Articles | Volume 26, issue 8
https://doi.org/10.5194/acp-26-5713-2026
© Author(s) 2026. 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-26-5713-2026
© Author(s) 2026. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Apr 2026
Research article |
| 27 Apr 2026
| 27 Apr 2026
Rapid secondary organic aerosol formation at the air–water interface from methoxyphenols in wildfire emissions: UVA-driven S(IV) photooxidation to organosulfates
Baohua Cai
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Yuanlong Huang
Ningbo Institute of Digital Twin, Eastern Institute of Technology, Ningbo 315201, China
Wenqing Jiang
Department of Environmental Toxicology, University of California, Davis, California 95616, United States
Yanchen Li
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Yali Li
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Jinghao Zhai
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Yaling Zeng
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Jianhuai Ye
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Huizhong Shen
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Chen Wang
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Tzung-May Fu
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
Department of Environmental Toxicology, University of California, Davis, California 95616, United States
Shenzhen Key Laboratory of Precision Measurement and Early Warning Technology for Urban Environmental Health Risks, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, China
Guangdong Provincial Field Observation and Research Station for Coastal Atmosphere and Climate of the Greater Bay Area, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China
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Atmos. Meas. Tech., 17, 423–439, https://doi.org/10.5194/amt-17-423-2024, https://doi.org/10.5194/amt-17-423-2024, 2024
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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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Atmos. Chem. Phys., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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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.
Lei Shu, Lei Zhu, Juseon Bak, Peter Zoogman, Han Han, Song Liu, Xicheng Li, Shuai Sun, Juan Li, Yuyang Chen, Dongchuan Pu, Xiaoxing Zuo, Weitao Fu, Xin Yang, and Tzung-May Fu
Atmos. Chem. Phys., 23, 3731–3748, https://doi.org/10.5194/acp-23-3731-2023, https://doi.org/10.5194/acp-23-3731-2023, 2023
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We quantify the benefit of multisource observations (GEMS, LEO satellite, and surface) on ozone simulations in Asia. Data assimilation improves the monitoring of exceedance, spatial pattern, and diurnal variation of surface ozone, with the regional mean bias reduced from −2.1 to −0.2 ppbv. Data assimilation also better represents ozone vertical distributions in the middle to upper troposphere at low latitudes. Our results offer a valuable reference for future ozone simulations.
Nathaniel W. May, Noah Bernays, Ryan Farley, Qi Zhang, and Daniel A. Jaffe
Atmos. Chem. Phys., 23, 2747–2764, https://doi.org/10.5194/acp-23-2747-2023, https://doi.org/10.5194/acp-23-2747-2023, 2023
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In summer 2019 at Mt. Bachelor Observatory, we observed smoke from wildfires with transport times ranging from less than a day up to 2 weeks. Aerosol absorption of multi-day transported smoke was dominated by black carbon, while smoke with shorter transport times had greater brown carbon absorption. Notably, Siberian smoke exhibited aerosol scattering and physical properties indicative of contributions from larger particles than typically observed in smoke.
Christopher R. Niedek, Fan Mei, Maria A. Zawadowicz, Zihua Zhu, Beat Schmid, and Qi Zhang
Atmos. Meas. Tech., 16, 955–968, https://doi.org/10.5194/amt-16-955-2023, https://doi.org/10.5194/amt-16-955-2023, 2023
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This novel micronebulization aerosol mass spectrometry (MS) technique requires a low sample volume (10 μL) and can quantify nanogram levels of organic and inorganic particulate matter (PM) components when used with 34SO4. This technique was successfully applied to PM samples collected from uncrewed atmospheric measurement platforms and provided chemical information that agrees well with real-time data from a co-located aerosol chemical speciation monitor and offline data from secondary ion MS.
Amir H. Souri, Matthew S. Johnson, Glenn M. Wolfe, James H. Crawford, Alan Fried, Armin Wisthaler, William H. Brune, Donald R. Blake, Andrew J. Weinheimer, Tijl Verhoelst, Steven Compernolle, Gaia Pinardi, Corinne Vigouroux, Bavo Langerock, Sungyeon Choi, Lok Lamsal, Lei Zhu, Shuai Sun, Ronald C. Cohen, Kyung-Eun Min, Changmin Cho, Sajeev Philip, Xiong Liu, and Kelly Chance
Atmos. Chem. Phys., 23, 1963–1986, https://doi.org/10.5194/acp-23-1963-2023, https://doi.org/10.5194/acp-23-1963-2023, 2023
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We have rigorously characterized different sources of error in satellite-based HCHO / NO2 tropospheric columns, a widely used metric for diagnosing near-surface ozone sensitivity. Specifically, the errors were categorized/quantified into (i) an inherent chemistry error, (ii) the decoupled relationship between columns and the near-surface concentration, (iii) the spatial representativeness error of ground satellite pixels, and (iv) the satellite retrieval errors.
