Articles | Volume 23, issue 22
https://doi.org/10.5194/acp-23-14437-2023
© Author(s) 2023. 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-23-14437-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
22 Nov 2023
Research article |
| 22 Nov 2023
| 22 Nov 2023
pH dependence of brown-carbon optical properties in cloud water
Christopher J. Hennigan
CORRESPONDING AUTHOR
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Michael McKee
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Vikram Pratap
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Bryanna Boegner
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Jasper Reno
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Lucia Garcia
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Madison McLaren
Department of Chemical, Biochemical and Environmental Engineering, University of Maryland, Baltimore County, Baltimore, 21250, USA
Sara M. Lance
Atmospheric Sciences Research Center (ASRC), University at Albany, Albany, 12226, USA
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Michael A. Battaglia Jr., Nicholas Balasus, Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
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This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
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Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
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This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Christopher E. Lawrence, Paul Casson, Richard Brandt, James J. Schwab, James E. Dukett, Phil Snyder, Elizabeth Yerger, Daniel Kelting, Trevor C. VandenBoer, and Sara Lance
Atmos. Chem. Phys., 23, 1619–1639, https://doi.org/10.5194/acp-23-1619-2023, https://doi.org/10.5194/acp-23-1619-2023, 2023
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Atmospheric aqueous chemistry can have profound effects on our environment, as illustrated by historical data from Whiteface Mountain (WFM) that were critical for uncovering the process of acid rain. The current study updates the long-term trends in cloud water composition at WFM for the period 1994 to 2021. We highlight the emergence of a new chemical regime at WFM dominated by organics and ammonium, quite different from the highly acidic regime observed in the past but not necessarily
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Michael A. Battaglia Jr., Nicholas Balasus, Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 18271–18281, https://doi.org/10.5194/acp-21-18271-2021, https://doi.org/10.5194/acp-21-18271-2021, 2021
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This study characterizes aerosol liquid water content and aerosol pH at a land–water transition site near Baltimore, Maryland. We characterize the effects of unique meteorology associated with the close proximity to the Chesapeake Bay and episodic NH3 events derived from industrial and agricultural sources on aerosol chemistry during the summer. We also examine two events where primary Bay emissions underwent aging in the polluted urban atmosphere.
Nicholas Balasus, Michael A. Battaglia Jr., Katherine Ball, Vanessa Caicedo, Ruben Delgado, Annmarie G. Carlton, and Christopher J. Hennigan
Atmos. Chem. Phys., 21, 13051–13065, https://doi.org/10.5194/acp-21-13051-2021, https://doi.org/10.5194/acp-21-13051-2021, 2021
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Measurements of aerosol and gas composition were carried out at a land–water transition site near Baltimore, MD. Gas-phase ammonia concentrations were highly elevated compared to measurements at a nearby inland site. Our analysis reveals that NH2 was from both industrial and agricultural sources. This had a pronounced effect on aerosol chemical composition at the site, most notably contributing to episodic spikes of aerosol nitrate.
Havala O. T. Pye, Athanasios Nenes, Becky Alexander, Andrew P. Ault, Mary C. Barth, Simon L. Clegg, Jeffrey L. Collett Jr., Kathleen M. Fahey, Christopher J. Hennigan, Hartmut Herrmann, Maria Kanakidou, James T. Kelly, I-Ting Ku, V. Faye McNeill, Nicole Riemer, Thomas Schaefer, Guoliang Shi, Andreas Tilgner, John T. Walker, Tao Wang, Rodney Weber, Jia Xing, Rahul A. Zaveri, and Andreas Zuend
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Acid rain is recognized for its impacts on human health and ecosystems, and programs to mitigate these effects have had implications for atmospheric acidity. Historical measurements indicate that cloud and fog droplet acidity has changed in recent decades in response to controls on emissions from human activity, while the limited trend data for suspended particles indicate acidity may be relatively constant. This review synthesizes knowledge on the acidity of atmospheric particles and clouds.
Michael A. Battaglia Jr., Rodney J. Weber, Athanasios Nenes, and Christopher J. Hennigan
Atmos. Chem. Phys., 19, 14607–14620, https://doi.org/10.5194/acp-19-14607-2019, https://doi.org/10.5194/acp-19-14607-2019, 2019
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The effects of water-soluble organic carbon (WSOC) on aerosol pH were characterized for aqueous-phase particles containing a mixture of inorganics and organics. The ISORROPIA-II and E-AIM models were used in conjunction with AIOMFAC to quantify the effect of organics on aerosol pH through (1) changes to the aerosol liquid water content and (2) changes to the hydrogen ion activity coefficient. The study included both organic acids and nonacids, at RH levels ranging from 70 to 90 %.
