Articles | Volume 24, issue 7
https://doi.org/10.5194/acp-24-4473-2024
© Author(s) 2024. 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-24-4473-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
17 Apr 2024
Research article |
| 17 Apr 2024
| 17 Apr 2024
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Stephanie Arciva
Department of Land, Air and Water Resources, University of California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Lan Ma
Department of Land, Air and Water Resources, University of California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
now at: SGS-CSTC Standards Technical Services Co. Ltd., Hangzhou, Zhejiang Province, 310052, China
Camille Mavis
Department of Land, Air and Water Resources, University of California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
now at: Department of Atmospheric Science, Colorado State University, Fort Collins, CO 80521, USA
Chrystal Guzman
Department of Land, Air and Water Resources, University of California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
now at: Department of Pharmacology, University of Washington, Seattle, WA 98195, USA
Department of Land, Air and Water Resources, University of California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
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Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2026-241, https://doi.org/10.5194/essd-2026-241, 2026
Preprint under review for ESSD
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This article summarizes the data sets collected during the Arctic Radiation Cloud aerosol Sea ice Interaction eXperiment (ARCSIX), NASA's most comprehensive Arctic field campaign to date. The overarching goal was to quantify the contributions of surface, clouds, aerosol particles, and precipitation to summer sea ice melt. This paper describes the ARCSIX implementation including the flight strategy, instruments, complementary data sets, access, and usage details.
Keighan J. Gemmell, Laura Marie Dahler Heinlein, Emma A. Petersen-Sonn, Claudia Sardena, Zhongyu Guo, Nory Mariño-Ocampo, Belinda Heyne, Christian George, Cort Anastasio, and Nadine Borduas-Dedekind
Atmos. Meas. Tech., 19, 3961–3982, https://doi.org/10.5194/amt-19-3961-2026, https://doi.org/10.5194/amt-19-3961-2026, 2026
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Molecular singlet oxygen (1O2*) is the first excited state of O2 and is produced when sunlight excites light-absorbing molecules in aerosols in the atmosphere. 1O2* can drive oxidation reactions and impact aerosol properties. This study is an inter-comparison of photoreactors, light sources and data analysis across 3 atmospheric chemistry laboratories, yielding a critical assessment of practices and recommendations for intercomparing 1O2* measurements and extrapolating to ambient particles.
Samuel Ephraim, Paquita Zuidema, Aaron Bansemer, Lintong Cai, Markus Petters, Elise Rosky, Jefferson R. Snider, Zhien Wang, Sarah Woods, Kevin Barry, Theresa Campos, Owen Cruikshank, Sabine Eckhardt, Nikolaos Evangeliou, Romanos Foskinis, Jeffrey R. French, Bart Geerts, Coltin Grasmick, Silvia Henning, Varun Kumar, Andreas Massling, Camille Mavis, Greg M. McFarquhar, Athanasios Nenes, Gunnar Noer, Ryan Patnaude, Russell Perkins, Lise Lotte Sorensen, Henrik Skov, Tyler Tatro, Florian Tornow, and Lu Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2026-2940, https://doi.org/10.5194/egusphere-2026-2940, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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The processes that establish how mixed-phase closed-cell clouds transition to more open cellular structures are poorly known. First-of-its kind aircraft observations document such a transition in the presence of anomalously high aerosol concentrations over the Nordic Seas at cloud temperatures < -15 °C. The reduces the drop size, discouraging riming. Eventually, ice precipitation produces surface cold pools that drive the convective transition, despite strong counteracting surface fluxes.
Hannah C. Frostenberg, Jessie M. Creamean, Erik S. Thomson, Heather Guy, Roman Pohorsky, Camille Mavis, Ian M. Brooks, Nicolas Fauré, Lea Haberstock, Julia Kojoj, Sonja Murto, Julia Schmale, Michael Tjernström, Paul Zieger, and Luisa Ickes
EGUsphere, https://doi.org/10.5194/egusphere-2026-2403, https://doi.org/10.5194/egusphere-2026-2403, 2026
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Arctic low clouds containing both droplets and ice crystals strongly impact sea ice and therefore require accurate modeling. Using a high-resolution atmospheric model, we found that particle and ice concentrations, alongside ice crystal shape, strongly dictate the simulated cloud. Therefore, these specific properties should be prioritized during future Arctic observational campaigns. Furthermore, atmospheric models must be able to represent a variety of ice crystal shapes.