Qian Zhang, Yujie Zhang, Zhichun Wu, Bin Zhang, Yaling Zeng, Jian Sun, Hongmei Xu, Qiyuan Wang, Zhihua Li, Junji Cao, and Zhenxing Shen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-801, https://doi.org/10.5194/acp-2022-801, 2022
Revised manuscript not accepted
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We identified the brown carbon (BrC) molecules and their absorbing abilities on a molecular level from animal dung fuel combustion over the Tibetan Plateau region in China. The ultra-high performance liquid chromatography quadrupole time-of-flight mass spectrometer coupled with the partial least squares regression were precisely applied to characterize the molecular absorptions, key molecular markers, and radiative effects of BrC from household combustion scenarios at the high-altitude area.
Xun Li, Momei Qin, Lin Li, Kangjia Gong, Huizhong Shen, Jingyi Li, and Jianlin Hu
Atmos. Chem. Phys., 22, 14799–14811, https://doi.org/10.5194/acp-22-14799-2022, https://doi.org/10.5194/acp-22-14799-2022, 2022
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Photochemical indicators have been widely used to predict O3–NOx–VOC sensitivity with given thresholds. Here we assessed the effectiveness of four indicators with a case study in the Yangtze River Delta, China. The overall performance was good, while some indicators showed inconsistencies with the O3 isopleths. The methodology used to determine the thresholds may produce uncertainties. These results would improve our understanding of the use of photochemical indicators in policy implications.
Xinghua Zhang, Wenhui Zhao, Lixiang Zhai, Miao Zhong, Jinsen Shi, Junying Sun, Yanmei Liu, Conghui Xie, Yulong Tan, Kemei Li, Xinlei Ge, Qi Zhang, Shichang Kang, and Jianzhong Xu
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-211, https://doi.org/10.5194/essd-2022-211, 2022
Manuscript not accepted for further review
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A comprehensive aerosol observation project was carried out in the Tibetan Plateau (TP) in recent years to investigate the properties and sources of atmospheric aerosols as well as their regional differences by performing multiple short-term intensive field observations. The real-time online high-time-resolution (hourly) data of aerosol properties in the different TP region are integrated in a new dataset and can provide supporting for related studies in in the TP.
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.
Xiaotian Xu, Xu Feng, Haipeng Lin, Peng Zhang, Shaojian Huang, Zhengcheng Song, Yiming Peng, Tzung-May Fu, and Yanxu Zhang
Geosci. Model Dev., 15, 3845–3859, https://doi.org/10.5194/gmd-15-3845-2022, https://doi.org/10.5194/gmd-15-3845-2022, 2022
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Mercury is one of the most toxic pollutants in the environment, and wet deposition is a major process for atmospheric mercury to enter, causing ecological and human health risks. High-mercury wet deposition in the southeastern US has been a problem for many years. Here we employed a newly developed high-resolution WRF-GC model with the capability to simulate mercury to study this problem. We conclude that deep convection caused enhanced mercury wet deposition in the southeastern US.
Sophia M. Charan, Yuanlong Huang, Reina S. Buenconsejo, Qi Li, David R. Cocker III, and John H. Seinfeld
Atmos. Chem. Phys., 22, 917–928, https://doi.org/10.5194/acp-22-917-2022, https://doi.org/10.5194/acp-22-917-2022, 2022
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In this study, we investigate the secondary organic aerosol formation potential of decamethylcyclopentasiloxane (D5), which is used as a tracer for volatile chemical products and measured in high concentrations both outdoors and indoors. By performing experiments in different types of reactors, we find that D5’s aerosol formation is highly dependent on OH, and, at low OH concentrations or exposures, D5 forms little aerosol. We also reconcile results from other studies.
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 %.
Fan Mei, Jian Wang, Shan Zhou, Qi Zhang, Sonya Collier, and Jianzhong Xu
Atmos. Chem. Phys., 21, 13019–13029, https://doi.org/10.5194/acp-21-13019-2021, https://doi.org/10.5194/acp-21-13019-2021, 2021
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This work focuses on understanding aerosol's ability to act as cloud condensation nuclei (CCN) and its variations with organic oxidation level and volatility using measurements at a rural site. Aerosol properties were examined from four air mass sources. The results help improve the accurate representation of aerosol from different ambient aerosol emissions, transformation pathways, and atmospheric processes in a climate model.