Jie Zhang, Sara Lance, Jeffrey M. Freedman, Yele Sun, Brian A. Crandall, Xiuli Wei, and James J. Schwab
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Preprint retracted
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The impact of fireworks (FW) events on air quality was studied using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and collocated instruments during the Independence Day (July 4) holiday. The Independence Day FW events resulted in significant increases in both organic and inorganic (potassium, sulfate, chloride) chemical components, and the contribution from different aerosol sources was discussed.
Marwa M. H. El-Sayed, Diana L. Ortiz-Montalvo, and Christopher J. Hennigan
Atmos. Chem. Phys., 18, 1171–1184, https://doi.org/10.5194/acp-18-1171-2018, https://doi.org/10.5194/acp-18-1171-2018, 2018
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We characterized the reversibility of aqSOA formed from isoprene at a location in the eastern United States. WSOCp evaporation with drying was observed systematically throughout the late spring and summer, indicating reversible aqSOA formation. The absolute reversible aqSOA concentrations, as well as the relative amount of reversible aqSOA, increased with decreasing NOx / isoprene ratios, suggesting that IEPOX or other low-NOx oxidation products were responsible for these effects.
C. J. Hennigan, J. Izumi, A. P. Sullivan, R. J. Weber, and A. Nenes
Atmos. Chem. Phys., 15, 2775–2790, https://doi.org/10.5194/acp-15-2775-2015, https://doi.org/10.5194/acp-15-2775-2015, 2015
Short summary
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We show that the ion balance and molar ratio methods are unsuitable for use as aerosol pH proxies. Our recommendation is that 1) thermodynamic equilibrium models constrained by both gas and aerosol inputs run in the forward (open) mode, and 2) the phase partitioning of ammonia provides the best predictions of aerosol pH. Given the significance of acidity for numerous chemical processes in the atmosphere, the implications of this study are important and far reaching.
R. Saleh, C. J. Hennigan, G. R. McMeeking, W. K. Chuang, E. S. Robinson, H. Coe, N. M. Donahue, and A. L. Robinson
Atmos. Chem. Phys., 13, 7683–7693, https://doi.org/10.5194/acp-13-7683-2013, https://doi.org/10.5194/acp-13-7683-2013, 2013
Related subject area
Subject: Aerosols | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Xiao He, Xuan Zheng, Shuwen Guo, Lewei Zeng, Ting Chen, Bohan Yang, Shupei Xiao, Qiongqiong Wang, Zhiyuan Li, Yan You, Shaojun Zhang, and Ye Wu
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This study introduces an innovative method for identifying and quantifying complex organic vapors and aerosols. By combining advanced analytical techniques and new algorithms, we categorized thousands of compounds from heavy-duty diesel vehicles and ambient air and highlighted specific tracers for emission sources. The innovative approach enhances peak identification, reduces quantification uncertainties, and offers new insights for air quality management and atmospheric chemistry.
Yu Xu, Tang Liu, Yi-Jia Ma, Qi-Bin Sun, Hong-Wei Xiao, Hao Xiao, Hua-Yun Xiao, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 10531–10542, https://doi.org/10.5194/acp-24-10531-2024, https://doi.org/10.5194/acp-24-10531-2024, 2024
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This study investigates the characteristics of aminiums and ammonium in PM2.5 on clean and polluted winter days in 11 Chinese cities, highlighting the possibility of the competitive uptake of ammonia versus amines on acidic aerosols or the displacement of aminiums by ammonia under high-ammonia conditions. The overall results deepen the understanding of the spatiotemporal differences in aminium characteristics and formation in China.
Cassidy Soloff, Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Francesca Gallo, Johnathan W. Hair, Miguel Ricardo A. Hilario, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 10385–10408, https://doi.org/10.5194/acp-24-10385-2024, https://doi.org/10.5194/acp-24-10385-2024, 2024
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Using aircraft measurements over the northwestern Atlantic between the US East Coast and Bermuda and trajectory modeling of continental outflow, we identify trace gas and particle properties that exhibit gradients with offshore distance and quantify these changes with high-resolution measurements of concentrations and particle chemistry, size, and scattering properties. This work furthers our understanding of the complex interactions between continental and marine environments.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
Atmos. Chem. Phys., 24, 10349–10361, https://doi.org/10.5194/acp-24-10349-2024, https://doi.org/10.5194/acp-24-10349-2024, 2024
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Ions enhance the formation and growth rates of new particles, affecting the Earth's radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Yuan Cheng, Xu-bing Cao, Sheng-qiang Zhu, Zhi-qing Zhang, Jiu-meng Liu, Hong-liang Zhang, Qiang Zhang, and Ke-bin He
Atmos. Chem. Phys., 24, 9869–9883, https://doi.org/10.5194/acp-24-9869-2024, https://doi.org/10.5194/acp-24-9869-2024, 2024
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The agreement between observational and modeling results is essential for the development of efficient air pollution control strategies. Here we constrained the modeling results of carbonaceous aerosols by field observation in Northeast China, a historically overlooked but recently targeted region of national clean-air actions. Our study suggested that the simulation of agricultural fire emissions and secondary organic aerosols remains challenging.