Christopher Niedek, Wenqing Jiang, Antai Zhang, Cort Anastasio, and Qi Zhang
Atmos. Meas. Tech., 19, 2009–2023, https://doi.org/10.5194/amt-19-2009-2026, https://doi.org/10.5194/amt-19-2009-2026, 2026
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We developed a new photoreactor to study how organic compounds react in water under atmospheric-relevant conditions. Experiments were performed on smoke-related chemicals under controlled light, temperature, and humidity mimicking cloud and haze environments. Our results showed that saltier water speeds particle formation and changes their composition, providing new insights into atmospheric aerosol chemistry.
Laura M. D. Heinlein, Junwei He, Michael Oluwatoyin Sunday, Fangzhou Guo, James Campbell, Allison Moon, Sukriti Kapur, Ting Fang, Kasey Edwards, Meeta Cesler-Maloney, Alyssa J. Burns, Jack Dibb, William Simpson, Manabu Shiraiwa, Becky Alexander, Jingqiu Mao, James H. Flynn III, Jochen Stutz, and Cort Anastasio
Atmos. Chem. Phys., 25, 9561–9581, https://doi.org/10.5194/acp-25-9561-2025, https://doi.org/10.5194/acp-25-9561-2025, 2025
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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.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
Atmos. Chem. Phys., 25, 5087–5100, https://doi.org/10.5194/acp-25-5087-2025, https://doi.org/10.5194/acp-25-5087-2025, 2025
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that the illumination of brown carbon can rapidly form HOOH within particles, even under the low-sunlight conditions of Fairbanks, Alaska, during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
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.
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.
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.
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.
Cited articles
Aguilera, R., Corringham, T., Gershunov, A., and Benmarhnia, T.: Wildfire smoke impacts respiratory health more than fine particles from other sources: observational evidence from Southern California., Nat. Commun., 12, 1493, https://doi.org/10.1038/s41467-021-21708-0, 2021.
Akagi, S. K., Yokelson, R. J., Wiedinmyer, C., Alvarado, M. J., Reid, J. S., Karl, T., Crounse, J. D., and Wennberg, P. O.: Emission factors for open and domestic biomass burning for use in atmospheric models, Atmos. Chem. Phys., 11, 4039–4072, https://doi.org/10.5194/acp-11-4039-2011, 2011.
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.
Andreae, M. O.: Emission of trace gases and aerosols from biomass burning – an updated assessment, Atmos. Chem. Phys., 19, 8523–8546, https://doi.org/10.5194/acp-19-8523-2019, 2019.
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.
Berndt, T. and Böge, O.: Gas-phase reaction of OH radicals with phenol, Phys. Chem. Chem. Phys., 5, 342–350, https://doi.org/10.1039/B208187C, 2003.
Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J.-H., and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res.-Atmos., 109, D14203, https://doi.org/10.1029/2003JD003697, 2004.
Buxton, G. V., Greenstock, C. L., Helman, W. P., and Ross, A. B.: Critical Review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals (OH/O- in Aqueous Solution, J. Phys. Chem. Ref. Data, 17, 513–886, https://doi.org/10.1063/1.555805, 1988.
Chang, J. L. and Thompson, J. E.: Characterization of colored products formed during irradiation of aqueous solutions containing H2O2 and phenolic compounds, Atmos. Environ., 44, 541–551, https://doi.org/10.1016/j.atmosenv.2009.10.042, 2010.
Coeur-Tourneur, C., Cassez, A., and Wenger, J. C.: Rate coefficients for the gas-phase reaction of hydroxyl radicals with 2-methoxyphenol (guaiacol) and related compounds., J. Phys. Chem. A, 114, 11645–11650, https://doi.org/10.1021/jp1071023, 2010.
Di Lorenzo, R. A., Washenfelder, R. A., Attwood, A. R., Guo, H., Xu, L., Ng, N. L., Weber, R. J., Baumann, K., Edgerton, E., and Young, C. J.: Molecular-Size-Separated Brown Carbon Absorption for Biomass-Burning Aerosol at Multiple Field Sites, Environ. Sci. Technol., 51, 3128–3137, https://doi.org/10.1021/acs.est.6b06160, 2017.
