Research article
24 Aug 2018
Research article
| 24 Aug 2018
Effectiveness of ammonia reduction on control of fine particle nitrate
Hongyu Guo et al.
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources, but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
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We use the WRF-Chem model with new implementations of GOES-16 fire radiative power (FRP) based wildfire emissions and plume-rise to interpret aerosol observations during the 2019 NASA-NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
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Wildfires emit aerosol particles containing brown carbon material that affects visibility, global climate, and are toxic. Brown carbon is poorly characterized due to measurement limitations and their evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, T. Nash Skipper, and Armistead G. Russell
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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.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
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Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
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Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
Pamela Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-309, https://doi.org/10.5194/acp-2022-309, 2022
Preprint under review for ACP
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources, but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
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.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip Thomas Michael Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-239, https://doi.org/10.5194/acp-2022-239, 2022
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This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model-measurements discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
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.
Aditya Kumar, R. Bradley Pierce, Ravan Ahmadov, Gabriel Pereira, Saulo Freitas, Georg Grell, Chris Schmidt, Allen Lenzen, Joshua P. Schwarz, Anne E. Perring, Joseph M. Katich, John Hair, Jose L. Jimenez, Pedro Campuzano-Jost, and Hongyu Guo
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-33, https://doi.org/10.5194/acp-2022-33, 2022
Preprint under review for ACP
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We use the WRF-Chem model with new implementations of GOES-16 fire radiative power (FRP) based wildfire emissions and plume-rise to interpret aerosol observations during the 2019 NASA-NOAA FIREX-AQ field campaign and perform model evaluations. The model shows significant improvements in simulating the variety of aerosol loading environments sampled during FIREX-AQ. Our results also highlight the importance of accurate wildfire diurnal cycle and aerosol chemical mechanisms in models.
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.
Zhi-Hui Zhang, Elena Hartner, Battist Utinger, Benjamin Gfeller, Andreas Paul, Martin Sklorz, Hendryk Czech, Bin Xia Yang, Xin Yi Su, Gert Jakobi, Jürgen Orasche, Jürgen Schnelle-Kreis, Seongho Jeong, Thomas Gröger, Michal Pardo, Thorsten Hohaus, Thomas Adam, Astrid Kiendler-Scharr, Yinon Rudich, Ralf Zimmermann, and Markus Kalberer
Atmos. Chem. Phys., 22, 1793–1809, https://doi.org/10.5194/acp-22-1793-2022, https://doi.org/10.5194/acp-22-1793-2022, 2022
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Using a novel setup, we comprehensively characterized the formation of particle-bound reactive oxygen species (ROS) in anthropogenic and biogenic secondary organic aerosols (SOAs). We found that more than 90 % of all ROS components in both SOA types have a short lifetime. Our results also show that photochemical aging promotes particle-bound ROS production and enhances the oxidative potential of the aerosols. We found consistent results between chemical-based and biological-based ROS analyses.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-85, https://doi.org/10.5194/acp-2022-85, 2022
Preprint under review for ACP
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The oxidation of limonene, a common volatile emitted by trees and by chemical products, by NO3, an nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10–30 compounds. Many HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted a major fraction. Their formation can be explained the chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
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. Discuss., https://doi.org/10.5194/acp-2021-1000, https://doi.org/10.5194/acp-2021-1000, 2022
Preprint under review for ACP
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Widespread biomass burning (BB) events occur annually in Africa, which contribute about one-third of global BB emissions. These emissions contain a large family of light-absorbing organics, known as brown carbon (BrC), whose absorption of incident solar radiation is difficult to estimate, leading to large uncertainties in the global radiative forcing estimation. This study quantified the BrC absorption of aged BB particles and highlighted the importance of absorbing iron in the meanwhile.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-70, https://doi.org/10.5194/acp-2022-70, 2022
Preprint under review for ACP
Short summary
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Wildfires emit aerosol particles containing brown carbon material that affects visibility, global climate, and are toxic. Brown carbon is poorly characterized due to measurement limitations and their evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
Douglas A. Day, Pedro Campuzano-Jost, Benjamin A. Nault, Brett B. Palm, Weiwei Hu, Hongyu Guo, Paul J. Wooldridge, Ronald C. Cohen, Kenneth S. Docherty, J. Alex Huffman, Suzane S. de Sá, Scot T. Martin, and Jose L. Jimenez
Atmos. Meas. Tech., 15, 459–483, https://doi.org/10.5194/amt-15-459-2022, https://doi.org/10.5194/amt-15-459-2022, 2022
Short summary
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Particle-phase nitrates are an important component of atmospheric aerosols and chemistry. In this paper, we systematically explore the application of aerosol mass spectrometry (AMS) to quantify the organic and inorganic nitrate fractions of aerosols in the atmosphere. While AMS has been used for a decade to quantify nitrates, methods are not standardized. We make recommendations for a more universal approach based on this analysis of a large range of field and laboratory observations.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-432, https://doi.org/10.5194/amt-2021-432, 2022
Preprint under review for AMT
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
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.
Ralf Tillmannn, Georgios I. Gkatzelis, Franz Rohrer, Benjamin Winter, Christian Wesolek, Tobias Schuldt, Anne Caroline Lange, Philipp Franke, Elmar Friese, Michael Decker, Robert Wegener, Morten Hundt, Oleg Aseev, and Astrid Kiendler-Scharr
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-360, https://doi.org/10.5194/amt-2021-360, 2021
Revised manuscript accepted for AMT
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We report in-situ measurements of air pollutant concentrations within the planetary boundary layer on board a Zeppelin in Germany. The low costs of commercial flights provide an affordable and efficient method to improve our understanding of changes in emissions in space and time. The experimental setup expands the capabilities of this platform and provides insights into primary and secondary pollution observations and planetary boundary layer dynamics which determine air quality significantly.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
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The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
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.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Linghan Zeng, Amy P. Sullivan, Rebecca A. Washenfelder, Jack Dibb, Eric Scheuer, Teresa L. Campos, Joseph M. Katich, Ezra Levin, Michael A. Robinson, and Rodney J. Weber
Atmos. Meas. Tech., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, https://doi.org/10.5194/amt-14-6357-2021, 2021
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Three online systems for measuring water-soluble brown carbon are compared. A mist chamber and two different particle-into-liquid samplers were deployed on separate research aircraft targeting wildfires and followed a similar detection method using a long-path liquid waveguide with a spectrometer to measure the light absorption from 300 to 700 nm. Detection limits, signal hysteresis and other sampling issues are compared, and further improvements of these liquid-based systems are provided.
Caroline Dang, Michal Segal-Rozenhaimer, Haochi Che, Lu Zhang, Paola Formenti, Jonathan Taylor, Amie Dobracki, Sara Purdue, Pui-Shan Wong, Athanios Nenes, Arthur Sedlacek, Hugh Coe, Jens Redemann, Paquita Zuidema, and James Haywood
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-724, https://doi.org/10.5194/acp-2021-724, 2021
Revised manuscript accepted for ACP
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We used TEM to analyze aged biomass burning aerosol from Africa. 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 change biomass burning aerosol through incorporation of sodium into particles. We found regions dominated by chloride particles without the presence of Na, and that marine salts are more processed when mixed with biomass burning plumes.
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.
Janne Lampilahti, Hanna E. Manninen, Tuomo Nieminen, Sander Mirme, Mikael Ehn, Iida Pullinen, Katri Leino, Siegfried Schobesberger, Juha Kangasluoma, Jenni Kontkanen, Emma Järvinen, Riikka Väänänen, Taina Yli-Juuti, Radovan Krejci, Katrianne Lehtipalo, Janne Levula, Aadu Mirme, Stefano Decesari, Ralf Tillmann, Douglas R. Worsnop, Franz Rohrer, Astrid Kiendler-Scharr, Tuukka Petäjä, Veli-Matti Kerminen, Thomas F. Mentel, and Markku Kulmala
Atmos. Chem. Phys., 21, 12649–12663, https://doi.org/10.5194/acp-21-12649-2021, https://doi.org/10.5194/acp-21-12649-2021, 2021
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We studied aerosol particle formation and growth in different parts of the planetary boundary layer at two different locations (Po Valley, Italy, and Hyytiälä, Finland). The observations consist of airborne measurements on board an instrumented Zeppelin and a small airplane combined with comprehensive ground-based measurements.
Luisa Hantschke, Anna Novelli, Birger Bohn, Changmin Cho, David Reimer, Franz Rohrer, Ralf Tillmann, Marvin Glowania, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, https://doi.org/10.5194/acp-21-12665-2021, 2021
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The reactions of Δ3-carene with ozone and the hydroxyl radical (OH) and the photolysis and OH reaction of caronaldehyde were investigated in the simulation chamber SAPHIR. Reaction rate constants of these reactions were determined. Caronaldehyde yields of the ozonolysis and OH reaction were determined. The organic nitrate yield of the reaction of Δ3-carene and caronaldehyde-derived peroxy radicals with NO was determined. The ROx budget (ROx = OH+HO2+RO2) was also investigated.
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
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.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
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.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, https://doi.org/10.5194/acp-21-9681-2021, 2021
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The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthropogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
Yuhan Yang, Dong Gao, and Rodney J. Weber
Atmos. Meas. Tech., 14, 4707–4719, https://doi.org/10.5194/amt-14-4707-2021, https://doi.org/10.5194/amt-14-4707-2021, 2021
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Iron and copper are commonly found in ambient aerosols and have been linked to adverse health effects. We describe a relatively simple benchtop instrument that can be used to quantify these metals in aqueous solutions and verify the method by comparison with inductively coupled plasma mass spectrometry. The approach is based on forming light-absorbing metal–ligand complexes that can be measured with high sensitivity utilizing a long-path liquid waveguide capillary cell.
Richard H. Moore, Elizabeth B. Wiggins, Adam T. Ahern, Stephen Zimmerman, Lauren Montgomery, Pedro Campuzano Jost, Claire E. Robinson, Luke D. Ziemba, Edward L. Winstead, Bruce E. Anderson, Charles A. Brock, Matthew D. Brown, Gao Chen, Ewan C. Crosbie, Hongyu Guo, Jose L. Jimenez, Carolyn E. Jordan, Ming Lyu, Benjamin A. Nault, Nicholas E. Rothfuss, Kevin J. Sanchez, Melinda Schueneman, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Nicholas L. Wagner, and Jian Wang
Atmos. Meas. Tech., 14, 4517–4542, https://doi.org/10.5194/amt-14-4517-2021, https://doi.org/10.5194/amt-14-4517-2021, 2021
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Atmospheric particles are everywhere and exist in a range of sizes, from a few nanometers to hundreds of microns. Because particle size determines the behavior of chemical and physical processes, accurately measuring particle sizes is an important and integral part of atmospheric field measurements! Here, we discuss the performance of two commonly used particle sizers and how changes in particle composition and optical properties may result in sizing uncertainties, which we quantify.
Djacinto Monteiro dos Santos, Luciana Varanda Rizzo, Samara Carbone, Patrick Schlag, and Paulo Artaxo
Atmos. Chem. Phys., 21, 8761–8773, https://doi.org/10.5194/acp-21-8761-2021, https://doi.org/10.5194/acp-21-8761-2021, 2021
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The metropolitan area of São Paulo (MASP), with very extensive biofuel use, has unique atmospheric chemistry among world megacities. In this study, we examine the complex relationships between aerosol chemical composition and particle size distribution. Our findings provide a better understanding of the dynamics of the physicochemical properties of submicron particles and highlight the key role of secondary organic aerosol formation in the pollution levels in São Paulo.
Marvin Glowania, Franz Rohrer, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Meas. Tech., 14, 4239–4253, https://doi.org/10.5194/amt-14-4239-2021, https://doi.org/10.5194/amt-14-4239-2021, 2021
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Three instruments that use different techniques to measure gaseous formaldehyde concentrations were compared in experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. The results demonstrated the need to correct the baseline in measurements by instruments that use the Hantzsch reaction or make use of cavity ring-down spectroscopy. After applying corrections, all three methods gave accurate and precise measurements within their specifications.
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.
Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Douglas A. Day, Jason C. Schroder, Dongwook Kim, Jack E. Dibb, Maximilian Dollner, Bernadett Weinzierl, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 3631–3655, https://doi.org/10.5194/amt-14-3631-2021, https://doi.org/10.5194/amt-14-3631-2021, 2021
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We utilize a set of high-quality datasets collected during the NASA Atmospheric Tomography Mission to investigate the impact of differences in observable particle sizes across aerosol instruments in aerosol measurement comparisons. Very good agreement was found between chemically and physically derived submicron aerosol volume. Results support a lack of significant unknown biases in the response of an Aerodyne aerosol mass spectrometer (AMS) when sampling remote aerosols across the globe.
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.
Clara Betancourt, Christoph Küppers, Tammarat Piansawan, Uta Sager, Andrea B. Hoyer, Heinz Kaminski, Gerhard Rapp, Astrid C. John, Miriam Küpper, Ulrich Quass, Thomas Kuhlbusch, Jochen Rudolph, Astrid Kiendler-Scharr, and Iulia Gensch
Atmos. Chem. Phys., 21, 5953–5964, https://doi.org/10.5194/acp-21-5953-2021, https://doi.org/10.5194/acp-21-5953-2021, 2021
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For the first time, we included stable isotopes in the Lagrangian particle dispersion model FLEXPART to investigate firewood home heating aerosol. This is an innovative source apportionment methodology since comparison of stable isotope ratio model predictions with observations delivers quantitative understanding of atmospheric processes. The main outcome of this study is that the home heating aerosol in residential areas was not of remote origin.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
Changmin Cho, Andreas Hofzumahaus, Hendrik Fuchs, Hans-Peter Dorn, Marvin Glowania, Frank Holland, Franz Rohrer, Vaishali Vardhan, Astrid Kiendler-Scharr, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 14, 1851–1877, https://doi.org/10.5194/amt-14-1851-2021, https://doi.org/10.5194/amt-14-1851-2021, 2021
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This study describes the implementation and characterization of the chemical modulation reactor (CMR) used in the laser-induced fluorescence instrument of the Forschungszentrum Jülich. The CMR allows for interference-free OH radical measurement in ambient air. During a field campaign in a rural environment, the observed interference was mostly below the detection limit of the instrument and fully explained by the known ozone interference.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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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.
Jens Redemann, Robert Wood, Paquita Zuidema, Sarah J. Doherty, Bernadette Luna, Samuel E. LeBlanc, Michael S. Diamond, Yohei Shinozuka, Ian Y. Chang, Rei Ueyama, Leonhard Pfister, Ju-Mee Ryoo, Amie N. Dobracki, Arlindo M. da Silva, Karla M. Longo, Meloë S. Kacenelenbogen, Connor J. Flynn, Kristina Pistone, Nichola M. Knox, Stuart J. Piketh, James M. Haywood, Paola Formenti, Marc Mallet, Philip Stier, Andrew S. Ackerman, Susanne E. Bauer, Ann M. Fridlind, Gregory R. Carmichael, Pablo E. Saide, Gonzalo A. Ferrada, Steven G. Howell, Steffen Freitag, Brian Cairns, Brent N. Holben, Kirk D. Knobelspiesse, Simone Tanelli, Tristan S. L'Ecuyer, Andrew M. Dzambo, Ousmane O. Sy, Greg M. McFarquhar, Michael R. Poellot, Siddhant Gupta, Joseph R. O'Brien, Athanasios Nenes, Mary Kacarab, Jenny P. S. Wong, Jennifer D. Small-Griswold, Kenneth L. Thornhill, David Noone, James R. Podolske, K. Sebastian Schmidt, Peter Pilewskie, Hong Chen, Sabrina P. Cochrane, Arthur J. Sedlacek, Timothy J. Lang, Eric Stith, Michal Segal-Rozenhaimer, Richard A. Ferrare, Sharon P. Burton, Chris A. Hostetler, David J. Diner, Felix C. Seidel, Steven E. Platnick, Jeffrey S. Myers, Kerry G. Meyer, Douglas A. Spangenberg, Hal Maring, and Lan Gao
Atmos. Chem. Phys., 21, 1507–1563, https://doi.org/10.5194/acp-21-1507-2021, https://doi.org/10.5194/acp-21-1507-2021, 2021
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Southern Africa produces significant biomass burning emissions whose impacts on regional and global climate are poorly understood. ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) is a 5-year NASA investigation designed to study the key processes that determine these climate impacts. The main purpose of this paper is to familiarize the broader scientific community with the ORACLES project, the dataset it produced, and the most important initial findings.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Georgia Sotiropoulou, Étienne Vignon, Gillian Young, Hugh Morrison, Sebastian J. O'Shea, Thomas Lachlan-Cope, Alexis Berne, and Athanasios Nenes
Atmos. Chem. Phys., 21, 755–771, https://doi.org/10.5194/acp-21-755-2021, https://doi.org/10.5194/acp-21-755-2021, 2021
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Summer clouds have a significant impact on the radiation budget of the Antarctic surface and thus on ice-shelf melting. However, these are poorly represented in climate models due to errors in their microphysical structure, including the number of ice crystals that they contain. We show that breakup from ice particle collisions can substantially magnify the ice crystal number concentration with significant implications for surface radiation. This process is currently missing in climate models.
