Articles | Volume 25, issue 16
https://doi.org/10.5194/acp-25-9561-2025
© Author(s) 2025. 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-25-9561-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Aug 2025
Research article |
| 29 Aug 2025
| 29 Aug 2025
Surprisingly robust photochemistry in subarctic particles during winter: evidence from photooxidants
Laura M. D. Heinlein
Department of Land, Air and Water Resources, University of California, Davis, CA 95616, USA
Junwei He
Department of Land, Air and Water Resources, University of California, Davis, CA 95616, USA
Michael Oluwatoyin Sunday
Department of Land, Air and Water Resources, University of California, Davis, CA 95616, USA
now at: California Air Resources Board, Sacramento, CA, USA
Fangzhou Guo
Department of Earth & Atmospheric Sciences, University of Houston, Houston, TX 77204, USA
now at: Center for Atmospheric and Environmental Chemistry, Aerodyne Research Inc, Billerica, MA 01821, USA
James Campbell
Department of Chemistry and Biochemistry, University of Alaska, Fairbanks, AK 99775, USA
Allison Moon
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
Sukriti Kapur
Department of Chemistry, University of California, Irvine, CA 92697, USA
Ting Fang
Department of Chemistry, University of California, Irvine, CA 92697, USA
now at: Sustainable Energy and Environment Thrust, The Hong Kong University of Science and Technology (Guangzhou), Guangzhou, Guangdong 511400, China
Kasey Edwards
Department of Chemistry, University of California, Irvine, CA 92697, USA
Meeta Cesler-Maloney
Department of Chemistry and Biochemistry, University of Alaska, Fairbanks, AK 99775, USA
now at: Louisville Metro Air Pollution Control District, Louisville, KY 40203, USA
Alyssa J. Burns
Department of Land, Air and Water Resources, University of California, Davis, CA 95616, USA
Jack Dibb
College of Engineering & Physical Sciences, University of New Hampshire, Durham, NH 03824, USA
William Simpson
Department of Chemistry and Biochemistry, University of Alaska, Fairbanks, AK 99775, USA
Manabu Shiraiwa
Department of Chemistry, University of California, Irvine, CA 92697, USA
Becky Alexander
Department of Atmospheric Sciences, University of Washington, Seattle, WA 98195, USA
Jingqiu Mao
Department of Chemistry and Biochemistry, University of Alaska, Fairbanks, AK 99775, USA
James H. Flynn III
Department of Earth & Atmospheric Sciences, University of Houston, Houston, TX 77204, USA
Jochen Stutz
Department of Atmospheric & Oceanic Sciences, University of California, Los Angeles, CA 90095, USA
Department of Land, Air and Water Resources, University of California, Davis, CA 95616, USA
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Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
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Zhuang Jiang, Becky Alexander, Joel Savarino, and Lei Geng
Atmos. Chem. Phys., 24, 4895–4914, https://doi.org/10.5194/acp-24-4895-2024, https://doi.org/10.5194/acp-24-4895-2024, 2024
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Zhiqiang Zhang, Ying Li, Haiyan Ran, Junling An, Yu Qu, Wei Zhou, Weiqi Xu, Weiwei Hu, Hongbin Xie, Zifa Wang, Yele Sun, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 4809–4826, https://doi.org/10.5194/acp-24-4809-2024, https://doi.org/10.5194/acp-24-4809-2024, 2024
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Santo Fedele Colosimo, Nathaniel Brockway, Vijay Natraj, Robert Spurr, Klaus Pfeilsticker, Lisa Scalone, Max Spolaor, Sarah Woods, and Jochen Stutz
Atmos. Meas. Tech., 17, 2367–2385, https://doi.org/10.5194/amt-17-2367-2024, https://doi.org/10.5194/amt-17-2367-2024, 2024
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Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
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.
Meeta Cesler-Maloney, William Simpson, Jonas Kuhn, Jochen Stutz, Jennie Thomas, Tjarda Roberts, Deanna Huff, and Sol Cooperdock
EGUsphere, https://doi.org/10.5194/egusphere-2023-3082, https://doi.org/10.5194/egusphere-2023-3082, 2024
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We used a one-dimensional model to simulate how pollution in Fairbanks, Alaska, accumulates in shallow layers near the ground when temperature inversions are present. We find pollution accumulates in a 20 m to 50 m thick layer. The model agrees with observations of SO2 pollution using only home heating emissions sources, which shows that ground-based sources dominate sulfur pollution in downtown Fairbanks. Air residence times in downtown are only a few hours, limiting chemical transformations.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Wei Li, Yuxuan Wang, Xueying Liu, Ehsan Soleimanian, Travis Griggs, James Flynn, and Paul Walter
Atmos. Chem. Phys., 23, 13685–13699, https://doi.org/10.5194/acp-23-13685-2023, https://doi.org/10.5194/acp-23-13685-2023, 2023
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This study examined high offshore ozone events in Galveston Bay and the Gulf of Mexico, using boat data and WRF–CAMx modeling during the TRACER-AQ 2021 field campaign. On average, high ozone is caused by chemistry due to the regional transport of volatile organic compounds and downwind advection of NOx from the ship channel. Two case studies show advection of ozone can be another process leading to high ozone, and accurate wind prediction is crucial for air quality forecasting in coastal areas.
Sujan Shrestha, Shan Zhou, Manisha Mehra, Meghan Guagenti, Subin Yoon, Sergio L. Alvarez, Fangzhou Guo, Chun-Ying Chao, James H. Flynn III, Yuxuan Wang, Robert J. Griffin, Sascha Usenko, and Rebecca J. Sheesley
Atmos. Chem. Phys., 23, 10845–10867, https://doi.org/10.5194/acp-23-10845-2023, https://doi.org/10.5194/acp-23-10845-2023, 2023
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We evaluated different methods for assessing the influence of long-range transport of biomass burning (BB) plumes at a coastal site in Texas, USA. We show that the aerosol composition and optical properties exhibited good agreement, while CO and acetonitrile trends were less specific for assessing BB source influence. Our results demonstrate that the network of aerosol optical measurements can be useful for identifying the influence of aged BB plumes in anthropogenically influenced areas.
Xueying Liu, Yuxuan Wang, Shailaja Wasti, Wei Li, Ehsan Soleimanian, James Flynn, Travis Griggs, Sergio Alvarez, John T. Sullivan, Maurice Roots, Laurence Twigg, Guillaume Gronoff, Timothy Berkoff, Paul Walter, Mark Estes, Johnathan W. Hair, Taylor Shingler, Amy Jo Scarino, Marta Fenn, and Laura Judd
Geosci. Model Dev., 16, 5493–5514, https://doi.org/10.5194/gmd-16-5493-2023, https://doi.org/10.5194/gmd-16-5493-2023, 2023
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With a comprehensive suite of ground-based and airborne remote sensing measurements during the 2021 TRacking Aerosol Convection ExpeRiment – Air Quality (TRACER-AQ) campaign in Houston, this study evaluates the simulation of the planetary boundary layer (PBL) height and the ozone vertical profile by a high-resolution (1.33 km) 3-D photochemical model Weather Research and Forecasting-driven GEOS-Chem (WRF-GC).
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.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
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Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, https://doi.org/10.5194/acp-23-7103-2023, 2023
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Haihui Zhu, Randall V. Martin, Betty Croft, Shixian Zhai, Chi Li, Liam Bindle, Jeffrey R. Pierce, Rachel Y.-W. Chang, Bruce E. Anderson, Luke D. Ziemba, Johnathan W. Hair, Richard A. Ferrare, Chris A. Hostetler, Inderjeet Singh, Deepangsu Chatterjee, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jack E. Dibb, Joshua S. Schwarz, and Andrew Weinheimer
Atmos. Chem. Phys., 23, 5023–5042, https://doi.org/10.5194/acp-23-5023-2023, https://doi.org/10.5194/acp-23-5023-2023, 2023
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Particle size of atmospheric aerosol is important for estimating its climate and health effects, but simulating atmospheric aerosol size is computationally demanding. This study derives a simple parameterization of the size of organic and secondary inorganic ambient aerosol that can be applied to atmospheric models. Applying this parameterization allows a better representation of the global spatial pattern of aerosol size, as verified by ground and airborne measurements.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
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Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Meredith Schervish and Manabu Shiraiwa
Atmos. Chem. Phys., 23, 221–233, https://doi.org/10.5194/acp-23-221-2023, https://doi.org/10.5194/acp-23-221-2023, 2023
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Secondary organic aerosols (SOAs) can exhibit complex non-ideal behavior and adopt an amorphous semisolid state. We simulate condensation of semi-volatile compounds into a phase-separated particle to investigate the effect of non-ideality and particle phase state on the equilibration timescale of SOA partitioning. Our results provide useful insights into the interpretation of experimental observations and the description and treatment of SOA in aerosol models.