Dulo, B., Phan, K., Githaiga, J., Raes, K., and De Meester, S.: Natural quinone dyes: A review on structure, extraction techniques, analysis and application potential, Waste Biomass Valor., 12, 6339–6374, https://doi.org/10.1007/s12649-021-01443-9, 2021.
Fleming, L. T., Lin, P., Roberts, J. M., Selimovic, V., Yokelson, R., Laskin, J., Laskin, A., and Nizkorodov, S. A.: Molecular composition and photochemical lifetimes of brown carbon chromophores in biomass burning organic aerosol, Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, 2020.
Garofalo, L. A., Pothier, M. A., Levin, E. J. T., Campos, T., Kreidenweis, S. M., and Farmer, D. K.: Emission and Evolution of Submicron Organic Aerosol in Smoke from Wildfires in the Western United States, ACS Earth Space Chem., 3, 1237–1247, https://doi.org/10.1021/acsearthspacechem.9b00125, 2019.
Graber, E. R. and Rudich, Y.: Atmospheric HULIS: How humic-like are they? A comprehensive and critical review, Atmos. Chem. Phys., 6, 729–753, https://doi.org/10.5194/acp-6-729-2006, 2006.
Grieshop, A. P., Logue, J. M., Donahue, N. M., and Robinson, A. L.: Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 1: measurement and simulation of organic aerosol evolution, Atmos. Chem. Phys., 9, 1263–1277, https://doi.org/10.5194/acp-9-1263-2009, 2009.
Gurol, M. D. and Nekouinaini, S.: Kinetic behavior of ozone in aqueous solutions of substituted phenols, Ind. Eng. Chem. Fund., 23, 54–60, https://doi.org/10.1021/i100013a011, 1984.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
Heald, C. L., Henze, D. K., Horowitz, L. W., Feddema, J., Lamarque, J. F., Guenther, A., Hess, P. G., Vitt, F., Seinfeld, J. H., Goldstein, A. H., and Fung, I.: Predicted change in global secondary organic aerosol concentrations in response to future climate, emissions, and land use change, J. Geophys. Res., 113, D05211, https://doi.org/10.1029/2007JD009092, 2008.
Hecobian, A., Zhang, X., Zheng, M., Frank, N., Edgerton, E. S., and Weber, R. J.: Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States, Atmos. Chem. Phys., 10, 5965–5977, https://doi.org/10.5194/acp-10-5965-2010, 2010.
Hems, R. F., Schnitzler, E. G., Bastawrous, M., Soong, R., Simpson, A. J., and Abbatt, J. P. D.: Aqueous photoreactions of wood smoke brown carbon, ACS Earth Space Chem., 4, 1149–1160, https://doi.org/10.1021/acsearthspacechem.0c00117, 2020.
Hems, R. F., Schnitzler, E. G., Liu-Kang, C., Cappa, C. D., and Abbatt, J. P. D.: Aging of atmospheric brown carbon aerosol, ACS Earth Space Chem., 5, 722–748, https://doi.org/10.1021/acsearthspacechem.0c00346, 2021.
Hennigan, C. J., Miracolo, M. A., Engelhart, G. J., May, A. A., Presto, A. A., Lee, T., Sullivan, A. P., McMeeking, G. R., Coe, H., Wold, C. E., Hao, W.-M., Gilman, J. B., Kuster, W. C., de Gouw, J., Schichtel, B. A., Collett Jr., J. L., Kreidenweis, S. M., and Robinson, A. L.: Chemical and physical transformations of organic aerosol from the photo-oxidation of open biomass burning emissions in an environmental chamber, Atmos. Chem. Phys., 11, 7669–7686, https://doi.org/10.5194/acp-11-7669-2011, 2011.
Huang, D. D., Zhang, Q., Cheung, H. H. Y., Yu, L., Zhou, S., Anastasio, C., Smith, J. D., and Chan, C. K.: Formation and Evolution of aqSOA from Aqueous-Phase Reactions of Phenolic Carbonyls: Comparison between Ammonium Sulfate and Ammonium Nitrate Solutions., Environ. Sci. Technol., 52, 9215–9224, https://doi.org/10.1021/acs.est.8b03441, 2018.
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.
