Articles | Volume 19, issue 9
https://doi.org/10.5194/acp-19-6579-2019
© Author(s) 2019. 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-19-6579-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Photooxidants from brown carbon and other chromophores in illuminated particle extracts
Richie Kaur
Department of Land, Air and Water Resources, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Jacqueline R. Labins
Department of Land, Air and Water Resources, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Scarlett S. Helbock
Department of Land, Air and Water Resources, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Wenqing Jiang
Department of Environmental Toxicology, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Keith J. Bein
Center for Health and the Environment, University of California, Davis,
One Shields Avenue, Davis, CA 95616-8627, USA
Department of Environmental Toxicology, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
Department of Land, Air and Water Resources, University of
California, Davis, One Shields Avenue, Davis, CA 95616-8627, USA
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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.
Wenqing Jiang, Lijuan Li, Lu Yu, Hwajin Kim, Yele Sun, and Qi Zhang
EGUsphere, https://doi.org/10.5194/egusphere-2025-3949, https://doi.org/10.5194/egusphere-2025-3949, 2025
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We studied how sunlight changes natural organic matter in fog droplets and the tiny airborne particles formed after the water evaporation. Advanced analyses showed that sunlight makes this material more oxidized, nitrogen-enriched, chemically transformed, and different in light absorption and volatility. These sunlight-driven changes influence the particles’ behavior in the air, affecting air quality, climate, and how long they remain suspended in the atmosphere.
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.
Fan Mei, Qi Zhang, Damao Zhang, Jerome D. Fast, Gourihar Kulkarni, Mikhail S. Pekour, Christopher R. Niedek, Susanne Glienke, Israel Silber, Beat Schmid, Jason M. Tomlinson, Hardeep S. Mehta, Xena Mansoura, Zezhen Cheng, Gregory W. Vandergrift, Nurun Nahar Lata, Swarup China, and Zihua Zhu
Atmos. Chem. Phys., 25, 3425–3444, https://doi.org/10.5194/acp-25-3425-2025, https://doi.org/10.5194/acp-25-3425-2025, 2025
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This study highlights the unique capability of the ArcticShark, an uncrewed aerial system, in measuring vertically resolved atmospheric properties. Data from 32 research flights in 2023 reveal seasonal patterns and correlations with conventional measurements. The consistency and complementarity of in situ and remote sensing methods are highlighted. The study demonstrates the ArcticShark’s versatility in bridging data gaps and improving the understanding of vertical atmospheric structures.
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.
Jianzhong Xu, Xinghua Zhang, Wenhui Zhao, Lixiang Zhai, Miao Zhong, Jinsen Shi, Junying Sun, Yanmei Liu, Conghui Xie, Yulong Tan, Kemei Li, Xinlei Ge, Qi Zhang, and Shichang Kang
Earth Syst. Sci. Data, 16, 1875–1900, https://doi.org/10.5194/essd-16-1875-2024, https://doi.org/10.5194/essd-16-1875-2024, 2024
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A comprehensive aerosol observation project was carried out in the Tibetan Plateau (TP) and its surroundings in recent years to investigate the properties and sources of atmospheric aerosols as well as their regional differences by performing multiple intensive field observations. The release of this dataset can provide basic and systematic data for related research in the atmospheric, cryospheric, and environmental sciences in this unique region.
Ryan N. Farley, James E. Lee, Laura-Hélèna Rivellini, Alex K. Y. Lee, Rachael Dal Porto, Christopher D. Cappa, Kyle Gorkowski, Abu Sayeed Md Shawon, Katherine B. Benedict, Allison C. Aiken, Manvendra K. Dubey, and Qi Zhang
Atmos. Chem. Phys., 24, 3953–3971, https://doi.org/10.5194/acp-24-3953-2024, https://doi.org/10.5194/acp-24-3953-2024, 2024
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The black carbon aerosol composition and mixing state were characterized using a soot particle aerosol mass spectrometer. Single-particle measurements revealed the major role of atmospheric processing in modulating the black carbon mixing state. A significant fraction of soot particles were internally mixed with oxidized organic aerosol and sulfate, with implications for activation as cloud nuclei.
