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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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
Short summary
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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
Short summary
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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
Short summary
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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
Short summary
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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
Short summary
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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.
Cited articles
Allan, B. J., Carslaw, N., Coe, H., Burgess, R. A., and Plane, J. M. C.:
Observations of the nitrate radical in the marine boundary layer, J. Atmos.
Chem., 33, 129–154, https://doi.org/10.1023/A:1005917203307, 1999.
Asaf, D., Tas, E., Pedersen, D., Peleg, M., and Luria, M.: Long-term
measurements of NO3 radical at a semiarid urban site: 2. Seasonal
trends and loss mechanisms, Environ. Sci. Technol., 44, 5901–5907,
https://doi.org/10.1021/es100967z, 2010.
Behnke, W., George, C., Scheer, V., and Zetzsch, C.: Production and decay of
ClNO2 from the reaction of gaseous N2O5 with NaCl solution:
Bulk and aerosol experiments, J. Geophys. Res., 102, 3795–3804,
https://doi.org/10.1029/96JD03057, 1997.
Bertram, T. H. and Thornton, J. A.: Toward a general parameterization of N2O5 reactivity on aqueous particles: the competing effects of particle liquid water, nitrate and chloride, Atmos. Chem. Phys., 9, 8351–8363, https://doi.org/10.5194/acp-9-8351-2009, 2009.
Bertram, T. H., Thornton, J. A., Riedel, T. P., Middlebrook, A. M.,
Bahreini, R., Bates, T. S., Quinn, P. K., and Coffman, D. J.: Direct
observations of N2O5 reactivity on ambient aerosol particles,
Geophys. Res. Lett., 36, 1–5, https://doi.org/10.1029/2009GL040248, 2009.
Brown, S. S., Dibb, J. E., Stark, H., Aldener, M., Vozella, M., Whitlow, S.,
Williams, E. J., Lerner, B. M., Jakoubek, R., Middlebrook, A. M., DeGouw, J.
A., Warneke, C., Goldan, P. D., Kuster, W. C., Angevine, W. M., Sueper, D.
T., Quinn, P. K., Bates, T. S., Meagher, J. F., Fehsenfeld, F. C., and
Ravishankara, A. R.: Nighttime removal of NOx in the summer marine
boundary layer, Geophys. Res. Lett., 31, 2–6, https://doi.org/10.1029/2004GL019412,
2004.
Brown, S. S., Dubé, W. P., Osthoff, H. D., Stutz, J., Ryerson, T. B.,
Wollny, A. G., Brock, C. A., Warneke, C., de Gouw, J. A., Atlas, E., Neuman,
J. A., Holloway, J. S., Lerner, B. M., Williams, E. J., Kuster, W. C.,
Goldan, P. D., Angevine, W. M., Trainer, M., Fehsenfeld, F. C., and
Ravishankara, A. R.: Vertical profiles in NO3 and N2O5
measured from an aircraft: Results from the NOAA P-3 and surface platforms
during the New England Air Quality Study 2004, J. Geophys. Res.-Atmos.,
112, 1–17, https://doi.org/10.1029/2007JD008883, 2007.
Brown, S. S., Dubé, W. P., Tham, Y. J., Zha, Q., Xue, L., Poon, S.,
Wang, Z., Blake, D. R., Tsui, W., Parrish, D. D., and Wang, T.: Nighttime
chemistry at a high altitude site above Hong Kong, J. Geophys. Res.-Atmos.,
121, 2457–2475, https://doi.org/10.1002/2015JD024566, 2016.
Chang, W. L., Bhave, P. V, Brown, S. S., Riemer, N., Stutz, J., and Dabdub,
D.: Heterogeneous Atmospheric Chemistry, Ambient Measurements, and Model
Calculations of N2O5: A Review, Aerosol Sci. Tech., 45,
665–695, https://doi.org/10.1080/02786826.2010.551672, 2011.
Chen, Q., Edebeli, J., McNamara, S. M., Kulju, K. D., May, N. W., Bertman,
S. B., Thanekar, S., Fuentes, J. D., and Pratt, K. A.: HONO, Particulate
Nitrite, and Snow Nitrite at a Midlatitude Urban Site during Wintertime, ACS
Earth Space Chem., 3, 811–822, https://doi.org/10.1021/acsearthspacechem.9b00023,
2019.
Christiansen, A. E., Carlton, A. G., and Henderson, B. H.: Differences in fine particle chemical composition on clear and cloudy days, Atmos. Chem. Phys., 20, 11607–11624, https://doi.org/10.5194/acp-20-11607-2020, 2020.