Huan Song, Xiaorui Chen, Keding Lu, Qi Zou, Zhaofeng Tan, Hendrik Fuchs, Alfred Wiedensohler, Daniel R. Moon, Dwayne E. Heard, María-Teresa Baeza-Romero, Mei Zheng, Andreas Wahner, Astrid Kiendler-Scharr, and Yuanhang Zhang
Atmos. Chem. Phys., 20, 15835–15850, https://doi.org/10.5194/acp-20-15835-2020, https://doi.org/10.5194/acp-20-15835-2020, 2020
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Accurate calculation of the HO2 uptake coefficient is one of the key parameters to quantify the co-reduction of both aerosol and ozone pollution. We modelled various lab measurements of γHO2 based on a gas-liquid phase kinetic model and developed a state-of-the-art parameterized equation. Based on a dataset from a comprehensive field campaign in the North China Plain, we proposed that the determination of the heterogeneous uptake process for HO2 should be included in future field campaigns.
Johannes Quaas, Antti Arola, Brian Cairns, Matthew Christensen, Hartwig Deneke, Annica M. L. Ekman, Graham Feingold, Ann Fridlind, Edward Gryspeerdt, Otto Hasekamp, Zhanqing Li, Antti Lipponen, Po-Lun Ma, Johannes Mülmenstädt, Athanasios Nenes, Joyce E. Penner, Daniel Rosenfeld, Roland Schrödner, Kenneth Sinclair, Odran Sourdeval, Philip Stier, Matthias Tesche, Bastiaan van Diedenhoven, and Manfred Wendisch
Atmos. Chem. Phys., 20, 15079–15099, https://doi.org/10.5194/acp-20-15079-2020, https://doi.org/10.5194/acp-20-15079-2020, 2020
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Anthropogenic pollution particles – aerosols – serve as cloud condensation nuclei and thus increase cloud droplet concentration and the clouds' reflection of sunlight (a cooling effect on climate). This Twomey effect is poorly constrained by models and requires satellite data for better quantification. The review summarizes the challenges in properly doing so and outlines avenues for progress towards a better use of aerosol retrievals and better retrievals of droplet concentrations.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Hongyu Guo, Duseong S. Jo, Anne V. Handschy, Demetrios Pagonis, Jason C. Schroder, Melinda K. Schueneman, Michael J. Cubison, Jack E. Dibb, Alma Hodzic, Weiwei Hu, Brett B. Palm, and Jose L. Jimenez
Atmos. Meas. Tech., 13, 6193–6213, https://doi.org/10.5194/amt-13-6193-2020, https://doi.org/10.5194/amt-13-6193-2020, 2020
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Collecting particulate matter, or aerosols, onto filters to be analyzed offline is a widely used method to investigate the mass concentration and chemical composition of the aerosol, especially the inorganic portion. Here, we show that acidic aerosol (sulfuric acid) collected onto filters and then exposed to high ammonia mixing ratios (from human emissions) will lead to biases in the ammonium collected onto filters, and the uptake of ammonia is rapid (< 10 s), which impacts the filter data.
Michael Rolletter, Marion Blocquet, Martin Kaminski, Birger Bohn, Hans-Peter Dorn, Andreas Hofzumahaus, Frank Holland, Xin Li, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 13701–13719, https://doi.org/10.5194/acp-20-13701-2020, https://doi.org/10.5194/acp-20-13701-2020, 2020
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The photooxidation of pinonaldehyde is investigated in a chamber study under natural sunlight and low NO conditions with and without an added hydroxyl radical (OH) scavenger. The experimentally determined pinonaldehyde photolysis frequency is faster by a factor of 3.5 than currently used parameterizations in atmospheric models. Yields of degradation products are measured in the presence and absence of OH. Measurements are compared to current atmospheric models and a theory-based mechanism.
Ari Laaksonen, Jussi Malila, and Athanasios Nenes
Atmos. Chem. Phys., 20, 13579–13589, https://doi.org/10.5194/acp-20-13579-2020, https://doi.org/10.5194/acp-20-13579-2020, 2020
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Aerosol particles containing black carbon are ubiquitous in the atmosphere and originate from combustion processes. We examine their capability to act as condensation centers for water vapor. We make use of published experimental data sets for different types of black carbon particles, ranging from very pure particles to particles that contain both black carbon and water soluble organic matter, and we show that a recently developed theory reproduces most of the experimental results.
Lanxiadi Chen, Chao Peng, Wenjun Gu, Hanjing Fu, Xing Jian, Huanhuan Zhang, Guohua Zhang, Jianxi Zhu, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 20, 13611–13626, https://doi.org/10.5194/acp-20-13611-2020, https://doi.org/10.5194/acp-20-13611-2020, 2020
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We investigated hygroscopic properties of a number of mineral dust particles in a quantitative manner, via measuring the sample mass at different relative humidities. The robust and comprehensive data obtained would significantly improve our knowledge of hygroscopicity of mineral dust and its impacts on atmospheric chemistry and climate.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Iida Pullinen, Sebastian Schmitt, Sungah Kang, Mehrnaz Sarrafzadeh, Patrick Schlag, Stefanie Andres, Einhard Kleist, Thomas F. Mentel, Franz Rohrer, Monika Springer, Ralf Tillmann, Jürgen Wildt, Cheng Wu, Defeng Zhao, Andreas Wahner, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 20, 10125–10147, https://doi.org/10.5194/acp-20-10125-2020, https://doi.org/10.5194/acp-20-10125-2020, 2020
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Biogenic and anthropogenic air masses mix in the atmosphere, bringing plant-emitted monoterpenes and traffic-related nitrogen oxides together. There is debate whether the presence of nitrogen oxides reduces or increases secondary aerosol formation. This is important as secondary aerosols have cooling effects in the climate system but also constitute a health risk in populated areas. We show that the presence of NOx alone should not much affect the mass yields of secondary organic aerosols.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Shunliu Zhao, Matthew G. Russell, Amir Hakami, Shannon L. Capps, Matthew D. Turner, Daven K. Henze, Peter B. Percell, Jaroslav Resler, Huizhong Shen, Armistead G. Russell, Athanasios Nenes, Amanda J. Pappin, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Charles O. Stanier, and Tianfeng Chai
Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, https://doi.org/10.5194/gmd-13-2925-2020, 2020
Jian Xu, Jia Chen, Na Zhao, Guochen Wang, Guangyuan Yu, Hao Li, Juntao Huo, Yanfen Lin, Qingyan Fu, Hongyu Guo, Congrui Deng, Shan-Hu Lee, Jianmin Chen, and Kan Huang
Atmos. Chem. Phys., 20, 7259–7269, https://doi.org/10.5194/acp-20-7259-2020, https://doi.org/10.5194/acp-20-7259-2020, 2020
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This study provided evidence that gas-particle partitioning of ammonia, as opposed to ammonia concentration, plays a critical role in the haze formation. A reduction in ammonia emissions alone may not reduce air pollution effectively, at least at rural agricultural sites in China.
Dong Gao, Krystal J. Godri Pollitt, James A. Mulholland, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 20, 5197–5210, https://doi.org/10.5194/acp-20-5197-2020, https://doi.org/10.5194/acp-20-5197-2020, 2020
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This study provides a direct intercomparison between two assays for quantifying oxidative potential (OP) of ambient particles: the synthetic respiratory-tract-lining fluid (RTLF) assay and the dithiothreitol (DTT) assay. The results suggest that the DTT assay and the ascorbic acid depletion in RTLF are associated with organic species, transition metal ions, and antagonistic interactions between species. The glutathione depletion in RTLF is strongly dependent on water-soluble copper.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Anna Novelli, Luc Vereecken, Birger Bohn, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, David Reimer, Franz Rohrer, Simon Rosanka, Domenico Taraborrelli, Ralf Tillmann, Robert Wegener, Zhujun Yu, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 20, 3333–3355, https://doi.org/10.5194/acp-20-3333-2020, https://doi.org/10.5194/acp-20-3333-2020, 2020
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Experimental evidence from a simulation chamber study shows that the regeneration efficiency of the hydroxyl radical is maintained globally at values higher than 0.5 for a wide range of nitrogen oxide concentrations as a result of isomerizations of peroxy radicals originating from the OH oxidation of isoprene. The available models were tested, and suggestions on how to improve their ability to reproduce the measured radical and oxygenated volatile organic compound concentrations are provided.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Mary Kacarab, K. Lee Thornhill, Amie Dobracki, Steven G. Howell, Joseph R. O'Brien, Steffen Freitag, Michael R. Poellot, Robert Wood, Paquita Zuidema, Jens Redemann, and Athanasios Nenes
Atmos. Chem. Phys., 20, 3029–3040, https://doi.org/10.5194/acp-20-3029-2020, https://doi.org/10.5194/acp-20-3029-2020, 2020
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We find that extensive biomass burning aerosol plumes from southern Africa can profoundly influence clouds in the southeastern Atlantic. Concurrent variations in vertical velocity, however, are found to magnify the relationship between boundary layer aerosol and the cloud droplet number. Neglecting these covariances may strongly bias the sign and magnitude of aerosol impacts on the cloud droplet number.
Yu Wang, Ying Chen, Zhijun Wu, Dongjie Shang, Yuxuan Bian, Zhuofei Du, Sebastian H. Schmitt, Rong Su, Georgios I. Gkatzelis, Patrick Schlag, Thorsten Hohaus, Aristeidis Voliotis, Keding Lu, Limin Zeng, Chunsheng Zhao, M. Rami Alfarra, Gordon McFiggans, Alfred Wiedensohler, Astrid Kiendler-Scharr, Yuanhang Zhang, and Min Hu
Atmos. Chem. Phys., 20, 2161–2175, https://doi.org/10.5194/acp-20-2161-2020, https://doi.org/10.5194/acp-20-2161-2020, 2020
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Severe haze events, with high particulate nitrate (pNO3−) burden, frequently prevail in Beijing. In this study, we demonstrate a mutual-promotion effect between aerosol water uptake and pNO3− formation backed up by theoretical calculations and field observations throughout a typical pNO3−-dominated haze event in Beijing wintertime. This self-amplified mutual-promotion effect between aerosol water content and particulate nitrate can rapidly deteriorate air quality and degrade visibility.
Aoxing Zhang, Yuhang Wang, Yuzhong Zhang, Rodney J. Weber, Yongjia Song, Ziming Ke, and Yufei Zou
Atmos. Chem. Phys., 20, 1901–1920, https://doi.org/10.5194/acp-20-1901-2020, https://doi.org/10.5194/acp-20-1901-2020, 2020
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Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosols. We developed a module to simulate the emissions, atmospheric processing and direct radiative effect of BrC in the Community Earth System Model (CESM). We found that globally BrC is a significant absorber and is more centered in the tropical free troposphere compared to BC. The contribution of BrC heating to the Hadley circulation and latitudinal expansion of the tropics is comparable to BC heating.
Arnaldo Negron, Natasha DeLeon-Rodriguez, Samantha M. Waters, Luke D. Ziemba, Bruce Anderson, Michael Bergin, Konstantinos T. Konstantinidis, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1817–1838, https://doi.org/10.5194/acp-20-1817-2020, https://doi.org/10.5194/acp-20-1817-2020, 2020
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Airborne biological particles impact human health, cloud formation, and ecosystems, but few techniques are available to characterize their atmospheric abundance. Combining a newly developed high-volume sampling/flow cytometry technique together with an laser-induced fluorescence instrument, we detect a highly dynamic bioaerosol community over urban Atlanta, composed of pollen, fungi, and bacteria with low and high nucleic acid content.
Georgia Sotiropoulou, Sylvia Sullivan, Julien Savre, Gary Lloyd, Thomas Lachlan-Cope, Annica M. L. Ekman, and Athanasios Nenes
Atmos. Chem. Phys., 20, 1301–1316, https://doi.org/10.5194/acp-20-1301-2020, https://doi.org/10.5194/acp-20-1301-2020, 2020
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Arctic clouds constitute a large source of uncertainty in predictions of future climate. Observations indicate that the number concentration of cloud ice crystals exceeds the concentration of aerosols that can act as ice-nucleating particles (INPs). We show that ice multiplication due to mechanical break-up upon collisions between the few primary ice crystals (formed from INPs) can explain the discrepancy. Including a description of the process in climate models can improve cloud representation.
Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Michael Rolletter, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 19, 11635–11649, https://doi.org/10.5194/acp-19-11635-2019, https://doi.org/10.5194/acp-19-11635-2019, 2019
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Here we present a study of the photooxidation of alpha-pinene, the most abundant monoterpene, by hydroxyl radicals (OH) conducted in the simulation chamber SAPHIR under low NOx and atmospheric alpha-pinene concentrations. Yields of the main degradation products acetone, formaldehyde, and pinonaldehyde were determined and the HOx (OH + HO2) radical budget was investigated. Measurements were used to test current atmospheric models and a theory-based mechanism.
Eleni Marinou, Matthias Tesche, Athanasios Nenes, Albert Ansmann, Jann Schrod, Dimitra Mamali, Alexandra Tsekeri, Michael Pikridas, Holger Baars, Ronny Engelmann, Kalliopi-Artemis Voudouri, Stavros Solomos, Jean Sciare, Silke Groß, Florian Ewald, and Vassilis Amiridis
Atmos. Chem. Phys., 19, 11315–11342, https://doi.org/10.5194/acp-19-11315-2019, https://doi.org/10.5194/acp-19-11315-2019, 2019
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We assess the feasibility of ground-based and spaceborne lidars to retrieve profiles of cloud-relevant aerosol concentrations and ice-nucleating particles. The retrieved profiles are in good agreement with airborne in situ measurements. Our methodology will be applied to satellite observations in the future so as to provide a global 3D product of cloud-relevant properties.
George S. Fanourgakis, Maria Kanakidou, Athanasios Nenes, Susanne E. Bauer, Tommi Bergman, Ken S. Carslaw, Alf Grini, Douglas S. Hamilton, Jill S. Johnson, Vlassis A. Karydis, Alf Kirkevåg, John K. Kodros, Ulrike Lohmann, Gan Luo, Risto Makkonen, Hitoshi Matsui, David Neubauer, Jeffrey R. Pierce, Julia Schmale, Philip Stier, Kostas Tsigaridis, Twan van Noije, Hailong Wang, Duncan Watson-Parris, Daniel M. Westervelt, Yang Yang, Masaru Yoshioka, Nikos Daskalakis, Stefano Decesari, Martin Gysel-Beer, Nikos Kalivitis, Xiaohong Liu, Natalie M. Mahowald, Stelios Myriokefalitakis, Roland Schrödner, Maria Sfakianaki, Alexandra P. Tsimpidi, Mingxuan Wu, and Fangqun Yu
Atmos. Chem. Phys., 19, 8591–8617, https://doi.org/10.5194/acp-19-8591-2019, https://doi.org/10.5194/acp-19-8591-2019, 2019
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Effects of aerosols on clouds are important for climate studies but are among the largest uncertainties in climate projections. This study evaluates the skill of global models to simulate aerosol, cloud condensation nuclei (CCN) and cloud droplet number concentrations (CDNCs). Model results show reduced spread in CDNC compared to CCN due to the negative correlation between the sensitivities of CDNC to aerosol number concentration (air pollution) and updraft velocity (atmospheric dynamics).