Yuan Dai, Junfeng Wang, Houjun Wang, Shijie Cui, Yunjiang Zhang, Haiwei Li, Yun Wu, Ming Wang, Eleonora Aruffo, and Xinlei Ge
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Short-term strict emission control can improve air quality, but its effectiveness needs assessment. During the 2021 summer COVID-19 lockdown in Yangzhou, we found that PM2.5 levels did not decrease despite reduced primary emissions. Aged black-carbon particles increased substantially due to higher O3 levels and transported pollutants. High humidity and low wind also played key roles. The results highlight the importance of a regionally balanced control strategy for future air quality management.
Xinya Liu, Diego Alves Gouveia, Bas Henzing, Arnoud Apituley, Arjan Hensen, Danielle van Dinther, Rujin Huang, and Ulrike Dusek
Atmos. Chem. Phys., 24, 9597–9614, https://doi.org/10.5194/acp-24-9597-2024, https://doi.org/10.5194/acp-24-9597-2024, 2024
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The vertical distribution of aerosol optical properties is important for their effect on climate. This is usually measured by lidar, which has limitations, most notably the assumption of a lidar ratio. Our study shows that routine surface-level aerosol measurements are able to predict this lidar ratio reasonably well within the lower layers of the atmosphere and thus provide a relatively simple and cost-effective method to improve lidar measurements.
Weiqi Xu, Ye Kuang, Wanyun Xu, Zhiqiang Zhang, Biao Luo, Xiaoyi Zhang, Jiangchuang Tao, Hongqin Qiao, Li Liu, and Yele Sun
Atmos. Chem. Phys., 24, 9387–9399, https://doi.org/10.5194/acp-24-9387-2024, https://doi.org/10.5194/acp-24-9387-2024, 2024
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We deployed an advanced aerosol–fog sampling system at a rural site in the North China Plain to investigate impacts of aerosol hygroscopic growth and activation on the physicochemical properties of submicron aerosols. Observed results highlighted remarkably different aqueous processing of primary and secondary submicron aerosol components under distinct ambient relative humidity (RH) conditions and that RH levels significantly impact aerosol sampling through the aerosol swelling effect.
Can Wu, Xiaodi Liu, Ke Zhang, Si Zhang, Cong Cao, Jianjun Li, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 9263–9275, https://doi.org/10.5194/acp-24-9263-2024, https://doi.org/10.5194/acp-24-9263-2024, 2024
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Brown carbon (BrC) is prevalent in the troposphere and can efficiently absorb solar and terrestrial radiation. Our observations show that the enhanced light absorption of BrC relative to black carbon at the tropopause can be attributed to the formation of nitrogen-containing organic compounds through the aqueous-phase reactions of carbonyls with ammonium.
Taiwo Ajayi, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Marta A. Fenn, Richard A. Ferrare, Johnathan W. Hair, Miguel Ricardo A. Hilario, Chris A. Hostetler, Simon Kirschler, Richard H. Moore, Taylor J. Shingler, Michael A. Shook, Cassidy Soloff, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9197–9218, https://doi.org/10.5194/acp-24-9197-2024, https://doi.org/10.5194/acp-24-9197-2024, 2024
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This study uses airborne data to examine vertical profiles of trace gases, aerosol particles, and meteorological variables over a remote marine area (Bermuda). Results show distinct differences based on both air mass source region (North America, Ocean, Caribbean/North Africa) and altitude for a given air mass type. This work highlights the sensitivity of remote marine areas to long-range transport and the importance of considering the vertical dependence of trace gas and aerosol properties.
Kira Zeider, Grace Betito, Anthony Bucholtz, Peng Xian, Annette Walker, and Armin Sorooshian
Atmos. Chem. Phys., 24, 9059–9083, https://doi.org/10.5194/acp-24-9059-2024, https://doi.org/10.5194/acp-24-9059-2024, 2024
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The predominant wind direction along the California coast (northerly) reverses several times during the summer (to southerly). The effects of these wind reversals on aerosol and cloud characteristics are not well understood. Using data from multiple datasets we found that southerly flow periods had enhanced signatures of anthropogenic emissions due to shipping and continental sources, and clouds had more but smaller droplets.