Jian Zhao, Valter Mickwitz, Yuanyuan Luo, Ella Häkkinen, Frans Graeffe, Jiangyi Zhang, Hilkka Timonen, Manjula Canagaratna, Jordan E. Krechmer, Qi Zhang, Markku Kulmala, Juha Kangasluoma, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 17, 1527–1543, https://doi.org/10.5194/amt-17-1527-2024, https://doi.org/10.5194/amt-17-1527-2024, 2024
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Organic aerosol constitutes a significant portion of atmospheric fine particles but is less characterized due to its vast number of constituents. Recently, we developed a system for online measurements of particle-phase highly oxygenated organic molecules (HOMs). In this work, we systematically characterized the system, developed a new unit to enhance its performance, and demonstrated the essential role of thermograms in inferring volatility and quantifying HOMs in organic aerosols.
Xinlei Ge, Yele Sun, Justin Trousdell, Mindong Chen, and Qi Zhang
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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This study aims to enhance the application of the Aerodyne high-resolution aerosol mass spectrometer (HR-AMS) in characterizing organic nitrogen (ON) species within aerosol particles and droplets. A thorough analysis was conducted on 75 ON standards that represent a diverse spectrum of ambient ON types. The results underscore the capacity of the HR-AMS in examining the concentration and chemistry of atmospheric ON compounds, thereby offering insights into their sources and environmental impacts.
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.
Ryan N. Farley, Sonya Collier, Christopher D. Cappa, Leah R. Williams, Timothy B. Onasch, Lynn M. Russell, Hwajin Kim, and Qi Zhang
Atmos. Chem. Phys., 23, 15039–15056, https://doi.org/10.5194/acp-23-15039-2023, https://doi.org/10.5194/acp-23-15039-2023, 2023
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Soot particles, also known as black carbon (BC), have important implications for global climate and regional air quality. After the particles are emitted, BC can be coated with other material, impacting the aerosol properties. We selectively measured the composition of particles containing BC to explore their sources and chemical transformations in the atmosphere. We focus on a persistent, multiday fog event in order to study the effects of chemical reactions occurring within liquid droplets.
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.
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.
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.
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.
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.
Junfeng Wang, Jianhuai Ye, Dantong Liu, Yangzhou Wu, Jian Zhao, Weiqi Xu, Conghui Xie, Fuzhen Shen, Jie Zhang, Paul E. Ohno, Yiming Qin, Xiuyong Zhao, Scot T. Martin, Alex K. Y. Lee, Pingqing Fu, Daniel J. Jacob, Qi Zhang, Yele Sun, Mindong Chen, and Xinlei Ge
Atmos. Chem. Phys., 20, 14091–14102, https://doi.org/10.5194/acp-20-14091-2020, https://doi.org/10.5194/acp-20-14091-2020, 2020
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We compared the organics in total submicron matter and those coated on BC cores during summertime in Beijing and found large differences between them. Traffic-related OA was associated significantly with BC, while cooking-related OA did not coat BC. In addition, a factor likely originated from primary biomass burning OA was only identified in BC-containing particles. Such a unique BBOA requires further field and laboratory studies to verify its presence and elucidate its properties and impacts.
Lawrence I. Kleinman, Arthur J. Sedlacek III, Kouji Adachi, Peter R. Buseck, Sonya Collier, Manvendra K. Dubey, Anna L. Hodshire, Ernie Lewis, Timothy B. Onasch, Jeffery R. Pierce, John Shilling, Stephen R. Springston, Jian Wang, Qi Zhang, Shan Zhou, and Robert J. Yokelson
Atmos. Chem. Phys., 20, 13319–13341, https://doi.org/10.5194/acp-20-13319-2020, https://doi.org/10.5194/acp-20-13319-2020, 2020
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Aerosols from wildfires affect the Earth's temperature by absorbing light or reflecting it back into space. This study investigates time-dependent chemical, microphysical, and optical properties of aerosols generated by wildfires in the Pacific Northwest, USA. Wildfire smoke plumes were traversed by an instrumented aircraft at locations near the fire and up to 3.5 h travel time downwind. Although there was no net aerosol production, aerosol particles grew and became more efficient scatters.
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Short summary
We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in illuminated aqueous particle extracts. After measuring the impact of dilution on oxidant concentrations, we extrapolated our results to predict them in ambient particles – 1O2* and 3C* concentrations appear to be greatly enhanced, while •OH appears largely unchanged. Two of these oxidants (1O2*, 3C*) are not yet included in atmospheric models, and our results make it possible to include them in the future.
We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in...
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