Jenny P. S. Wong, Maria Tsagkaraki, Irini Tsiodra, Nikolaos Mihalopoulos, Kalliopi Violaki, Maria Kanakidou, Jean Sciare, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, https://doi.org/10.5194/acp-19-7319-2019, 2019
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Biomass burning is a major source of light-absorbing organic species in atmospheric aerosols, and it can play an important role in climate and atmospheric chemistry. Through a combination of laboratory experiments and field observations, this work demonstrated that the light absorption properties of aged biomass burning organic aerosols are dominated by high-molecular-weight compounds. In addition, we found that total hydrated sugars may be a robust tracer for aged biomass burning aerosols.
Zhaofeng Tan, Keding Lu, Andreas Hofzumahaus, Hendrik Fuchs, Birger Bohn, Frank Holland, Yuhan Liu, Franz Rohrer, Min Shao, Kang Sun, Yusheng Wu, Limin Zeng, Yinsong Zhang, Qi Zou, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 19, 7129–7150, https://doi.org/10.5194/acp-19-7129-2019, https://doi.org/10.5194/acp-19-7129-2019, 2019
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Atmospheric OH, HO2, and RO2 radicals; OH reactivity; and trace gases measured in the Pearl River Delta in autumn 2014 are used for radical budget analyses. The RO2 budget suggests that unexplained OH reactivity is due to unmeasured volatile organic compounds. The OH budget points to a missing OH source and that of RO2 to a missing RO2 sink at low NO. This could indicate a common, unknown process that converts RO2 to OH without the involvement of NO, which would reduce ozone production by 30 %.
Panayiotis Kalkavouras, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Maria Tombrou, Athanasios Nenes, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 6185–6203, https://doi.org/10.5194/acp-19-6185-2019, https://doi.org/10.5194/acp-19-6185-2019, 2019
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We study how new particle formation (NPF) events affect clouds throughout the year at a ground site in the E Mediterranean. Using a new tools and evaluation metrics, NPF is found to affect only evening and nocturnal clouds by modestly increasing droplet number by 7 to 12 %. A conventional analysis based on CCN concentration at prescribed supersaturation levels or aerosol size can considerably bias the perceived influence of NPF events on regional clouds, the hydrological cycle, and climate.
Nønne L. Prisle, Jack J. Lin, Sara Purdue, Haisheng Lin, J. Carson Meredith, and Athanasios Nenes
Atmos. Chem. Phys., 19, 4741–4761, https://doi.org/10.5194/acp-19-4741-2019, https://doi.org/10.5194/acp-19-4741-2019, 2019
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We measure surface activity and cloud-forming potential of pollenkitt, an organic mixture coating pollen grains. Cloud droplet formation is affected through both surface tension and bulk depletion, with a consistent particle size-dependent signature. We observe nonideal solution effects in pollenkitt mixtures with ammonium sulfate salt. Our results suggest sensitivity of general water interactions, including cloud formation by pollen and their fragments, to both atmospheric humidity and aging.
Hongyu Guo, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 18, 17307–17323, https://doi.org/10.5194/acp-18-17307-2018, https://doi.org/10.5194/acp-18-17307-2018, 2018
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Overprediction of fine-particle ammonium-sulfate molar ratios (R) by thermodynamic models is suggested as evidence for organic aerosol limiting the condensation of ammonia onto particles, with significant impacts on aerosol chemistry. We find that the effects of small amounts of salt and dust, combined with measurement artifacts, explain the discrepancy in R. These results are highly insensitive to mixing state. This means that aerosol predictions are much more robust than thought before.
Sylvia C. Sullivan, Christian Barthlott, Jonathan Crosier, Ilya Zhukov, Athanasios Nenes, and Corinna Hoose
Atmos. Chem. Phys., 18, 16461–16480, https://doi.org/10.5194/acp-18-16461-2018, https://doi.org/10.5194/acp-18-16461-2018, 2018
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Ice crystal formation in clouds can occur via thermodynamic nucleation, but also via mechanical collisions between pre-existing crystals or co-existing droplets. When descriptions of this mechanical ice generation are implemented into the COSMO weather model, we find that the contributions to crystal number from thermodynamic and mechanical processes are of the same order. Mechanical ice generation also intensifies differences in precipitation intensity between dynamic and quiescent regions.
Stelios Myriokefalitakis, Akinori Ito, Maria Kanakidou, Athanasios Nenes, Maarten C. Krol, Natalie M. Mahowald, Rachel A. Scanza, Douglas S. Hamilton, Matthew S. Johnson, Nicholas Meskhidze, Jasper F. Kok, Cecile Guieu, Alex R. Baker, Timothy D. Jickells, Manmohan M. Sarin, Srinivas Bikkina, Rachel Shelley, Andrew Bowie, Morgane M. G. Perron, and Robert A. Duce
Biogeosciences, 15, 6659–6684, https://doi.org/10.5194/bg-15-6659-2018, https://doi.org/10.5194/bg-15-6659-2018, 2018
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The first atmospheric iron (Fe) deposition model intercomparison is presented in this study, as a result of the deliberations of the United Nations Joint Group of Experts on the Scientific Aspects of Marine Environmental Protection (GESAMP; http://www.gesamp.org/) Working Group 38. We conclude that model diversity over remote oceans reflects uncertainty in the Fe content parameterizations of dust aerosols, combustion aerosol emissions and the size distribution of transported aerosol Fe.
Sara Bacer, Sylvia C. Sullivan, Vlassis A. Karydis, Donifan Barahona, Martina Krämer, Athanasios Nenes, Holger Tost, Alexandra P. Tsimpidi, Jos Lelieveld, and Andrea Pozzer
Geosci. Model Dev., 11, 4021–4041, https://doi.org/10.5194/gmd-11-4021-2018, https://doi.org/10.5194/gmd-11-4021-2018, 2018
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The complexity of ice nucleation mechanisms and aerosol--ice interactions makes their representation still challenging in atmospheric models. We have implemented a comprehensive ice crystal formation parameterization in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations. The newly implemented parameterization takes into account processes which were previously neglected by the standard version of the model.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Jorge Saturno, Bruna A. Holanda, Christopher Pöhlker, Florian Ditas, Qiaoqiao Wang, Daniel Moran-Zuloaga, Joel Brito, Samara Carbone, Yafang Cheng, Xuguang Chi, Jeannine Ditas, Thorsten Hoffmann, Isabella Hrabe de Angelis, Tobias Könemann, Jošt V. Lavrič, Nan Ma, Jing Ming, Hauke Paulsen, Mira L. Pöhlker, Luciana V. Rizzo, Patrick Schlag, Hang Su, David Walter, Stefan Wolff, Yuxuan Zhang, Paulo Artaxo, Ulrich Pöschl, and Meinrat O. Andreae
Atmos. Chem. Phys., 18, 12817–12843, https://doi.org/10.5194/acp-18-12817-2018, https://doi.org/10.5194/acp-18-12817-2018, 2018
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Biomass burning emits light-absorbing aerosol particles that warm the atmosphere. One of them is the primarily emitted black carbon, which strongly absorbs radiation in the visible and UV spectral regions. Another one is the so-called brown carbon, a fraction of organic aerosol particles that are able to absorb radiation, especially in the UV spectral region. The contribution of both kinds of aerosol particles to light absorption over the Amazon rainforest is studied in this paper.
Petros Vasilakos, Armistead Russell, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys., 18, 12765–12775, https://doi.org/10.5194/acp-18-12765-2018, https://doi.org/10.5194/acp-18-12765-2018, 2018
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In this work, we investigated the role of emission reductions on aerosol acidity and particulate nitrate. We found that models exhibit positive biases in pH predictions, attributed to very high levels of crustal elements (Mg, Ca, K) in model simulations, which in turn led to an increasing aerosol pH trend over the past decade and allowed nitrate to become an important component of aerosol, which is inconsistent with the measurements, highlighting the importance of accurate pH prediction.
Zhaofeng Tan, Franz Rohrer, Keding Lu, Xuefei Ma, Birger Bohn, Sebastian Broch, Huabin Dong, Hendrik Fuchs, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Xin Li, Ying Liu, Yuhan Liu, Anna Novelli, Min Shao, Haichao Wang, Yusheng Wu, Limin Zeng, Min Hu, Astrid Kiendler-Scharr, Andreas Wahner, and Yuanhang Zhang
Atmos. Chem. Phys., 18, 12391–12411, https://doi.org/10.5194/acp-18-12391-2018, https://doi.org/10.5194/acp-18-12391-2018, 2018
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We present the first wintertime OH, HO2, and RO2 measurements in Beijing, China. OH concentrations are nearly 2-fold larger than those observed in foreign cities during wintertime. The high OH and large OH reactivities indicate photochemical processes can be effective even during wintertime. A box model largely underestimated HO2 and RO2 concentrations during pollution episodes correlated with high NOx, indicating a deficit current chemistry in the high NOx regime.
Anna Novelli, Martin Kaminski, Michael Rolletter, Ismail-Hakki Acir, Birger Bohn, Hans-Peter Dorn, Xin Li, Anna Lutz, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Frank Holland, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 18, 11409–11422, https://doi.org/10.5194/acp-18-11409-2018, https://doi.org/10.5194/acp-18-11409-2018, 2018
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The impact of photooxidation of 2-methyl-3-butene-2-ol (MBO) on the concentration of radical species was studied in the atmospheric simulation chamber SAPHIR. MBO is a volatile organic compound mainly emitted by ponderosa and lodgepole pines which are very abundant in forests in the central-west USA. A very good agreement between measured and modelled radical concentrations and products from the oxidation of MBO was observed in an environment with NO of ~ 200 pptv.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Mingjin Wang, Tong Zhu, Defeng Zhao, Florian Rubach, Andreas Wahner, Astrid Kiendler-Scharr, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 7345–7359, https://doi.org/10.5194/acp-18-7345-2018, https://doi.org/10.5194/acp-18-7345-2018, 2018
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Organic coatings modify hygroscopicity and CCN activation of mineral dust perticles. Small amounts of oleic acid coating (volume fraction (vf) ≤ 4.1 %) decreased the CCN activity of CaCO3 particles, while more oleic acid coating (vf ≥ 14.8 %) increased the CCN activity of CaCO3 particles, while malonic acid coating (vf = 0.4−42 %) even in smallest amounts increased the CCN activity of CaCO3 particles. Our laboratory results should also hold under conditions of the atmosphere.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Haiyan Li, Qiang Zhang, Bo Zheng, Chunrong Chen, Nana Wu, Hongyu Guo, Yuxuan Zhang, Yixuan Zheng, Xin Li, and Kebin He
Atmos. Chem. Phys., 18, 5293–5306, https://doi.org/10.5194/acp-18-5293-2018, https://doi.org/10.5194/acp-18-5293-2018, 2018
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This study revealed the driving role of nitrate in urban haze development in the North China Plain (NCP) during summertime. Several factors favoring the rapid nitrate formation were investigated in detail. The higher concentration and, in particular, the higher contribution of nitrate in PM1 suggest an urgent need to initiate ammonia emission control measures and further reduce NOx emissions over the NCP region.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Defeng Zhao, Sebastian H. Schmitt, Mingjin Wang, Ismail-Hakki Acir, Ralf Tillmann, Zhaofeng Tan, Anna Novelli, Hendrik Fuchs, Iida Pullinen, Robert Wegener, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 18, 1611–1628, https://doi.org/10.5194/acp-18-1611-2018, https://doi.org/10.5194/acp-18-1611-2018, 2018
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Air pollutants emitted by human activities such as NOx and SO2 can influence the abundance of secondary organic aerosol (SOA) from biogenic volatile organic compounds (VOCs). We found that NOx suppressed new particle formation and SOA mass formation. When both SO2 and NOx are present, the suppressing effect of NOx on SOA mass formation was counteracted by SO2. High NOx changed SOA chemical composition, forming more organic nitrate, because NOx changed radical chemistry during VOC oxidation.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Xuan Wang, Colette L. Heald, Jiumeng Liu, Rodney J. Weber, Pedro Campuzano-Jost, Jose L. Jimenez, Joshua P. Schwarz, and Anne E. Perring
Atmos. Chem. Phys., 18, 635–653, https://doi.org/10.5194/acp-18-635-2018, https://doi.org/10.5194/acp-18-635-2018, 2018
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Brown carbon (BrC) contributes significantly to uncertainty in estimating the global direct radiative effect (DRE) of aerosols. We develop a global model simulation of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental United States. We suggest that BrC DRE has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Dong Gao, Ting Fang, Vishal Verma, Linghan Zeng, and Rodney J. Weber
Atmos. Meas. Tech., 10, 2821–2835, https://doi.org/10.5194/amt-10-2821-2017, https://doi.org/10.5194/amt-10-2821-2017, 2017
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This work compares three methods to determine the optimal approach for quantifying the total oxidative potential (OP) of fine particles collected with filters using the dithiothreitol (DTT) assay. An automated system has been developed to facilitate the total OP measurements for use in generation of large data sets needed for epidemiology studies. The results from this study show that the water-insoluble components contribute to PM2.5 OP and the related DTT-active species are largely secondary.
Cheng Wu, Iida Pullinen, Stefanie Andres, Astrid Kiendler-Scharr, Einhard Kleist, Andreas Wahner, Jürgen Wildt, and Thomas F. Mentel
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-260, https://doi.org/10.5194/bg-2017-260, 2017
Manuscript not accepted for further review
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Biogenic volatile organic compounds are important for atmospheric chemistry. We showed by 13CO2 labelling experiments that biosynthesis is not restricted to the presence of light. In particular sesquiterpenes exhibit substantial de novo emissions in darkness with the carbon being delivered from alternative carbon sources. Our findings are of importance for future emissions under conditions of climate change as the response of de novo emissions to stresses differs from that of pool emissions.
Khairunnisa Yahya, Timothy Glotfelty, Kai Wang, Yang Zhang, and Athanasios Nenes
Geosci. Model Dev., 10, 2333–2363, https://doi.org/10.5194/gmd-10-2333-2017, https://doi.org/10.5194/gmd-10-2333-2017, 2017
Petros Vasilakos, Yong-Ηa Kim, Jeffrey R. Pierce, Sotira Yiacoumi, Costas Tsouris, and Athanasios Nenes
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2017-96, https://doi.org/10.5194/gmd-2017-96, 2017
Revised manuscript not accepted
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Radioactive charging can significantly impact the way radioactive aerosols behave, and as a result their lifetime, but such effects are neglected in predictive model studies of radioactive plumes. We extend a well-established model that simulates the evolution of atmospheric particulate matter to account for radioactive charging effects in an accurate and computationally efficient way. It is shown that radioactivity can strongly impact the deposition patterns of aerosol.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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Fine particle pH is linked to many environmental impacts by affecting particle concentration and composition. Predicted Pasadena, CA (CalNex campaign), PM1 pH is 1.9 and PM2.5 pH 2.7, the latter higher due to sea salts. The model predicted gas–particle partitionings of HNO3–NO3−, NH3–NH4+, and HCl–Cl− are in good agreement, verifying the model predictions. A summary of contrasting locations in the US and eastern Mediterranean shows fine particles are generally highly acidic, with pH below 3.