Jimenez, J. L., Canagaratna, M. R., Donahue, N. M., Prevot, A. S. H., Zhang, Q., Kroll, J. H., DeCarlo, P. F., Allan, J. D., Coe, H., Ng, N. L., Aiken, A. C., Docherty, K. S., Ulbrich, I. M., Grieshop, A. P., Robinson, A. L., Duplissy, J., Smith, J. D., Wilson, K. R., Lanz, V. A., Hueglin, C., Sun, Y. L., Tian, J., Laaksonen, A., Raatikainen, T., Rautiainen, J., Vaattovaara, P., Ehn, M., Kulmala, M., Tomlinson, J. M., Collins, D. R., Cubison, M. J., Dunlea, E. J., Huffman, J. A., Onasch, T. B., Alfarra, M. R., Williams, P. I., Bower, K., Kondo, Y., Schneider, J., Drewnick, F., Borrmann, S., Weimer, S., Demerjian, K., Salcedo, D., Cottrell, L., Griffin, R., Takami, A., Miyoshi, T., Hatakeyama, S., Shimono, A., Sun, J. Y., Zhang, Y. M., Dzepina, K., Kimmel, J. R., Sueper, D., Jayne, J. T., Herndon, S. C., Trimborn, A. M., Williams, L. R., Wood, E. C., Middlebrook, A. M., Kolb, C. E., Baltensperger, U., and Worsnop, D. R.: Evolution of organic aerosols in the atmosphere, Science, 326, 1525–1529, https://doi.org/10.1126/science.1180353, 2009.
Jo, D. S., Park, R. J., Lee, S., Kim, S.-W., and Zhang, X.: A global simulation of brown carbon: implications for photochemistry and direct radiative effect, Atmos. Chem. Phys., 16, 3413–3432, https://doi.org/10.5194/acp-16-3413-2016, 2016.
Kaeswurm, J. A. H., Scharinger, A., Teipel, J., and Buchweitz, M.: Absorption coefficients of phenolic structures in different solvents routinely used for experiments, Molecules, 26, 4656, https://doi.org/10.3390/molecules26154656, 2021.
Kanakidou, M., Seinfeld, J. H., Pandis, S. N., Barnes, I., Dentener, F. J., Facchini, M. C., Van Dingenen, R., Ervens, B., Nenes, A., Nielsen, C. J., Swietlicki, E., Putaud, J. P., Balkanski, Y., Fuzzi, S., Horth, J., Moortgat, G. K., Winterhalter, R., Myhre, C. E. L., Tsigaridis, K., Vignati, E., Stephanou, E. G., and Wilson, J.: Organic aerosol and global climate modelling: a review, Atmos. Chem. Phys., 5, 1053–1123, https://doi.org/10.5194/acp-5-1053-2005, 2005.
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, 2019a.
Kaur, R., Hudson, B. M., Draper, J., Tantillo, D. J., and Anastasio, C.: Aqueous reactions of organic triplet excited states with atmospheric alkenes, Atmos. Chem. Phys., 19, 5021–5032, https://doi.org/10.5194/acp-19-5021-2019, 2019b.
Kim, K.-H., Kabir, E., and Kabir, S.: A review on the human health impact of airborne particulate matter, Environ. Int., 74, 136–143, https://doi.org/10.1016/j.envint.2014.10.005, 2015.
Kirchstetter, T. W. and Thatcher, T. L.: Contribution of organic carbon to wood smoke particulate matter absorption of solar radiation, Atmos. Chem. Phys., 12, 6067–6072, https://doi.org/10.5194/acp-12-6067-2012, 2012.
Kleinman, L. I., Sedlacek III, A. J., Adachi, K., Buseck, P. R., Collier, S., Dubey, M. K., Hodshire, A. L., Lewis, E., Onasch, T. B., Pierce, J. R., Shilling, J., Springston, S. R., Wang, J., Zhang, Q., Zhou, S., and Yokelson, R. J.: Rapid evolution of aerosol particles and their optical properties downwind of wildfires in the western US, Atmos. Chem. Phys., 20, 13319–13341, https://doi.org/10.5194/acp-20-13319-2020, 2020.
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.
Liu, D., Li, S., Hu, D., Kong, S., Cheng, Y., Wu, Y., Ding, S., Hu, K., Zheng, S., Yan, Q., Zheng, H., Zhao, D., Tian, P., Ye, J., Huang, M., and Ding, D.: Evolution of Aerosol Optical Properties from Wood Smoke in Real Atmosphere Influenced by Burning Phase and Solar Radiation, Environ. Sci. Technol., 55, 5677–5688, https://doi.org/10.1021/acs.est.0c07569, 2021.