Crutzen, P. J.: The Role of NO and NO2 in the Chemistry of the
Troposphere and Stratosphere, Annu. Rev. Earth Pl. Sc., 7, 443–72,
https://doi.org/10.1146/annurev.ea.07.050179.002303, 1979.
Dall'Osto, M., Harrison, R. M., Coe, H., and Williams, P.: Real-time secondary aerosol formation during a fog event in London, Atmos. Chem. Phys., 9, 2459–2469, https://doi.org/10.5194/acp-9-2459-2009, 2009.
Davis, J. M., Bhave, P. V., and Foley, K. M.: Parameterization of N2O5 reaction probabilities on the surface of particles containing ammonium, sulfate, and nitrate, Atmos. Chem. Phys., 8, 5295–5311, https://doi.org/10.5194/acp-8-5295-2008, 2008.
Ervens, B.: Modeling the processing of aerosol and trace gases in clouds and fogs, Chem. Rev., 115, 4157–4198, https://doi.org/10.1021/cr5005887, 2015.
Evans, M. J. and Jacob, D. J.: Impact of new laboratory studies of
N2O5 hydrolysis on global model budgets of tropospheric nitrogen
oxides, ozone, and OH, Geophys. Res. Lett., 32, 1–4,
https://doi.org/10.1029/2005GL022469, 2005.
Fickert, S., Helleis, F., Adams, J. W., Moortgat, G. K., and Crowley, J. N.:
Reactive uptake of ClNO2 on aqueous bromide solutions, J. Phys. Chem.
A, 102, 10689–10696, https://doi.org/10.1021/jp983004n, 1998.
Finlayson-Pitts, B. J. and Pitts, J. N.: Formation of chemically active
chlorine compounds by reactions of atmospheric NaCl particles with gaseous
N2O5 and ClONO2, Nature, 337, 241–244,
https://doi.org/10.1038/337241a0, 1989.
Frenzel, A., Scheer, V., Sikorski, R., George, C., Behnke, W., and Zetzsch,
C.: Heterogeneous interconversion reactions of BrNO2, ClNO2, Br2, and Cl2,
J. Phys. Chem. A, 102, 1329–1337, https://doi.org/10.1021/jp973044b, 1998.
Ge, X., Zhang, Q., Sun, Y., Ruehl, C. R., and Setyan, A.: Effect of
aqueous-phase processing on aerosol chemistry and size distributions in
Fresno, California, during wintertime, Environ. Chem., 9, 221–235,
https://doi.org/10.1071/EN11168, 2012.
Geyer, A., Alicke, B., Konrad, S., Schmitz, T., Stutz, J., and Platt, U.:
Chemistry and oxidation capacity of the nitrate radical in the continental
boundary layer near Berlin, J. Geophys. Res.-Atmos., 106, 8013–8025,
https://doi.org/10.1029/2000JD900681, 2001.
Griffiths, P. T. and Cox, R. A.: Temperature dependence of heterogeneous
uptake of N2O5 by ammonium sulfate aerosol, Atmos. Sci. Lett., 10,
159–163, https://doi.org/10.1002/asl.225, 2009.
Gržinić, G., Bartels-Rausch, T., Türler, A., and Ammann, M.: Efficient bulk mass accommodation and dissociation of N2O5 in neutral aqueous aerosol, Atmos. Chem. Phys., 17, 6493–6502, https://doi.org/10.5194/acp-17-6493-2017, 2017.
Gunthe, S. S., Liu, P., Panda, U., Raj, S. S., Sharma, A., Darbyshire, E.,
Reyes-Villegas, E., Allan, J., Chen, Y., Wang, X., Song, S., Pöhlker, M.
L., Shi, L., Wang, Y., Kommula, S. M., Liu, T., Ravikrishna, R., McFiggans,
G., Mickley, L. J., Martin, S. T., Pöschl, U., Andreae, M. O., and Coe,
H.: Enhanced aerosol particle growth sustained by high continental chlorine
emission in India, Nat. Geosci., 14, 77–84,
https://doi.org/10.1038/s41561-020-00677-x, 2021.
Hallquist, M., Stewart, D. J., Stephenson, S. K., and Cox, R. A.: Hydrolysis
of N2O5 on sub-micron sulfate aerosols, Phys. Chem. Chem. Phys.,
5, 3453–3463, https://doi.org/10.1039/b301827j, 2003.