Vlassis A. Karydis, Alexandra P. Tsimpidi, Sara Bacer, Andrea Pozzer, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 17, 5601–5621, https://doi.org/10.5194/acp-17-5601-2017, https://doi.org/10.5194/acp-17-5601-2017, 2017
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The importance of mineral dust for cloud droplet formation is studied by considering the adsorption activation of insoluble dust particles and the thermodynamic interactions between mineral cations and inorganic anions. This study demonstrates that a comprehensive treatment of the CCN activity of mineral dust and its chemical and thermodynamic interactions with inorganic species by chemistry climate models is important to realistically account for aerosol–chemistry–cloud–climate interaction.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
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Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Wing Y. Tuet, Yunle Chen, Lu Xu, Shierly Fok, Dong Gao, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 17, 839–853, https://doi.org/10.5194/acp-17-839-2017, https://doi.org/10.5194/acp-17-839-2017, 2017
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Secondary organic aerosols (SOA) comprise a significant fraction of particulate matter (PM) and may have health implications. The water-soluble oxidative potentials of various SOA systems were determined using dithiothreitol consumption. Results from this study demonstrate that precursor identity was more influential than reaction condition in determining SOA oxidative potential and highlight a need to consider SOA contributions from anthropogenic hydrocarbons to PM-induced health effects.
Alexandra Tsekeri, Vassilis Amiridis, Franco Marenco, Athanasios Nenes, Eleni Marinou, Stavros Solomos, Phil Rosenberg, Jamie Trembath, Graeme J. Nott, James Allan, Michael Le Breton, Asan Bacak, Hugh Coe, Carl Percival, and Nikolaos Mihalopoulos
Atmos. Meas. Tech., 10, 83–107, https://doi.org/10.5194/amt-10-83-2017, https://doi.org/10.5194/amt-10-83-2017, 2017
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The In situ/Remote sensing aerosol Retrieval Algorithm (IRRA) provides vertical profiles of aerosol optical, microphysical and hygroscopic properties from airborne in situ and remote sensing measurements. The algorithm is highly advantageous for aerosol characterization in humid conditions, employing the ISORROPIA II model for acquiring the particle hygroscopic growth. IRRA can find valuable applications in aerosol–cloud interaction schemes and in validation of active space-borne sensors.
Havala O. T. Pye, Benjamin N. Murphy, Lu Xu, Nga L. Ng, Annmarie G. Carlton, Hongyu Guo, Rodney Weber, Petros Vasilakos, K. Wyat Appel, Sri Hapsari Budisulistiorini, Jason D. Surratt, Athanasios Nenes, Weiwei Hu, Jose L. Jimenez, Gabriel Isaacman-VanWertz, Pawel K. Misztal, and Allen H. Goldstein
Atmos. Chem. Phys., 17, 343–369, https://doi.org/10.5194/acp-17-343-2017, https://doi.org/10.5194/acp-17-343-2017, 2017
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We use a chemical transport model to examine how organic compounds in the atmosphere interact with water present in particles. Organic compounds themselves lead to water uptake, and organic compounds interact with water associated with inorganic compounds in the rural southeast atmosphere. Including interactions of organic compounds with water requires a treatment of nonideality to more accurately represent aerosol observations during the Southern Oxidant and Aerosol Study (SOAS) 2013.
Panayiotis Kalkavouras, Elissavet Bossioli, Spiros Bezantakos, Aikaterini Bougiatioti, Nikos Kalivitis, Iasonas Stavroulas, Giorgos Kouvarakis, Anna P. Protonotariou, Aggeliki Dandou, George Biskos, Nikolaos Mihalopoulos, Athanasios Nenes, and Maria Tombrou
Atmos. Chem. Phys., 17, 175–192, https://doi.org/10.5194/acp-17-175-2017, https://doi.org/10.5194/acp-17-175-2017, 2017
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Concentrations of chemically and size-resolved submicron aerosol particles along with concentrations of gases and meteorological variables were measured at Santorini and Finokalia (central and southern Aegean Sea) during the Etesians. Particle nucleation bursts were recorded. The NPF can double CCN number (at 0.1 % supersaturation), but the resulting strong competition for water vapor in cloudy updrafts decreases maximum supersaturation by 14 % and augments the potential droplet number by 12 %.
Stelios Myriokefalitakis, Athanasios Nenes, Alex R. Baker, Nikolaos Mihalopoulos, and Maria Kanakidou
Biogeosciences, 13, 6519–6543, https://doi.org/10.5194/bg-13-6519-2016, https://doi.org/10.5194/bg-13-6519-2016, 2016
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The global atmospheric cycle of P is simulated accounting for natural and anthropogenic sources, acid dissolution of dust aerosol and changes in atmospheric acidity. Simulations show that P-containing dust dissolution flux may have increased in the last 150 years but is expected to decrease in the future, and biological particles are important carriers of bioavailable P to the ocean. These insights to the P cycle have important implications for marine ecosystem responses to climate change.
Amelia F. Longo, David J. Vine, Laura E. King, Michelle Oakes, Rodney J. Weber, Lewis Gregory Huey, Armistead G. Russell, and Ellery D. Ingall
Atmos. Chem. Phys., 16, 13389–13398, https://doi.org/10.5194/acp-16-13389-2016, https://doi.org/10.5194/acp-16-13389-2016, 2016
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New synchrotron-based techniques were applied to characterize the oxidation state and composition of sulfur in ambient aerosol and emission sources. Individual particles were found to contain surprisingly high levels of elemental sulfur, a form of sulfur found in only one of the emission sources analyzed. We also show metal sulfates as a key component of urban aerosols. These metal sulfate phases are highly soluble and are indicative of acidic processes transforming metals in the environment.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Mehrnaz Sarrafzadeh, Jürgen Wildt, Iida Pullinen, Monika Springer, Einhard Kleist, Ralf Tillmann, Sebastian H. Schmitt, Cheng Wu, Thomas F. Mentel, Defeng Zhao, Donald R. Hastie, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 16, 11237–11248, https://doi.org/10.5194/acp-16-11237-2016, https://doi.org/10.5194/acp-16-11237-2016, 2016
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We investigated NOx impacts on the formation of secondary organic aerosol (SOA) mass from b-pinene and we could reveal two different mechanisms of impacts. One of them was the impact of NOx on OH that could explain increasing SOA yield with increasing NOx at low NOx conditions. The other was the suppression of new particle formation limiting the condensational sink for the SOA precursors. This effect could explain a substantial fraction of the decrease of SOA yield observed at high NOx.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Aikaterini Bougiatioti, Spiros Bezantakos, Iasonas Stavroulas, Nikos Kalivitis, Panagiotis Kokkalis, George Biskos, Nikolaos Mihalopoulos, Alexandros Papayannis, and Athanasios Nenes
Atmos. Chem. Phys., 16, 7389–7409, https://doi.org/10.5194/acp-16-7389-2016, https://doi.org/10.5194/acp-16-7389-2016, 2016
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BBOA from long-range transport exhibits increased CCN concentrations for particles larger than 100 nm. At the same time the hygroscopicity parameter decreased for all particle sizes, as sub-100 nm particles appear to be richer in less hygroscopic organic material, while larger particles become less hygroscopic due to condensation of less hygroscopic gaseous compounds. Finally, atmospheric processing of freshly emitted BBOA to more oxidized organic aerosol can result in a 2-fold increase of κ.
Bernadette Rosati, Martin Gysel, Florian Rubach, Thomas F. Mentel, Brigitta Goger, Laurent Poulain, Patrick Schlag, Pasi Miettinen, Aki Pajunoja, Annele Virtanen, Henk Klein Baltink, J. S. Bas Henzing, Johannes Größ, Gian Paolo Gobbi, Alfred Wiedensohler, Astrid Kiendler-Scharr, Stefano Decesari, Maria Cristina Facchini, Ernest Weingartner, and Urs Baltensperger
Atmos. Chem. Phys., 16, 7295–7315, https://doi.org/10.5194/acp-16-7295-2016, https://doi.org/10.5194/acp-16-7295-2016, 2016
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This study presents PEGASOS project data from field campaigns in the Po Valley, Italy and the Netherlands. Vertical profiles of aerosol hygroscopicity and chemical composition were investigated with airborne measurements on board a Zeppelin NT airship. A special focus was on the evolution of different mixing layers within the PBL as a function of daytime. A closure study showed that variations in aerosol hygroscopicity can well be explained by the variations in chemical composition.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Weruka Rattanavaraha, Kevin Chu, Sri Hapsari Budisulistiorini, Matthieu Riva, Ying-Hsuan Lin, Eric S. Edgerton, Karsten Baumann, Stephanie L. Shaw, Hongyu Guo, Laura King, Rodney J. Weber, Miranda E. Neff, Elizabeth A. Stone, John H. Offenberg, Zhenfa Zhang, Avram Gold, and Jason D. Surratt
Atmos. Chem. Phys., 16, 4897–4914, https://doi.org/10.5194/acp-16-4897-2016, https://doi.org/10.5194/acp-16-4897-2016, 2016
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The mechanisms by which specific anthropogenic pollutants enhance isoprene SOA in ambient PM2.5 remain unclear. As one aspect of an investigation to examine how anthropogenic pollutants influence isoprene-derived SOA formation, high-volume PM2.5 filter samples were collected from Birmingham, AL, during the 2013 Southern Oxidant and Aerosol Study (SOAS). Isoprene SOA tracers were measured from these samples and compared to gas and aerosol data collected from the SEARCH network.
Aikaterini Bougiatioti, Panayiota Nikolaou, Iasonas Stavroulas, Giorgos Kouvarakis, Rodney Weber, Athanasios Nenes, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 16, 4579–4591, https://doi.org/10.5194/acp-16-4579-2016, https://doi.org/10.5194/acp-16-4579-2016, 2016
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Atmospheric aerosols and relevant parameters were measured in the eastern Mediterranean during summer and fall 2012. Submicron aerosol water can contribute up to 33 % of total mass, and 27.5 % of this can be associated with organics. Using these data, the pH of the submicron aerosols was calculated to be highly acidic, varying from 0.5 to 2.8 and independently of air masses origin. Such pH values could increase nutrient availability and thus sea water productivity of the Mediterranean Sea.
Christopher R. Hoyle, Clare S. Webster, Harald E. Rieder, Athanasios Nenes, Emanuel Hammer, Erik Herrmann, Martin Gysel, Nicolas Bukowiecki, Ernest Weingartner, Martin Steinbacher, and Urs Baltensperger
Atmos. Chem. Phys., 16, 4043–4061, https://doi.org/10.5194/acp-16-4043-2016, https://doi.org/10.5194/acp-16-4043-2016, 2016
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A simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from the high-altitude site Jungfraujoch. It is found that cloud droplet formation at the Jungfraujoch is predominantly controlled by the number concentration of aerosol particles. A statistical model based on only the number of particles larger than 80nm can explain 79 % of the observed variance in droplet numbers.
Ting Fang, Vishal Verma, Josephine T. Bates, Joseph Abrams, Mitchel Klein, Matthew J. Strickland, Stefanie E. Sarnat, Howard H. Chang, James A. Mulholland, Paige E. Tolbert, Armistead G. Russell, and Rodney J. Weber
Atmos. Chem. Phys., 16, 3865–3879, https://doi.org/10.5194/acp-16-3865-2016, https://doi.org/10.5194/acp-16-3865-2016, 2016
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Ascorbic acid (AA) and Dithiothreitol (DTT) assay measures of water-soluble PM2.5 oxidative potential (OP) are compared in terms of spatiotemporal trends, chemical selectivity, sources, and health impacts based on an epidemiological study with backcast estimated OP. Both assays point to metals from brake/tire wear, but only the DTT assay also identifies organics from combustion. DTT is associated with emergency department visits for asthma/wheeze and congestive heart failure, whereas AA is not.
T. Hohaus, U. Kuhn, S. Andres, M. Kaminski, F. Rohrer, R. Tillmann, A. Wahner, R. Wegener, Z. Yu, and A. Kiendler-Scharr
Atmos. Meas. Tech., 9, 1247–1259, https://doi.org/10.5194/amt-9-1247-2016, https://doi.org/10.5194/amt-9-1247-2016, 2016
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As an extension of the atmosphere simulation chamber SAPHIR, an environmentally-controlled dynamic (flow-through) plant chamber under SAPHIR (SAPHIR-PLUS) was developed. This facility allows for feeding a natural blend of biogenic trace gases into SAPHIR. PLUS is utilized to characterize the atmospheric chemistry of natural trace gas mixtures at close to ambient concentration levels. In this study, the results of the initial characterization experiments are presented in detail.
Yong-ha Kim, Sotira Yiacoumi, Athanasios Nenes, and Costas Tsouris
Atmos. Chem. Phys., 16, 3449–3462, https://doi.org/10.5194/acp-16-3449-2016, https://doi.org/10.5194/acp-16-3449-2016, 2016
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Three microphysical approaches are proposed to incorporate mutual effects of particle charging and coagulation in predictions of transient charge and size distributions of atmospheric particles, including radioactive aerosols. The three approaches have different levels of complexities and are applicable to various laboratory and field atmospheric studies. Also, these approaches can be easily incorporated into aerosol transport models at different scales to account for particle charging effects.
Andrea Ghirardo, Junfei Xie, Xunhua Zheng, Yuesi Wang, Rüdiger Grote, Katja Block, Jürgen Wildt, Thomas Mentel, Astrid Kiendler-Scharr, Mattias Hallquist, Klaus Butterbach-Bahl, and Jörg-Peter Schnitzler
Atmos. Chem. Phys., 16, 2901–2920, https://doi.org/10.5194/acp-16-2901-2016, https://doi.org/10.5194/acp-16-2901-2016, 2016
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Trees can impact urban air quality. Large emissions of plant volatiles are emitted in Beijing as a stress response to the urban polluted environment, but their impacts on secondary particulate matter remain relatively low compared to those originated from anthropogenic activities. The present study highlights the importance of including stress-induced compounds when studying plant volatile emissions.
Sylvia C. Sullivan, Ricardo Morales Betancourt, Donifan Barahona, and Athanasios Nenes
Atmos. Chem. Phys., 16, 2611–2629, https://doi.org/10.5194/acp-16-2611-2016, https://doi.org/10.5194/acp-16-2611-2016, 2016
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We use the adjoint model of a cirrus parameterization to quantify sources of crystal variability for various ice-nucleating spectra and output from CAM5.
The sensitivities can be directly linked to nucleation regime and
efficiency of various INP.
The lab-based spectrum calculates much higher INP efficiencies than field-based ones, owing to aerosol surface properties.
The sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters.
M. Dal Maso, L. Liao, J. Wildt, A. Kiendler-Scharr, E. Kleist, R. Tillmann, M. Sipilä, J. Hakala, K. Lehtipalo, M. Ehn, V.-M. Kerminen, M. Kulmala, D. Worsnop, and T. Mentel
Atmos. Chem. Phys., 16, 1955–1970, https://doi.org/10.5194/acp-16-1955-2016, https://doi.org/10.5194/acp-16-1955-2016, 2016
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In this paper, we present the first direct laboratory observations of nanoparticle formation from sulfuric acid and realistic BVOC precursor vapour mixtures performed at atmospherically relevant concentration levels. We found that the formation rate was proportional to the product of sulphuric acid and biogenic VOC emission strength, and that the formation rates were consistent with a mechanism in which nucleating BVOC oxidation products are rapidly formed and activate with sulfuric acid.
D. F. Zhao, A. Buchholz, B. Kortner, P. Schlag, F. Rubach, H. Fuchs, A. Kiendler-Scharr, R. Tillmann, A. Wahner, Å. K. Watne, M. Hallquist, J. M. Flores, Y. Rudich, K. Kristensen, A. M. K. Hansen, M. Glasius, I. Kourtchev, M. Kalberer, and Th. F. Mentel
Atmos. Chem. Phys., 16, 1105–1121, https://doi.org/10.5194/acp-16-1105-2016, https://doi.org/10.5194/acp-16-1105-2016, 2016
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This study investigated the cloud droplet activation behavior and hygroscopic growth of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Cloud droplet activation behaviors of different types of SOA were similar. In contrast, the hygroscopicity of ASOA was higher than BSOA and ABSOA. ASOA components enhanced the hygroscopicity of the ABSOA. Yet this enhancement cannot be described by a linear mixing of pure SOA systems.
