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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Global maps of the NH3 emissions over 2019–2022 are derived using IASI NH3 spaceborne observations, the LMDZ-INCA chemistry transport model at 1.27°×2.5° resolution, and the mass-balance approach. The average global NH3 emissions over the period are ~97 Tg NH3 yr-1, which is significantly higher than three reference inventories. The analysis provides confidence in the seasonal variability and regional budgets and provides new insights into NH3 emissions at global and regional scales.
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EGUsphere, https://doi.org/10.5194/egusphere-2025-4659, https://doi.org/10.5194/egusphere-2025-4659, 2025
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Mixed-phase clouds play a key role in Earth’s climate but remain poorly represented in climate models. We improved their representation in the EC-Earth model by introducing an aerosol-sensitive scheme for ice formation and a machine-learning approach for secondary ice production. These advances produce more realistic cloud properties and radiative effects, highlighting that both processes are essential for reliable climate projections.
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EGUsphere, https://doi.org/10.5194/egusphere-2025-4120, https://doi.org/10.5194/egusphere-2025-4120, 2025
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Volatile organic compounds (VOCs) affect air quality and climate, but their behavior in the atmosphere is still uncertain. We launched a global research effort to compare how different models represent these compounds and to improve their accuracy. By analyzing model results alongside observations and satellite data, we aim to better understand the atmospheric composition of these compounds.
Lara Noppen, Lieven Clarisse, Frederik Tack, Thomas Ruhtz, Martin Van Damme, Michel Van Roozendael, Dirk Schuettemeyer, and Pierre Coheur
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Current infrared satellite sounders offer high spectral but low spatial resolution, limiting their ability to quantify atmospheric ammonia (NH3) at small scales. Through simulations and analysis of real data, we show that NH3 can be measured effectively from spectra with reduced resolution, either in a contiguous spectral range or in select well-chosen bands. This approach opens possibilities for the development of smaller dedicated instruments for observing NH3 at high spatial resolution.
Lorenzo Fabris, Nicolas Theys, Lieven Clarisse, Bruno Franco, Jonas Vlietinck, Huan Yu, Hugues Brenot, Thomas Danckaert, Pascal Hedelt, and Michel Van Roozendael
EGUsphere, https://doi.org/10.5194/egusphere-2025-4026, https://doi.org/10.5194/egusphere-2025-4026, 2025
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In this study, we developed an improved algorithm to retrieve the plume height and column density of sulfur dioxide emitted by volcanoes using data from the spectral band 2 of TROPOMI (S-5P). We tested its sensitivity to various conditions and applied it to real volcanic eruptions. Overall, our approach shows high precision, accuracy and sensitivity, and the results are consistent with other satellite measurements.
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
Atmos. Chem. Phys., 25, 9085–9111, https://doi.org/10.5194/acp-25-9085-2025, https://doi.org/10.5194/acp-25-9085-2025, 2025
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We show distinct seasonal and geographical patterns in the contributions of mineral dust, marine aerosol, and terrestrial biological particles to ice-nucleating particle (INP) concentrations that lead to atmospheric ice formation, a major source of uncertainty in climate projections. Bioaerosols are the major source of INPs at high temperatures, while mineral dust influences the global INP population at lower temperatures. These particles can satisfactorily reproduce INPs in a climate model.
Anam M. Khan, Olivia E. Clifton, Jesse O. Bash, Sam Bland, Nathan Booth, Philip Cheung, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christian Hogrefe, 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, Donna Schwede, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, Leiming Zhang, and Paul C. Stoy
Atmos. Chem. Phys., 25, 8613–8635, https://doi.org/10.5194/acp-25-8613-2025, https://doi.org/10.5194/acp-25-8613-2025, 2025
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Vegetation removes tropospheric ozone through stomatal uptake, and accurately modeling the stomatal uptake of ozone is important for modeling dry deposition and air quality. We evaluated the stomatal component of ozone dry deposition modeled by atmospheric chemistry models at six sites. We find that models and observation-based estimates agree at times during the growing season at all sites, but some models overestimated the stomatal component during the dry summers at a seasonally dry site.
Sijia Lou, Manish Shrivastava, Alexandre Albinet, Sophie Tomaz, Deepchandra Srivastava, Olivier Favez, Huizhong Shen, and Aijun Ding
Atmos. Chem. Phys., 25, 8163–8183, https://doi.org/10.5194/acp-25-8163-2025, https://doi.org/10.5194/acp-25-8163-2025, 2025
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Polycyclic aromatic hydrocarbons (PAHs), emitted from incomplete combustion, pose serious health risks due to their carcinogenic properties. This research demonstrates that viscous organic aerosol coatings significantly hinder PAH oxidation, with spatial distributions sensitive to the degradation modeling approach. Our findings emphasize the need for accurate modeling of PAH oxidation processes in risk assessments, considering both fresh and oxidized PAHs in evaluating human health risks.