Hameed, S. and Sperber, K. R.: Rate of precipitation scavenging of nitrates on central Long Island, J. Geophys. Res.-Atmos., 91, 11833–11839, https://doi.org/10.1029/JD091iD11p11833, 1986.
Heintz, F., Platt, U., Flentje, H., and Dubois, R.: Long-term observation of
nitrate radicals at the Tor Station, Kap Arkona (Rügen), J. Geophys.
Res., 101, 22891–22910, 1996.
Huey, L. G., Tanner, D. J., Slusher, D. L., Dibb, J. E., Arimoto, R., Chen,
G., Davis, D., Buhr, M. P., Nowak, J. B., Mauldin, R. L., Eisele, F. L., and
Kosciuch, E.: CIMS measurements of HNO3 and SO2 at the South Pole
during ISCAT 2000, Atmos. Environ., 38, 5411–5421,
https://doi.org/10.1016/j.atmosenv.2004.04.037, 2004.
Jacob, J.: Chemistry of OH in Remote Clouds and Its Role in the Production
of Formic Acid and Peroxymonosulfate, J. Geophys. Res., 91, 9807–9826, 1986.
Johnson, C. A., Sigg, L., and Zobrist, J.: Case studies on the chemical
composition of fogwater: The influence of local gaseous emissions, Atmos.
Environ., 21, 2365–2374, https://doi.org/10.1016/0004-6981(87)90371-4, 1987.
Kercher, J. P., Riedel, T. P., and Thornton, J. A.: Chlorine activation by N2O5: simultaneous, in situ detection of ClNO2 and N2O5 by chemical ionization mass spectrometry, Atmos. Meas. Tech., 2, 193–204, https://doi.org/10.5194/amt-2-193-2009, 2009.
Kolesar, K. R., Mattson, C. N., Peterson, P. K., May, N. W., Prendergast, R. K., and Pratt, K.A.: Increases in wintertime PM2.5 sodium and chloride linked to snowfall and road salt application. Atmos. Environ., 177, 195–202, https://doi.org/10.1016/j.atmosenv.2018.01.008, 2018.
Kulju, K. and Pratt, K. A.: N2O5, ClNO2, PM2.5 chloride,
and PM2.5 nitrate in Kalamazoo, Michigan, USA during January–February
2018, PANGAEA [data set], https://doi.org/10.1594/PANGAEA.933765, 2021.
Leblanc, T. and Hauchecorne, A.: Recent observations of mesospheric
temperature inversions, J. Geophys. Res.-Atmos., 102, 19471–19482,
https://doi.org/10.1029/97JD01445, 1997.
Liao, J., Sihler, H., Huey, L. G., Neuman, J. A., Tanner, D. J., Friess, U.,
Platt, U., Flocke, F. M., Orlando, J. J., Shepson, P. B., Beine, H. J.,
Weinheimer, A. J., Sjostedt, S. J., Nowak, J. B., Knapp, D. J., Staebler, R.
M., Zheng, W., Sander, R., Hall, S. R., and Ullmann, K.: A comparison of
Arctic BrO measurements by chemical ionization mass spectrometry and long
path-differential optical absorption spectroscopy, J. Geophys. Res.-Atmos.,
116, 1–14, https://doi.org/10.1029/2010JD014788, 2011.
Lillis, D., Cruz, C. N., Collett, J., Willard Richards, L., and Pandis, S.
N.: Production and removal of aerosol in a polluted fog layer: Model
evaluation and fog effect on PM, Atmos. Environ., 33, 4797–4816,
https://doi.org/10.1016/S1352-2310(99)00264-2, 1999.
Lopez-Hilfiker, F. D., Constantin, K., Kercher, J. P., and Thornton, J. A.: Temperature dependent halogen activation by N2O5 reactions on halide-doped ice surfaces, Atmos. Chem. Phys., 12, 5237–5247, https://doi.org/10.5194/acp-12-5237-2012, 2012.
Markovic, M. Z., Vandenboer, T. C., and Murphy, J. G.: Characterization and
optimization of an online system for the simultaneous measurement of
atmospheric water-soluble constituents in the gas and particle phases, J.
Environ. Monit., 14, 1872–1884, https://doi.org/10.1039/c2em00004k, 2012.