Saleh Alzahrani, Doğuşhan Kılıç, Michael Flynn, Paul I. Williams, and James Allan
Atmos. Chem. Phys., 24, 9045–9058, https://doi.org/10.5194/acp-24-9045-2024, https://doi.org/10.5194/acp-24-9045-2024, 2024
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This paper investigates emissions from aviation activities at an international airport to evaluate their impact on local air quality. The study provides detailed insights into the chemical composition of aerosols and key pollutants in the airport environment. Source apportionment analysis using positive matrix factorisation (PMF) identified three significant sources: less oxidised oxygenated organic aerosol, alkane organic aerosol, and more oxidised oxygenated organic aerosol.
Mikko Heikkilä, Krista Luoma, Timo Mäkelä, and Tiia Grönholm
Atmos. Chem. Phys., 24, 8927–8941, https://doi.org/10.5194/acp-24-8927-2024, https://doi.org/10.5194/acp-24-8927-2024, 2024
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Black carbon (BC) concentration was measured from 211 ship exhaust gas plumes at a remote marine station. Emission factors of BC were calculated in grams per kilogram of fuel. Ships with an exhaust gas cleaning system (EGCS) were found to have median BC emissions per fuel consumed 5 times lower than ships without an EGCS. However, this might be because of non-EGCS ships running at low engine loads rather than the EGCS itself. A local speed restriction would increase BC emissions of ships.
Olga Zografou, Maria Gini, Prodromos Fetfatzis, Konstantinos Granakis, Romanos Foskinis, Manousos Ioannis Manousakas, Fotios Tsopelas, Evangelia Diapouli, Eleni Dovrou, Christina N. Vasilakopoulou, Alexandros Papayannis, Spyros N. Pandis, Athanasios Nenes, and Konstantinos Eleftheriadis
Atmos. Chem. Phys., 24, 8911–8926, https://doi.org/10.5194/acp-24-8911-2024, https://doi.org/10.5194/acp-24-8911-2024, 2024
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Characterization of PM1 and positive matrix factorization (PMF) source apportionment of organic and inorganic fractions were conducted at the high-altitude station (HAC)2. Cloud presence reduced PM1, affecting sulfate more than organics. Free-troposphere (FT) conditions showed more black carbon (eBC) than planetary boundary layer (PBL) conditions.
Yuanyuan Qin, Xinghua Zhang, Wei Huang, Juanjuan Qin, Xiaoyu Hu, Yuxuan Cao, Tianyi Zhao, Yang Zhang, Jihua Tan, Ziyin Zhang, Xinming Wang, and Zhenzhen Wang
Atmos. Chem. Phys., 24, 8737–8750, https://doi.org/10.5194/acp-24-8737-2024, https://doi.org/10.5194/acp-24-8737-2024, 2024
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Environmental persistent free radicals (EPFRs) and reactive oxygen species (ROSs) play an active role in the atmosphere. Despite control measures having effectively reduced their emissions, reductions were less than in PM2.5. Emission control measures performed well in achieving Parade Blue, but reducing the impact of the atmosphere on human health remains challenging. Thus, there is a need to reassess emission control measures to better address the challenges posed by EPFRs and ROSs.
Fenghua Wei, Xing Peng, Liming Cao, Mengxue Tang, Ning Feng, Xiaofeng Huang, and Lingyan He
Atmos. Chem. Phys., 24, 8507–8518, https://doi.org/10.5194/acp-24-8507-2024, https://doi.org/10.5194/acp-24-8507-2024, 2024
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The water solubility of secondary organic aerosols (SOAs) is a crucial factor in determining their hygroscopicity and climatic impact. Stable carbon isotope and mass spectrometry techniques were combined to assess the water solubility of SOAs with different aging degrees in a coastal megacity in China. This work revealed a much higher water-soluble fraction of aged SOA compared to fresh SOA, indicating that the aging degree of SOA has considerable impacts on its water solubility.
Zijun Zhang, Weiqi Xu, Yi Zhang, Wei Zhou, Xiangyu Xu, Aodong Du, Yinzhou Zhang, Hongqin Qiao, Ye Kuang, Xiaole Pan, Zifa Wang, Xueling Cheng, Lanzhong Liu, Qingyan Fu, Douglas R. Worsnop, Jie Li, and Yele Sun
Atmos. Chem. Phys., 24, 8473–8488, https://doi.org/10.5194/acp-24-8473-2024, https://doi.org/10.5194/acp-24-8473-2024, 2024
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We investigated aerosol composition and sources and the interaction between secondary organic aerosol (SOA) and clouds at a regional mountain site in southeastern China. Clouds efficiently scavenge more oxidized SOA; however, cloud evaporation leads to the production of less oxidized SOA. The unexpectedly high presence of nitrate in aerosol particles indicates that nitrate formed in polluted areas has undergone interactions with clouds, significantly influencing the regional background site.