L. M. Zamora, R. A. Kahn, M. J. Cubison, G. S. Diskin, J. L. Jimenez, Y. Kondo, G. M. McFarquhar, A. Nenes, K. L. Thornhill, A. Wisthaler, A. Zelenyuk, and L. D. Ziemba
Atmos. Chem. Phys., 16, 715–738, https://doi.org/10.5194/acp-16-715-2016, https://doi.org/10.5194/acp-16-715-2016, 2016
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Based on extensive aircraft campaigns, we quantify how biomass burning smoke affects subarctic and Arctic liquid cloud microphysical properties. Enhanced cloud albedo may decrease short-wave radiative flux by between 2 and 4 Wm2 or more in some subarctic conditions. Smoke halved average cloud droplet diameter. In one case study, it also appeared to limit droplet formation. Numerous Arctic background Aitken particles can also interact with combustion particles, perhaps affecting their properties.
M. Paramonov, V.-M. Kerminen, M. Gysel, P. P. Aalto, M. O. Andreae, E. Asmi, U. Baltensperger, A. Bougiatioti, D. Brus, G. P. Frank, N. Good, S. S. Gunthe, L. Hao, M. Irwin, A. Jaatinen, Z. Jurányi, S. M. King, A. Kortelainen, A. Kristensson, H. Lihavainen, M. Kulmala, U. Lohmann, S. T. Martin, G. McFiggans, N. Mihalopoulos, A. Nenes, C. D. O'Dowd, J. Ovadnevaite, T. Petäjä, U. Pöschl, G. C. Roberts, D. Rose, B. Svenningsson, E. Swietlicki, E. Weingartner, J. Whitehead, A. Wiedensohler, C. Wittbom, and B. Sierau
Atmos. Chem. Phys., 15, 12211–12229, https://doi.org/10.5194/acp-15-12211-2015, https://doi.org/10.5194/acp-15-12211-2015, 2015
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The research paper presents the first comprehensive overview of field measurements with the CCN Counter performed at a large number of locations around the world within the EUCAARI framework. The paper sheds light on the CCN number concentrations and activated fractions around the world and their dependence on the water vapour supersaturation ratio, the dependence of aerosol hygroscopicity on particle size, and seasonal and diurnal variation of CCN activation and hygroscopic properties.
T. Fang, H. Guo, V. Verma, R. E. Peltier, and R. J. Weber
Atmos. Chem. Phys., 15, 11667–11682, https://doi.org/10.5194/acp-15-11667-2015, https://doi.org/10.5194/acp-15-11667-2015, 2015
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This work presented a new method of quantifying water-soluble elements in PM2.5 aqueous extracts (N~500) with an X-ray fluorescence analyzer. The results indicate that water-soluble elements had marked spatial and temporal patterns. Four sources were resolved: brake/tire wear, biomass burning, secondary formation, and mineral dust. The findings have informed studies on aerosol oxidative potential and provided insights into the health effects of water-soluble metals, especially Cu, Fe, Mn and Zn.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
N. Kalivitis, V.-M. Kerminen, G. Kouvarakis, I. Stavroulas, A. Bougiatioti, A. Nenes, H. E. Manninen, T. Petäjä, M. Kulmala, and N. Mihalopoulos
Atmos. Chem. Phys., 15, 9203–9215, https://doi.org/10.5194/acp-15-9203-2015, https://doi.org/10.5194/acp-15-9203-2015, 2015
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Cloud condensation nuclei (CCN) production associated with atmospheric new particle formation (NPF) is presented, and this is the first direct evidence of CCN production resulting from NPF in the eastern Mediterranean atmosphere. We show that condensation of both gaseous sulfuric acid and organic compounds from multiple sources leads to the rapid growth of nucleated particles. Sub-100nm particles were found to be substantially less hygroscopic than larger particles during the active NPF period.
S. H. Budisulistiorini, X. Li, S. T. Bairai, J. Renfro, Y. Liu, Y. J. Liu, K. A. McKinney, S. T. Martin, V. F. McNeill, H. O. T. Pye, A. Nenes, M. E. Neff, E. A. Stone, S. Mueller, C. Knote, S. L. Shaw, Z. Zhang, A. Gold, and J. D. Surratt
Atmos. Chem. Phys., 15, 8871–8888, https://doi.org/10.5194/acp-15-8871-2015, https://doi.org/10.5194/acp-15-8871-2015, 2015
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Isoprene epoxydiols (IEPOX) are major gas-phase products from the atmospheric oxidation of isoprene that yield secondary organic aerosol (SOA) by reactive uptake onto acidic sulfate aerosol. We report a substantial contribution of IEPOX-derived SOA to the total fine aerosol collected during summer. IEPOX-derived SOA measured by online and offline mass spectrometry techniques is correlated with acidic sulfate aerosol, demonstrating the critical role of anthropogenic emissions in its formation.
K. M. Cerully, A. Bougiatioti, J. R. Hite Jr., H. Guo, L. Xu, N. L. Ng, R. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 8679–8694, https://doi.org/10.5194/acp-15-8679-2015, https://doi.org/10.5194/acp-15-8679-2015, 2015
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The hygroscopicity of SE US aerosol is mostly water-soluble, with a hygroscopicity that is insensitive to partial volatilization in a thermodenuder.
The most and least oxidized components of the aerosol are the most hygroscopic of organic constituents.
No clear relationship was found between organic aerosol hygroscopicity and oxygen-to-carbon ratio.
The aerosol factors covary in a way that induces the observed diurnal invariance in total organic hygroscopicity.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
J. Liu, E. Scheuer, J. Dibb, G. S. Diskin, L. D. Ziemba, K. L. Thornhill, B. E. Anderson, A. Wisthaler, T. Mikoviny, J. J. Devi, M. Bergin, A. E. Perring, M. Z. Markovic, J. P. Schwarz, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, and R. J. Weber
Atmos. Chem. Phys., 15, 7841–7858, https://doi.org/10.5194/acp-15-7841-2015, https://doi.org/10.5194/acp-15-7841-2015, 2015
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Brown carbon (BrC) is found throughout the US continental troposphere during a summer of extensive biomass burning and its prevalence relative to black carbon (BC) increases with altitude. A radiative transfer model based on direct measurements of aerosol scattering and absorption by BC and BrC shows BrC reduces top-of-atmosphere forcing by 20%. A method to estimate BrC radiative forcing efficiencies from surface-based measurements is provided.
Y. Shinozuka, A. D. Clarke, A. Nenes, A. Jefferson, R. Wood, C. S. McNaughton, J. Ström, P. Tunved, J. Redemann, K. L. Thornhill, R. H. Moore, T. L. Lathem, J. J. Lin, and Y. J. Yoon
Atmos. Chem. Phys., 15, 7585–7604, https://doi.org/10.5194/acp-15-7585-2015, https://doi.org/10.5194/acp-15-7585-2015, 2015
L. Xu, S. Suresh, H. Guo, R. J. Weber, and N. L. Ng
Atmos. Chem. Phys., 15, 7307–7336, https://doi.org/10.5194/acp-15-7307-2015, https://doi.org/10.5194/acp-15-7307-2015, 2015
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Year-long comprehensive characterization of ambient aerosol was performed in both rural and urban sites in the southeastern US as part of Southeastern Center of Air Pollution and Epidemiology (SCAPE) study and Southeastern Oxidant and Aerosol Study (SOAS). Three independent methods were applied to estimate the concentration of particle-phase organic nitrates. The spatial distribution of organic aerosol is investigated by comparing simultaneous HR-ToF-AMS and ACSM measurements at different sites.
S. Myriokefalitakis, N. Daskalakis, N. Mihalopoulos, A. R. Baker, A. Nenes, and M. Kanakidou
Biogeosciences, 12, 3973–3992, https://doi.org/10.5194/bg-12-3973-2015, https://doi.org/10.5194/bg-12-3973-2015, 2015
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The global atmospheric cycle of Fe is simulated accounting for natural and combustion sources, proton- and organic ligand-promoted Fe dissolution from dust aerosol and changes in anthropogenic emissions, and thus in atmospheric acidity. Simulations show that Fe dissolution may have increased in the last 150 years and is expected to decrease due to air pollution regulations. Reductions in dissolved-Fe deposition can further limit the primary productivity over high-nutrient-low-chlorophyll water.
H. Guo, L. Xu, A. Bougiatioti, K. M. Cerully, S. L. Capps, J. R. Hite Jr., A. G. Carlton, S.-H. Lee, M. H. Bergin, N. L. Ng, A. Nenes, and R. J. Weber
Atmos. Chem. Phys., 15, 5211–5228, https://doi.org/10.5194/acp-15-5211-2015, https://doi.org/10.5194/acp-15-5211-2015, 2015
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Particle pH can affect many aerosol processes, including gas-particle partitioning, SOA formation, and mobilization of toxic redox metals. pH is challenging to directly measure and often improperly characterized by proxies like ion balances or molar ratios of measured aerosol ionic species. We present a detailed analysis predicting pH with a thermodynamic model, verify the prediction, and test pH sensitivity to model inputs based on data from the SOAS field campaign.
J. W. Taylor, J. D. Allan, D. Liu, M. Flynn, R. Weber, X. Zhang, B. L. Lefer, N. Grossberg, J. Flynn, and H. Coe
Atmos. Meas. Tech., 8, 1701–1718, https://doi.org/10.5194/amt-8-1701-2015, https://doi.org/10.5194/amt-8-1701-2015, 2015
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When using the SP2 to report black carbon core/shell coating thickness, the core density and refractive index must be estimated from literature values. We systematically vary the assumed parameters and the instrument calibration, and quantify the effects in the derived coatings. The technique is highly sensitive to the core refractive index but has only a minor sensitivity to the core density and coating refractive index. We identify the most appropriate values to use in future analysis.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
B. Yuan, P. R. Veres, C. Warneke, J. M. Roberts, J. B. Gilman, A. Koss, P. M. Edwards, M. Graus, W. C. Kuster, S.-M. Li, R. J. Wild, S. S. Brown, W. P. Dubé, B. M. Lerner, E. J. Williams, J. E. Johnson, P. K. Quinn, T. S. Bates, B. Lefer, P. L. Hayes, J. L. Jimenez, R. J. Weber, R. Zamora, B. Ervens, D. B. Millet, B. Rappenglück, and J. A. de Gouw
Atmos. Chem. Phys., 15, 1975–1993, https://doi.org/10.5194/acp-15-1975-2015, https://doi.org/10.5194/acp-15-1975-2015, 2015
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In this work, secondary formation of formic acid at an urban site and a site in an oil and gas production region is studied. We investigated various gas phase formation pathways of formic acid, including those recently proposed, using a box model. The contributions from aerosol-related processes, fog events and air-snow exchange to formic acid are also quantified.
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
T. Fang, V. Verma, H. Guo, L. E. King, E. S. Edgerton, and R. J. Weber
Atmos. Meas. Tech., 8, 471–482, https://doi.org/10.5194/amt-8-471-2015, https://doi.org/10.5194/amt-8-471-2015, 2015
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This work summarizes a newly developed semi-automated system for quantifying the oxidative potential of aerosol aqueous extracts using the dithiothreitol (DTT) assay. 500 sample analyses indicate that DTT activity in the southeast US is likely not dominated by a unique local source, and sources change with season. The unique large data set generated with the technique described in this paper allows new studies on DTT sources and investigating linkages between reactive oxygen species and health.
D. F. Zhao, M. Kaminski, P. Schlag, H. Fuchs, I.-H. Acir, B. Bohn, R. Häseler, A. Kiendler-Scharr, F. Rohrer, R. Tillmann, M. J. Wang, R. Wegener, J. Wildt, A. Wahner, and Th. F. Mentel
Atmos. Chem. Phys., 15, 991–1012, https://doi.org/10.5194/acp-15-991-2015, https://doi.org/10.5194/acp-15-991-2015, 2015
C. Wu, I. Pullinen, S. Andres, G. Carriero, S. Fares, H. Goldbach, L. Hacker, T. Kasal, A. Kiendler-Scharr, E. Kleist, E. Paoletti, A. Wahner, J. Wildt, and Th. F. Mentel
Biogeosciences, 12, 177–191, https://doi.org/10.5194/bg-12-177-2015, https://doi.org/10.5194/bg-12-177-2015, 2015
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Impacts of soil moisture on de novo monoterpene emissions from several tree species were studied. Mild drought slightly increased MT emissions, but with further progressing drought the emissions decreased to almost zero. Increases of MT emissions were explainable by increases of leaf temperature due to lowered transpirational cooling. The decrease of emissions observed when soil moisture fell below certain thresholds was parameterized, allowing considering impacts of soil moisture in models.
V. Verma, T. Fang, H. Guo, L. King, J. T. Bates, R. E. Peltier, E. Edgerton, A. G. Russell, and R. J. Weber
Atmos. Chem. Phys., 14, 12915–12930, https://doi.org/10.5194/acp-14-12915-2014, https://doi.org/10.5194/acp-14-12915-2014, 2014
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The major emission sources of the reactive oxygen species (ROS) associated with ambient particulate matter in the southeastern United States were identified. The study shows biomass burning and secondary aerosol formation as the major sources contributing to the ROS-generating capability of ambient particles. The ubiquitous nature of these two sources suggests widespread population exposures to the toxic aerosol components.
Y. You, V. P. Kanawade, J. A. de Gouw, A. B. Guenther, S. Madronich, M. R. Sierra-Hernández, M. Lawler, J. N. Smith, S. Takahama, G. Ruggeri, A. Koss, K. Olson, K. Baumann, R. J. Weber, A. Nenes, H. Guo, E. S. Edgerton, L. Porcelli, W. H. Brune, A. H. Goldstein, and S.-H. Lee
Atmos. Chem. Phys., 14, 12181–12194, https://doi.org/10.5194/acp-14-12181-2014, https://doi.org/10.5194/acp-14-12181-2014, 2014
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Amiens play important roles in atmospheric secondary aerosol formation and human health, but the fast response measurements of amines are lacking. Here we show measurements in a southeastern US forest and a moderately polluted midwestern site. Our results show that gas to particle conversion is an important process that controls ambient amine concentrations and that biomass burning is an important source of amines.