McDuffie, E. E., Fibiger, D. L., Dubé, W. P., Lopez Hilfiker, F., Lee,
B. H., Jaeglé, L., Guo, H., Weber, R. J., Reeves, J. M., Weinheimer, A.
J., Schroder, J. C., Campuzano-Jost, P., Jimenez, J. L., Dibb, J. E., Veres,
P., Ebben, C., Sparks, T. L., Wooldridge, P. J., Cohen, R. C., Campos, T.,
Hall, S. R., Ullmann, K., Roberts, J. M., Thornton, J. A., and Brown, S. S.:
ClNO2 Yields From Aircraft Measurements During the 2015 WINTER Campaign
and Critical Evaluation of the Current Parameterization, J. Geophys. Res.-Atmos., 123, 12994–13015, https://doi.org/10.1029/2018JD029358, 2018.
McNamara, S. M., Raso, A. R. W., Wang, S., Thanekar, S., Boone, E. J.,
Kolesar, K. R., Peterson, P. K., Simpson, W. R., Fuentes, J. D., Shepson, P.
B., and Pratt, K. A.: Springtime Nitrogen Oxide-Influenced Chlorine Chemistry
in the Coastal Arctic, Environ. Sci. Technol., 53, 8057–8067,
https://doi.org/10.1021/acs.est.9b01797, 2019.
McNamara, S. M., Kolesar, K. R., Wang, S., Kirpes, R. M., May, N. W.,
Gunsch, M. J., Cook, R. D., Fuentes, J. D., Hornbrook, R. S., Apel, E. C.,
China, S., Laskin, A., and Pratt, K. A.: Observation of Road Salt Aerosol
Driving Inland Wintertime Atmospheric Chlorine Chemistry, ACS Cent. Sci., 6, 684–694,
https://doi.org/10.1021/acscentsci.9b00994, 2020.
McNamara, S. M., Chen, Q., Edebeli, J., Kulju, K. D., Mumpfield, J.,
Fuentes, J. D., Bertman, S. B., and Pratt, K. A.: Observation of N2O5
deposition and ClNO2 production on the saline snowpack, ACS Earth Space Chem., 5, 1020–1031,
https://doi.org/10.1021/acsearthspacechem.0c00317, 2021.
Mielke, L. H., Furgeson, A., and Osthoff, H. D.: Observation of ClNO2 in
a Mid-Continental Urban Environment, Environ. Sci. Technol, 45, 8889–8896,
https://doi.org/10.1021/es201955u, 2011.
Monin, A. S. and Obukhov, A. M.: Basic laws of turbulent mixing in the
surface layer of the atmosphere,
https://gibbs.science/teaching/efd/handouts/monin_obukhov_1954.pdf (last access: 31 May 2019), 1954.
Neuman, J. A., Huey, L. G., Dissly, R. W., Fehsenfeld, F. C., Flocke, F.,
Holecek, J. C., Holloway, J. S., Hübler, G., Jakoubek, R., Nicks, D. K.,
Parrish, D. D., Ryerson, T. B., Sueper, D. T., and Weinheimer, A. J.:
Fast-response airborne in situ measurements of HNO3 during the Texas
2000 Air Quality Study, J. Geophys. Res.-Atmos., 107, 1–12,
https://doi.org/10.1029/2001JD001437, 2002.
Osthoff, H. D., Sommariva, R., Baynard, T., Pettersson, A., Williams, E. J.,
Lerner, B. M., Roberts, J. M., Stark, H., Goldan, P. D., Kuster, W. C.,
Bates, T. S., Coffman, D., Ravishankara, A. R., and Brown, S. S.: Observation
of daytime N2O5 in the marine boundary layer during New England
Air Quality Study – Intercontinental Transport and Chemical Transformation
2004, J. Geophys. Res.-Atmos., 111, 1–13, https://doi.org/10.1029/2006JD007593,
2006.
Osthoff, H. D., Roberts, J. M., Ravishankara, A. R., Williams, E. J.,
Lerner, B. M., Sommariva, R., Bates, T. S., Coffman, D., Quinn, P. K., Dibb,
J. E., Stark, H., Burkholder, J. B., Talukdar, R. K., Meagher, J.,
Fehsenfeld, F. C., and Brown, S. S.: High levels of nitryl chloride in the
polluted subtropical marine boundary layer, Nat. Geosci., 1, 324–328,
https://doi.org/10.1038/ngeo177, 2008.
Osthoff, H. D., Odame-Ankrah, C. A., Taha, Y. M., Tokarek, T. W., Schiller, C. L., Haga, D., Jones, K., and Vingarzan, R.: Low levels of nitryl chloride at ground level: nocturnal nitrogen oxides in the Lower Fraser Valley of British Columbia, Atmos. Chem. Phys., 18, 6293–6315, https://doi.org/10.5194/acp-18-6293-2018, 2018.