Pamela S. 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, Jeff Peischl, 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., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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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.
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.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
Yanzhi Cao, Zhuang Jiang, Becky Alexander, Jihong Cole-Dai, Joel Savarino, Joseph Erbland, and Lei Geng
Atmos. Chem. Phys., 22, 13407–13422, https://doi.org/10.5194/acp-22-13407-2022, https://doi.org/10.5194/acp-22-13407-2022, 2022
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We investigate the potential of ice-core preserved nitrate isotopes as proxies of stratospheric ozone variability by measuring nitrate isotopes in a shallow ice core from the South Pole. The large variability in the snow accumulation rate and its slight increase after the 1970s masked any signals caused by the ozone hole. Moreover, the nitrate oxygen isotope decrease may reflect changes in the atmospheric oxidation environment in the Southern Ocean.
Subin Yoon, Alexander Kotsakis, Sergio L. Alvarez, Mark G. Spychala, Elizabeth Klovenski, Paul Walter, Gary Morris, Ernesto Corrales, Alfredo Alan, Jorge A. Diaz, and James H. Flynn
Atmos. Meas. Tech., 15, 4373–4384, https://doi.org/10.5194/amt-15-4373-2022, https://doi.org/10.5194/amt-15-4373-2022, 2022
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SO2 is adverse to human health and the environment. A single SO2 sonde was developed to provide direct SO2 measurement with a greater vertical extent, a lower limit of detection, and less uncertainty relative to the previous dual-sonde method. The single sonde was tested in the field near volcanoes and anthropogenic sources where the sonde measured SO2 ranging from 0.5 to 940 ppb. This lighter-weight payload can be a great candidate to attach to small drones and unmanned aerial vehicles.
Zhuang Jiang, Joel Savarino, Becky Alexander, Joseph Erbland, Jean-Luc Jaffrezo, and Lei Geng
The Cryosphere, 16, 2709–2724, https://doi.org/10.5194/tc-16-2709-2022, https://doi.org/10.5194/tc-16-2709-2022, 2022
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A record of year-round atmospheric nitrate isotopic composition along with snow nitrate isotopic data from Summit, Greenland, revealed apparent enrichments in nitrogen isotopes in snow nitrate compared to atmospheric nitrate, in addition to a relatively smaller degree of changes in oxygen isotopes. The results suggest that at this site post-depositional processing takes effect, which should be taken into account when interpreting ice-core nitrate isotope records.
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., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its 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.
Katherine R. Travis, James H. Crawford, Gao Chen, Carolyn E. Jordan, Benjamin A. Nault, Hwajin Kim, Jose L. Jimenez, Pedro Campuzano-Jost, Jack E. Dibb, Jung-Hun Woo, Younha Kim, Shixian Zhai, Xuan Wang, Erin E. McDuffie, Gan Luo, Fangqun Yu, Saewung Kim, Isobel J. Simpson, Donald R. Blake, Limseok Chang, and Michelle J. Kim
Atmos. Chem. Phys., 22, 7933–7958, https://doi.org/10.5194/acp-22-7933-2022, https://doi.org/10.5194/acp-22-7933-2022, 2022
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The 2016 Korea–United States Air Quality (KORUS-AQ) field campaign provided a unique set of observations to improve our understanding of PM2.5 pollution in South Korea. Models typically have errors in simulating PM2.5 in this region, which is of concern for the development of control measures. We use KORUS-AQ observations to improve our understanding of the mechanisms driving PM2.5 and the implications of model errors for determining PM2.5 that is attributable to local or foreign sources.
Tianlang Zhao, Jingqiu Mao, William R. Simpson, Isabelle De Smedt, Lei Zhu, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Gonzalo González Abad, Caroline R. Nowlan, Barbara Barletta, Simone Meinardi, Donald R. Blake, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Chem. Phys., 22, 7163–7178, https://doi.org/10.5194/acp-22-7163-2022, https://doi.org/10.5194/acp-22-7163-2022, 2022
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Monitoring formaldehyde (HCHO) can help us understand Arctic vegetation change. Here, we compare satellite data and model and show that Alaska summertime HCHO is largely dominated by a background from methane oxidation during mild wildfire years and is dominated by wildfire (largely from direct emission of fire) during strong fire years. Consequently, it is challenging to use satellite HCHO to study vegetation change in the Arctic region.
Ted Hullar, Theo Tran, Zekun Chen, Fernanda Bononi, Oliver Palmer, Davide Donadio, and Cort Anastasio
Atmos. Chem. Phys., 22, 5943–5959, https://doi.org/10.5194/acp-22-5943-2022, https://doi.org/10.5194/acp-22-5943-2022, 2022
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Chemicals are commonly found in snowpacks throughout the world and may be degraded by sunlight; some previous research has reported faster decay rates for chemicals on the surface of snow and ice compared to in water. We found photodegradation on snow can be as much as 30 times faster than in solution for the three dimethoxybenzene isomers. Our computational modeling found light absorbance by dimethoxybenzenes increases on the snow surface, but this only partially explains the decay rate.
Carlos Alberti, Frank Hase, Matthias Frey, Darko Dubravica, Thomas Blumenstock, Angelika Dehn, Paolo Castracane, Gregor Surawicz, Roland Harig, Bianca C. Baier, Caroline Bès, Jianrong Bi, Hartmut Boesch, André Butz, Zhaonan Cai, Jia Chen, Sean M. Crowell, Nicholas M. Deutscher, Dragos Ene, Jonathan E. Franklin, Omaira García, David Griffith, Bruno Grouiez, Michel Grutter, Abdelhamid Hamdouni, Sander Houweling, Neil Humpage, Nicole Jacobs, Sujong Jeong, Lilian Joly, Nicholas B. Jones, Denis Jouglet, Rigel Kivi, Ralph Kleinschek, Morgan Lopez, Diogo J. Medeiros, Isamu Morino, Nasrin Mostafavipak, Astrid Müller, Hirofumi Ohyama, Paul I. Palmer, Mahesh Pathakoti, David F. Pollard, Uwe Raffalski, Michel Ramonet, Robbie Ramsay, Mahesh Kumar Sha, Kei Shiomi, William Simpson, Wolfgang Stremme, Youwen Sun, Hiroshi Tanimoto, Yao Té, Gizaw Mengistu Tsidu, Voltaire A. Velazco, Felix Vogel, Masataka Watanabe, Chong Wei, Debra Wunch, Marcia Yamasoe, Lu Zhang, and Johannes Orphal
Atmos. Meas. Tech., 15, 2433–2463, https://doi.org/10.5194/amt-15-2433-2022, https://doi.org/10.5194/amt-15-2433-2022, 2022
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Space-borne greenhouse gas missions require ground-based validation networks capable of providing fiducial reference measurements. Here, considerable refinements of the calibration procedures for the COllaborative Carbon Column Observing Network (COCCON) are presented. Laboratory and solar side-by-side procedures for the characterization of the spectrometers have been refined and extended. Revised calibration factors for XCO2, XCO and XCH4 are provided, incorporating 47 new spectrometers.
Meloë S. F. Kacenelenbogen, Qian Tan, Sharon P. Burton, Otto P. Hasekamp, Karl D. Froyd, Yohei Shinozuka, Andreas J. Beyersdorf, Luke Ziemba, Kenneth L. Thornhill, Jack E. Dibb, Taylor Shingler, Armin Sorooshian, Reed W. Espinosa, Vanderlei Martins, Jose L. Jimenez, Pedro Campuzano-Jost, Joshua P. Schwarz, Matthew S. Johnson, Jens Redemann, and Gregory L. Schuster
Atmos. Chem. Phys., 22, 3713–3742, https://doi.org/10.5194/acp-22-3713-2022, https://doi.org/10.5194/acp-22-3713-2022, 2022
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The impact of aerosols on Earth's radiation budget and human health is important and strongly depends on their composition. One desire of our scientific community is to derive the composition of the aerosol from satellite sensors. However, satellites observe aerosol optical properties (and not aerosol composition) based on remote sensing instrumentation. This study assesses how much aerosol optical properties can tell us about aerosol composition.
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.