Li, X., Tao, Y., Zhu, L., Ma, S., Luo, S., Zhao, Z., Sun, N., Ge, X., and Ye, Z.: Optical and chemical properties and oxidative potential of aqueous-phase products from OH and 3C∗-initiated photooxidation of eugenol, Atmos. Chem. Phys., 22, 7793–7814, https://doi.org/10.5194/acp-22-7793-2022, 2022.
Li, Y. J., Huang, D. D., Cheung, H. Y., Lee, A. K. Y., and Chan, C. K.: Aqueous-phase photochemical oxidation and direct photolysis of vanillin – a model compound of methoxy phenols from biomass burning, Atmos. Chem. Phys., 14, 2871–2885, https://doi.org/10.5194/acp-14-2871-2014, 2014.
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., 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.
McFall, A. S., Johnson, A. W., and Anastasio, C.: Air-Water Partitioning of Biomass-Burning Phenols and the Effects of Temperature and Salinity, Environ. Sci. Technol., 54, 3823–3830, https://doi.org/10.1021/acs.est.9b06443, 2020.
Misovich, M. V., Hettiyadura, A. P. S., Jiang, W., Zhang, Q., and Laskin, A.: Molecular-Level Study of the Photo-Oxidation of Aqueous-Phase Guaiacyl Acetone in the Presence of 3C*: Formation of Brown Carbon Products, ACS Earth Space Chem., https://doi.org/10.1021/acsearthspacechem.1c00103, 2021.
O'Dell, K., Bilsback, K., Ford, B., Martenies, S. E., Magzamen, S., Fischer, E. V., and Pierce, J. R.: Estimated mortality and morbidity attributable to smoke plumes in the united states: not just a western US problem, GeoHealth, 5, e2021GH000457, https://doi.org/10.1029/2021GH000457, 2021.
Ortega, A. M., Day, D. A., Cubison, M. J., Brune, W. H., Bon, D., de Gouw, J. A., and Jimenez, J. L.: Secondary organic aerosol formation and primary organic aerosol oxidation from biomass-burning smoke in a flow reactor during FLAME-3, Atmos. Chem. Phys., 13, 11551–11571, https://doi.org/10.5194/acp-13-11551-2013, 2013.
Palm, B. B., Peng, Q., Fredrickson, C. D., Lee, B. H., Garofalo, L. A., Pothier, M. A., Kreidenweis, S. M., Farmer, D. K., Pokhrel, R. P., Shen, Y., Murphy, S. M., Permar, W., Hu, L., Campos, T. L., Hall, S. R., Ullmann, K., Zhang, X., Flocke, F., Fischer, E. V., and Thornton, J. A.: Quantification of organic aerosol and brown carbon evolution in fresh wildfire plumes, P. Natl. Acad. Sci. USA, 117, 29469–29477, https://doi.org/10.1073/pnas.2012218117, 2020.
Powelson, M. H., Espelien, B. M., Hawkins, L. N., Galloway, M. M., and De Haan, D. O.: Brown carbon formation by aqueous-phase carbonyl compound reactions with amines and ammonium sulfate, Environ. Sci. Technol., 48, 985–993, https://doi.org/10.1021/es4038325, 2014.
Reid, J. S., Koppmann, R., Eck, T. F., and Eleuterio, D. P.: A review of biomass burning emissions part II: intensive physical properties of biomass burning particles, Atmos. Chem. Phys., 5, 799–825, https://doi.org/10.5194/acp-5-799-2005, 2005.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking organic aerosols: semivolatile emissions and photochemical aging., Science, 315, 1259–1262, https://doi.org/10.1126/science.1133061, 2007.
Saleh, R.: From Measurements to Models: Toward Accurate Representation of Brown Carbon in Climate Calculations, Curr. Pollut. Reports, 6, 90–104, https://doi.org/10.1007/s40726-020-00139-3, 2020.
Saleh, R., Hennigan, C. J., McMeeking, G. R., Chuang, W. K., Robinson, E. S., Coe, H., Donahue, N. M., and Robinson, A. L.: Absorptivity of brown carbon in fresh and photo-chemically aged biomass-burning emissions, Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, 2013.