Abdulamid A. Fakoya, Jens Redemann, Pablo E. Saide, Lan Gao, Logan T. Mitchell, Calvin Howes, Amie Dobracki, Ian Chang, Gonzalo A. Ferrada, Kristina Pistone, Samuel E. Leblanc, Michal Segal-Rozenhaimer, Arthur J. Sedlacek III, Thomas Eck, Brent Holben, Pawan Gupta, Elena Lind, Paquita Zuidema, Gregory Carmichael, and Connor J. Flynn
Atmos. Chem. Phys., 25, 7879–7902, https://doi.org/10.5194/acp-25-7879-2025, https://doi.org/10.5194/acp-25-7879-2025, 2025
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Tiny atmospheric particles from wildfire smoke impact the climate by interacting with sunlight and clouds, the extent of which is uncertain due to gaps in understanding how smoke changes over time. We developed a new method using remote sensing instruments to track how these particles evolve during atmospheric transport. Our results show that the ability of these particles to absorb sunlight increases as they travel. This discovery could help improve predictions of future climate scenarios.
Jinghao Zhai, Yin Zhang, Pengfei Liu, Yujie Zhang, Antai Zhang, Yaling Zeng, Baohua Cai, Jingyi Zhang, Chunbo Xing, Honglong Yang, Xiaofei Wang, Jianhuai Ye, Chen Wang, Tzung-May Fu, Lei Zhu, Huizhong Shen, Shu Tao, and Xin Yang
Atmos. Chem. Phys., 25, 7959–7972, https://doi.org/10.5194/acp-25-7959-2025, https://doi.org/10.5194/acp-25-7959-2025, 2025
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Our study shows that the optical properties of brown carbon depend on its source. Brown carbon from ozone pollution had the weakest light absorption but the strongest wavelength dependence, while biomass burning brown carbon showed the strongest absorption and the weakest wavelength dependence. Nitrogen-containing organic carbon compounds were identified as key light absorbers. These results improve understanding of brown carbon sources and help refine climate models.
Benjamin C. Sapper, Sean Youn, Daven K. Henze, Manjula Canagaratna, Harald Stark, and Jose L. Jimenez
Geosci. Model Dev., 18, 2891–2919, https://doi.org/10.5194/gmd-18-2891-2025, https://doi.org/10.5194/gmd-18-2891-2025, 2025
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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 error-weighted PMF that drastically reduces the computational costs of previously developed algorithms. We use this technique to deliver interpretable factors and solution diagnostics from an atmospheric chemistry dataset.
Petra Bauerová, Josef Keder, Adriana Šindelářová, Ondřej Vlček, William Patiño, Pavel Krč, Jan Geletič, Hynek Řezníček, Martin Bureš, Kryštof Eben, Michal Belda, Jelena Radović, Vladimír Fuka, Radek Jareš, Igor Esau, and Jaroslav Resler
Atmos. Chem. Phys., 25, 4477–4504, https://doi.org/10.5194/acp-25-4477-2025, https://doi.org/10.5194/acp-25-4477-2025, 2025
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The study explored urban air quality in Prague using low-cost sensors and highlighted the multivariate adaptive regression splines (MARS) correction method's effectiveness in enhancing accuracy. Results showed traffic's impact on nitrogen dioxide levels and atmospheric dynamics on particulate matter. The research confirmed MARS-corrected sensors as cost-effective for monitoring, despite challenges like sensor ageing and data quality control.
Sara L. Farrell, Havala O. T. Pye, Robert Gilliam, George Pouliot, Deanna Huff, Golam Sarwar, William Vizuete, Nicole Briggs, Fengkui Duan, Tao Ma, Shuping Zhang, and Kathleen Fahey
Atmos. Chem. Phys., 25, 3287–3312, https://doi.org/10.5194/acp-25-3287-2025, https://doi.org/10.5194/acp-25-3287-2025, 2025
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In this work we implement heterogeneous sulfur chemistry into the Community Multiscale Air Quality (CMAQ) model. This new chemistry accounts for the formation of sulfate via aqueous oxidation of SO2 in aerosol liquid water and the formation of hydroxymethanesulfonate (HMS) – often confused by measurement techniques as sulfate. Model performance in predicting sulfur PM2.5 in Fairbanks, Alaska, and other places that experience dark and cold winters is improved.