T. K. V. Nguyen, M. D. Petters, S. R. Suda, H. Guo, R. J. Weber, and A. G. Carlton
Atmos. Chem. Phys., 14, 10911–10930, https://doi.org/10.5194/acp-14-10911-2014, https://doi.org/10.5194/acp-14-10911-2014, 2014
R. Morales Betancourt and A. Nenes
Geosci. Model Dev., 7, 2345–2357, https://doi.org/10.5194/gmd-7-2345-2014, https://doi.org/10.5194/gmd-7-2345-2014, 2014
C. Fountoukis, A. G. Megaritis, K. Skyllakou, P. E. Charalampidis, C. Pilinis, H. A. C. Denier van der Gon, M. Crippa, F. Canonaco, C. Mohr, A. S. H. Prévôt, J. D. Allan, L. Poulain, T. Petäjä, P. Tiitta, S. Carbone, A. Kiendler-Scharr, E. Nemitz, C. O'Dowd, E. Swietlicki, and S. N. Pandis
Atmos. Chem. Phys., 14, 9061–9076, https://doi.org/10.5194/acp-14-9061-2014, https://doi.org/10.5194/acp-14-9061-2014, 2014
D. Barahona, A. Molod, J. Bacmeister, A. Nenes, A. Gettelman, H. Morrison, V. Phillips, and A. Eichmann
Geosci. Model Dev., 7, 1733–1766, https://doi.org/10.5194/gmd-7-1733-2014, https://doi.org/10.5194/gmd-7-1733-2014, 2014
B. Gantt, J. He, X. Zhang, Y. Zhang, and A. Nenes
Atmos. Chem. Phys., 14, 7485–7497, https://doi.org/10.5194/acp-14-7485-2014, https://doi.org/10.5194/acp-14-7485-2014, 2014
S. H. Budisulistiorini, M. R. Canagaratna, P. L. Croteau, K. Baumann, E. S. Edgerton, M. S. Kollman, N. L. Ng, V. Verma, S. L. Shaw, E. M. Knipping, D. R. Worsnop, J. T. Jayne, R.J. Weber, and J. D. Surratt
Atmos. Meas. Tech., 7, 1929–1941, https://doi.org/10.5194/amt-7-1929-2014, https://doi.org/10.5194/amt-7-1929-2014, 2014
M. Crippa, F. Canonaco, V. A. Lanz, M. Äijälä, J. D. Allan, S. Carbone, G. Capes, D. Ceburnis, M. Dall'Osto, D. A. Day, P. F. DeCarlo, M. Ehn, A. Eriksson, E. Freney, L. Hildebrandt Ruiz, R. Hillamo, J. L. Jimenez, H. Junninen, A. Kiendler-Scharr, A.-M. Kortelainen, M. Kulmala, A. Laaksonen, A. A. Mensah, C. Mohr, E. Nemitz, C. O'Dowd, J. Ovadnevaite, S. N. Pandis, T. Petäjä, L. Poulain, S. Saarikoski, K. Sellegri, E. Swietlicki, P. Tiitta, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 14, 6159–6176, https://doi.org/10.5194/acp-14-6159-2014, https://doi.org/10.5194/acp-14-6159-2014, 2014
J. M. Flores, D. F. Zhao, L. Segev, P. Schlag, A. Kiendler-Scharr, H. Fuchs, Å. K. Watne, N. Bluvshtein, Th. F. Mentel, M. Hallquist, and Y. Rudich
Atmos. Chem. Phys., 14, 5793–5806, https://doi.org/10.5194/acp-14-5793-2014, https://doi.org/10.5194/acp-14-5793-2014, 2014
G. Drozd, J. Woo, S. A. K. Häkkinen, A. Nenes, and V. F. McNeill
Atmos. Chem. Phys., 14, 5205–5215, https://doi.org/10.5194/acp-14-5205-2014, https://doi.org/10.5194/acp-14-5205-2014, 2014
S. Romakkaniemi, A. Jaatinen, A. Laaksonen, A. Nenes, and T. Raatikainen
Atmos. Meas. Tech., 7, 1377–1384, https://doi.org/10.5194/amt-7-1377-2014, https://doi.org/10.5194/amt-7-1377-2014, 2014
A. Bougiatioti, I. Stavroulas, E. Kostenidou, P. Zarmpas, C. Theodosi, G. Kouvarakis, F. Canonaco, A. S. H. Prévôt, A. Nenes, S. N. Pandis, and N. Mihalopoulos
Atmos. Chem. Phys., 14, 4793–4807, https://doi.org/10.5194/acp-14-4793-2014, https://doi.org/10.5194/acp-14-4793-2014, 2014
R. Morales Betancourt and A. Nenes
Atmos. Chem. Phys., 14, 4809–4826, https://doi.org/10.5194/acp-14-4809-2014, https://doi.org/10.5194/acp-14-4809-2014, 2014
J. Wildt, T. F. Mentel, A. Kiendler-Scharr, T. Hoffmann, S. Andres, M. Ehn, E. Kleist, P. Müsgen, F. Rohrer, Y. Rudich, M. Springer, R. Tillmann, and A. Wahner
Atmos. Chem. Phys., 14, 2789–2804, https://doi.org/10.5194/acp-14-2789-2014, https://doi.org/10.5194/acp-14-2789-2014, 2014
M. Paglione, A. Kiendler-Scharr, A. A. Mensah, E. Finessi, L. Giulianelli, S. Sandrini, M. C. Facchini, S. Fuzzi, P. Schlag, A. Piazzalunga, E. Tagliavini, J. S. Henzing, and S. Decesari
Atmos. Chem. Phys., 14, 25–45, https://doi.org/10.5194/acp-14-25-2014, https://doi.org/10.5194/acp-14-25-2014, 2014
J. Liu, M. Bergin, H. Guo, L. King, N. Kotra, E. Edgerton, and R. J. Weber
Atmos. Chem. Phys., 13, 12389–12404, https://doi.org/10.5194/acp-13-12389-2013, https://doi.org/10.5194/acp-13-12389-2013, 2013
M. Trail, A. P. Tsimpidi, P. Liu, K. Tsigaridis, Y. Hu, A. Nenes, and A. G. Russell
Geosci. Model Dev., 6, 1429–1445, https://doi.org/10.5194/gmd-6-1429-2013, https://doi.org/10.5194/gmd-6-1429-2013, 2013
Th. F. Mentel, E. Kleist, S. Andres, M. Dal Maso, T. Hohaus, A. Kiendler-Scharr, Y. Rudich, M. Springer, R. Tillmann, R. Uerlings, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 13, 8755–8770, https://doi.org/10.5194/acp-13-8755-2013, https://doi.org/10.5194/acp-13-8755-2013, 2013
Y. Cheng, G. Engling, K.-B. He, F.-K. Duan, Y.-L. Ma, Z.-Y. Du, J.-M. Liu, M. Zheng, and R. J. Weber
Atmos. Chem. Phys., 13, 7765–7781, https://doi.org/10.5194/acp-13-7765-2013, https://doi.org/10.5194/acp-13-7765-2013, 2013
L. E. King and R. J. Weber
Atmos. Meas. Tech., 6, 1647–1658, https://doi.org/10.5194/amt-6-1647-2013, https://doi.org/10.5194/amt-6-1647-2013, 2013
Y. P. Li, H. Elbern, K. D. Lu, E. Friese, A. Kiendler-Scharr, Th. F. Mentel, X. S. Wang, A. Wahner, and Y. H. Zhang
Atmos. Chem. Phys., 13, 6289–6304, https://doi.org/10.5194/acp-13-6289-2013, https://doi.org/10.5194/acp-13-6289-2013, 2013
S. Lance, T. Raatikainen, T. B. Onasch, D. R. Worsnop, X.-Y. Yu, M. L. Alexander, M. R. Stolzenburg, P. H. McMurry, J. N. Smith, and A. Nenes
Atmos. Chem. Phys., 13, 5049–5062, https://doi.org/10.5194/acp-13-5049-2013, https://doi.org/10.5194/acp-13-5049-2013, 2013
H.-P. Dorn, R. L. Apodaca, S. M. Ball, T. Brauers, S. S. Brown, J. N. Crowley, W. P. Dubé, H. Fuchs, R. Häseler, U. Heitmann, R. L. Jones, A. Kiendler-Scharr, I. Labazan, J. M. Langridge, J. Meinen, T. F. Mentel, U. Platt, D. Pöhler, F. Rohrer, A. A. Ruth, E. Schlosser, G. Schuster, A. J. L. Shillings, W. R. Simpson, J. Thieser, R. Tillmann, R. Varma, D. S. Venables, and A. Wahner
Atmos. Meas. Tech., 6, 1111–1140, https://doi.org/10.5194/amt-6-1111-2013, https://doi.org/10.5194/amt-6-1111-2013, 2013
R. H. Moore, V. A. Karydis, S. L. Capps, T. L. Lathem, and A. Nenes
Atmos. Chem. Phys., 13, 4235–4251, https://doi.org/10.5194/acp-13-4235-2013, https://doi.org/10.5194/acp-13-4235-2013, 2013
E. U. Emanuelsson, M. Hallquist, K. Kristensen, M. Glasius, B. Bohn, H. Fuchs, B. Kammer, A. Kiendler-Scharr, S. Nehr, F. Rubach, R. Tillmann, A. Wahner, H.-C. Wu, and Th. F. Mentel
Atmos. Chem. Phys., 13, 2837–2855, https://doi.org/10.5194/acp-13-2837-2013, https://doi.org/10.5194/acp-13-2837-2013, 2013
T. L. Lathem, A. J. Beyersdorf, K. L. Thornhill, E. L. Winstead, M. J. Cubison, A. Hecobian, J. L. Jimenez, R. J. Weber, B. E. Anderson, and A. Nenes
Atmos. Chem. Phys., 13, 2735–2756, https://doi.org/10.5194/acp-13-2735-2013, https://doi.org/10.5194/acp-13-2735-2013, 2013
M. Frosch, M. Bilde, A. Nenes, A. P. Praplan, Z. Jurányi, J. Dommen, M. Gysel, E. Weingartner, and U. Baltensperger
Atmos. Chem. Phys., 13, 2283–2297, https://doi.org/10.5194/acp-13-2283-2013, https://doi.org/10.5194/acp-13-2283-2013, 2013
Y. C. Sud, D. Lee, L. Oreopoulos, D. Barahona, A. Nenes, and M. J. Suarez
Geosci. Model Dev., 6, 57–79, https://doi.org/10.5194/gmd-6-57-2013, https://doi.org/10.5194/gmd-6-57-2013, 2013
E. Kleist, T. F. Mentel, S. Andres, A. Bohne, A. Folkers, A. Kiendler-Scharr, Y. Rudich, M. Springer, R. Tillmann, and J. Wildt
Biogeosciences, 9, 5111–5123, https://doi.org/10.5194/bg-9-5111-2012, https://doi.org/10.5194/bg-9-5111-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Measurement report: Optical properties and sources of water-soluble brown carbon in Tianjin, North China – insights from organic molecular compositions
Trends in secondary inorganic aerosol pollution in China and its responses to emission controls of precursors in wintertime
Measurement report: Source apportionment of carbonaceous aerosol using dual-carbon isotopes (13C and 14C) and levoglucosan in three northern Chinese cities during 2018–2019
Chemically speciated mass size distribution, particle density, shape and origin of non-refractory PM1 measured at a rural background site in central Europe
Offline analysis of the chemical composition and hygroscopicity of submicrometer aerosol at an Asian outflow receptor site and comparison with online measurements
High number concentrations of transparent exopolymer particles in ambient aerosol particles and cloud water – a case study at the tropical Atlantic Ocean
Micro-spectroscopic and freezing characterization of ice-nucleating particles collected in the marine boundary layer in the eastern North Atlantic
Oxidation pathways and emission sources of atmospheric particulate nitrate in Seoul: based on δ15N and Δ17O measurements
Measurement report: Characterization and source apportionment of coarse particulate matter in Hong Kong: insights into the constituents of unidentified mass and source origins in a coastal city in southern China
The optical properties and in-situ observational evidence for the formation of brown carbon in clouds
High atmospheric oxidation capacity drives wintertime nitrate pollution in the eastern Yangtze River Delta of China
Development and evolution of an anomalous Asian dust event across Europe in March 2020
What caused a record high PM10 episode in northern Europe in October 2020?
Sensitivity of low-level clouds and precipitation to anthropogenic aerosol emission in southern West Africa: a DACCIWA case study
Pan-Arctic seasonal cycles and long-term trends of aerosol properties from 10 observatories
Analysis of reduced and oxidized nitrogen-containing organic compounds at a coastal site in summer and winter
Evolution of source attributed organic aerosols and gases in a megacity of central China
Sources and processes of iron aerosols in a megacity in Eastern China
Reversible and irreversible gas-particle partitioning of dicarbonyl compounds observed in the real atmosphere
Linking Switzerland's PM10 and PM2.5 oxidative potential (OP) with emission sources
Mapping gaseous dimethylamine, trimethylamine, ammonia, and their particulate counterparts in marine atmospheres of China’s marginal seas – Part 2: Spatiotemporal heterogeneity, causes, and hypothesis
Single-particle characterization of polycyclic aromatic hydrocarbons in background air in northern Europe
Regional heterogeneities in the emission of airborne primary sugar compounds and biogenic secondary organic aerosols in the East Asian outflow: evidence for coal combustion as a source of levoglucosan
Measurement report: Hygroscopic growth of ambient fine particles measured at five sites of China
Influence of organic aerosol molecular composition on particle absorptive properties in autumn Beijing
The importance of alkyl nitrates and sea ice emissions to atmospheric NOx sources and cycling in the summertime Southern Ocean marine boundary layer
Field observational constraints on the controllers in glyoxal (CHOCHO) reactive uptake to aerosol
Polycyclic aromatic hydrocarbons (PAHs) and their alkylated-, nitro- and oxy-derivatives in the atmosphere over the Mediterranean and Middle East seas
Measurement report: Particle-size-dependent fluorescence properties of water-soluble organic compounds (WSOCs) and their atmospheric implications for the aging of WSOCs
Molecular Characteristics of Organosulfur Compounds in Guangzhou, South China: Heterogeneous Secondary Reactions Drivers the Molecular Distribution
Impact of non-ideality on reconstructing spatial and temporal variations in aerosol acidity with multiphase buffer theory
Mercury isotopic compositions in fine particles and offshore surface seawater in a coastal area of East China: implications for Hg sources and atmospheric transformations
Real-time chemical speciation and source apportionment of organic aerosol components in Delhi, India, using extractive electrospray ionization mass spectrometry
Urban aerosol chemistry at a land–water transition site during summer – Part 2: Aerosol pH and liquid water content
First insights into northern Africa high-altitude background aerosol chemical composition and source influences
Impact of dry intrusion events on the composition and mixing state of particles during the winter Aerosol and Cloud Experiment in the Eastern North Atlantic (ACE-ENA)
Diverse mixing states of amine-containing single particles in Nanjing, China
Long-range transport of anthropogenic air pollutants into the marine air: insight into fine particle transport and chloride depletion on sea salts
Response of atmospheric composition to COVID-19 lockdown measures during spring in the Paris region (France)
Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest
Origin of water-soluble organic aerosols at the Maïdo high-altitude observatory, Réunion Island, in the tropical Indian Ocean
Sources and nature of ice-nucleating particles in the free troposphere at Jungfraujoch in winter 2017
Spatiotemporal variability in the oxidative potential of ambient fine particulate matter in the Midwestern United States
Measurement report: Spatiotemporal and policy-related variations of PM2.5 composition and sources during 2015–2019 at multiple sites in a Chinese megacity
Contribution of combustion Fe in marine aerosols over the northwestern Pacific estimated by Fe stable isotope ratios
Fluorescent biological aerosol particles over the central Pacific Ocean: covariation with ocean surface biological activity indicators
Dramatic changes in Harbin aerosol during 2018–2020: the roles of open burning policy and secondary aerosol formation
Time-dependent source apportionment of submicron organic aerosol for a rural site in an alpine valley using a rolling positive matrix factorisation (PMF) window
Characterization of non-refractory (NR) PM1 and source apportionment of organic aerosol in Kraków, Poland
Sources of black carbon at residential and traffic environments obtained by two source apportionment methods
Junjun Deng, Hao Ma, Xinfeng Wang, Shujun Zhong, Zhimin Zhang, Jialei Zhu, Yanbing Fan, Wei Hu, Libin Wu, Xiaodong Li, Lujie Ren, Chandra Mouli Pavuluri, Xiaole Pan, Yele Sun, Zifa Wang, Kimitaka Kawamura, and Pingqing Fu
Atmos. Chem. Phys., 22, 6449–6470, https://doi.org/10.5194/acp-22-6449-2022, https://doi.org/10.5194/acp-22-6449-2022, 2022
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Light-absorbing brown carbon (BrC) plays an important role in climate change and atmospheric chemistry. Here we investigated the seasonal and diurnal variations in water-soluble BrC in PM2.5 in the megacity Tianjin in coastal China. Results of the source apportionments from the combination with organic molecular compositions and optical properties of water-soluble BrC reveal a large contribution from primary bioaerosol particles to BrC in the urban atmosphere.
Fanlei Meng, Yibo Zhang, Jiahui Kang, Mathew R. Heal, Stefan Reis, Mengru Wang, Lei Liu, Kai Wang, Shaocai Yu, Pengfei Li, Jing Wei, Yong Hou, Ying Zhang, Xuejun Liu, Zhenling Cui, Wen Xu, and Fusuo Zhang
Atmos. Chem. Phys., 22, 6291–6308, https://doi.org/10.5194/acp-22-6291-2022, https://doi.org/10.5194/acp-22-6291-2022, 2022
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PM2.5 pollution is a pressing environmental issue threatening human health and food security globally. We combined a meta-analysis of nationwide measurements and air quality modeling to identify efficiency gains by striking a balance between controlling NH3 and acid gas emissions. Persistent secondary inorganic aerosol pollution in China is limited by acid gas emissions, while an additional control on NH3 emissions would become more important as reductions in SO2 and NOx emissions progress.