Weimeng Kong, Stavros Amanatidis, Huajun Mai, Changhyuk Kim, Benjamin C. Schulze, Yuanlong Huang, Gregory S. Lewis, Susanne V. Hering, John H. Seinfeld, and Richard C. Flagan
Atmos. Meas. Tech., 14, 5429–5445, https://doi.org/10.5194/amt-14-5429-2021, https://doi.org/10.5194/amt-14-5429-2021, 2021
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We present the design, modeling, and experimental characterization of the nano-scanning electrical mobility spectrometer (nSEMS), a recently developed instrument that probes particle physical properties in the 1.5–25 nm range. The nSEMS has proven to be extremely powerful in examining atmospheric nucleation and the subsequent growth of nanoparticles in the CERN CLOUD experiment, which provides a valuable asset to study atmospheric nanoparticles and to evaluate their impact on climate.
Xu Feng, Haipeng Lin, Tzung-May Fu, Melissa P. Sulprizio, Jiawei Zhuang, Daniel J. Jacob, Heng Tian, Yaping Ma, Lijuan Zhang, Xiaolin Wang, Qi Chen, and Zhiwei Han
Geosci. Model Dev., 14, 3741–3768, https://doi.org/10.5194/gmd-14-3741-2021, https://doi.org/10.5194/gmd-14-3741-2021, 2021
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WRF-GC is an online coupling of the WRF meteorological model and GEOS-Chem chemical transport model for regional atmospheric chemistry and air quality modeling. In WRF-GC v2.0, we implemented the aerosol–radiation interactions and aerosol–cloud interactions, as well as the capability to nest multiple domains for high-resolution simulations based on the modular framework of WRF-GC v1.0. This allows the GEOS-Chem users to investigate the meteorology–atmospheric chemistry interactions.
Stavros Amanatidis, Yuanlong Huang, Buddhi Pushpawela, Benjamin C. Schulze, Christopher M. Kenseth, Ryan X. Ward, John H. Seinfeld, Susanne V. Hering, and Richard C. Flagan
Atmos. Meas. Tech., 14, 4507–4516, https://doi.org/10.5194/amt-14-4507-2021, https://doi.org/10.5194/amt-14-4507-2021, 2021
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We assess the performance of a highly portable mobility analyzer, the Spider DMA, in measuring ambient aerosol particle size distributions, with specific attention to its moderate sizing resolution (R=3). Long-term field testing showed excellent correlation with a conventional mobility analyzer (R=10) over the 17–500 nm range, suggesting that moderate resolution may be sufficient to obtain key properties of ambient size distributions, enabling smaller instruments and better counting statistics.
Bingqing Zhang, Huizhong Shen, Pengfei Liu, Hongyu Guo, Yongtao Hu, Yilin Chen, Shaodong Xie, Ziyan Xi, T. Nash Skipper, and Armistead G. Russell
Atmos. Chem. Phys., 21, 8341–8356, https://doi.org/10.5194/acp-21-8341-2021, https://doi.org/10.5194/acp-21-8341-2021, 2021
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Extended ground-level measurements are coupled with model simulations to comprehensively compare the aerosol acidity in China and the United States. Aerosols in China are significantly less acidic than those in the United States, with pH values 1–2 units higher. Higher aerosol mass concentrations and the abundance of ammonia and ammonium in China, compared to the United States, are leading causes of the pH difference between these two countries.
Cited articles
Abbatt, J. P. D., Benz, S., Cziczo, D. J., Kanji, Z., Lohmann, U., and Möhler, O.: Solid Ammonium Sulfate Aerosols as Ice Nuclei: A Pathway for Cirrus Cloud Formation, Science, 313, 1770–1773, https://doi.org/10.1126/science.1129726, 2006.
Bai, C.-B., Wang, N.-X., Lan, X.-W., Wang, Y.-J., Xing, Y., Wen, J.-L., Gao, X.-W., and Zhang, W.: An Unexpected Controlled New Oxidant:
Brandt, C. and van Eldik, R.: Transition Metal-Catalyzed Oxidation of Sulfur(IV) Oxides. Atmospheric-Relevant Processes and Mechanisms, Chem. Rev., 95, 119–190, https://doi.org/10.1021/cr00033a006, 1995.
Canagaratna, M. R., Jayne, J. T., Jimenez, J. L., Allan, J. D., Alfarra, M. R., Zhang, Q., Onasch, T. B., Drewnick, F., Coe, H., Middlebrook, A., Delia, A., Williams, L. R., Trimborn, A. M., Northway, M. J., DeCarlo, P. F., Kolb, C. E., Davidovits, P., and Worsnop, D. R.: Chemical and microphysical characterization of ambient aerosols with the aerodyne aerosol mass spectrometer, Mass Spectrom. Rev., 26, 185–222, https://doi.org/10.1002/mas.20115, 2007.