Paul A. Makar, Philip Cheung, Christian Hogrefe, Ayodeji Akingunola, Ummugulsum Alyuz, Jesse O. Bash, Michael D. Bell, Roberto Bellasio, Roberto Bianconi, Tim Butler, Hazel Cathcart, Olivia E. Clifton, Alma Hodzic, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Jason A. Lynch, Kester Momoh, Juan L. Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Thomas Scheuschner, Mark W. Shephard, Ranjeet S. Sokhi, and Stefano Galmarini
Atmos. Chem. Phys., 25, 3049–3107, https://doi.org/10.5194/acp-25-3049-2025, https://doi.org/10.5194/acp-25-3049-2025, 2025
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The large range of sulfur and nitrogen deposition estimates from air quality models results in a large range of predicted impacts. We used models and deposition diagnostics to identify the processes controlling atmospheric sulfur and nitrogen deposition variability. Controlling factors included the uptake of gases and aerosols by hydrometeors, aerosol inorganic chemistry, particle dry deposition, ammonia bidirectional fluxes, gas deposition via plant cuticles and soil, and land use data.
Yuzhi Jin, Jiandong Wang, Chao Liu, David C. Wong, Golam Sarwar, Kathleen M. Fahey, Shang Wu, Jiaping Wang, Jing Cai, Zeyuan Tian, Zhouyang Zhang, Jia Xing, Aijun Ding, and Shuxiao Wang
Atmos. Chem. Phys., 25, 2613–2630, https://doi.org/10.5194/acp-25-2613-2025, https://doi.org/10.5194/acp-25-2613-2025, 2025
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Black carbon (BC) affects climate and the environment, and its aging process alters its properties. Current models, like WRF-CMAQ, lack full accounting for it. We developed the WRF-CMAQ-BCG model to better represent BC aging by introducing bare and coated BC species and their conversion. The WRF-CMAQ-BCG model introduces the capability to simulate BC mixing states and bare and coated BC wet deposition, and it improves the accuracy of BC mass concentration and aerosol optics.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Min Huang, Gregory R. Carmichael, 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
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use 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 pollutant budgets in this area as local anthropogenic emissions drop.
Alexandros Milousis, Klaus Klingmüller, Alexandra P. Tsimpidi, Jasper F. Kok, Maria Kanakidou, Athanasios Nenes, and Vlassis A. Karydis
Atmos. Chem. Phys., 25, 1333–1351, https://doi.org/10.5194/acp-25-1333-2025, https://doi.org/10.5194/acp-25-1333-2025, 2025
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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 m−2, respectively, mainly affecting the shortwave spectrum. Sensitivity simulations evaluated the influence of mineral dust composition and emissions on the results.
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 Dieudonné, 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
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled 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.
Hyerim Kim, Xi Chen, Jun Wang, Zhendong Lu, Meng Zhou, Gregory R. Carmichael, Sang Seo Park, and Jhoon Kim
Atmos. Meas. Tech., 18, 327–349, https://doi.org/10.5194/amt-18-327-2025, https://doi.org/10.5194/amt-18-327-2025, 2025
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We compare passive aerosol layer height (ALH) retrievals from the Earth Polychromatic Imaging Camera (EPIC), TROPOspheric Monitoring Instrument (TROPOMI), and Geostationary Environment Monitoring Spectrometer (GEMS) with lidar. GEMS shows a lower correlation (R = 0.64) than EPIC and TROPOMI (R > 0.7) but with minimal bias (0.1 km vs. overestimated by ~0.8 km). GEMS performance is improved for an ultraviolet aerosol index ≥ 3. EPIC and GEMS ALH diurnal variation differs slightly.
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
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In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
T. Nash Skipper, Christian Hogrefe, Barron H. Henderson, Rohit Mathur, Kristen M. Foley, and Armistead G. Russell
Geosci. Model Dev., 17, 8373–8397, https://doi.org/10.5194/gmd-17-8373-2024, https://doi.org/10.5194/gmd-17-8373-2024, 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 and 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.
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
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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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, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O'Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
Atmos. Chem. Phys., 24, 12749–12773, https://doi.org/10.5194/acp-24-12749-2024, https://doi.org/10.5194/acp-24-12749-2024, 2024
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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 2 different years, we characterize emissions and evolutions of up to 8 h of PM2.5 mass, black carbon (BC), and brown carbon (BrC) in smoke from burning of forested lands in the southeastern USA.
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
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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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 explain the weaker hourly variation in NO2 columns than at the surface.
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
Geosci. Model Dev., 17, 7513–7537, https://doi.org/10.5194/gmd-17-7513-2024, https://doi.org/10.5194/gmd-17-7513-2024, 2024
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Detailed modeling of urban air quality in stable conditions is a challenge. We show the unprecedented sensitivity of a large eddy simulation (LES) model to meteorological boundary conditions and model parameters in an urban environment under stable conditions. We demonstrate the crucial role of boundary conditions for the comparability of results with observations. The study reveals a strong sensitivity of the results to model parameters and model numerical instabilities during such conditions.