Feifei Li, Shanshan Tang, Jitao Lv, Shiyang Yu, Xu Sun, Dong Cao, Yawei Wang, and Guibin Jiang
Atmos. Chem. Phys., 24, 8397–8411, https://doi.org/10.5194/acp-24-8397-2024, https://doi.org/10.5194/acp-24-8397-2024, 2024
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Targeted derivatization and non-targeted analysis with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) were used to reveal the molecular composition of carbonyl molecules in PM2.5, and the important role of carbonyls in increasing the oxidative potential of organic aerosol was found in real samples.
Maya Abou-Ghanem, Daniel M. Murphy, Gregory P. Schill, Michael J. Lawler, and Karl D. Froyd
Atmos. Chem. Phys., 24, 8263–8275, https://doi.org/10.5194/acp-24-8263-2024, https://doi.org/10.5194/acp-24-8263-2024, 2024
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Using particle analysis by laser mass spectrometry, we examine vanadium-containing ship exhaust particles measured on NASA's DC-8 during the Atmospheric Tomography Mission (ATom). Our results reveal ship exhaust particles are sufficiently widespread in the marine atmosphere and experience atmospheric aging. Finally, we use laboratory calibrations to determine the vanadium, sulfate, and organic single-particle mass fractions of vanadium-containing ship exhaust particles.
Cassandra J. Gaston, Joseph M. Prospero, Kristen Foley, Havala O. T. Pye, Lillian Custals, Edmund Blades, Peter Sealy, and James A. Christie
Atmos. Chem. Phys., 24, 8049–8066, https://doi.org/10.5194/acp-24-8049-2024, https://doi.org/10.5194/acp-24-8049-2024, 2024
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To understand how changing emissions have impacted aerosols in remote regions, we measured nitrate and sulfate in Barbados and compared them to model predictions from EPA’s Air QUAlity TimE Series (EQUATES). Nitrate was stable, except for spikes in 2008 and 2010 due to transported smoke. Sulfate decreased in the 1990s due to reductions in sulfur dioxide (SO2) in the US and Europe; then it increased in the 2000s, likely due to anthropogenic emissions from Africa.
Jie Zhang, Tianyu Zhu, Alexandra Catena, Yaowei Li, Margaret Schwab, Pengfei Liu, Akua Asa-Awuku, and James Schwab
EGUsphere, https://doi.org/10.5194/egusphere-2024-1390, https://doi.org/10.5194/egusphere-2024-1390, 2024
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This study shows the derived organic aerosol hygroscopicity under high humidity conditions based on a simple optical scatter monitor system, including two nephelometric monitors (pDR-1500), after knowing the aerosol chemical composition.
Jiao Xue, Tian Zhang, Keyhong Park, Jinpei Yan, Young Jun Yoon, Jiyeon Park, and Bingbing Wang
Atmos. Chem. Phys., 24, 7731–7754, https://doi.org/10.5194/acp-24-7731-2024, https://doi.org/10.5194/acp-24-7731-2024, 2024
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Ice formation by particles is an important way of making mixed-phase and ice clouds. We found that particles collected in the marine atmosphere exhibit diverse ice nucleation abilities and mixing states. Sea salt mixed-sulfate particles were enriched in ice-nucleating particles. Selective aging on sea salt particles made particle populations more externally mixed. Characterizations of particles and their mixing state are needed for a better understanding of aerosol–cloud interactions.
Yangzhi Mo, Jun Li, Guangcai Zhong, Sanyuan Zhu, Shizhen Zhao, Jiao Tang, Hongxing Jiang, Zhineng Cheng, Chongguo Tian, Yingjun Chen, and Gan Zhang
Atmos. Chem. Phys., 24, 7755–7772, https://doi.org/10.5194/acp-24-7755-2024, https://doi.org/10.5194/acp-24-7755-2024, 2024
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In this study, we found that biomass burning (31.0 %) and coal combustion (31.1 %) were the dominant sources of water-insoluble organic carbon in China, with coal combustion sources exhibiting the strongest light-absorbing capacity. Additionally, we propose a light-absorbing carbonaceous continuum, revealing that components enriched with fossil sources tend to have stronger light-absorbing capacity, higher aromaticity, higher molecular weights, and greater recalcitrance in the atmosphere.
Jing Duan, Ru-Jin Huang, Ying Wang, Wei Xu, Haobin Zhong, Chunshui Lin, Wei Huang, Yifang Gu, Jurgita Ovadnevaite, Darius Ceburnis, and Colin O'Dowd
Atmos. Chem. Phys., 24, 7687–7698, https://doi.org/10.5194/acp-24-7687-2024, https://doi.org/10.5194/acp-24-7687-2024, 2024
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The chemical composition of atmospheric particles has shown significant changes in recent years. We investigated the potential effects of changes in inorganics on aerosol water uptake and, thus, secondary organic aerosol formation in wintertime haze based on the size-resolved measurements of non-refractory fine particulate matter (NR-PM2.5) in Xi’an, northwestern China. We highlight the key role of aerosol water as a medium to link inorganics and organics in their multiphase processes.
