Articles | Volume 22, issue 4
https://doi.org/10.5194/acp-22-2553-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-22-2553-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
25 Feb 2022
Research article |
| 25 Feb 2022
| 25 Feb 2022
Urban inland wintertime N2O5 and ClNO2 influenced by snow-covered ground, air turbulence, and precipitation
Kathryn D. Kulju
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
Stephen M. McNamara
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
Qianjie Chen
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
currently at: Department of Civil and Environmental Engineering, The
Hong Kong Polytechnic University, Hong Kong SAR, China
Hannah S. Kenagy
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
Jacinta Edebeli
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
Paul Scherrer Institut, 5232 Villigen, Switzerland
Jose D. Fuentes
Department of Meteorology and Atmospheric Science, Pennsylvania State
University, University Park, Pennsylvania 16802, USA
Steven B. Bertman
Institute of the Environment and Sustainability, Western Michigan
University, Kalamazoo, Michigan 49008, USA
Department of Chemistry, University of Michigan, Ann Arbor, MI 48109,
USA
Department of Earth and Environmental Sciences, University of
Michigan, Ann Arbor, MI 48109, USA
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Patrick C. Taylor, Armin Sorooshian, Rei Ueyama, Sebastian Schmidt, Ihab Abboud, Quincy Allison, Kevin Barry, Sebastian Becker, Holly A. Bender, Joseph R. Bennett, James B. Blair, Niklas Bohn, Linette Boisvert, Matthew D. Brown, Roelof Bruintjes, Anthony Bucholtz, Megan Buzanowicz, Brian Cairns, Filippo Calì Quaglia, Eduard Chemyakin, Bo Chen, Gao Chen, Hong Chen, Yu-Wen Chen, Zezhen Cheng, Swarup China, Dan Chirica, Yonghoon Choi, Peter Colarco, Brian Collister, Ewan Crosbie, Maurice J. Cross, Janet Daniels, Paul DeMott, Joshua P. DiGangi, Alcide Giorgio di Sarra, Glenn S. Diskin, Erica K. Dolinar, Eva-Lou Edwards, Samuel Ephraim, Nikolaos Evangeliou, Romanos Foskinis, Francesca Gallo, Lan Gao, José Luis Gómez-Amo, Daisy Gonzalez, Christine Groot Zwaaftink, Pawan Gupta, Ivan Heckman, Michael Hendrickson, Miguel Ricardo A. Hilario, Ken Hirata, Michelle Hofton, Andrew L. Holen, Ulas Im, Alia L. Khan, Ralph Kahn, Alexei V. Korolev, Sonia Kreidenweis, Thomas Krumpen, Nathan Kurtz, Leslie Lait, Bradley Lamkin, Jack Landy, Nurun Nahar Lata, Paul Lawson, Samuel LeBlanc, Sean Leavor, Jing Li, Thorsten Markus, Hal Maring, Andreas H. Massling, Camille Mavis, Flynn McGinnity, Kerry Meyer, Gabriel Mojica, Richard H. Moore, Parker Morris, Giovanni Muscari, Vikas Nataraja, Amin R. Nehrir, Athanasios Nenes, Edward P. Nowottnick, Matteo Ottaviani, Chelsea Parker, Ryan Patnaude, Michael Perez, Russell J. Perkins, Colten Peterson, Alek Petty, Stevie Phothisane, Chris Polashenski, Kerri A. Pratt, Kayla M. Preisler, John Prytherch, David Rabine, Jens Redemann, Ju-Mee Ryoo, Joseph S. Schlosser, Vanessa Selimovic, Michael A. Shook, Morgan Silverman, Henrik Skov, Alexander Smirnov, Cassidy Soloff, Amy Solomon, Snorre Stamnes, Azusa Takeishi, David R. Thompson, K. Lee Thornhill, Rachel Tilling, Michael Tjernström, Monica Tosco, Pedro C. Valdelomar, David Van Gilst, Jian Wang, Zhien Wang, Andrzej Wasilewski, Manfred Wendisch, Brent Wilder, Edward L. Winstead, Albert Wu, Peng Xian, Lauren M. Zamora, Jiaoshi Zhang, Lei Zhang, Lu Zhang, Luke Ziemba, and Paquita Zuidema
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2026-241, https://doi.org/10.5194/essd-2026-241, 2026
Preprint under review for ESSD
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This article summarizes the data sets collected during the Arctic Radiation Cloud aerosol Sea ice Interaction eXperiment (ARCSIX), NASA's most comprehensive Arctic field campaign to date. The overarching goal was to quantify the contributions of surface, clouds, aerosol particles, and precipitation to summer sea ice melt. This paper describes the ARCSIX implementation including the flight strategy, instruments, complementary data sets, access, and usage details.