Jiemei Liu, Jesper H. Christensen, Zhuyun Ye, Shikui Dong, Camilla Geels, Jørgen Brandt, Athanasios Nenes, Yuan Yuan, and Ulas Im
Atmos. Chem. Phys., 24, 10849–10867, https://doi.org/10.5194/acp-24-10849-2024, https://doi.org/10.5194/acp-24-10849-2024, 2024
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China was chosen as an example to conduct a quantitative analysis using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from the Weather Research and Forecasting (WRF) model. Meteorological conditions and emission inventories contributed 46 % (65 %) and 54 % (35 %) to the variations in PM2.5 concentrations (oxidative potential – OP), respectively, highlighting secondary aerosol formation and biomass burning as the primary contributors to PM2.5 and OP levels.
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
Geosci. Model Dev., 17, 6903–6927, https://doi.org/10.5194/gmd-17-6903-2024, https://doi.org/10.5194/gmd-17-6903-2024, 2024
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Aerosol–cloud interactions occur at a range of spatio-temporal scales. While evaluating recent developments in EC-Earth3-AerChem, this study aims to understand the extent to which the Twomey effect manifests itself at larger scales. We find a reduction in the warm bias over the Southern Ocean due to model improvements. While we see footprints of the Twomey effect at larger scales, the negative relationship between cloud droplet number and liquid water drives the shortwave radiative effect.
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 Papayannis, Konstantinos Eleftheridadis, Ottmar Möhler, and Athanasios Nenes
Atmos. Chem. Phys., 24, 9939–9974, https://doi.org/10.5194/acp-24-9939-2024, https://doi.org/10.5194/acp-24-9939-2024, 2024
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Ice nucleating particle (INP) concentrations are required for correct predictions of clouds and precipitation in a changing climate, but they are poorly constrained in climate models. We unravel source contributions to INPs in the eastern Mediterranean and find that biological particles are important, regardless of their origin. The parameterizations developed exhibit superior performance and enable models to consider biological-particle effects on INPs.
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
Atmos. Chem. Phys., 24, 9827–9842, https://doi.org/10.5194/acp-24-9827-2024, https://doi.org/10.5194/acp-24-9827-2024, 2024
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Analysis of modeling, in situ, and remote sensing measurements reveals the microphysical state of orographic clouds and their response to aerosol from the boundary layer and free troposphere. We show that cloud response 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 allows for novel model constraints and remote sensing products.
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
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Irene C. Dedoussi, Daven K. Henze, Sebastian D. Eastham, Raymond L. Speth, and Steven R. H. Barrett
Geosci. Model Dev., 17, 5689–5703, https://doi.org/10.5194/gmd-17-5689-2024, https://doi.org/10.5194/gmd-17-5689-2024, 2024
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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.
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.
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).
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.
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.
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.
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.
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.
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.
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.
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.
Cited articles
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Bash, J. O., Cooter, E. J., Dennis, R. L., Walker, J. T., and Pleim, J. E.: Evaluation of a regional air-quality model with bidirectional NH3 exchange coupled to an agroecosystem model, Biogeosciences, 10, 1635–1645, https://doi.org/10.5194/bg-10-1635-2013, 2013.
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Clarisse, L., Van Damme, M., Clerbaux, C., and Coheur, P.-F.: Tracking down global NH3 point sources with wind-adjusted superresolution, Atmos. Meas. Tech., 12, 5457–5473, https://doi.org/10.5194/amt-12-5457-2019, 2019.
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Cooter, E. J., Bash, J. O., Benson, V., and Ran, L.: Linking agricultural crop management and air quality models for regional to national-scale nitrogen assessments, Biogeosciences, 9, 4023–4035, https://doi.org/10.5194/bg-9-4023-2012, 2012.
Dammers, E., Palm, M., Van Damme, M., Vigouroux, C., Smale, D., Conway, S., Toon, G. C., Jones, N., Nussbaumer, E., Warneke, T., Petri, C., Clarisse, L., Clerbaux, C., Hermans, C., Lutsch, E., Strong, K., Hannigan, J. W., Nakajima, H., Morino, I., Herrera, B., Stremme, W., Grutter, M., Schaap, M., Wichink Kruit, R. J., Notholt, J., Coheur, P.-F., and Erisman, J. W.: An evaluation of IASI-NH3 with ground-based Fourier transform infrared spectroscopy measurements, Atmos. Chem. Phys., 16, 10351–10368, https://doi.org/10.5194/acp-16-10351-2016, 2016.
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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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