Hongyong Li, Xiaopu Lyu, Likun Xue, Yunxi Huo, Dawen Yao, Haoxian Lu, and Hai Guo
Atmos. Chem. Phys., 24, 7085–7100, https://doi.org/10.5194/acp-24-7085-2024, https://doi.org/10.5194/acp-24-7085-2024, 2024
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Organic aerosol is ubiquitous in the atmosphere and largely explains the gap between current levels of fine particulate matter in many cities and the World Health Organization guideline values. This study highlights the dominant contributions of cooking emissions to organic aerosol when marine air prevailed in Hong Kong, which were occasionally overwhelmed by aromatics-derived secondary organic aerosol in continental ouflows.
Shao Shi, Jinghao Zhai, Xin Yang, Yechun Ruan, Yuanlong Huang, Xujian Chen, Antai Zhang, Jianhuai Ye, Guomao Zheng, Baohua Cai, Yaling Zeng, Yixiang Wang, Chunbo Xing, Yujie Zhang, Tzung-May Fu, Lei Zhu, Huizhong Shen, and Chen Wang
Atmos. Chem. Phys., 24, 7001–7012, https://doi.org/10.5194/acp-24-7001-2024, https://doi.org/10.5194/acp-24-7001-2024, 2024
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The determination of ions in the mass spectra of individual particles remains uncertain. We have developed a standard-free mass calibration algorithm applicable to more than 98 % of ambient particles. With our algorithm, ions with ~ 0.05 Th mass difference could be determined. Therefore, many more atmospheric species could be determined and involved in the source apportionment of aerosols, the study of chemical reaction mechanisms, and the analysis of single-particle mixing states.
Wei Sun, Xiaodong Hu, Yuzhen Fu, Guohua Zhang, Yujiao Zhu, Xinfeng Wang, Caiqing Yan, Likun Xue, He Meng, Bin Jiang, Yuhong Liao, Xinming Wang, Ping'an Peng, and Xinhui Bi
Atmos. Chem. Phys., 24, 6987–6999, https://doi.org/10.5194/acp-24-6987-2024, https://doi.org/10.5194/acp-24-6987-2024, 2024
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The formation pathways of nitrogen-containing compounds (NOCs) in the atmosphere remain unclear. We investigated the composition of aerosols and fog water by state-of-the-art mass spectrometry and compared the formation pathways of NOCs. We found that NOCs in aerosols were mainly formed through nitration reaction, while ammonia addition played a more important role in fog water. The results deepen our understanding of the processes of organic particulate pollution.
Fuzhen Shen, Michaela I. Hegglin, and Yue Yuan
Atmos. Chem. Phys., 24, 6539–6553, https://doi.org/10.5194/acp-24-6539-2024, https://doi.org/10.5194/acp-24-6539-2024, 2024
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We attempt to use a novel structural self-organising map and machine learning models to identify a weather system and quantify the importance of each meteorological factor in driving the unexpected PM2.5 and O3 changes under the specific weather system during the COVID-19 lockdown in China. The result highlights that temperature under the double-centre high-pressure system plays the most crucial role in abnormal events.
Wenshuai Li, Yuxuan Qi, Yingchen Liu, Guanru Wu, Yanjing Zhang, Jinhui Shi, Wenjun Qu, Lifang Sheng, Wencai Wang, Daizhou Zhang, and Yang Zhou
Atmos. Chem. Phys., 24, 6495–6508, https://doi.org/10.5194/acp-24-6495-2024, https://doi.org/10.5194/acp-24-6495-2024, 2024
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Aerosol particles from mainland can transport to oceans and deposit, providing soluble Fe and affecting phytoplankton growth. Thus, we studied the dissolution process of aerosol Fe and found that photochemistry played a key role in promoting Fe dissolution in clean conditions. RH-dependent reactions were more influential in slightly polluted conditions. These results highlight the distinct roles of two weather-related parameters (radiation and RH) in influencing geochemical cycles related to Fe.