Phillips, G. J., Tang, M. J., Thieser, J., Brickwedde, B., Schuster, G.,
Bohn, B., Lelieveld, J., and Crowley, J. N.: Significant concentrations of
nitryl chloride observed in rural continental Europe associated with the
influence of sea salt chloride and anthropogenic emissions, Geophys. Res.
Lett., 39, 1–5, https://doi.org/10.1029/2012GL051912, 2012.
Pruppacher, H. R. and Klett, J. D.: Microphysics of Clouds and
Precipitation, 2nd Edn., Kluwer Academic Publishers, Dordrecht, ISBN 0-7923-4211-9, 1997.
Riedel, T. P., Wagner, N. L., Dubé, W. P., Middlebrook, A. M., Young, C.
J., Öztürk, F., Bahreini, R., Vandenboer, T. C., Wolfe, D. E.,
Williams, E. J., Roberts, J. M., Brown, S. S., and Thornton, J. A.: Chlorine
activation within urban or power plant plumes: Vertically resolved
ClNO2 and Cl2 measurements from a tall tower in a polluted
continental setting, J. Geophys. Res.-Atmos., 118, 8702–8715,
https://doi.org/10.1002/jgrd.50637, 2013.
Roberts, J. M., Osthoff, H. D., Brown, S. S., Ravishankara, A. R., Coffman,
D., Quinn, P., and Bates, T.: Laboratory studies of products of
N2O5 uptake on Cl- containing substrates, Geophys. Res. Lett.,
36, 1–5, https://doi.org/10.1029/2009GL040448, 2009.
Sander, R.: Compilation of Henry's law constants (version 4.0) for water as solvent, Atmos. Chem. Phys., 15, 4399–4981, https://doi.org/10.5194/acp-15-4399-2015, 2015.
Sarwar, G., Simon, H., Xing, J., and Mathur, R.: Importance of tropospheric
ClNO2 chemistry across the Northern Hemisphere, Geophys. Res. Lett.,
41, 4050–4058, https://doi.org/10.1002/2014GL059962, 2014.
Simpson, W. R., Brown, S. S., Saiz-Lopez, A., Thornton, J. A., and Von
Glasow, R.: Tropospheric Halogen Chemistry: Sources, Cycling, and Impacts,
Chem. Rev., 115, 4035–4062, https://doi.org/10.1021/cr5006638, 2015.
Slusher, D. L., Huey, L. G., Tanner, D. J., Flocke, F. M., and Roberts, J.
M.: A thermal dissociation – Chemical ionization mass spectrometry (TD-CIMS)
technique for the simultaneous measurement of peroxyacyl nitrates and
dinitrogen pentoxide, J. Geophys. Res.-Atmos., 109, 1–13,
https://doi.org/10.1029/2004JD004670, 2004.
Sommariva, R., Osthoff, H. D., Brown, S. S., Bates, T. S., Baynard, T., Coffman, D., de Gouw, J. A., Goldan, P. D., Kuster, W. C., Lerner, B. M., Stark, H., Warneke, C., Williams, E. J., Fehsenfeld, F. C., Ravishankara, A. R., and Trainer, M.: Radicals in the marine boundary layer during NEAQS 2004: a model study of day-time and night-time sources and sinks, Atmos. Chem. Phys., 9, 3075–3093, https://doi.org/10.5194/acp-9-3075-2009, 2009.
Stanier, C., Singh, A., Adamski, W., Baek, J., Caughey, M., Carmichael, G., Edgerton, E., Kenski, D., Koerber, M., Oleson, J., Rohlf, T., Lee, S. R., Riemer, N., Shaw, S., Sousan, S., and Spak, S. N.: Overview of the LADCO winter nitrate study: hourly ammonia, nitric acid and PM2.5 composition at an urban and rural site pair during PM2.5 episodes in the US Great Lakes region, Atmos. Chem. Phys., 12, 11037–11056, https://doi.org/10.5194/acp-12-11037-2012, 2012.
Stull, R.: Practical Meteorology: An Algebra-based Survey of Atmospheric
Science, 1.02b., Univ. of British Columbia, Vancouver, ISBN 978-0-88865-283-6, 2017.
Stull, R. B.: An Introduction to Boundary Layer Meteorology, Kluwer Academic Publishers, Dordrecht, ISBN 978-90-277-2768-8, 1988.