Amir H. Souri, Kelly Chance, Juseon Bak, Caroline R. Nowlan, Gonzalo González Abad, Yeonjin Jung, David C. Wong, Jingqiu Mao, and Xiong Liu
Atmos. Chem. Phys., 21, 18227–18245, https://doi.org/10.5194/acp-21-18227-2021, https://doi.org/10.5194/acp-21-18227-2021, 2021
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The global pandemic is believed to have an impact on emissions of air pollutants such as nitrogen dioxide (NO2) and formaldehyde (HCHO). This study quantifies the changes in the amount of NOx and VOC emissions via state-of-the-art inverse modeling technique using satellite observations during the lockdown 2020 with respect to a baseline over Europe, which in turn, it permits unraveling atmospheric processes being responsible for ozone formation in a less cloudy month.
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.
Shixian Zhai, Daniel J. Jacob, Jared F. Brewer, Ke Li, Jonathan M. Moch, Jhoon Kim, Seoyoung Lee, Hyunkwang Lim, Hyun Chul Lee, Su Keun Kuk, Rokjin J. Park, Jaein I. Jeong, Xuan Wang, Pengfei Liu, Gan Luo, Fangqun Yu, Jun Meng, Randall V. Martin, Katherine R. Travis, Johnathan W. Hair, Bruce E. Anderson, Jack E. Dibb, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jung-Hun Woo, Younha Kim, Qiang Zhang, and Hong Liao
Atmos. Chem. Phys., 21, 16775–16791, https://doi.org/10.5194/acp-21-16775-2021, https://doi.org/10.5194/acp-21-16775-2021, 2021
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Geostationary satellite aerosol optical depth (AOD) has tremendous potential for monitoring surface fine particulate matter (PM2.5). Our study explored the physical relationship between AOD and PM2.5 by integrating data from surface networks, aircraft, and satellites with the GEOS-Chem chemical transport model. We quantitatively showed that accurate simulation of aerosol size distributions, boundary layer depths, relative humidity, coarse particles, and diurnal variations in PM2.5 are essential.
Nicole Jacobs, William R. Simpson, Kelly A. Graham, Christopher Holmes, Frank Hase, Thomas Blumenstock, Qiansi Tu, Matthias Frey, Manvendra K. Dubey, Harrison A. Parker, Debra Wunch, Rigel Kivi, Pauli Heikkinen, Justus Notholt, Christof Petri, and Thorsten Warneke
Atmos. Chem. Phys., 21, 16661–16687, https://doi.org/10.5194/acp-21-16661-2021, https://doi.org/10.5194/acp-21-16661-2021, 2021
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Spatial patterns of carbon dioxide seasonal cycle amplitude and summer drawdown timing derived from the OCO-2 satellite over northern high latitudes agree well with corresponding estimates from two models. The Asian boreal forest is anomalous with the largest amplitude and earliest seasonal drawdown. Modeled land contact tracers suggest that accumulated CO2 exchanges during atmospheric transport play a major role in shaping carbon dioxide seasonality in northern high-latitude regions.
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.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
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.
Zhuang Jiang, Becky Alexander, Joel Savarino, Joseph Erbland, and Lei Geng
The Cryosphere, 15, 4207–4220, https://doi.org/10.5194/tc-15-4207-2021, https://doi.org/10.5194/tc-15-4207-2021, 2021
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We used a snow photochemistry model (TRANSITS) to simulate the seasonal nitrate snow profile at Summit, Greenland. Comparisons between model outputs and observations suggest that at Summit post-depositional processing is active and probably dominates the snowpack δ15N seasonality. We also used the model to assess the degree of snow nitrate loss and the consequences in its isotopes at present and in the past, which helps for quantitative interpretations of ice-core nitrate records.
Jiajue Chai, Jack E. Dibb, Bruce E. Anderson, Claire Bekker, Danielle E. Blum, Eric Heim, Carolyn E. Jordan, Emily E. Joyce, Jackson H. Kaspari, Hannah Munro, Wendell W. Walters, and Meredith G. Hastings
Atmos. Chem. Phys., 21, 13077–13098, https://doi.org/10.5194/acp-21-13077-2021, https://doi.org/10.5194/acp-21-13077-2021, 2021
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Nitrous acid (HONO) derived from wildfire emissions plays a key role in controlling atmospheric oxidation chemistry. However, the HONO budget remains poorly constrained. By combining the field-observed concentrations and novel isotopic composition (N and O) of HONO and nitrogen oxides (NOx), we quantitatively constrained the relative contribution of each pathway to secondary HONO production and the relative importance of major atmospheric oxidants (ozone versus peroxy) in aged wildfire smoke.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Tommaso Galeazzo, Richard Valorso, Ying Li, Marie Camredon, Bernard Aumont, and Manabu Shiraiwa
Atmos. Chem. Phys., 21, 10199–10213, https://doi.org/10.5194/acp-21-10199-2021, https://doi.org/10.5194/acp-21-10199-2021, 2021
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We simulate SOA viscosity with explicit modeling of gas-phase oxidation of isoprene and α-pinene. While the viscosity dependence on relative humidity and mass loadings is captured well by simulations, the model underestimates measured viscosity, indicating missing processes. Kinetic limitations and reduction in mass accommodation may cause an increase in viscosity. The developed model is powerful for investigation of the interplay among gas reactions, chemical composition and phase state.
Kun Wang, Shohei Hattori, Mang Lin, Sakiko Ishino, Becky Alexander, Kazuki Kamezaki, Naohiro Yoshida, and Shichang Kang
Atmos. Chem. Phys., 21, 8357–8376, https://doi.org/10.5194/acp-21-8357-2021, https://doi.org/10.5194/acp-21-8357-2021, 2021
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
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.
Candice L. Sirmollo, Don R. Collins, Jordan M. McCormick, Cassandra F. Milan, Matthew H. Erickson, James H. Flynn, Rebecca J. Sheesley, Sascha Usenko, Henry W. Wallace, Alexander A. T. Bui, Robert J. Griffin, Matthew Tezak, Sean M. Kinahan, and Joshua L. Santarpia
Atmos. Meas. Tech., 14, 3351–3370, https://doi.org/10.5194/amt-14-3351-2021, https://doi.org/10.5194/amt-14-3351-2021, 2021
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The newly developed portable 1 m3 CAGE chamber systems were characterized using data acquired during a 2-month field study in 2016 in a forested area north of Houston, TX, USA. Concentrations of several oxidant and organic compounds measured in the chamber were found to closely agree with those calculated with a zero-dimensional model. By tracking the modes of injected monodisperse particles, a pattern change was observed for hourly averaged growth rates between late summer and early fall.
Jake Wilson, Ulrich Pöschl, Manabu Shiraiwa, and Thomas Berkemeier
Atmos. Chem. Phys., 21, 6175–6198, https://doi.org/10.5194/acp-21-6175-2021, https://doi.org/10.5194/acp-21-6175-2021, 2021
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This work explores the gas–particle partitioning of PAHs on soot with a kinetic model. We show that the equilibration timescale depends on PAH molecular structure, temperature, and particle number concentration. We explore scenarios in which the particulate fraction is perturbed from equilibrium by chemical loss and discuss implications for chemical transport models that assume instantaneous equilibration at each model time step.
Melinda K. Schueneman, Benjamin A. Nault, Pedro Campuzano-Jost, Duseong S. Jo, Douglas A. Day, Jason C. Schroder, Brett B. Palm, Alma Hodzic, Jack E. Dibb, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 2237–2260, https://doi.org/10.5194/amt-14-2237-2021, https://doi.org/10.5194/amt-14-2237-2021, 2021
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This work focuses on two important properties of the aerosol, acidity, and sulfate composition, which is important for our understanding of aerosol health and environmental impacts. We explore different methods to understand the composition of the aerosol with measurements from a specific instrument and apply those methods to a large dataset. These measurements are confounded by other factors, making it challenging to predict aerosol sulfate composition; pH estimations, however, show promise.
Miguel Ricardo A. Hilario, Ewan Crosbie, Michael Shook, Jeffrey S. Reid, Maria Obiminda L. Cambaliza, James Bernard B. Simpas, Luke Ziemba, Joshua P. DiGangi, Glenn S. Diskin, Phu Nguyen, F. Joseph Turk, Edward Winstead, Claire E. Robinson, Jian Wang, Jiaoshi Zhang, Yang Wang, Subin Yoon, James Flynn, Sergio L. Alvarez, Ali Behrangi, and Armin Sorooshian
Atmos. Chem. Phys., 21, 3777–3802, https://doi.org/10.5194/acp-21-3777-2021, https://doi.org/10.5194/acp-21-3777-2021, 2021
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This study characterizes long-range transport from major Asian pollution sources into the tropical northwest Pacific and the impact of scavenging on these air masses. We combined aircraft observations, HYSPLIT trajectories, reanalysis, and satellite retrievals to reveal distinct composition and size distribution profiles associated with specific emission sources and wet scavenging. The results of this work have implications for international policymaking related to climate and health.