Huiyizhe Zhao, Zhenchuan Niu, Weijian Zhou, Sen Wang, Xue Feng, Shugang Wu, Xuefeng Lu, and Hua Du
Atmos. Chem. Phys., 22, 6255–6274, https://doi.org/10.5194/acp-22-6255-2022, https://doi.org/10.5194/acp-22-6255-2022, 2022
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In this study, we investigated the characteristics and changes in the sources of carbonaceous aerosols in northern Chinese cities using dual-carbon isotopes (13C and 14C) and levoglucosan during 2018 to 2019 and compared them with the research in previous decades. The results show that the contribution of fossil sources has decreased (6–16%) significantly, and non-fossil sources have become the main part of carbonaceous aerosols, which verified the effectiveness of air quality management.
Petra Pokorná, Naděžda Zíková, Petr Vodička, Radek Lhotka, Saliou Mbengue, Adéla Holubová Šmejkalová, Véronique Riffault, Jakub Ondráček, Jaroslav Schwarz, and Vladimír Ždímal
Atmos. Chem. Phys., 22, 5829–5858, https://doi.org/10.5194/acp-22-5829-2022, https://doi.org/10.5194/acp-22-5829-2022, 2022
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By examining individual episodes of high mass and number concentrations, we show that the seasonality in the physicochemical properties of aerosol particles was caused by the sources' diversity and was related to the different air masses and meteorology. We also confirmed the relation between particle size and age that is reflected in oxidation state and shape (difference in densities; effective vs. material). The results have general validity and thus transcend the study regional character.
Yange Deng, Hiroaki Fujinari, Hikari Yai, Kojiro Shimada, Yuzo Miyazaki, Eri Tachibana, Dhananjay K. Deshmukh, Kimitaka Kawamura, Tomoki Nakayama, Shiori Tatsuta, Mingfu Cai, Hanbing Xu, Fei Li, Haobo Tan, Sho Ohata, Yutaka Kondo, Akinori Takami, Shiro Hatakeyama, and Michihiro Mochida
Atmos. Chem. Phys., 22, 5515–5533, https://doi.org/10.5194/acp-22-5515-2022, https://doi.org/10.5194/acp-22-5515-2022, 2022
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Offline analyses of the hygroscopicity and composition of atmospheric aerosols are complementary to online analyses in view of the applicability to broader sizes, specific compound groups, and investigations at remote sites. This offline study characterized the composition of water-soluble matter in aerosols and their humidity-dependent hygroscopicity on Okinawa, a receptor site of East Asian outflow. Further, comparison with online analyses showed the appropriateness of the offline method.
Manuela van Pinxteren, Tiera-Brandy Robinson, Sebastian Zeppenfeld, Xianda Gong, Enno Bahlmann, Khanneh Wadinga Fomba, Nadja Triesch, Frank Stratmann, Oliver Wurl, Anja Engel, Heike Wex, and Hartmut Herrmann
Atmos. Chem. Phys., 22, 5725–5742, https://doi.org/10.5194/acp-22-5725-2022, https://doi.org/10.5194/acp-22-5725-2022, 2022
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A class of marine particles (transparent exopolymer particles, TEPs) that is ubiquitously found in the world oceans was measured for the first time in ambient marine aerosol particles and marine cloud waters in the tropical Atlantic Ocean. TEPs are likely to have good properties for influencing clouds. We show that TEPs are transferred from the ocean to the marine atmosphere via sea-spray formation and our results suggest that they can also form directly in aerosol particles and in cloud water.
Daniel A. Knopf, Joseph C. Charnawskas, Peiwen Wang, Benny Wong, Jay M. Tomlin, Kevin A. Jankowski, Matthew Fraund, Daniel P. Veghte, Swarup China, Alexander Laskin, Ryan C. Moffet, Mary K. Gilles, Josephine Y. Aller, Matthew A. Marcus, Shira Raveh-Rubin, and Jian Wang
Atmos. Chem. Phys., 22, 5377–5398, https://doi.org/10.5194/acp-22-5377-2022, https://doi.org/10.5194/acp-22-5377-2022, 2022
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Marine boundary layer aerosols collected in the remote region of the eastern North Atlantic induce immersion freezing and deposition ice nucleation under typical mixed-phase and cirrus cloud conditions. Corresponding ice nucleation parameterizations for model applications have been derived. Chemical imaging of ambient aerosol and ice-nucleating particles demonstrates that the latter is dominated by sea salt and organics while also representing a major particle type in the particle population.
Saehee Lim, Meehye Lee, Joel Savarino, and Paolo Laj
Atmos. Chem. Phys., 22, 5099–5115, https://doi.org/10.5194/acp-22-5099-2022, https://doi.org/10.5194/acp-22-5099-2022, 2022
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We determined δ15N(NO3−) and Δ17O(NO3−) of PM2.5 in Seoul during 2018–2019 and estimated quantitatively the contribution of oxidation pathways to NO3− formation and NOx emission sources. The nighttime pathway played a significant role in NO3− formation during the winter, and its contribution further increased up to 70 % on haze days when PM2.5 was greater than 75 µg m−3. Vehicle emissions were confirmed as a main NO3− source with an increasing contribution from coal combustion in winter.
Yee Ka Wong, Kin Man Liu, Claisen Yeung, Kenneth K. M. Leung, and Jian Zhen Yu
Atmos. Chem. Phys., 22, 5017–5031, https://doi.org/10.5194/acp-22-5017-2022, https://doi.org/10.5194/acp-22-5017-2022, 2022
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Coarse particulate matter (PM) has been shown to cause adverse health impacts, but compared to PM2.5, the source of coarse PM is less studied through field measurements. We collected chemical composition data for coarse PM in Hong Kong for a 1-year period. Using statistical models, we found that regional transport of fugitive dust is responsible for the elevated coarse PM. This work sets an example of how field measurements can be effectively utilized for evidence-based policymaking.
Ziyong Guo, Yuxiang Yang, Xiaodong Hu, Xiaocong Peng, Yuzhen Fu, Wei Sun, Guohua Zhang, Duohong Chen, Xinhui Bi, Xinming Wang, and Ping'an Peng
Atmos. Chem. Phys., 22, 4827–4839, https://doi.org/10.5194/acp-22-4827-2022, https://doi.org/10.5194/acp-22-4827-2022, 2022
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We show that in-cloud aqueous processing facilitates the formation of brown carbon (BrC), based on the simultaneous measurements of the light-absorption properties of the cloud residuals, cloud interstitial, and cloud-free particles. While extensive laboratory evidence indicated the formation of BrC in aqueous phase, our study represents the first attempt to show the possibility in real clouds, which would have potential implications in the atmospheric evolution and radiation forcing of BrC.
Han Zang, Yue Zhao, Juntao Huo, Qianbiao Zhao, Qingyan Fu, Yusen Duan, Jingyuan Shao, Cheng Huang, Jingyu An, Likun Xue, Ziyue Li, Chenxi Li, and Huayun Xiao
Atmos. Chem. Phys., 22, 4355–4374, https://doi.org/10.5194/acp-22-4355-2022, https://doi.org/10.5194/acp-22-4355-2022, 2022
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Particulate nitrate plays an important role in wintertime haze pollution in eastern China, yet quantitative constraints on detailed nitrate formation mechanisms remain limited. Here we quantified the contributions of the heterogeneous N2O5 hydrolysis (66 %) and gas-phase OH + NO2 reaction (32 %) to nitrate formation in this region and identified the atmospheric oxidation capacity (i.e., availability of O3 and OH radicals) as the driving factor of nitrate formation from both processes.
Laura Tositti, Erika Brattich, Claudio Cassardo, Pietro Morozzi, Alessandro Bracci, Angela Marinoni, Silvana Di Sabatino, Federico Porcù, and Alessandro Zappi
Atmos. Chem. Phys., 22, 4047–4073, https://doi.org/10.5194/acp-22-4047-2022, https://doi.org/10.5194/acp-22-4047-2022, 2022
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We present a thorough investigation of an anomalous transport of mineral dust over a region renowned for excess airborne particulate matter, the Italian Po Valley, which occurred in late March 2021. Both the origin of this dust outbreak, which was localized in central Asia (i.e., the so-called Aralkum Desert), and the upstream synoptic conditions, investigated here in extreme detail using multiple integrated observations including in situ measurements and remote sensing, were atypical.
Christine D. Groot Zwaaftink, Wenche Aas, Sabine Eckhardt, Nikolaos Evangeliou, Paul Hamer, Mona Johnsrud, Arve Kylling, Stephen M. Platt, Kerstin Stebel, Hilde Uggerud, and Karl Espen Yttri
Atmos. Chem. Phys., 22, 3789–3810, https://doi.org/10.5194/acp-22-3789-2022, https://doi.org/10.5194/acp-22-3789-2022, 2022
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We investigate causes of a poor-air-quality episode in northern Europe in October 2020 during which EU health limits for air quality were vastly exceeded. Such episodes may trigger measures to improve air quality. Analysis based on satellite observations, transport simulations, and surface observations revealed two sources of pollution. Emissions of mineral dust in Central Asia and biomass burning in Ukraine arrived almost simultaneously in Norway, and transport continued into the Arctic.
Adrien Deroubaix, Laurent Menut, Cyrille Flamant, Peter Knippertz, Andreas H. Fink, Anneke Batenburg, Joel Brito, Cyrielle Denjean, Cheikh Dione, Régis Dupuy, Valerian Hahn, Norbert Kalthoff, Fabienne Lohou, Alfons Schwarzenboeck, Guillaume Siour, Paolo Tuccella, and Christiane Voigt
Atmos. Chem. Phys., 22, 3251–3273, https://doi.org/10.5194/acp-22-3251-2022, https://doi.org/10.5194/acp-22-3251-2022, 2022
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During the summer monsoon in West Africa, pollutants emitted in urbanized areas modify cloud cover and precipitation patterns. We analyze these patterns with the WRF-CHIMERE model, integrating the effects of aerosols on meteorology, based on the numerous observations provided by the Dynamics-Aerosol-Climate-Interactions campaign. This study adds evidence to recent findings that increased pollution levels in West Africa delay the breakup time of low-level clouds and reduce precipitation.
Julia Schmale, Sangeeta Sharma, Stefano Decesari, Jakob Pernov, Andreas Massling, Hans-Christen Hansson, Knut von Salzen, Henrik Skov, Elisabeth Andrews, Patricia K. Quinn, Lucia M. Upchurch, Konstantinos Eleftheriadis, Rita Traversi, Stefania Gilardoni, Mauro Mazzola, James Laing, and Philip Hopke
Atmos. Chem. Phys., 22, 3067–3096, https://doi.org/10.5194/acp-22-3067-2022, https://doi.org/10.5194/acp-22-3067-2022, 2022
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Long-term data sets of Arctic aerosol properties from 10 stations across the Arctic provide evidence that anthropogenic influence on the Arctic atmospheric chemical composition has declined in winter, a season which is typically dominated by mid-latitude emissions. The number of significant trends in summer is smaller than in winter, and overall the pattern is ambiguous with some significant positive and negative trends. This reflects the mixed influence of natural and anthropogenic emissions.
Jenna C. Ditto, Jo Machesky, and Drew R. Gentner
Atmos. Chem. Phys., 22, 3045–3065, https://doi.org/10.5194/acp-22-3045-2022, https://doi.org/10.5194/acp-22-3045-2022, 2022
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We analyzed gases and aerosols sampled in summer and winter in a coastal region that is often downwind of urban areas and observed large contributions of nitrogen-containing organic compounds influenced by a mix of biogenic, anthropogenic, and/or marine sources as well as photochemical and aqueous-phase atmospheric processes. The results show the prevalence of key reduced and oxidized nitrogen functional groups and advance knowledge on the chemical structure of nitrogen-containing compounds.
Siyuan Li, Dantong Liu, Shaofei Kong, Yangzhou Wu, Kang Hu, Huang Zheng, Yi Cheng, Shurui Zheng, Xiaotong Jiang, Shuo Ding, Dawei Hu, Quan Liu, Ping Tian, Delong Zhao, and Jiujiang Sheng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-141, https://doi.org/10.5194/acp-2022-141, 2022
Revised manuscript accepted for ACP
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The understanding for secondary organic aerosols is hindered by the aerosol-gas evolution by different oxidation mechanisms. By concurrently online measuring detailed mass spectra of aerosol and gas phases in a megacity, we identified the primary and secondary source sectors, and investigated the transformation between gas and aerosol phases influenced by photooxidation and moisture. The results will help understand the respective evolution of major sources in a typical urban environment.
Yanhong Zhu, Weijun Li, Yue Wang, Jian Zhang, Lei Liu, Liang Xu, Jingsha Xu, Jinhui Shi, Longyi Shao, Pingqing Fu, Daizhou Zhang, and Zongbo Shi
Atmos. Chem. Phys., 22, 2191–2202, https://doi.org/10.5194/acp-22-2191-2022, https://doi.org/10.5194/acp-22-2191-2022, 2022
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The solubilities of iron in fine particles in a megacity in Eastern China were studied under haze, fog, dust, clear, and rain weather conditions. For the first time, a receptor model was used to quantify the sources of dissolved and total iron aerosol. Microscopic analysis further confirmed the aging of iron aerosol during haze and fog conditions that facilitated dissolution of insoluble iron.
Jingcheng Hu, Zhongming Chen, Xuan Qin, and Ping Dong
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-86, https://doi.org/10.5194/acp-2022-86, 2022
Revised manuscript accepted for ACP
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In this study, glyoxal and methylglyoxal, two important carbonyl compounds in the atmosphere, in the gas and particle phase were simultaneously measured in five field observations. We find that irreversible pathways play a dominant role with a proportion of more than 90 % in the partitioning process and we recommend the uptake coefficient for dicarbonyls in the real atmosphere. We expect this study could make contribution to the model simulation of secondary organic aerosols formation.
Stuart Kenneth Grange, Gaëlle Uzu, Samuël Weber, Jean-Luc Jaffrezo, and Christoph Hueglin
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-979, https://doi.org/10.5194/acp-2021-979, 2022
Revised manuscript accepted for ACP
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Oxidative potential (OP), a biologically relevant metric for particulate matter (PM), was linked to PM10 and PM2.5 sources and constituents across Switzerland between 2018 and 2019. Wood burning and non-exhaust traffic emissions were identified as key processes which led to enhanced OP. Therefore, the make up of the PM mix was very important for OP. The results highlight the importance of management of wood burning and non-exhaust emissions to reduce OP, and presumably biological harm.
Yating Gao, Dihui Chen, Yanjie Shen, Yang Gao, Huiwang Gao, and Xiaohong Yao
Atmos. Chem. Phys., 22, 1515–1528, https://doi.org/10.5194/acp-22-1515-2022, https://doi.org/10.5194/acp-22-1515-2022, 2022
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This study focuses on spatiotemporal heterogeneity of observed gaseous amines, NH3, their particulate counterparts in PM2.5 over different sea zones, and the disproportional release of alkaline gases and corresponding particulate counterparts from seawater in the sea zones in terms of different extents of enrichment of TMAH+ and DMAH+ in the sea surface microlayer (SML). A novel hypothesis is delivered.
Johannes Passig, Julian Schade, Robert Irsig, Thomas Kröger-Badge, Hendryk Czech, Thomas Adam, Henrik Fallgren, Jana Moldanova, Martin Sklorz, Thorsten Streibel, and Ralf Zimmermann
Atmos. Chem. Phys., 22, 1495–1514, https://doi.org/10.5194/acp-22-1495-2022, https://doi.org/10.5194/acp-22-1495-2022, 2022
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The single-particle distribution of health-relevant polycyclic aromatic hydrocarbons (PAHs) was studied at the Swedish coast in autumn. We found PAHs bound to long-range transported particles from eastern and central Europe and also from ship emissions and local sources. This is the first field study using a new technology revealing single-particle data from both inorganic components and PAHs. We discuss PAH profiles that are indicative of several sources and atmospheric aging processes.