Cao, Y., Qiu, W., Li, J., Jiang, J., and Pang, S.: Review on UV/sulfite process for water and wastewater treatments in the presence or absence of O2, Sci. Total Environ., 765, 142762, https://doi.org/10.1016/j.scitotenv.2020.142762, 2021.
Cao, Y., Liu, J., Ma, Q., Zhang, C., Zhang, P., Chen, T., Wang, Y., Chu, B., Zhang, X., Francisco, J. S., and He, H.: Photoactivation of Chlorine and Its Catalytic Role in the Formation of Sulfate Aerosols, J. Am. Chem. Soc., 146, 1467–1475, https://doi.org/10.1021/jacs.3c10840, 2024a.
Cao, Y., Wang, Z., Liu, J., Ma, Q., Li, S., Liu, J., Li, H., Zhang, P., Chen, T., Wang, Y., Chu, B., Zhang, X., Saiz-Lopez, A., Francisco, J. S., and He, H.: Spontaneous molecular bromine production in sea salt aerosols, Angew. Chem. Int. Edit., 63, e202409779, https://doi.org/10.1002/anie.202409779, 2024b.
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, e1601530, https://doi.org/10.1126/sciadv.1601530, 2016.
Coddens, E. M., Huang, L., Wong, C., and Grassian, V. H.: Influence of Glyoxal on the Catalytic Oxidation of S(IV) in Acidic Aqueous Media, ACS Earth Space Chem., 3, 142–149, https://doi.org/10.1021/acsearthspacechem.8b00168, 2018.
Cope, J. D., Bates, K. H., Tran, L. N., Abellar, K. A., and Nguyen, T. B.: Sulfur radical formation from the tropospheric irradiation of aqueous sulfate aerosols, P. Natl. Acad. Sci. USA, 119, e2202857119, https://doi.org/10.1073/pnas.2202857119, 2022.
Darer, A. I., Cole-Filipiak, N. C., O'Connor, A. E., and Elrod, M. J.: Formation and stability of atmospherically relevant isoprene-derived organosulfates and organonitrates, Environ. Sci. Technol., 45, 1895–1902, https://doi.org/10.1021/es103797z, 2011.
DeCarlo, P. F., Kimmel, J. R., Trimborn, A., Northway, M. J., Jayne, J. T., Aiken, A. C., Gonin, M., Fuhrer, K., Horvath, T., Docherty, K. S., Worsnop, D. R., and Jimenez, J. L.: Field-Deployable, High-Resolution, Time-of-Flight Aerosol Mass Spectrometer, Anal. Chem., 78, 8281–8289, https://doi.org/10.1029/2001jd001213, 2006.
Duporté, G., Flaud, P. M., Kammer, J., Geneste, E., Augagneur, S., Pangui, E., Lamkaddam, H., Gratien, A., Doussin, J. F., Budzinski, H., Villenave, E., and Perraudin, E.: Experimental Study of the Formation of Organosulfates from α-Pinene Oxidation. 2. Time Evolution and Effect of Particle Acidity, J. Phys. Chem. A, 124, 409–421, https://doi.org/10.1021/acs.jpca.9b07156, 2020.
Frisch, M., Trucks, G., Schlegel, H., Scuseria, G., Robb, M., Cheeseman, J., Scalmani, G., Barone, V., Petersson, G., and Nakatsuji, H.: Gaussian 16, Revision A.03, Gaussian [code], https://gaussian.com/gaussian16/ (last access: 23 April 2026), 2016.
Gao, Y., Zhang, M., Guo, J., and Xu, L.: Impact of the oxidation of SO2 by NO2 on regional sulfate concentrations over the North China Plain, Atmos. Pollut. Res., 13, 101337, https://doi.org/10.1016/j.apr.2022.101337, 2022.
George, C., Ammann, M., D'Anna, B., Donaldson, D. J., and Nizkorodov, S. A.: Heterogeneous photochemistry in the atmosphere, Chem. Rev., 115, 4218–4258, https://doi.org/10.1021/cr500648z, 2015.
Gong, C., Yuan, X., Xing, D., Zhang, D., Martins-Costa, M. T. C., Anglada, J. M., Ruiz-Lopez, M. F., Francisco, J. S., and Zhang, X.: Fast Sulfate Formation Initiated by the Spin-Forbidden Excitation of SO2 at the Air-Water Interface, J. Am. Chem. Soc., 144, 22302–22308, https://doi.org/10.1021/jacs.2c10830, 2022.
Guo, Y., Riplinger, C., Becker, U., Liakos, D. G., Minenkov, Y., Cavallo, L., and Neese, F.: Communication: An improved linear scaling perturbative triples correction for the domain based local pair-natural orbital based singles and doubles coupled cluster method [DLPNO-CCSD(T)], J. Chem. Phys., 148, 011101, https://doi.org/10.1063/1.5011798, 2018.