Manabu Shiraiwa and Ulrich Pöschl
Atmos. Chem. Phys., 21, 1565–1580, https://doi.org/10.5194/acp-21-1565-2021, https://doi.org/10.5194/acp-21-1565-2021, 2021
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Mass accommodation is a crucial process in secondary organic aerosol partitioning that depends on volatility, diffusivity, reactivity, and particle penetration depth of the chemical species involved. For efficient kinetic modeling, we introduce an effective mass accommodation coefficient that accounts for the above influencing factors, can be applied in the common Fuchs–Sutugin approximation, and helps to resolve inconsistencies and shortcomings of earlier experimental and model investigations.
Sabin Kasparoglu, Ying Li, Manabu Shiraiwa, and Markus D. Petters
Atmos. Chem. Phys., 21, 1127–1141, https://doi.org/10.5194/acp-21-1127-2021, https://doi.org/10.5194/acp-21-1127-2021, 2021
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Viscosity is important because it determines the lifetime, impact, and fate of particulate matter. We collected new data to rigorously test a framework that is used to constrain the phase state in global simulations. We find that the framework is accurate as long as appropriate compound specific inputs are available.
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.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Nicole Jacobs, William R. Simpson, Debra Wunch, Christopher W. O'Dell, Gregory B. Osterman, Frank Hase, Thomas Blumenstock, Qiansi Tu, Matthias Frey, Manvendra K. Dubey, Harrison A. Parker, Rigel Kivi, and Pauli Heikkinen
Atmos. Meas. Tech., 13, 5033–5063, https://doi.org/10.5194/amt-13-5033-2020, https://doi.org/10.5194/amt-13-5033-2020, 2020
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The boreal forest is the largest seasonally varying biospheric CO2-exchange region on Earth. This region is also undergoing amplified climate warming, leading to concerns about the potential for altered regional carbon exchange. Satellite missions, such as the Orbiting Carbon Observatory-2 (OCO-2) project, can measure CO2 abundance over the boreal forest but need validation for the assurance of accuracy. Therefore, we carried out a ground-based validation of OCO-2 CO2 data at three locations.
Rui Cheng, Troy S. Magney, Debsunder Dutta, David R. Bowling, Barry A. Logan, Sean P. Burns, Peter D. Blanken, Katja Grossmann, Sophia Lopez, Andrew D. Richardson, Jochen Stutz, and Christian Frankenberg
Biogeosciences, 17, 4523–4544, https://doi.org/10.5194/bg-17-4523-2020, https://doi.org/10.5194/bg-17-4523-2020, 2020
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We measured reflected sunlight from an evergreen canopy for a year to detect changes in pigments that play an important role in regulating the seasonality of photosynthesis. Results show a strong mechanistic link between spectral reflectance features and pigment content, which is validated using a biophysical model. Our results show spectrally where, why, and when spectral features change over the course of the season and show promise for estimating photosynthesis remotely.
Cited articles
Anastasio, C. and McGregor, K. G.: Chemistry of fog waters in California's Central Valley: 1. In situ photoformation of hydroxyl radical and singlet molecular oxygen, Atmos. Environ., 35, 1079–1089, https://doi.org/10.1016/S1352-2310(00)00281-8, 2001.
Anastasio, C., Faust, B. C., and Rao, C. J.: Aromatic Carbonyl Compounds as Aqueous-Phase Photochemical Sources of Hydrogen Peroxide in Acidic Sulfate Aerosols, Fogs, and Clouds. 1. Non-Phenolic Methoxybenzaldehydes and Methoxyacetophenones with Reductants (Phenols), Environ. Sci. Technol., 31, 218–232, https://doi.org/10.1021/es960359g, 1997.
Appiani, E. and McNeill, K.: Photochemical production of singlet oxygen from particulate organic matter, Environ. Sci. Technol., 49, 3514–3522, https://doi.org/10.1021/es505712e, 2015.
Appiani, E., Ossola, R., Latch, D. E., Erickson, P. R., and McNeill, K.: Aqueous singlet oxygen reaction kinetics of furfuryl alcohol: Effect of temperature, pH, and salt content, Environ. Sci. Process. Impacts, 19, 507–516, https://doi.org/10.1039/c6em00646a, 2017.
Arakaki, T., Anastasio, C., Kuroki, Y., Nakajima, H., Okada, K., Kotani, Y., Handa, D., Azechi, S., Kimura, T., Tsuhako, A., and Miyagi, Y.: A General Scavenging Rate Constant for Reaction of Hydroxyl Radical with Organic Carbon in Atmospheric Waters, Environ. Sci. Technol., 47, 8196–8203, https://doi.org/10.1021/es401927b, 2013.
Arciva, S., Niedek, C., Mavis, C., Yoon, M., Sanchez, M. E., Zhang, Q., and Anastasio, C.: Aqueous ⚫OH Oxidation of Highly Substituted Phenols as a Source of Secondary Organic Aerosol, Environ. Sci. Technol., 56, 9959–9967, https://doi.org/10.1021/acs.est.2c02225, 2022.
Arnold, S. R., Law, K. S., Brock, C. A., Thomas, J. L., Starkweather, S. M., Von Salzen, K., Stohl, A., Sharma, S., Lund, M. T., Flanner, M. G., Petäjä, T., Tanimoto, H., Gamble, J., Dibb, J. E., Melamed, M., Johnson, N., Fidel, M., Tynkkynen, V. P., Baklanov, A., Eckhardt, S., Monks, S. A., Browse, J., and Bozem, H.: Arctic air pollution: Challenges and opportunities for the next decade, Elementa, 4, 000104, https://doi.org/10.12952/journal.elementa.000104, 2016.
Atwi, K., Cheng, Z., El Hajj, O., Perrie, C., and Saleh, R.: A dominant contribution to light absorption by methanol-insoluble brown carbon produced in the combustion of biomass fuels typically consumed in wildland fires in the United States, Environ. Sci.-Atmospheres, 2, 182–191, https://doi.org/10.1039/d1ea00065a, 2022.
Badali, K. M., Zhou, S., Aljawhary, D., Antiñolo, M., Chen, W. J., Lok, A., Mungall, E., Wong, J. P. S., Zhao, R., and Abbatt, J. P. D.: Formation of hydroxyl radicals from photolysis of secondary organic aerosol material, Atmos. Chem. Phys., 15, 7831––7840, https://doi.org/10.5194/acp-15-7831-2015, 2015.
Bali, K., Banerji, S., Campbell, J. R., Bhakta, A. V., Chen, L. W. A., Holmes, C. D., and Mao, J.: Measurements of brown carbon and its optical properties from boreal forest fires in Alaska summer, Atmos. Environ., 324, 120436, https://doi.org/10.1016/j.atmosenv.2024.120436, 2024.
Bielski, B. H., Babelli, D. E., Arudi, R. L., and Ross, A. B.: Reactivity of HO2/O
Bodesheim, M., Schlitz, M., and Schmidt, R.: Triplet state energy dependence of the competitive formation of
Bogler, S., Daellenbach, K. R., Bell, D. M., Prévôt, A. S. H., El Haddad, I., and Borduas-Dedekind, N.: Singlet Oxygen Seasonality in Aqueous PM10 is Driven by Biomass Burning and Anthropogenic Secondary Organic Aerosol, Environ. Sci. Technol., 56, 15389–15397, https://doi.org/10.1021/acs.est.2c04554, 2022.
Brett, N., Law, K. S., Arnold, S. R., Fochesatto, J. G., Raut, J.-C., Onishi, T., Gilliam, R., Fahey, K., Huff, D., Pouliot, G., Barret, B., Dieudonné, E., Pohorsky, R., Schmale, J., Baccarini, A., Bekki, S., Pappaccogli, G., Scoto, F., Decesari, S., Donateo, A., Cesler-Maloney, M., Simpson, W., Medina, P., D'Anna, B., Temime-Roussel, B., Savarino, J., Albertin, S., Mao, J., Alexander, B., Moon, A., DeCarlo, P. F., Selimovic, V., Yokelson, R., and Robinson, E. S.: Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022, Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, 2025.
Campbell, J. R., Battaglia, M., Dingilian, K., Cesler-Maloney, M., St Clair, J. M., Hanisco, T. F., Robinson, E., Decarlo, P., Simpson, W., Nenes, A., Weber, R. J., and Mao, J.: Source and Chemistry of Hydroxymethanesulfonate (HMS) in Fairbanks, Alaska, Environ. Sci. Technol., 56, 7657–7667, https://doi.org/10.1021/acs.est.2c00410, 2022.