Yanqin Ren, Zhenhai Wu, Yuanyuan Ji, Fang Bi, Junling Li, Haijie Zhang, Hao Zhang, Hong Li, and Gehui Wang
Atmos. Chem. Phys., 24, 6525–6538, https://doi.org/10.5194/acp-24-6525-2024, https://doi.org/10.5194/acp-24-6525-2024, 2024
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Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) in PM2.5 were examined from an urban area in Beijing during the autumn and winter. The OPAH and NAC concentrations were much higher during heating than before heating. They majorly originated from the combustion of biomass and automobile emissions, and the secondary generation was the major contributor throughout the whole sampling period.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O’Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
EGUsphere, https://doi.org/10.5194/egusphere-2024-1485, https://doi.org/10.5194/egusphere-2024-1485, 2024
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Prescribed burning is an important method for managing ecosystems and preventing wildfires, however, smoke from prescribed fires can have a significant impact on air quality. Here, using a network of fixed sites and sampling throughout an extended prescribed burning period in two different years, we characterize the emissions and evolution up to 8 hours of PM2.5 mass, BC, and BrC in smoke from burning of forested lands in the southeastern US.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Tomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
EGUsphere, https://doi.org/10.5194/egusphere-2024-1399, https://doi.org/10.5194/egusphere-2024-1399, 2024
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Using single-particle mass spectrometry, we show that trace concentrations of bromine and iodine are ubiquitous in remote tropospheric aerosol, and suggest that aerosols are an important part of the global reactive iodine budget. Comparisons to a global climate model with detailed iodine chemistry are favorable in the background atmosphere; however, the model cannot replicate our measurements near the ocean surface, in biomass burning plumes, and in the stratosphere.
Marco Paglione, David C. S. Beddows, Anna Jones, Thomas Lachlan-Cope, Matteo Rinaldi, Stefano Decesari, Francesco Manarini, Mara Russo, Karam Mansour, Roy M. Harrison, Andrea Mazzanti, Emilio Tagliavini, and Manuel Dall'Osto
Atmos. Chem. Phys., 24, 6305–6322, https://doi.org/10.5194/acp-24-6305-2024, https://doi.org/10.5194/acp-24-6305-2024, 2024
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Applying factor analysis techniques to H-NMR spectra, we present the organic aerosol (OA) source apportionment of PM1 samples collected in parallel at two Antarctic stations, namely Signy and Halley, allowing investigation of aerosol–climate interactions in an unperturbed atmosphere. Our results show remarkable differences between pelagic (open-ocean) and sympagic (sea-ice-influenced) air masses and indicate that various sources and processes are controlling Antarctic aerosols.
Zhichao Dong, Chandra Mouli Pavuluri, Peisen Li, Zhanjie Xu, Junjun Deng, Xueyan Zhao, Xiaomai Zhao, Pingqing Fu, and Cong-Qiang Liu
Atmos. Chem. Phys., 24, 5887–5905, https://doi.org/10.5194/acp-24-5887-2024, https://doi.org/10.5194/acp-24-5887-2024, 2024
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Comprehensive study of optical properties of brown carbon (BrC) in fine aerosols from Tianjin, China, implied that biological emissions are major sources of BrC in summer, whereas fossil fuel combustion and biomass burning emissions are in cold periods. The direct radiation absorption caused by BrC in short wavelengths contributed about 40 % to that caused by BrC in 300–700 nm. Water-insoluble but methanol-soluble BrC contains more protein-like chromophores (PLOM) than that of water-soluble BrC.
Kumiko Goto-Azuma, Yoshimi Ogawa-Tsukagawa, Kaori Fukuda, Koji Fujita, Motohiro Hirabayashi, Remi Dallmayr, Jun Ogata, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Sumito Matoba, and Teruo Aoki
EGUsphere, https://doi.org/10.5194/egusphere-2024-1498, https://doi.org/10.5194/egusphere-2024-1498, 2024
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Monthly records spanning 350 years from a Greenland ice core reveal trends in black carbon (BC) concentrations and sizes. BC concentrations have risen since the late 19th century due to the inflow of anthropogenic BC, with these particles being larger than those from biomass burning (BB). High BB BC concentration peaks in summer originating from BB could reduce albedo. However, BB BC showed no upward trend until the early 2000s. Our findings are crucial for validating aerosol and climate models.
Shan Wang, Kezheng Liao, Zijing Zhang, Yuk Ying Cheng, Qiongqiong Wang, Hanzhe Chen, and Jian Zhen Yu
Atmos. Chem. Phys., 24, 5803–5821, https://doi.org/10.5194/acp-24-5803-2024, https://doi.org/10.5194/acp-24-5803-2024, 2024
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In this work, hourly primary and secondary organic carbon were estimated by a novel Bayesian inference approach in suburban Hong Kong. Their multi-temporal-scale variations and evolution characteristics during PM2.5 episodes were examined. The methodology could serve as a guide for other locations with similar monitoring capabilities. The observation-based results are helpful for understanding the evolving nature of secondary organic aerosols and refining the accuracy of model simulations.