Harris, E., Sinha, B., van Pinxteren, D., Tilgner, A., Fomba, K. W., Schneider, J., Roth, A., Gnauk, T., Fahlbusch, B., Mertes, S., Lee, T., Collett, J., Foley, S., Borrmann, S., Hoppe, P., and Herrmann, H.: Enhanced Role of Transition Metal Ion Catalysis During In-Cloud Oxidation of SO2, Science, 340, 727–730, https://doi.org/10.1126/science.1230911, 2013.
He, Y., Zhao, B., Wang, S., Valorso, R., Chang, X., Yin, D., Feng, B., Camredon, M., Aumont, B., Dearden, A., Jathar, S. H., Shrivastava, M., Jiang, Z., Cappa, C. D., Yee, L. D., Seinfeld, J. H., Hao, J., and Donahue, N. M.: Formation of secondary organic aerosol from wildfire emissions enhanced by long-time ageing, Nat. Geosci., 17, 124–129, https://doi.org/10.1038/s41561-023-01355-4, 2024.
Herrmann, H., Schaefer, T., Tilgner, A., Styler, S. A., Weller, C., Teich, M., and Otto, T.: Tropospheric aqueous-phase chemistry: kinetics, mechanisms, and its coupling to a changing gas phase, Chem. Rev., 115, 4259–4334, https://doi.org/10.1021/cr500447k, 2015.
Hess, B., Kutzner, C., van der Spoel, D., and Lindahl, E.: GROMACS 4: Algorithms for Highly Efficient, Load-Balanced, and Scalable Molecular Simulation, J. Chem. Theory Comput., 4, 435–447, https://doi.org/10.1021/ct700301q, 2008.
Hoffmann, M. R.: On the kinetics and mechanism of oxidation of aquated sulfur dioxide by ozone, Atmos. Environ., 20, 1145–1154, https://doi.org/10.1016/0004-6981(86)90147-2, 1986.
Huang, Y., Barraza, K. M., Kenseth, C. M., Zhao, R., Wang, C., Beauchamp, J. L., and Seinfeld, J. H.: Probing the OH Oxidation of Pinonic Acid at the Air–Water Interface Using Field-Induced Droplet Ionization Mass Spectrometry (FIDI-MS), J. Phys. Chem. A, 122, 6445–6456, https://doi.org/10.1021/acs.jpca.8b05353, 2018.
Hughes, D. D., Christiansen, M. B., Milani, A., Vermeuel, M. P., Novak, G. A., Alwe, H. D., Dickens, A. F., Pierce, R. B., Millet, D. B., Bertram, T. H., Stanier, C. O., and Stone, E. A.: PM2.5 chemistry, organosulfates, and secondary organic aerosol during the 2017 Lake Michigan Ozone Study, Atmos. Environ., 244, 117939, https://doi.org/10.1016/j.atmosenv.2020.117939, 2021.
Humphrey, W., Dalke, A., and Schulten, K.: VMD: Visual molecular dynamics, J. Mol. Graphics, 14, 33–38, https://doi.org/10.1016/0263-7855(96)00018-5, 1996.
Iinuma, Y., Müller, C., Berndt, T., Böge, O., Claeys, M., and Herrmann, H.: Evidence for the Existence of Organosulfates from β-Pinene Ozonolysis in Ambient Secondary Organic Aerosol, Environ. Sci. Technol., 41, 6678–6683, https://doi.org/10.1021/es070938t, 2007.
Khan, F., Chen, Y., Hartwell, H. J., Yan, J., Lin, Y.-H., Freedman, A., Zhang, Z., Zhang, Y., Lambe, A. T., Turpin, B. J., Gold, A., Ault, A. P., Szmigielski, R., Fry, R. C., and Surratt, J. D.: Heterogeneous Oxidation Products of Fine Particulate Isoprene Epoxydiol-Derived Methyltetrol Sulfates Increase Oxidative Stress and Inflammatory Gene Responses in Human Lung Cells, Chem. Res. Toxicol., 36, 1814–1825, https://doi.org/10.1021/acs.chemrestox.3c00278, 2023.
Lan, Y., Wheeler, S. E., and Houk, K. N.: Extraordinary Difference in Reactivity of Ozone (OOO) and Sulfur Dioxide (OSO): A Theoretical Study, J. Chem. Theory Comput., 7, 2104–2111, https://doi.org/10.1021/ct200293w, 2011.
Li, F., Zhou, S., Du, L., Zhao, J., Hang, J., and Wang, X.: Aqueous-phase chemistry of atmospheric phenolic compounds: A critical review of laboratory studies, Sci. Total Environ., 856, 158895, https://doi.org/10.1016/j.scitotenv.2022.158895, 2023a.