Jing Chen, Xianyi Sun, Chuang Qin, Jie Li, Qianjie Chen, and Xiao Fu
Atmos. Chem. Phys., 26, 9809–9826, https://doi.org/10.5194/acp-26-9809-2026, https://doi.org/10.5194/acp-26-9809-2026, 2026
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By incorporating an iron-mediated molecular chlorine (Cl2) formation pathway into the GEOS-Chem global atmospheric chemistry transport model, simulated surface Cl2 concentrations align better with observations. Reactive chlorine species increase substantially, thereby altering atmospheric oxidative capacity. Stronger oxidation elevates PM2.5 levels in polluted regions, especially in winter, underscoring the need to consider iron–halogen coupling chemistry in future air-quality mitigation.
Shengjin Xie, Xuelei Zhang, Aijun Xiu, Hong Qi, Shengrui Tong, Qianjie Chen, Chao Gao, Hongmei Zhao, Shichun Zhang, Stephen Dauda Yabo, Yiming Liu, Siting Li, and Mengduo Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-5338, https://doi.org/10.5194/egusphere-2025-5338, 2026
This preprint is open for discussion and under review for The Cryosphere (TC).
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This study examines how snow-covered surfaces affect air pollution in Northeast China. Using numerical simulations, we explore chlorine-related chemical reactions that generate reactive species, enhancing fine particles and ozone. Results show that snow-surface reactions drive nighttime pollutant accumulation and notably improve model performance, providing new insights into how snow and surface chemistry influence regional air quality.
Zhouxing Zou, Tianshu Chen, Qianjie Chen, Weihang Sun, Shichun Han, Zhuoyue Ren, Xinyi Li, Wei Song, Aoqi Ge, Qi Wang, Xiao Tian, Chenglei Pei, Xinming Wang, Yanli Zhang, and Tao Wang
Atmos. Chem. Phys., 25, 8147–8161, https://doi.org/10.5194/acp-25-8147-2025, https://doi.org/10.5194/acp-25-8147-2025, 2025
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We measured ambient OH and HO2* (HO2 and contribution from RO2, organic peroxyl radicals) concentrations at a subtropical rural site and compared our observations with model results. During warm periods, the model overestimated concentrations of OH and HO2, leading to overestimation of ozone and nitric acid production. Our findings highlight the need to better understand how OH and HO2 are formed and removed, which is important for accurate air quality and climate predictions.