Campbell, J., Battaglia Jr., M., Dingilian, K., Cesler-Maloney, M., Simpson, W., Robinson, E., DeCarlo, P., Temime-Roussel, B., D'Anna, B., Holen, A., Wu, J., Pratt, K., Dibb, J., Nenes, A., Weber, R., and Mao, J.: Enhanced aqueous formation and neutralization of fine atmospheric particles driven by extreme cold, Fairbanks, Alaska, 2022, Arctic Data Center [data set], https://doi.org/10.18739/A2G73757K, 2024a.
Campbell, J. R., Battaglia Jr., M., Dingilian, K. K., Cesler-Maloney, M., Simpson, W. R., Robinson, E. S., DeCarlo, P. F., Temime-Roussel, B., Holen, A. L., Wu, J., Pratt, K. A., Dibb, J. E., Nenes, A., Weber, R. J., and Mao, J.: Enhanced aqueous formation and neutralization of fine atmospheric particles driven by extreme cold, Sci. Adv., 10, 4373, https://doi.org/10.1126/sciadv.ado4373, 2024b.
Cesler-Maloney, M., Simpson, W. R., Miles, T., Mao, J., Law, K. S., and Roberts, T. J.: Differences in Ozone and Particulate Matter Between Ground Level and 20 m Aloft are Frequent During Wintertime Surface-Based Temperature Inversions in Fairbanks, Alaska, J. Geophys. Res.-Atmos., 127, 036215, https://doi.org/10.1029/2021JD036215, 2022.
Cesler-Maloney, M., Simpson, W., Kuhn, J., Stutz, J., Thomas, J., Roberts, T., Huff, D., and Cooperdock, S.: Shallow boundary layer heights controlled by the surface-based temperature inversion strength are responsible for trapping home heating emissions near the ground level in Fairbanks, Alaska, EGUsphere [preprint], https://doi.org/10.5194/egusphere-2023-3082, 2024.
Chen, H., Ge, X., and Ye, Z.: Aqueous-Phase Secondary Organic Aerosol Formation Via Reactions with Organic Triplet Excited States – a Short Review, Current Pollution Reports, 4, 8–12, https://doi.org/10.1007/s40726-018-0079-7, 2018.
Cheng, Y., Zheng, G., Wei, C., Mu, Q., Zheng, B., Wang, Z., Gao, M., Zhang, Q., He, K., Carmichael, G., Pöschl, U., and Su, H.: Reactive nitrogen chemistry in aerosol water as a source of sulfate during haze events in China, Sci. Adv., 2, 1601530, https://doi.org/10.1126/sciadv.1601530, 2016.
Corral Arroyo, P., David, G., Alpert, P. A., Parmentier, E. A., Ammann, M., and Signorell, R.: Amplification of light within aerosol particles accelerates in-particle photochemistry, Science, 376, 293–296, https://doi.org/10.1126/science.abm7915, 2022.
Crawford, J., Shetter, R. E., Lefer, B., Cantrell, C., Junkermann, W., Madronich, S., and Calvert, J.: Cloud impacts on UV spectral actinic flux observed during the International Photolysis Frequency Measurement and Model Intercomparison (IPMMI), J. Geophys. Res.-Atmos., 108, 8545, https://doi.org/10.1029/2002jd002731, 2003.
Cziczo, D. J. and Abbatt, J. P. D.: Deliquescence, efflorescence, and supercooling of ammonium sulfate aerosols at low temperature: Implications for cirrus cloud formation and aerosol phase in the atmosphere, J. Geophys. Res.-Atmos., 104, 13781–13790, https://doi.org/10.1029/1999JD900112, 1999.
Dingilian, K., Hebert, E., Battaglia, M., Campbell, J., Cesler-Maloney, M., Simpson, W., St. Clair, J., Dibb, J., Temime-Roussel, B., D'Anna, B., Moon, A., Alexander, B., Yang, Y., Nenes, A., Mao, J., and Weber, R.: Hydroxymethanesulfonate and Sulfur (IV) in Fairbanks Winter During the Alaskan Layered Pollution and Chemical Analysis (ALPACA) Study, 2022, Arctic Data Center [data set], https://doi.org/10.18739/A2VD6P65Q, 2024a.
Dingilian, K., Hebert, E., Battaglia, M., Campbell, J. R., Cesler-Maloney, M., Simpson, W., St. Clair, J. M., Dibb, J., Temime-Roussel, B., D'Anna, B., Moon, A., Alexander, B., Yang, Y., Nenes, A., Mao, J., and Weber, R. J.: Hydroxymethanesulfonate and Sulfur(IV) in Fairbanks Winter During the ALPACA Study, ACS ES&T Air, 1, 646–659, https://doi.org/10.1021/acsestair.4c00012, 2024b.
Edwards, K. C., Kapur, S., Fang, T., Cesler-Maloney, M., Yang, Y., Holen, A. L., Wu, J., Robinson, E. S., DeCarlo, P. F., Pratt, K. A., Weber, R. J., Simpson, W. R., and Shiraiwa, M.: Residential Wood Burning and Vehicle Emissions as Major Sources of Environmentally Persistent Free Radicals in Fairbanks, Alaska, Environ. Sci. Technol., 58, 14293–14305, https://doi.org/10.1021/acs.est.4c01206, 2024.
Farley, R., Bernays, N., Jaffe, D. A., Ketcherside, D., Hu, L., Zhou, S., Collier, S., and Zhang, Q.: Persistent Influence of Wildfire Emissions in the Western United States and Characteristics of Aged Biomass Burning Organic Aerosols under Clean Air Conditions, Environ. Sci. Technol., 56, 3645–3657, https://doi.org/10.1021/acs.est.1c07301, 2022.
Finlayson-Pitts, B. J. and Pitts Jr., J. N.: Chemistry of the Upper and Lower Atmosphere: Theory, Experiments, and Applications, Academic Press, https://doi.org/10.1016/B978-0-12-257060-5.X5000-X, 2000.
Galbavy, E. S., Ram, K., and Anastasio, C.: 2-Nitrobenzaldehyde as a chemical actinometer for solution and ice photochemistry, J. Photochem. Photobiol. A Chem., 209, 186–192, https://doi.org/10.1016/j.jphotochem.2009.11.013, 2010.
Gerritz, L., Schervish, M., Lakey, P. S. J., Oeij, T., Wei, J., Nizkorodov, S. A., and Shiraiwa, M.: Photoenhanced Radical Formation in Aqueous Mixtures of Levoglucosan and Benzoquinone: Implications to Photochemical Aging of Biomass-Burning Organic Aerosols, J. Phys. Chem. A, 127, 5209–5221, https://doi.org/10.1021/acs.jpca.3c01794, 2023.
Gerritz, L., Wei, J., Fang, T., Wong, C., Klodt, A. L., Nizkorodov, S. A., and Shiraiwa, M.: Reactive Oxygen Species Formation and Peroxide and Carbonyl Decomposition in Aqueous Photolysis of Secondary Organic Aerosols, Environ. Sci. Technol., 58, 4716–4726, https://doi.org/10.1021/acs.est.3c08662, 2024.
Hearn, J. D. and Smith, G. D.: Measuring rates of reaction in supercooled organic particles with implications for atmospheric aerosol, Phys. Chem. Chem. Phys., 7, 2549–2551, https://doi.org/10.1039/b506424d, 2005.
Helms, J. R., Stubbins, A., Ritchie, J. D., Minor, E. C., Kieber, D. J., and Mopper, K.: Absorption spectral slopes and slope ratios as indicators of molecular weight, source, and photobleaching of chromophoric dissolved organic matter, Limnol. Oceanogr., 53, 955–969, https://doi.org/10.4319/lo.2008.53.3.0955, 2008.
Ibusuki, T. and Takeuchi, K.: Sulfur dioxide oxidation by oxygen catalyzed by mixtures of manganese(II) and iron(III) in aqueous solutions at environmental reaction conditions, Atmos. Environ., 21, 1555–1560, https://doi.org/10.1016/0004-6981(87)90317-9, 1986.
Ijaz, A., Temime-Roussel, B., Chazeau, B., Albertin, S., Arnold, S. R., Barrett, B., Bekki, S., Brett, N., Cesler-Maloney, M., Dieudonne, E., Dingilian, K. K., Fochesatto, J. G., Mao, J., Moon, A., Savarino, J., Simpson, W., Weber, R. J., Law, K. S., and D'Anna, B.: Complementary aerosol mass spectrometry elucidates sources of wintertime sub-micron particle pollution in Fairbanks, Alaska, during ALPACA 2022 , EGUsphere [preprint], https://doi.org/10.5194/egusphere-2024-3789, 2024.