Li, M., Duan, P., Huo, Y., Jiang, J., Zhou, Y., Ma, Y., Jin, Z., Mei, Q., Xie, J., and He, M.: The multiple roles of phenols in the degradation of aniline contaminants by sulfate radicals: A combined study of DFT calculations and experiments, J. Hazard. Mater., 443, 130216, https://doi.org/10.1016/j.jhazmat.2022.130216, 2023b.
Liang, C. and Su, H.-W.: Identification of Sulfate and Hydroxyl Radicals in Thermally Activated Persulfate, Ind. Eng. Chem. Res., 48, 5558–5562, https://doi.org/10.1021/ie9002848, 2009.
Liu, C., Chen, D., and Chen, X.: Atmospheric Reactivity of Methoxyphenols: A Review, Environ. Sci. Technol., 56, 2897–2916, https://doi.org/10.1021/acs.est.1c06535, 2022.
Liu, T. and Abbatt, J. P. D.: Oxidation of sulfur dioxide by nitrogen dioxide accelerated at the interface of deliquesced aerosol particles, Nat. Chem., 13, 1173–1177, https://doi.org/10.1038/s41557-021-00777-0, 2021.
Liu, T., Clegg, S. L., and Abbatt, J. P. D.: Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles, P. Natl. Acad. Sci. USA, 117, 1354–1359, https://doi.org/10.1073/pnas.1916401117, 2020.
Liu, Y., Li, X., Ge, Q., Fang, X., Wang, T., You, W., Wang, W., Xie, L., Li, K., Gong, K., Yang, L., Wang, R., Wang, J., Wang, L., Ma, M., Huang, T., Fu, H., Chen, J., Dong, X., and Zhang, L.: Carbonate radical ion as a key driver of rapid atmospheric sulfate formation, npj Clim. Atmos. Sci., 8, 45, https://doi.org/10.1038/s41612-025-00905-4, 2025.
Lu, T. and Chen, F.: Multiwfn: A multifunctional wavefunction analyzer, J. Comput. Chem., 33, 580–592, https://doi.org/10.1002/jcc.22885, 2012.
Lu, T. and Chen, Q.: Shermo: A general code for calculating molecular thermochemistry properties, Comput. Theor. Chem., 1200, 113249, https://doi.org/10.1016/j.comptc.2021.113249, 2021.
Marenich, A. V., Cramer, C. J., and Truhlar, D. G.: Performance of SM6, SM8, and SMD on the SAMPL1 Test Set for the Prediction of Small-Molecule Solvation Free Energies, J. Phys. Chem. B, 113, 4538–4543, https://doi.org/10.1021/jp809094y, 2009.
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.
Neese, F.: Software update: the ORCA program system – Version 6.0, WIRes Comput. Mol. Sci., 15, e70019, https://doi.org/10.1002/wcms.70019, 2025.
Noga, J. and Bartlett, R. J.: The full CCSDT model for molecular electronic structure, J. Chem. Phys., 86, 7041–7050, https://doi.org/10.1063/1.452353, 1987.
Pan, Y., Zhang, F., Tan, W., and Feng, X.: New insight into wastewater treatment by activation of sulfite with humic acid under visible light irradiation, Water Res., 258, 121773, https://doi.org/10.1016/j.watres.2024.121773, 2024.
Passananti, M., Kong, L., Shang, J., Dupart, Y., Perrier, S., Chen, J., Donaldson, D. J., and George, C.: Organosulfate Formationthrough the Heterogeneous Reactionof Sulfur Dioxide with Unsaturated Fatty Acids and Long-Chain Alkenes, Angew. Chem. Int. Edit., 55, 10336–10339, https://doi.org/10.1002/anie.201605266, 2016.
Peng, C., Razafindrambinina, P. N., Malek, K. A., Chen, L., Wang, W., Huang, R.-J., Zhang, Y., Ding, X., Ge, M., Wang, X., Asa-Awuku, A. A., and Tang, M.: Interactions of organosulfates with water vapor under sub- and supersaturated conditions, Atmos. Chem. Phys., 21, 7135–7148, https://doi.org/10.5194/acp-21-7135-2021, 2021.
Ren, H., Sedlak, J. A., and Elrod, M. J.: General Mechanism for Sulfate Radical Addition to Olefinic Volatile Organic Compounds in Secondary Organic Aerosol, Environ. Sci. Technol., 55, 1456–1465, https://doi.org/10.1021/acs.est.0c05256, 2021.