Schauer, J. J., Kleeman, M. J., Cass, G. R., and Simoneit, B. R.: Measurement of emissions from air pollution sources. 3. C1-C29 organic compounds from fireplace combustion of wood, Environ. Sci. Technol., 35, 1716–1728, https://doi.org/10.1021/es001331e, 2001.
Schnitzler, E. G., Gerrebos, N. G. A., Carter, T. S., Huang, Y., Heald, C. L., Bertram, A. K., and Abbatt, J. P. D.: Rate of atmospheric brown carbon whitening governed by environmental conditions, P. Natl. Acad. Sci. USA, 119, e2205610119, https://doi.org/10.1073/pnas.2205610119, 2022.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B., Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T., Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J., Smith, J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R., Zaveri, R. A., Zelenyuk, A., and Zhang, Q.: Recent advances in understanding secondary organic aerosol: Implications for global climate forcing, Rev. Geophys., 55, 509–559, https://doi.org/10.1002/2016RG000540, 2017.
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.
Sun, Y. L., Zhang, Q., Anastasio, C., and Sun, J.: Insights into secondary organic aerosol formed via aqueous-phase reactions of phenolic compounds based on high resolution mass spectrometry, Atmos. Chem. Phys., 10, 4809–4822, https://doi.org/10.5194/acp-10-4809-2010, 2010.
Volkamer, R., Jimenez, J. L., San Martini, F., Dzepina, K., Zhang, Q., Salcedo, D., Molina, L. T., Worsnop, D. R., and Molina, M. J.: Secondary organic aerosol formation from anthropogenic air pollution: Rapid and higher than expected, Geophys. Res. Lett., 33, L17811, https://doi.org/10.1029/2006GL026899, 2006.
Wang, Y., Huang, W., Tian, L., Wang, Y., Li, F., Huang, D. D., Zhang, R., Go Mabato, B. R., Huang, R.-J., Chen, Q., Ge, X., Du, L., Ma, Y. G., Gen, M., Hoi, K. I., Mok, K. M., Yu, J. Z., Chan, C. K., Li, X., and Li, Y. J.: Decay Kinetics and Absorption Changes of Methoxyphenols and Nitrophenols during Nitrate-Mediated Aqueous Photochemical Oxidation at 254 and 313 nm, ACS Earth Space Chem., 6, 1115–1125, https://doi.org/10.1021/acsearthspacechem.2c00021, 2022.
Yee, L. D., Kautzman, K. E., Loza, C. L., Schilling, K. A., Coggon, M. M., Chhabra, P. S., Chan, M. N., Chan, A. W. H., Hersey, S. P., Crounse, J. D., Wennberg, P. O., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from biomass burning intermediates: phenol and methoxyphenols, Atmos. Chem. Phys., 13, 8019–8043, https://doi.org/10.5194/acp-13-8019-2013, 2013.
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, A., Wang, Y., Zhang, Y., Weber, R. J., Song, Y., Ke, Z., and Zou, Y.: Modeling the global radiative effect of brown carbon: a potentially larger heating source in the tropical free troposphere than black carbon, Atmos. Chem. Phys., 20, 1901–1920, https://doi.org/10.5194/acp-20-1901-2020, 2020.
Zhao, R., Lee, A. K. Y., Huang, L., Li, X., Yang, F., and Abbatt, J. P. D.: Photochemical processing of aqueous atmospheric brown carbon, Atmos. Chem. Phys., 15, 6087–6100, https://doi.org/10.5194/acp-15-6087-2015, 2015.
Zhong, M. and Jang, M.: Dynamic light absorption of biomass-burning organic carbon photochemically aged under natural sunlight, Atmos. Chem. Phys., 14, 1517–1525, https://doi.org/10.5194/acp-14-1517-2014, 2014.
Zhou, X., Josey, K., Kamareddine, L., Caine, M. C., Liu, T., Mickley, L. J., Cooper, M., and Dominici, F.: Excess of COVID-19 cases and deaths due to fine particulate matter exposure during the 2020 wildfires in the United States, Sci. Adv., 7, eabi8789, https://doi.org/10.1126/sciadv.abi8789, 2021.
Short summary
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.
We measured changes in light absorption during the aqueous oxidation of six phenols with...
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