Tham, Y. J., Wang, Z., Li, Q., Yun, H., Wang, W., Wang, X., Xue, L., Lu, K., Ma, N., Bohn, B., Li, X., Kecorius, S., Größ, J., Shao, M., Wiedensohler, A., Zhang, Y., and Wang, T.: Significant concentrations of nitryl chloride sustained in the morning: investigations of the causes and impacts on ozone production in a polluted region of northern China, Atmos. Chem. Phys., 16, 14959–14977, https://doi.org/10.5194/acp-16-14959-2016, 2016.
Tham, Y. J., Wang, Z., Li, Q., Wang, W., Wang, X., Lu, K., Ma, N., Yan, C., Kecorius, S., Wiedensohler, A., Zhang, Y., and Wang, T.: Heterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: roles of aerosol water content and chemical composition, Atmos. Chem. Phys., 18, 13155–13171, https://doi.org/10.5194/acp-18-13155-2018, 2018.
Thornton, J. A. and Abbatt, J. P. D.: N2O5 Reaction on Submicron
Sea Salt Aerosol: Kinetics, Products, and the Effect of Surface Active
Organics, J. Phys. Chem. A, 109, 10004–10012, https://doi.org/10.1021/jp054183t, 2005.
Thornton, J. A., Kercher, J. P., Riedel, T. P., Wagner, N. L., Cozic, J.,
Holloway, J. S., Dubé, W. P., Wolfe, G. M., Quinn, P. K., Middlebrook,
A. M., Alexander, B., and Brown, S. S.: A large atomic chlorine source
inferred from mid-continental reactive nitrogen chemistry, Nature, 464,
271–274, https://doi.org/10.1038/nature08905, 2010.
Wagner, N. L., Riedel, T. P., Young, C. J., Bahreini, R., Brock, C. A.,
Dubé, W. P., Kim, S., Middlebrook, A. M., Öztürk, F., Roberts,
J. M., Russo, R., Sive, B., Swarthout, R., Thornton, J. A., VandenBoer, T.
C., Zhou, Y., and Brown, S. S.: N2O5 uptake coefficients and
nocturnal NO2 removal rates determined from ambient wintertime
measurements, J. Geophys. Res.-Atmos., 118, 9331–9350,
https://doi.org/10.1002/jgrd.50653, 2013.
Wang, S., Ackermann, R., and Stutz, J.: Vertical profiles of O3 and NOx chemistry in the polluted nocturnal boundary layer in Phoenix, AZ: I. Field observations by long-path DOAS, Atmos. Chem. Phys., 6, 2671–2693, https://doi.org/10.5194/acp-6-2671-2006, 2006.
Wang, S., McNamara, S. M., Kolesar, K. R., May, N. W., Fuentes, J. D., Cook,
R. D., Gunsch, M. J., Mattson, C. N., Hornbrook, R. S., Apel, E. C., and
Pratt, K. A.: Urban Snowpack ClNO2 Production and Fate: A
One-Dimensional Modeling Study, ACS Earth Space Chem., 4, 1140–1148,
https://doi.org/10.1021/acsearthspacechem.0c00116, 2020.
Wang, X., Wang, H., Xue, L., Wang, T., Wang, L., Gu, R., Wang, W., Tham, Y.
J., Wang, Z., Yang, L., Chen, J., and Wang, W.: Observations of
N2O5 and ClNO2 at a polluted urban surface site in North
China: High N2O5 uptake coefficients and low ClNO2 product
yields, Atmos. Environ., 156, 125–134, https://doi.org/10.1016/j.atmosenv.2017.02.035,
2017.
Wood, E. C., Bertram, T. H., Wooldridge, P. J., and Cohen, R. C.: Measurements of N2O5, NO2, and O3 east of the San Francisco Bay, Atmos. Chem. Phys., 5, 483–491, https://doi.org/10.5194/acp-5-483-2005, 2005.
Young, C. J., Washenfelder, R. A., Edwards, P. M., Parrish, D. D., Gilman, J. B., Kuster, W. C., Mielke, L. H., Osthoff, H. D., Tsai, C., Pikelnaya, O., Stutz, J., Veres, P. R., Roberts, J. M., Griffith, S., Dusanter, S., Stevens, P. S., Flynn, J., Grossberg, N., Lefer, B., Holloway, J. S., Peischl, J., Ryerson, T. B., Atlas, E. L., Blake, D. R., and Brown, S. S.: Chlorine as a primary radical: evaluation of methods to understand its role in initiation of oxidative cycles, Atmos. Chem. Phys., 14, 3427–3440, https://doi.org/10.5194/acp-14-3427-2014, 2014.
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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