Ursula A. Jongebloed, Jacob I. Chalif, Linia Tashmim, William C. Porter, Kelvin H. Bates, Qianjie Chen, Erich C. Osterberg, Bess G. Koffman, Jihong Cole-Dai, Dominic A. Winski, David G. Ferris, Karl J. Kreutz, Cameron P. Wake, and Becky Alexander
Atmos. Chem. Phys., 25, 4083–4106, https://doi.org/10.5194/acp-25-4083-2025, https://doi.org/10.5194/acp-25-4083-2025, 2025
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Marine phytoplankton emit dimethyl sulfide (DMS), which forms methanesulfonic acid (MSA) and sulfate. MSA concentrations in ice cores decreased over the industrial era, which has been attributed to pollution-driven changes in DMS chemistry. We use a model to investigate DMS chemistry compared to observations of DMS, MSA, and sulfate. We find that modeled DMS, MSA, and sulfate are influenced by pollution-sensitive oxidant concentrations, characterization of DMS chemistry, and other variables.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiia Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
Atmos. Chem. Phys., 25, 2207–2241, https://doi.org/10.5194/acp-25-2207-2025, https://doi.org/10.5194/acp-25-2207-2025, 2025
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Limited aerosol measurements in the central Arctic hinder our understanding of aerosol–climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Local wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
Mohammad Allouche, Vladislav I. Sevostianov, Einara Zahn, Mark A. Zondlo, Nelson Luís Dias, Gabriel G. Katul, Jose D. Fuentes, and Elie Bou-Zeid
Atmos. Chem. Phys., 24, 9697–9711, https://doi.org/10.5194/acp-24-9697-2024, https://doi.org/10.5194/acp-24-9697-2024, 2024
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The significance of surface–atmosphere exchanges of aerosol species to atmospheric composition is underscored by their rising concentrations that are modulating the Earth's climate and having detrimental consequences for human health and the environment. Estimating these exchanges, using field measurements, and offering alternative models are the aims here. Limitations in measuring some species misrepresent their actual exchanges, so our proposed models serve to better quantify them.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Zhouxing Zou, Qianjie Chen, Men Xia, Qi Yuan, Yi Chen, Yanan Wang, Enyu Xiong, Zhe Wang, and Tao Wang
Atmos. Chem. Phys., 23, 7057–7074, https://doi.org/10.5194/acp-23-7057-2023, https://doi.org/10.5194/acp-23-7057-2023, 2023
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We present OH observation and model simulation results at a coastal site in Hong Kong. The model predicted the OH concentration under high-NOx well but overpredicted it under low-NOx conditions. This implies an insufficient understanding of OH chemistry under low-NOx conditions. We show evidence of missing OH sinks as a possible cause of the overprediction.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
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Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Qianjie Chen, Jessica A. Mirrielees, Sham Thanekar, Nicole A. Loeb, Rachel M. Kirpes, Lucia M. Upchurch, Anna J. Barget, Nurun Nahar Lata, Angela R. W. Raso, Stephen M. McNamara, Swarup China, Patricia K. Quinn, Andrew P. Ault, Aaron Kennedy, Paul B. Shepson, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 15263–15285, https://doi.org/10.5194/acp-22-15263-2022, https://doi.org/10.5194/acp-22-15263-2022, 2022
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During a spring field campaign in the coastal Arctic, ultrafine particles were enhanced during high wind speeds, and coarse-mode particles were reduced during blowing snow. Calculated periods blowing snow were overpredicted compared to observations. Sea spray aerosols produced by sea ice leads affected the composition of aerosols and snowpack. An improved understanding of aerosol emissions from leads and blowing snow is critical for predicting the future climate of the rapidly warming Arctic.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Andrew D. Polasky, Jenni L. Evans, and Jose D. Fuentes
EGUsphere, https://doi.org/10.5194/egusphere-2022-282, https://doi.org/10.5194/egusphere-2022-282, 2022
Preprint withdrawn
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Statistical downscaling provides methods to bridge the gap between the global climate models and the scale of information needed to understand the impacts of climate change. This paper describes a new software package that provides a number of statistical downscaling approaches, as well as evaluation metrics for these methods. The goal of this work is to provide a new tool for researchers carrying out downscaling studies, and enable the easy use and comparison of different downscaling methods.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
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Short summary
N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and highly reactive Cl radicals that impact air quality. In the inland urban atmosphere, ClNO2 was elevated during lower air turbulence and over snow-covered ground, from snowpack ClNO2 production. N2O5 and ClNO2 levels were lowest, on average, during rainfall and fog because of scavenging, with N2O5 scavenging by fog droplets likely contributing to observed increased particulate nitrate concentrations.
N2O5 uptake by chloride-containing surfaces produces ClNO2, which photolyzes, producing NO2 and...
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