Jiang, W., Misovich, M. V., Hettiyadura, A. P. S., Laskin, A., McFall, A. S., Anastasio, C., and Zhang, Q.: Photosensitized Reactions of a Phenolic Carbonyl from Wood Combustion in the Aqueous Phase – Chemical Evolution and Light Absorption Properties of AqSOA, Environ. Sci. Technol., 55, 5199–5211, https://doi.org/10.1021/acs.est.0c07581, 2021.
Jiang, W., Ma, L., Niedek, C., Anastasio, C., and Zhang, Q.: Chemical and Light-Absorption Properties of Water-Soluble Organic Aerosols in Northern California and Photooxidant Production by Brown Carbon Components, ACS Earth Space Chem., 7, 1107–1119, https://doi.org/10.1021/acsearthspacechem.3c00022, 2023a.
Jiang, W., Niedek, C., Anastasio, C., and Zhang, Q.: Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants, Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, 2023b.
Joo, T., Machesky, J. E., Zeng, L., Hass-Mitchell, T., Weber, R. J., Gentner, D. R., and Ng, N. L.: Secondary Brown Carbon Formation From Photooxidation of Furans From Biomass Burning, Geophys. Res. Lett., 51, 104900, https://doi.org/10.1029/2023GL104900, 2024.
Kapur, S., Edwards, K. C., Fang, T., Schervish, M., Lakey, P. S. J., Yang, Y., Robinson, E. S., DeCarlo, P. F., Simpson, W. R., Weber, R. J., and Shiraiwa, M.: Reactive oxygen species, environmentally persistent free radicals, and oxidative potential of outdoor and indoor particulate matter in Wintertime Fairbanks, Alaska, Aerosol Sci. Technol., 1–18, https://doi.org/10.1080/02786826.2024.2433656, 2024.
Kaur, R. and Anastasio, C.: First Measurements of Organic Triplet Excited States in Atmospheric Waters, Environ. Sci. Technol., 52, 5218–5226, https://doi.org/10.1021/acs.est.7b06699, 2018.
Kaur, R., Labins, J. R., Helbock, S. S., Jiang, W., Bein, K. J., Zhang, Q., and Anastasio, C.: Photooxidants from brown carbon and other chromophores in illuminated particle extracts, Atmos. Chem. Phys., 19, 6579–6594, https://doi.org/10.5194/acp-19-6579-2019, 2019.
Kiland, K. J., Mahrt, F., Peng, L., Nikkho, S., Zaks, J., Crescenzo, G. V., and Bertram, A. K.: Viscosity, Glass Formation, and Mixing Times within Secondary Organic Aerosol from Biomass Burning Phenolics, ACS Earth Space Chem., 7, 1388–1400, https://doi.org/10.1021/acsearthspacechem.3c00039, 2023.
Koop, T., Bookhold, J., Shiraiwa, M., and Pöschl, U.: Glass transition and phase state of organic compounds: Dependency on molecular properties and implications for secondary organic aerosols in the atmosphere, Phys. Chem. Chem. Phys., 13, 19238–19255, https://doi.org/10.1039/c1cp22617g, 2011.
Kotchenruther, R. A.: Source apportionment of PM2.5 at multiple Northwest U.S. sites: Assessing regional winter wood smoke impacts from residential wood combustion, Atmos. Environ., 142, 210–219, https://doi.org/10.1016/j.atmosenv.2016.07.048, 2016.
Kuhn, J., Stutz, J., Bartels-Rausch, T., Thomas, J. L., Cesler-Maloney, M., Simpson, W., Dibb, J. E., Heinlein, L. M. D., and Anastasio, C.: The interplay between snow and polluted air masses in cold urban environments, Faraday Discuss, 258, 502–520, https://doi.org/10.1039/D4FD00176A, 2024.
Laskin, A., Laskin, J., and Nizkorodov, S. A.: Chemistry of Atmospheric Brown Carbon, Chem. Rev., 115, 4335–4382, https://doi.org/10.1021/cr5006167, 2015.
Laskin, A., West, C. P., and Hettiyadura, A. P. S.: Molecular insights into the composition, sources, and aging of atmospheric brown carbon, Chem. Soc. Rev., 54, 1583–1612, https://doi.org/10.1039/D3CS00609C, 2025.
Leresche, F., Salazar, J. R., Pfotenhauer, D. J., Hannigan, M. P., Majestic, B. J., and Rosario-Ortiz, F. L.: Photochemical Aging of Atmospheric Particulate Matter in the Aqueous Phase, Environ. Sci. Technol., 55, 13152–13163, https://doi.org/10.1021/acs.est.1c00978, 2021.
Li, J., Zhang, Q., Wang, G., Li, J., Wu, C., Liu, L., Wang, J., Jiang, W., Li, L., Ho, K. F., and Cao, J.: Optical properties and molecular compositions of water-soluble and water-insoluble brown carbon (BrC) aerosols in northwest China, Atmos. Chem. Phys., 20, 4889–4904, https://doi.org/10.5194/acp-20-4889-2020, 2020.
Liang, Z., Zhou, L., Chang, Y., Qin, Y., and Chan, C. K.: Biomass-burning organic aerosols as a pool of atmospheric reactive triplets to drive multiphase sulfate formation, P. Natl. Acad. Sci. USA, 121, e2416803121, https://doi.org/10.1073/pnas.2416803121, 2024.
Lyu, Y., Lam, Y. H., Li, Y., Borduas-Dedekind, N., and Nah, T.: Seasonal variations in the production of singlet oxygen and organic triplet excited states in aqueous PM2.5 in Hong Kong SAR, South China, Atmos. Chem. Phys., 23, 9245–9263, https://doi.org/10.5194/acp-23-9245-2023, 2023.
Ma, L., Guzman, C., Niedek, C., Tran, T., Zhang, Q., and Anastasio, C.: Kinetics and Mass Yields of Aqueous Secondary Organic Aerosol from Highly Substituted Phenols Reacting with a Triplet Excited State, Environ. Sci. Technol., 55, 5772–5781, https://doi.org/10.1021/acs.est.1c00575, 2021.
Ma, L., Worland, R., Tran, T., and Anastasio, C.: Evaluation of Probes to Measure Oxidizing Organic Triplet Excited States in Aerosol Liquid Water, Environ. Sci. Technol., 57, 6052–6062, https://doi.org/10.1021/acs.est.2c09672, 2022.
Ma, L., Worland, R., Jiang, W., Niedek, C., Guzman, C., Bein, K. J., Zhang, Q., and Anastasio, C.: Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles, Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, 2023.
Ma, L., Worland, R., Heinlein, L., Guzman, C., Jiang, W., Niedek, C., Bein, K. J., Zhang, Q., and Anastasio, C.: Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles, Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, 2024.
Madronich, S. and Flocke, S.: The role of solar radiation in atmospheric chemistry, in: Handbook of Environmental Chemistry, Springer-Verlag, 1–26, https://doi.org/10.1007/978-3-540-69044-3_1, 1998.
Manfrin, A., Nizkorodov, S. A., Malecha, K. T., Getzinger, G. J., McNeill, K., and Borduas-Dedekind, N.: Reactive Oxygen Species Production from Secondary Organic Aerosols: The Importance of Singlet Oxygen, Environ. Sci. Technol., 53, 8553–8562, https://doi.org/10.1021/acs.est.9b01609, 2019.
Mao, J., Fan, S., Jacob, D. J., and Travis, K. R.: Radical loss in the atmosphere from Cu-Fe redox coupling in aerosols, Atmos. Chem. Phys., 13, 509–519, https://doi.org/10.5194/acp-13-509-2013, 2013.
Mao, J., Bali, K., Campbell, J. R., Robinson, E. S., DeCarlo, P. F., Ijaz, A., Temime-Roussel, B., Barbara, D., Ketcherside, D., Yokelson, R. J., Hu, L., Cesler-Maloney, M., Simpson, W., Guo, F., Flynn, J., St. Clair, J., Nenes, A., and Weber, R.: Multiphase sulfur chemistry facilitates particle growth in a cold and dark urban environment, Faraday Discuss, 258, 357–374, https://doi.org/10.1039/D4FD00170B, 2024.
Martin, L. R. and Hill, M. W.: The Effect of Ionic Strength on the Manganese Catalyzed Oxidation of Sulfur (IV), Atmos. Environ., 21, 2267–2270, https://doi.org/10.1016/0004-6981(87)90361-1, 1987.