Md. Mozammel Haque, Yanlin Zhang, Srinivas Bikkina, Meehye Lee, and Kimitaka Kawamura
Atmos. Chem. Phys., 22, 1373–1393, https://doi.org/10.5194/acp-22-1373-2022, https://doi.org/10.5194/acp-22-1373-2022, 2022
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We attempt to understand the current state of East Asian organic aerosols with both the molecular marker approach and 14° C data of carbonaceous components. A significant positive correlation of nonfossil- and fossil-derived organic carbon with levoglucosan suggests the importance of biomass burning (BB) and coal combustion sources in the East Asian outflow. Thus, attribution of ambient levoglucosan levels over the western North Pacific to the impact of BB emission may cause large uncertainty.
Lu Chen, Fang Zhang, Dongmei Zhang, Xinming Wang, Wei Song, Jieyao Liu, Jingye Ren, Sihui Jiang, Xue Li, and Zhanqing Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-912, https://doi.org/10.5194/acp-2021-912, 2022
Revised manuscript accepted for ACP
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Aerosol hygroscopicity is critical when evaluating its effect on visibility and climate. Here, the size-resolved particle hygroscopicity at five sites of China is characterized using field measurements. We show distinct particles hygroscopic behaviors during pollution evolution among the five sites. Moreover, different hygroscopic behaviors during NPF events were also observed. The dataset is helpful for understanding the spatial variability of particles composition and formation mechanisms.
Jing Cai, Cheng Wu, Jiandong Wang, Wei Du, Feixue Zheng, Simo Hakala, Xiaolong Fan, Biwu Chu, Lei Yao, Zemin Feng, Yongchun Liu, Yele Sun, Jun Zheng, Chao Yan, Federico Bianchi, Markku Kulmala, Claudia Mohr, and Kaspar R. Daellenbach
Atmos. Chem. Phys., 22, 1251–1269, https://doi.org/10.5194/acp-22-1251-2022, https://doi.org/10.5194/acp-22-1251-2022, 2022
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This study investigates the connection between organic aerosol (OA) molecular composition and particle absorptive properties in autumn in Beijing. We find that the molecular properties of OA compounds in different episodes influence particle light absorption properties differently: the light absorption enhancement of black carbon and light absorption coefficient of brown carbon were mostly related to more oxygenated OA (low C number and four O atoms) and aromatics/nitro-aromatics, respectively.
Jessica M. Burger, Julie Granger, Emily Joyce, Meredith G. Hastings, Kurt A. M. Spence, and Katye E. Altieri
Atmos. Chem. Phys., 22, 1081–1096, https://doi.org/10.5194/acp-22-1081-2022, https://doi.org/10.5194/acp-22-1081-2022, 2022
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The nitrogen (N) isotopic composition of atmospheric nitrate in the Southern Ocean (SO) marine boundary layer (MBL) reveals the importance of oceanic alkyl nitrate emissions as a source of reactive N to the atmosphere. The oxygen isotopic composition suggests peroxy radicals contribute up to 63 % to NO oxidation and that nitrate forms via the OH pathway. This work improves our understanding of reactive N sources and cycling in a remote marine region, a proxy for the pre-industrial atmosphere.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Marco Wietzoreck, Marios Kyprianou, Benjamin A. Musa Bandowe, Siddika Celik, John N. Crowley, Frank Drewnick, Philipp Eger, Nils Friedrich, Minas Iakovides, Petr Kukučka, Jan Kuta, Barbora Nežiková, Petra Pokorná, Petra Přibylová, Roman Prokeš, Roland Rohloff, Ivan Tadic, Sebastian Tauer, Jake Wilson, Hartwig Harder, Jos Lelieveld, Ulrich Pöschl, Euripides G. Stephanou, and Gerhard Lammel
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-32, https://doi.org/10.5194/acp-2022-32, 2022
Revised manuscript accepted for ACP
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A unique dataset of concentrations and sources of PAHs and their alkylated, oxygenated and nitrated derivatives, in total 74 individual species, in the marine atmosphere is presented. Exposure to these substances poses a major health risk. We found very low concentrations over the Arabian Sea, while both local and long-range transported pollution caused elevated levels over the Mediterranean Sea and the Arabian Gulf.
Juanjuan Qin, Jihua Tan, Xueming Zhou, Yanrong Yang, Yuanyuan Qin, Xiaobo Wang, Shaoxuan Shi, Kang Xiao, and Xinming Wang
Atmos. Chem. Phys., 22, 465–479, https://doi.org/10.5194/acp-22-465-2022, https://doi.org/10.5194/acp-22-465-2022, 2022
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Water-soluble organic compounds (WSOCs) play important roles in atmospheric particle formation, migration, and transformation processes. In this work, size-segregated atmospheric particles were collected in a rural area of Beijing, and 3D fluorescence spectroscopy was used to investigate the optical properties of WSOCs as a means of inferring information about their atmospheric sources. It was found that these data could efficiently reveal the secondary transformation processes of WSOCs.
Hongxing Jiang, Jun Li, Jiao Tang, Min Cui, Shizhen Zhao, Yangzhi Mo, Chongguo Tian, Xiangyun Zhang, Bin Jiang, Yuhong Liao, Yinjun Chen, and Gan Zhang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1069, https://doi.org/10.5194/acp-2021-1069, 2022
Revised manuscript accepted for ACP
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We conducted field observation employing Fourier transform ion cyclotron resonance mass spectrometry to characterize the molecular composition and major formation pathways or sources of organosulfur compounds in Guangzhou, where is heavily influenced by biogenic−anthropogenic interactions and has high relative humidity and temperature. We suggested that heterogeneous reactions such as SO2 uptake and heterogeneous oxidations are important to the molecular variations of organosulfur compounds.
Guangjie Zheng, Hang Su, Siwen Wang, Andrea Pozzer, and Yafang Cheng
Atmos. Chem. Phys., 22, 47–63, https://doi.org/10.5194/acp-22-47-2022, https://doi.org/10.5194/acp-22-47-2022, 2022
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The recently proposed multiphase buffer theory provides a framework to reconstruct long-term trends and spatial variations in aerosol pH, while non-ideality is a major limitation for its broad applications. Here we proposed a parameterization method to estimate the impact of non-ideality and validated it against long-term observations and global simulations. With this method, the multiphase buffer theory can reproduce well aerosol pH variations estimated by comprehensive thermodynamic models.
Lingling Xu, Jiayan Shi, Yuping Chen, Yanru Zhang, Mengrong Yang, Yanting Chen, Liqian Yin, Lei Tong, Hang Xiao, and Jinsheng Chen
Atmos. Chem. Phys., 21, 18543–18555, https://doi.org/10.5194/acp-21-18543-2021, https://doi.org/10.5194/acp-21-18543-2021, 2021
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Mercury (Hg) isotopic compositions in aerosols are the mixed results of emission sources and atmospheric processes. This study presents Hg isotopic compositions in PM2.5 from different types of locations and total Hg from offshore surface seawater. The results indicate that atmospheric transformations induce significant mass independent fractionation of Hg isotopes, which obscures Hg isotopic signatures of initial emissions.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-1033, https://doi.org/10.5194/acp-2021-1033, 2021
Revised manuscript accepted for ACP
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionisation time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of OA, in particular the SOA fraction. Here, we are able to apportion not only POA but also SOA to specific sources, which is done for the first time in Delhi.
Michael A. Battaglia Jr., Nicholas Balasus, Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 18271–18281, https://doi.org/10.5194/acp-21-18271-2021, https://doi.org/10.5194/acp-21-18271-2021, 2021
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This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
Nabil Deabji, Khanneh Wadinga Fomba, Souad El Hajjaji, Abdelwahid Mellouki, Laurent Poulain, Sebastian Zeppenfeld, and Hartmut Herrmann
Atmos. Chem. Phys., 21, 18147–18174, https://doi.org/10.5194/acp-21-18147-2021, https://doi.org/10.5194/acp-21-18147-2021, 2021
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Mountain and high-altitude sites provide representative data for the lower free troposphere, various pathways for aerosol interactions, and changing boundary layer heights useful in understanding atmospheric composition. However, only few studies exist in African regions despite diversity in both natural and anthropogenic emissions. This study provides detailed atmospheric studies in the northern African high-altitude region.
Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
Atmos. Chem. Phys., 21, 18123–18146, https://doi.org/10.5194/acp-21-18123-2021, https://doi.org/10.5194/acp-21-18123-2021, 2021
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Analysis of individual atmospheric particles shows that aerosol transported from North America during meteorological dry intrusion episodes may have a substantial impact on the mixing state and particle-type population over the mid-Atlantic, as organic contribution and particle-type diversity are significantly enhanced during these periods. These observations need to be considered in current atmospheric models.
Qi En Zhong, Chunlei Cheng, Zaihua Wang, Lei Li, Mei Li, Dafeng Ge, Lei Wang, Yuanyuan Li, Wei Nie, Xuguang Chi, Aijun Ding, Suxia Yang, Duohong Chen, and Zhen Zhou
Atmos. Chem. Phys., 21, 17953–17967, https://doi.org/10.5194/acp-21-17953-2021, https://doi.org/10.5194/acp-21-17953-2021, 2021
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Particulate amines play important roles in new particle formation, aerosol acidity, and hygroscopicity. Most of the field observations did not distinguish the different behavior of each type amine under the same ambient influencing factors. In this study, two amine-containing single particles exhibited different mixing states and disparate enrichment of secondary organics, which provide insight into the discriminated fates of organics during the formation and evolution processes.
Liang Xu, Xiaohuan Liu, Huiwang Gao, Xiaohong Yao, Daizhou Zhang, Lei Bi, Lei Liu, Jian Zhang, Yinxiao Zhang, Yuanyuan Wang, Qi Yuan, and Weijun Li
Atmos. Chem. Phys., 21, 17715–17726, https://doi.org/10.5194/acp-21-17715-2021, https://doi.org/10.5194/acp-21-17715-2021, 2021
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We quantified different types of marine aerosols and explored the Cl depletion of sea salt aerosol (SSA) in the eastern China seas and the northwestern Pacific Ocean. We found that anthropogenic acidic gases in the troposphere were transported longer distances compared to the anthropogenic aerosols and could significantly impact remote marine aerosols. Meanwhile, variations of chloride depletion in SSA can serve as a potential indicator for anthropogenic gaseous pollutants in remote marine air.
Jean-Eudes Petit, Jean-Charles Dupont, Olivier Favez, Valérie Gros, Yunjiang Zhang, Jean Sciare, Leila Simon, François Truong, Nicolas Bonnaire, Tanguy Amodeo, Robert Vautard, and Martial Haeffelin
Atmos. Chem. Phys., 21, 17167–17183, https://doi.org/10.5194/acp-21-17167-2021, https://doi.org/10.5194/acp-21-17167-2021, 2021
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The COVID-19 outbreak led to lockdowns at national scales in spring 2020. Large cuts in emissions occurred, but the quantitative assessment of their role from observations is hindered by weather and interannual variability. That is why we developed an innovative methodology in order to best characterize the impact of lockdown on atmospheric chemistry. We find that a local decrease in traffic-related pollutants triggered a decrease of secondary aerosols and an increase in ozone.
Alexander A. T. Bui, Henry W. Wallace, Sarah Kavassalis, Hariprasad D. Alwe, James H. Flynn, Matt H. Erickson, Sergio Alvarez, Dylan B. Millet, Allison L. Steiner, and Robert J. Griffin
Atmos. Chem. Phys., 21, 17031–17050, https://doi.org/10.5194/acp-21-17031-2021, https://doi.org/10.5194/acp-21-17031-2021, 2021
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Differences in atmospheric species above and below a forest canopy provide insight into the relative importance of local mixing, long-range transport, and chemical processes in determining vertical gradients in atmospheric particles in a forested environment. This helps in understanding the flux of climate-relevant material out of the forest to the atmosphere. We studied this in a remote forest using vertically resolved measurements of gases and particles.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Haoran Yu, Joseph Varghese Puthussery, Yixiang Wang, and Vishal Verma
Atmos. Chem. Phys., 21, 16363–16386, https://doi.org/10.5194/acp-21-16363-2021, https://doi.org/10.5194/acp-21-16363-2021, 2021
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We assessed the oxidative potential (OP) of ambient PM2.5 collected from many sites in the US Midwest through multiple acellular endpoints. Compared to homogeneously distributed PM2.5, OP showed higher spatiotemporal variation. Poor correlations for the regression between mass and OP indicated a limited role of mass in determining the OP. Moreover, weak correlations among different OP endpoints justify the need for using multiple assays to determine oxidative levels of particles.
Xinyao Feng, Yingze Tian, Qianqian Xue, Danlin Song, Fengxia Huang, and Yinchang Feng
Atmos. Chem. Phys., 21, 16219–16235, https://doi.org/10.5194/acp-21-16219-2021, https://doi.org/10.5194/acp-21-16219-2021, 2021
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This study focused on PM2.5 compositions and sources and explored their spatiotemporal and policy-related variations based on observation at 19 sites during wintertime of 2015–2019 in a fast-developing megacity. We found that PM2.5 compositions for the outermost zone in 2019 were similar to those for the core zone 2 or 3 years ago. Percentage contributions of coal and biomass combustion dramatically declined in the core zone, while the traffic source showed an increasing trend.
Minako Kurisu, Kohei Sakata, Mitsuo Uematsu, Akinori Ito, and Yoshio Takahashi
Atmos. Chem. Phys., 21, 16027–16050, https://doi.org/10.5194/acp-21-16027-2021, https://doi.org/10.5194/acp-21-16027-2021, 2021
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Aerosol iron (Fe) input can enhance oceanic primary production. We analyzed Fe isotope ratios of size-fractionated aerosols over the northwestern Pacific to evaluate the contribution of natural and combustion Fe. It was found that combustion Fe was an important soluble Fe source in marine aerosols and possibly in surface seawater when air masses were from East Asia. This study shows the applicability of Fe isotope ratios for a more quantitative understanding of the Fe cycle in the surface ocean.
Kaori Kawana, Kazuhiko Matsumoto, Fumikazu Taketani, Takuma Miyakawa, and Yugo Kanaya
Atmos. Chem. Phys., 21, 15969–15983, https://doi.org/10.5194/acp-21-15969-2021, https://doi.org/10.5194/acp-21-15969-2021, 2021
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Atmospheric autofluorescent particles observed over the central Pacific Ocean were identified as bioaerosols from comparisons to a DNA-nuclear-staining method. Their number concentrations in the pristine marine air masses showed high correlations with concentrations of bacteria and transparent exopolymer particles in the surface seawater, providing strong evidence of their marine origins. We propose equations to derive the atmospheric bioaerosol number concentrations from oceanic parameters.
Yuan Cheng, Qin-qin Yu, Jiu-meng Liu, Xu-bing Cao, Ying-jie Zhong, Zhen-yu Du, Lin-lin Liang, Guan-nan Geng, Wan-li Ma, Hong Qi, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 21, 15199–15211, https://doi.org/10.5194/acp-21-15199-2021, https://doi.org/10.5194/acp-21-15199-2021, 2021
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Open burning policies in Heilongjiang Province experienced a rapid transition during 2018 to 2020. This study evaluated the responses of PM2.5 pollution to this transition and suggested that neither of the policies could be considered successful. In addition, heterogeneous reactions were found to be at play in secondary aerosol formation, even in the frigid atmosphere in Heilongjiang. The unique haze in northeast China deserves more attention.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Sanna Saarikoski, Jarkko V. Niemi, Minna Aurela, Liisa Pirjola, Anu Kousa, Topi Rönkkö, and Hilkka Timonen
Atmos. Chem. Phys., 21, 14851–14869, https://doi.org/10.5194/acp-21-14851-2021, https://doi.org/10.5194/acp-21-14851-2021, 2021
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This study presents the main sources of black carbon (BC) at two urban environments. The largest fraction of BC originated from biomass burning at the residential site (38 %) and from vehicular emissions (57 %) in the street canyon. Also, a significant fraction of BC was associated with urban background or long-range transport. The data are needed by modelers and authorities when assessing climate and air quality impact of BC as well as directing the emission legislation and mitigation actions.