Mingfu Cai, Chenshuo Ye, Bin Yuan, Shan Huang, E Zheng, Suxia Yang, Zelong Wang, Yi Lin, Tiange Li, Weiwei Hu, Wei Chen, Qicong Song, Wei Li, Yuwen Peng, Baolin Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
EGUsphere, https://doi.org/10.5194/egusphere-2024-887, https://doi.org/10.5194/egusphere-2024-887, 2024
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This study investigated the daytime secondary organic aerosol (SOA) formation in urban plumes. We observed a significant daytime SOA formation through gas-particle partitioning when the site was affected by urban plumes. Box model simulation indicated that urban pollutants (nitrogen oxide and volatile organic compounds) could enhance the oxidizing capacity, while the elevated volatile organic compounds were mainly responsible for promoting daytime SOA formation.
James Brean, David C. S. Beddows, Eija Asmi, Ari Virkkula, Lauriane L. J. Quéléver, Mikko Sipilä, Floortje Van Den Heuvel, Thomas Lachlan-Cope, Anna Jones, Markus Frey, Angelo Lupi, Jiyeon Park, Young Jun Yoon, Ralf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall´Osto
EGUsphere, https://doi.org/10.5194/egusphere-2024-987, https://doi.org/10.5194/egusphere-2024-987, 2024
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Our results emphasize how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Qun He, Zhaowen Wang, Houfeng Liu, Pengju Xu, Rongbao Duan, Caihong Xu, Jianmin Chen, and Min Wei
EGUsphere, https://doi.org/10.5194/egusphere-2024-841, https://doi.org/10.5194/egusphere-2024-841, 2024
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Coastal environments provide an ideal setting for investigating the intermixing processes of terrestrial and marine aerosols. Terrestrial air mass constituted a larger proportion during severe air pollution, harboring more animal and human pathogens. A relative shift towards marine air-mass with respect to pollution elimination, where saprophytic bacteria and fungi were predominant. Mixed air-mass reveals the intermixing processes of terrestrial and marine sources.
Yi-Jia Ma, Yu Xu, Ting Yang, Hong-Wei Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 24, 4331–4346, https://doi.org/10.5194/acp-24-4331-2024, https://doi.org/10.5194/acp-24-4331-2024, 2024
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This study provides field-based evidence about the differential impacts of combustion of fresh and aged biomass materials on aerosol nitrogen-containing organic compounds (NOCs) in different seasons in Ürümqi, bridging the linkages between the observations and previous laboratory studies showing the formation mechanisms of NOCs.
Maud Leriche, Pierre Tulet, Laurent Deguillaume, Frédéric Burnet, Aurélie Colomb, Agnès Borbon, Corinne Jambert, Valentin Duflot, Stéphan Houdier, Jean-Luc Jaffrezo, Mickaël Vaïtilingom, Pamela Dominutti, Manon Rocco, Camille Mouchel-Vallon, Samira El Gdachi, Maxence Brissy, Maroua Fathalli, Nicolas Maury, Bert Verreyken, Crist Amelynck, Niels Schoon, Valérie Gros, Jean-Marc Pichon, Mickael Ribeiro, Eric Pique, Emmanuel Leclerc, Thierry Bourrianne, Axel Roy, Eric Moulin, Joël Barrie, Jean-Marc Metzger, Guillaume Péris, Christian Guadagno, Chatrapatty Bhugwant, Jean-Mathieu Tibere, Arnaud Tournigand, Evelyn Freney, Karine Sellegri, Anne-Marie Delort, Pierre Amato, Muriel Joly, Jean-Luc Baray, Pascal Renard, Angelica Bianco, Anne Réchou, and Guillaume Payen
Atmos. Chem. Phys., 24, 4129–4155, https://doi.org/10.5194/acp-24-4129-2024, https://doi.org/10.5194/acp-24-4129-2024, 2024
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Aerosol particles in the atmosphere play a key role in climate change and air pollution. A large number of aerosol particles are formed from the oxidation of volatile organic compounds (VOCs and secondary organic aerosols – SOA). An important field campaign was organized on Réunion in March–April 2019 to understand the formation of SOA in a tropical atmosphere mostly influenced by VOCs emitted by forest and in the presence of clouds. This work synthesizes the results of this campaign.
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.
Wei Yuan, Ru-Jin Huang, Chao Luo, Lu Yang, Wenjuan Cao, Jie Guo, and Huinan Yang
EGUsphere, https://doi.org/10.5194/egusphere-2024-680, https://doi.org/10.5194/egusphere-2024-680, 2024
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We characterized water-soluble oxidative potential (OP) levels in wintertime PM2.5 in the south and north of Beijing. Our results show that the volume normalized DTT (DTTv) in the north was comparable to that in the south, while the mass normalized DTT (DTTm) in the north was almost twice that in the south. Traffic-related emissions and biomass burning were the main sources of DTTv in the south, and traffic-related emissions contributed the most of DTTv in the north.
Cited articles
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Short summary
This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
This study characterized the optical properties of light-absorbing organic compounds, called...
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