McNeill, K. and Canonica, S.: Triplet state dissolved organic matter in aquatic photochemistry: Reaction mechanisms, substrate scope, and photophysical properties, Environ. Sci. Process. Impacts, 18, 1381–1399, https://doi.org/10.1039/c6em00408c, 2016.
Moon, A., Jongebloed, U., Dingilian, K., Schauer, A., Chan, Y.-C., Cesler-Maloney, M., Simpson, W., Weber, R., Tsiang, L., Yazbeck, F., Zhai, S., Wedum, A., Turner, A., Albertin, S., Bekki, S., Savarino, J., Gribanov, K., Pratt, K., Costa, E., Anastasio, C., Sunday, M., Heinlein, L., Mao, J., and Alexander, B.: Fairbanks sulfate isotope measurements during ALPACA (2022), Arctic Data Center [data set], https://doi.org/10.18739/A2Q52FF68, 2023.
Moon, A., Jongebloed, U., Dingilian, K. K., Schauer, A. J., Chan, Y.-C., Cesler-Maloney, M., Simpson, W. R., Weber, R. J., Tsiang, L., Yazbeck, F., Zhai, S., Wedum, A., Turner, A. J., Albertin, S., Bekki, S., Savarino, J., Gribanov, K., Pratt, K. A., Costa, E. J., Anastasio, C., Sunday, M. O., Heinlein, L. M. D., Mao, J., and Alexander, B.: Primary Sulfate Is the Dominant Source of Particulate Sulfate during Winter in Fairbanks, Alaska, ES&T Air, 1, 139–149, https://doi.org/10.1021/acsestair.3c00023, 2024.
Mu, Y., Chen, J., Herrmann, H., Ye, C., Chen, H., Hoffmann, E. H., Mettke, P., Tilgner, A., He, L., Mutzel, A., Brüggemann, M., Poulain, L., Schaefer, T., Heinold, B., Ma, Z., Liu, P., Xue, C., Zhao, X., Zhang, C., Zhang, F., Sun, H., Li, Q., Wang, L., Yang, X., Wang, J., Liu, C., and Xing, C.: Particle-phase photoreactions of Hulis and TMIs establish a strong source of H2O2 and particulate sulfate in the winter North China Plain, Environ. Sci. Technol., 55, 7818–7830, https://doi.org/10.1021/acs.est.1c00561, 2021.
Önnby, L., Salhi, E., McKay, G., Rosario-Ortiz, F. L., and von Gunten, U.: Ozone and chlorine reactions with dissolved organic matter – Assessment of oxidant-reactive moieties by optical measurements and the electron donating capacities, Water Res., 144, 64–75, https://doi.org/10.1016/j.watres.2018.06.059, 2018.
Ossola, R., Jönsson, O. M., Moor, K., and McNeill, K.: Singlet Oxygen Quantum Yields in Environmental Waters, Chem. Rev., 121, 4100–4146, https://doi.org/10.1021/acs.chemrev.0c00781, 2021.
Peuravuori, J. and Pihlaja, K.: Molecular size distribution and spectroscopic properties of aquatic humic substances, Anal. Chim. Acta, 337, 133–149, 1997.
Reid, J. P., Bertram, A. K., Topping, D. O., Laskin, A., Martin, S. T., Petters, M. D., Pope, F. D., and Rovelli, G.: The viscosity of atmospherically relevant organic particles, Nat. Commun., 9, 956, https://doi.org/10.1038/s41467-018-03027-z, 2018.
Remke, S. C., Bürgin, T. H., Ludvíková, L., Heger, D., Wenger, O. S., von Gunten, U., and Canonica, S.: Photochemical oxidation of phenols and anilines mediated by phenoxyl radicals in aqueous solution, Water Res., 213, 118095, https://doi.org/10.1016/j.watres.2022.118095, 2022.
Robinson, E. S., Cesler-Maloney, M., Tan, X., Mao, J., Simpson, W., and DeCarlo, P. F.: Wintertime spatial patterns of particulate matter in Fairbanks, AK during ALPACA 2022, Environ. Sci.-Atmospheres, 3, 568–580, https://doi.org/10.1039/d2ea00140c, 2023.
Robinson, E. S., Battaglia, M., Campbell, J. R., Cesler-Maloney, M., Simpson, W., Mao, J., Weber, R. J., and DeCarlo, P. F.: Multi-year, high-time resolution aerosol chemical composition and mass measurements from Fairbanks, Alaska, Environ. Sci.-Atmospheres, 4, 685–698, https://doi.org/10.1039/d4ea00008k, 2024.
Sander, R.: Compilation of Henry's law constants (version 5.0.0) for water as solvent, Atmos. Chem. Phys., 23, 10901–12440, https://doi.org/10.5194/acp-23-10901-2023, 2023.
Schmale, J., Arnold, S. R., Law, K. S., Thorp, T., Anenberg, S., Simpson, W. R., Mao, J., and Pratt, K. A.: Local Arctic Air Pollution: A Neglected but Serious Problem, Earths Fut., 6, 1385–1412, https://doi.org/10.1029/2018EF000952, 2018.
Schweitzer, G., Gronheid, R., Jordens, S., Lor, M., De Belder, G., Weil, T., Reuther, E., Müllen, K., and De Schryver, F. C.: Intramolecular directional energy transfer processes in dendrimers containing perylene and terrylene chromophores, J. Phys. Chem. A, 107, 3199–3207, https://doi.org/10.1021/jp026459s, 2003.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, 3rd edn., Wiley, ISBN-13: 978-1118947401, 2016.
Shiraiwa, M., Li, Y., Tsimpidi, A. P., Karydis, V. A., Berkemeier, T., Pandis, S. N., Lelieveld, J., Koop, T., and Pöschl, U.: Global distribution of particle phase state in atmospheric secondary organic aerosols, Nat. Commun., 8, 15002, https://doi.org/10.1038/ncomms15002, 2017.
Simpson, W., Law, K., Schmale, J., Pratt, K., Arnold, S., Mao, J., Alexander, B., Anenberg, S., Baklanov, A., Bell, D., Brown, S., Creamean, J., de Boer, G., DeCarlo, P., Descari, S., Elleman, R., Flynn, J., Fochesatto, J., Ganzenfeld, L., Griffin, R., Järvi, L., Kaspari, S., Konstantinov, P., Murphy, J., Petäjä, T., Pye, H., Jean-Christophe Raut, J.-C., Roberts, T., Shiraiwa, M., Stutz, J., Thomas, J., Thornton, J., Weber, R., Webley, P., and Williams, B.: Alaskan Layered Pollution And Chemical Analysis (ALPACA) White Paper, 2019.
Simpson, W., Cesler-Maloney, M., and Hoskins-Chaddon, R.: Gas and meteorological measurements at the CTC site and Birch Hill in Fairbanks, Alaska, during the ALPACA-2022 field study, Arctic Data Center [data set], https://doi.org/10.18739/A27D2Q87W, 2023.
Simpson, W. R., Mao, J., Fochesatto, G. J., Law, K. S., DeCarlo, P. F., Schmale, J., Pratt, K. A., Arnold, S. R., Stutz, J., Dibb, J. E., Creamean, J. M., Weber, R. J., Williams, B. J., Alexander, B., Hu, L., Yokelson, R. J., Shiraiwa, M., Decesari, S., Anastasio, C., D'Anna, B., Gilliam, R. C., Nenes, A., St. Clair, J. M., Trost, B., Flynn, J. H., Savarino, J., Conner, L. D., Kettle, N., Heeringa, K. M., Albertin, S., Baccarini, A., Barret, B., Battaglia, M. A., Bekki, S., Brado, T. J., Brett, N., Brus, D., Campbell, J. R., Cesler-Maloney, M., Cooperdock, S., Cysneiros de Carvalho, K., Delbarre, H., DeMott, P. J., Dennehy, C. J. S., Dieudonné, E., Dingilian, K. K., Donateo, A., Doulgeris, K. M., Edwards, K. C., Fahey, K., Fang, T., Guo, F., Heinlein, L. M. D., Holen, A. L., Huff, D., Ijaz, A., Johnson, S., Kapur, S., Ketcherside, D. T., Levin, E., Lill, E., Moon, A. R., Onishi, T., Pappaccogli, G., Perkins, R., Pohorsky, R., Raut, J.-C., Ravetta, F., Roberts, T., Robinson, E. S., Scoto, F., Selimovic, V., Sunday, M. O., Temime-Roussel, B., Tian, X., Wu, J., and Yang, Y.: Overview of the Alaskan Layered Pollution and Chemical Analysis (ALPACA) Field Experiment, ACS ES&T Air, 1, 200–222, https://doi.org/10.1021/acsestair.3c00076, 2024.
