duflot, Dominique Fonteyn, Jean-François Müller, Jean-Marc Metzger, Christian Hermans, Nicolas Kumps, Michel Ramonet, Morgan Lopez, Emmanuel Mahieu, and Martine De Mazière
Atmos. Chem. Phys., 22, 7763–7792, https://doi.org/10.5194/acp-22-7763-2022, https://doi.org/10.5194/acp-22-7763-2022, 2022
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A regional atmospheric transport model is used to analyze the factors contributing to CO2, CH4, and CO observations at Réunion Island. We show that the surface observations are dominated by local fluxes and dynamical processes, while the column data are influenced by larger-scale mechanisms such as biomass burning plumes. The model is able to capture the measured time series well; however, the results are highly dependent on accurate boundary conditions and high-resolution emission inventories.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
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Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Ying Li, Xiangjun Zhao, Xuejiao Deng, and Jinhui Gao
Atmos. Chem. Phys., 22, 3861–3873, https://doi.org/10.5194/acp-22-3861-2022, https://doi.org/10.5194/acp-22-3861-2022, 2022
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This study finds a new phenomenon of weak wind deepening (WWD) associated with the peripheral circulation of typhoon and gives the influence mechanism of WWD on its contribution to daily variation during sustained ozone episodes. The WWD provides the premise for pollution accumulation in the whole PBL and continued enhancement of ground-level ozone via vertical mixing processes. These findings could benefit the daily daytime ozone forecast in the PRD region and other areas.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
Xiaomeng Wu, Daoyuan Yang, Ruoxi Wu, Jiajun Gu, Yifan Wen, Shaojun Zhang, Rui Wu, Renjie Wang, Honglei Xu, K. Max Zhang, Ye Wu, and Jiming Hao
Atmos. Chem. Phys., 22, 1939–1950, https://doi.org/10.5194/acp-22-1939-2022, https://doi.org/10.5194/acp-22-1939-2022, 2022
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Our work pioneered land-use machine learning methods for developing link-level emission inventories, utilizing hourly traffic profiles, including volume, speed, and fleet mix, obtained from the governmental intercity highway monitoring network in the "capital circles" of China. This research provides a platform to realize the near-real-time process of establishing high-resolution vehicle emission inventories for policy makers to engage in sophisticated traffic management.
Chenchao Zhan and Min Xie
Atmos. Chem. Phys., 22, 1351–1371, https://doi.org/10.5194/acp-22-1351-2022, https://doi.org/10.5194/acp-22-1351-2022, 2022
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The changes of land use and anthropogenic heat (AH) derived from urbanization can affect meteorology and in turn O3 evolution. In this study, we briefly describe the general features of O3 pollution in the Yangtze River Delta (YRD) based on in situ observational data. Then, the impacts of land use and anthropogenic heat on O3 via changing the meteorological factors and local circulations are investigated in this region using the WRF-Chem model.
Hélène Peiro, Sean Crowell, Andrew Schuh, David F. Baker, Chris O'Dell, Andrew R. Jacobson, Frédéric Chevallier, Junjie Liu, Annmarie Eldering, David Crisp, Feng Deng, Brad Weir, Sourish Basu, Matthew S. Johnson, Sajeev Philip, and Ian Baker
Atmos. Chem. Phys., 22, 1097–1130, https://doi.org/10.5194/acp-22-1097-2022, https://doi.org/10.5194/acp-22-1097-2022, 2022
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Satellite CO2 observations are constantly improved. We study an ensemble of different atmospheric models (inversions) from 2015 to 2018 using separate ground-based data or two versions of the OCO-2 satellite. Our study aims to determine if different satellite data corrections can yield different estimates of carbon cycle flux. A difference in the carbon budget between the two versions is found over tropical Africa, which seems to show the impact of corrections applied in satellite data.
Shelley van der Graaf, Enrico Dammers, Arjo Segers, Richard Kranenburg, Martijn Schaap, Mark W. Shephard, and Jan Willem Erisman
Atmos. Chem. Phys., 22, 951–972, https://doi.org/10.5194/acp-22-951-2022, https://doi.org/10.5194/acp-22-951-2022, 2022
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CrIS NH3 satellite observations are assimilated into the LOTOS-EUROS model using two different methods. In the first method the data are used to fit spatially varying NH3 emission time factors. In the second method a local ensemble transform Kalman filter is used. Compared to in situ observations, combining both methods led to the most significant improvements in the modeled concentrations and deposition, illustrating the usefulness of CrIS NH3 to improve the spatiotemporal distribution of NH3.
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Short summary
Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3...
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