Riva, M., Tomaz, S., Cui, T., Lin, Y. H., Perraudin, E., Gold, A., Stone, E. A., Villenave, E., and Surratt, J. D.: Evidence for an unrecognized secondary anthropogenic source of organosulfates and sulfonates: gas-phase oxidation of polycyclic aromatic hydrocarbons in the presence of sulfate aerosol, Environ. Sci. Technol., 49, 6654–6664, https://doi.org/10.1021/acs.est.5b00836, 2015.
Riva, M., Chen, Y., Zhang, Y., Lei, Z., Olson, N. E., Boyer, H. C., Narayan, S., Yee, L. D., Green, H. S., Cui, T., Zhang, Z., Baumann, K., Fort, M., Edgerton, E., Budisulistiorini, S. H., Rose, C. A., Ribeiro, I. O., Oliveira, R. L., Dos Santos, E. O., Machado, C. M. D., Szopa, S., Zhao, Y., Alves, E. G., de Sa, S. S., Hu, W., Knipping, E. M., Shaw, S. L., Duvoisin Junior, S., de Souza, R. A. F., Palm, B. B., Jimenez, J. L., Glasius, M., Goldstein, A. H., Pye, H. O. T., Gold, A., Turpin, B. J., Vizuete, W., Martin, S. T., Thornton, J. A., Dutcher, C. S., Ault, A. P., and Surratt, J. D.: Increasing Isoprene Epoxydiol-to-Inorganic Sulfate Aerosol Ratio Results in Extensive Conversion of Inorganic Sulfate to Organosulfur Forms: Implications for Aerosol Physicochemical Properties, Environ. Sci. Technol., 53, 8682–8694, https://doi.org/10.1021/acs.est.9b01019, 2019.
Romero, F. and Oehme, M.: Organosulfates – A New Component of Humic-Like Substances in Atmospheric Aerosols?, J. Atmos. Chem., 52, 283–294, https://doi.org/10.1007/s10874-005-0594-y, 2005.
Rudziński, K. J., Gmachowski, L., and Kuznietsova, I.: Reactions of isoprene and sulphoxy radical-anions – a possible source of atmospheric organosulphites and organosulphates, Atmos. Chem. Phys., 9, 2129–2140, https://doi.org/10.5194/acp-9-2129-2009, 2009.
Ruiz-Lopez, M. F., Francisco, J. S., Martins-Costa, M. T. C., and Anglada, J. M.: Molecular reactions at aqueous interfaces, Nat. Rev. Chem., 4, 459–475, https://doi.org/10.1038/s41570-020-0203-2, 2020.
Schindelka, J., Iinuma, Y., Hoffmann, D., and Herrmann, H.: Sulfate radical-initiated formation of isoprene-derived organosulfates in atmospheric aerosols, Faraday Discuss., 165, 237–259, https://doi.org/10.1039/c3fd00042g, 2013.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From Air Pollution to Climate Change, in: 3rd Edn., Wiley, ISBN 9781119221166, 2016.
Shakya, K. M. and Peltier, R. E.: Non-sulfate sulfur in fine aerosols across the United States: Insight for organosulfate prevalence, Atmos. Environ., 100, 159–166, https://doi.org/10.1016/j.atmosenv.2014.10.058, 2015.
Surratt, J. D., Gómez-González, Y., Chan, A. W. H., Vermeylen, R., Shahgholi, M., Kleindienst, T. E., Edney, E. O., Offenberg, J. H., Lewandowski, M., Jaoui, M., Maenhaut, W., Claeys, M., Flagan, R. C., and Seinfeld, J. H.: Organosulfate Formation in Biogenic Secondary Organic Aerosol, J. Phys. Chem. A, 112, 8345–8378, https://doi.org/10.1021/jp802310p, 2008.
Teymoor Seydi, S., Abatzoglou, J. T., Jones, M. W., Kolden, C. A., Filippelli, G., Hurteau, M. D., AghaKouchak, A., Luce, C. H., Miao, C., and Sadegh, M.: Increasing global human exposure to wildland fires despite declining burned area, Science, 389, 826–829, https://doi.org/10.1126/science.adu6408, 2025.
Tolocka, M. P.: Contribution of Organosulfur Compounds to Organic Aerosol Mass, Environ. Sci. Technol., 46, 7978–7983, https://doi.org/10.1021/es300651v, 2012.
Tran, L. N., Abellar, K. A., Cope, J. D., and Nguyen, T. B.: Second-Order Kinetic Rate Coefficients for the Aqueous-Phase Sulfate Radical (
Wang, D., Li, Y., Yang, M., and Han, M.: Decomposition of polycyclic aromatic hydrocarbons in atmospheric aqueous droplets through sulfate anion radicals: An experimental and theoretical study, Sci. Total Environ., 393, 64–71, https://doi.org/10.1016/j.scitotenv.2007.11.036, 2008.