Smith, J. D., Sio, V., Yu, L., Zhang, Q., and Anastasio, C.: Secondary organic aerosol production from aqueous reactions of atmospheric phenols with an organic triplet excited state, Environ. Sci. Technol., 48, 1049–1057, https://doi.org/10.1021/es4045715, 2014.
Smith, J. D., Kinney, H., and Anastasio, C.: Aqueous benzene-diols react with an organic triplet excited state and hydroxyl radical to form secondary organic aerosol, Phys. Chem. Chem. Phys., 17, 10227–10237, https://doi.org/10.1039/c4cp06095d, 2015.
Smith, J. D., Kinney, H., and Anastasio, C.: Phenolic carbonyls undergo rapid aqueous photodegradation to form low-volatility, light-absorbing products, Atmos. Environ., 126, 36–44, https://doi.org/10.1016/j.atmosenv.2015.11.035, 2016.
Song, H., Lu, K., Ye, C., Dong, H., Li, S., Chen, S., Wu, Z., Zheng, M., Zeng, L., Hu, M., and Zhang, Y.: A comprehensive observation-based multiphase chemical model analysis of sulfur dioxide oxidations in both summer and winter, Atmos. Chem. Phys., 21, 13713–13727, https://doi.org/10.5194/acp-21-13713-2021, 2021.
Sunday, M. O., Dahler Heinlein, L. M., He, J., Moon, A., Kapur, S., Fang, T., Edwards, K. C., Guo, F., Dibb, J., Flynn III, J. H., Alexander, B., Shiraiwa, M., and Anastasio, C.: Hydrogen peroxide photoformation in particulate matter and its contribution to S(IV) oxidation during winter in Fairbanks, Alaska, Atmos. Chem. Phys., 25, 5087–5100, https://doi.org/10.5194/acp-25-5087-2025, 2025.
Tilgner, A., Schaefer, T., Alexander, B., Barth, M., Collett Jr., J. L., Fahey, K. M., Nenes, A., Pye, H. O. T., Herrmann, H., and McNeill, V. F.: Acidity and the multiphase chemistry of atmospheric aqueous particles and clouds, Atmos. Chem. Phys., 21, 13483–13536, https://doi.org/10.5194/acp-21-13483-2021, 2021.
Tomaz, S., Cui, T., Chen, Y., Sexton, K. G., Roberts, J. M., Warneke, C., Yokelson, R. J., Surratt, J. D., and Turpin, B. J.: Photochemical Cloud Processing of Primary Wildfire Emissions as a Potential Source of Secondary Organic Aerosol, Environ. Sci. Technol., 52, 11027–11037, https://doi.org/10.1021/acs.est.8b03293, 2018.
Tong, H., Arangio, A. M., Lakey, P. S. J., Berkemeier, T., Liu, F., Kampf, C. J., Brune, W. H., Pöschl, U., and Shiraiwa, M.: Hydroxyl radicals from secondary organic aerosol decomposition in water, Atmos. Chem. Phys., 16, 1761–1771, https://doi.org/10.5194/acp-16-1761-2016, 2016.
Virtanen, A., Joutsensaari, J., Koop, T., Kannosto, J., Yli-Pirilä, P., Leskinen, J., Mäkelä, J. M., Holopainen, J. K., Pöschl, U., Kulmala, M., Worsnop, D. R., and Laaksonen, A.: An amorphous solid state of biogenic secondary organic aerosol particles, Nature, 467, 824–827, https://doi.org/10.1038/nature09455, 2010.
Wang, J., Li, J., Ye, J., Zhao, J., Wu, Y., Hu, J., Liu, D., Nie, D., Shen, F., Huang, X., Huang, D. D., Ji, D., Sun, X., Xu, W., Guo, J., Song, S., Qin, Y., Liu, P., Turner, J. R., Lee, H. C., Hwang, S., Liao, H., Martin, S. T., Zhang, Q., Chen, M., Sun, Y., Ge, X., and Jacob, D. J.: Fast sulfate formation from oxidation of SO2 by NO2 and HONO observed in Beijing haze, Nat. Commun., 11, 2844, https://doi.org/10.1038/s41467-020-16683-x, 2020a.
Wang, W., Liu, M., Wang, T., Song, Y., Zhou, L., Cao, J., Hu, J., Tang, G., Chen, Z., Li, Z., Xu, Z., Peng, C., Lian, C., Chen, Y., Pan, Y., Zhang, Y., Sun, Y., Li, W., Zhu, T., Tian, H., and Ge, M.: Sulfate formation is dominated by manganese-catalyzed oxidation of SO2 on aerosol surfaces during haze events, Nat. Commun., 12, 1993, https://doi.org/10.1038/s41467-021-22091-6, 2021.
Wang, X., Gemayel, R., Hayeck, N., Perrier, S., Charbonnel, N., Xu, C., Chen, H., Zhu, C., Zhang, L., Wang, L., Nizkorodov, S. A., Wang, X., Wang, Z., Wang, T., Mellouki, A., Riva, M., Chen, J., and George, C.: Atmospheric Photosensitization: A New Pathway for Sulfate Formation, Environ. Sci. Technol., 54, 3114–3120, https://doi.org/10.1021/acs.est.9b06347, 2020b.
Xie, M., Hays, M. D., and Holder, A. L.: Light-Absorbing organic carbon from prescribed and laboratory biomass burning and gasoline vehicle emissions, Sci. Rep., 7, 7318, https://doi.org/10.1038/s41598-017-06981-8, 2017.
Ye, C., Mu, Y., Chen, J., Chen, H., Hoffmann, E. H., Mettke, P., Tilgner, A., He, L., Mutzel, A., Brüggemann, M., Herrmann, H., Poulain, L., Schaefer, T., Heinold, B., Ma, Z., Liu, P., Xue, C., Zhao, X., Zhang, C., Zhang, F., Sun, H., Li, Q., Wang, L., Yang, X., Wang, J., Liu, C., and Xing, C.: Particle-phase photoreactions of HULIS and TMIs establish a strong source of H2O2 and particulate sulfate in the winter North China Plain, Environ. Sci. Technol., 55, 7818–7830, https://doi.org/10.1021/acs.est.1c00561, 2021.
Yu, C., Liu, T., Ge, D., Nie, W., Chi, X., and Ding, A.: Ionic Strength Enhances the Multiphase Oxidation Rate of Sulfur Dioxide by Ozone in Aqueous Aerosols: Implications for Sulfate Production in the Marine Atmosphere, Environ. Sci. Technol., 57, 6609–6615, https://doi.org/10.1021/acs.est.3c00212, 2023.
Yu, L., Smith, J., Laskin, A., Anastasio, C., Laskin, J., and Zhang, Q.: Chemical characterization of SOA formed from aqueous-phase reactions of phenols with the triplet excited state of carbonyl and hydroxyl radical, Atmos. Chem. Phys., 14, 13801–13816, https://doi.org/10.5194/acp-14-13801-2014, 2014.
Yu, L., Smith, J., Laskin, A., George, K. M., Anastasio, C., Laskin, J., Dillner, A. M., and Zhang, Q.: Molecular transformations of phenolic SOA during photochemical aging in the aqueous phase: competition among oligomerization, functionalization, and fragmentation, Atmos. Chem. Phys., 16, 4511–4527, https://doi.org/10.5194/acp-16-4511-2016, 2016.
Zhang, J., Shrivastava, M., Zelenyuk, A., Zaveri, R. A., Surratt, J. D., Riva, M., Bell, D., and Glasius, M.: Observationally Constrained Modeling of the Reactive Uptake of Isoprene-Derived Epoxydiols under Elevated Relative Humidity and Varying Acidity of Seed Aerosol Conditions, ACS Earth Space Chem., 7, 788–799, https://doi.org/10.1021/acsearthspacechem.2c00358, 2022.
Zobrist, B., Marcolli, C., Pedernera, D. A., and Koop, T.: Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 8, 5221–5244, https://doi.org/10.5194/acp-8-5221-2008, 2008.
Short summary
High-latitude cities like Fairbanks, Alaska, experience severe wintertime pollution episodes. While conventional wisdom holds that oxidation is slow under these conditions, field measurements find oxidized products in particles. To explore this, we measured oxidants in aqueous extracts of winter particles from Fairbanks. We find high concentrations of oxidants during illumination experiments, indicating that particle photochemistry can be significant even in high latitudes during winter.
High-latitude cities like Fairbanks, Alaska, experience severe wintertime pollution episodes....
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