Wang, G., Zhang, R., Gomez, M. E., Yang, L., Levy Zamora, M., Hu, M., Lin, Y., Peng, J., Guo, S., Meng, J., Li, J., Cheng, C., Hu, T., Ren, Y., Wang, Y., Gao, J., Cao, J., An, Z., Zhou, W., Li, G., Wang, J., Tian, P., Marrero-Ortiz, W., Secrest, J., Du, Z., Zheng, J., Shang, D., Zeng, L., Shao, M., Wang, W., Huang, Y., Wang, Y., Zhu, Y., Li, Y., Hu, J., Pan, B., Cai, L., Cheng, Y., Ji, Y., Zhang, F., Rosenfeld, D., Liss, P. S., Duce, R. A., Kolb, C. E., and Molina, M. J.: Persistent sulfate formation from London Fog to Chinese haze, P. Natl. Acad. Sci. USA, 113, 13630–13635, https://doi.org/10.1073/pnas.1616540113, 2016.
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, W., Liu, Y., Wang, T., Ge, Q., Li, K., Liu, J., You, W., Wang, L., Xie, L., Fu, H., Chen, J., and Zhang, L.: Significantly Accelerated Photosensitized Formation of Atmospheric Sulfate at the Air–Water Interface of Microdroplets, J. Am. Chem. Soc., 146, 6580–6590, https://doi.org/10.1021/jacs.3c11892, 2024.
Wojnárovits, L. and Takács, E.: Rate constants of sulfate radical anion reactions with organic molecules: A review, Chemosphere, 220, 1014–1032, https://doi.org/10.1016/j.chemosphere.2018.12.156, 2019.
Xie, R., Guo, K., Li, Y., Zhang, Y., Zhong, H., Leung, D. Y. C., and Huang, H.: Harnessing air-water interface to generate interfacial ROS for ultrafast environmental remediation, Nat. Commun., 15, 8860, https://doi.org/10.1038/s41467-024-53289-z, 2024.
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.
Zhang, D., Wang, J., Chen, H., Gong, C., Xing, D., Liu, Z., Gladich, I., Francisco, J. S., and Zhang, X.: Fast Hydroxyl Radical Generation at the Air-Water Interface of Aerosols Mediated by Water-Soluble PM2.5 under Ultraviolet A Radiation, J. Am. Chem. Soc., 145, 6462–6470, https://doi.org/10.1021/jacs.3c00300, 2023.
Zhang, R. and Chan, C. K.: Simultaneous formation of sulfate and nitrate via co-uptake of SO2 and NO2 by aqueous NaCl droplets: combined effect of nitrate photolysis and chlorine chemistry, Atmos. Chem. Phys., 23, 6113–6126, https://doi.org/10.5194/acp-23-6113-2023, 2023.
Zhao, J., Zheng, B., Ciais, P., Chen, Y., Gasser, T., Canadell, J. G., Zhang, L., and Zhang, Q.: Global warming amplifies wildfire health burden and reshapes inequality, Nature, https://doi.org/10.1038/s41586-025-09612-9, 2025.
Zhao, Y. and Truhlar, D. G.: The M06 suite of density functionals for main group thermochemistry, thermochemical kinetics, noncovalent interactions, excited states, and transition elements: two new functionals and systematic testing of four M06-class functionals and 12 other functionals, Theor. Chem. Acc., 120, 215–241, https://doi.org/10.1007/s00214-007-0310-x, 2007.
Zheng, B., Zhang, Q., Zhang, Y., He, K. B., Wang, K., Zheng, G. J., Duan, F. K., Ma, Y. L., and Kimoto, T.: Heterogeneous chemistry: a mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China, Atmos. Chem. Phys., 15, 2031–2049, https://doi.org/10.5194/acp-15-2031-2015, 2015.
Zheng, J., Xu, X., and Truhlar, D. G.: Minimally augmented Karlsruhe basis sets, Theor. Chem. Acc., 128, 295–305, https://doi.org/10.1007/s00214-010-0846-z, 2010.
Zuo, Y., Zhan, J., and Wu, T.: Effects of Monochromatic UV-Visible Light and Sunlight on Fe(III)-Catalyzed Oxidation of Dissolved Sulfur Dioxide, J. Atmos. Chem., 50, 195–210, https://doi.org/10.1007/s10874-005-2813-y, 2005.
Short summary
This study reveals a novel Ultraviolet A-driven, metal-free mechanism for aqueous-phase tetravalent sulfur (S(IV)) oxidation that leads to organosulfates formation, addressing a critical knowledge gap in atmospheric sulfur and organic aerosol chemistry and highlighting a previously overlooked photochemical pathway with broad environmental implications.
This study reveals a novel Ultraviolet A-driven, metal-free mechanism for aqueous-phase...
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