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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Vikram Pratap, Christopher J. Hennigan, Bastian Stieger, Andreas Tilgner, Laurent Poulain, Dominik van Pinxteren, Gerald Spindler, and Hartmut Herrmann
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In this work, we characterize trends in aerosol pH and its controlling factors over the period of 2010 – 2019 at the Melpitz research station in eastern Germany. We find strong trends in aerosol pH and major inorganic species in response to changing emissions. We conduct a detailed thermodynamic analysis of the aerosol system and discuss implications for controlling PM2.5 in the region.
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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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.
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EGUsphere, https://doi.org/10.5194/egusphere-2025-457, https://doi.org/10.5194/egusphere-2025-457, 2025
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In this work, we characterize trends in aerosol pH and its controlling factors over the period of 2010 – 2019 at the Melpitz research station in eastern Germany. We find strong trends in aerosol pH and major inorganic species in response to changing emissions. We conduct a detailed thermodynamic analysis of the aerosol system and discuss implications for controlling PM2.5 in the region.
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This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 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
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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
clean.
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
Atmos. Chem. Phys., 20, 4809–4888, https://doi.org/10.5194/acp-20-4809-2020, https://doi.org/10.5194/acp-20-4809-2020, 2020
Short summary
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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
Short summary
Short summary
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
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Novel aerosol hygroscopicity analyses of CAMP2Ex (Cloud, Aerosol, and Monsoon Processes Philippines Experiment) field campaign data show low aerosol hygroscopicity values in Southeast Asia. Organic carbon from smoke decreases hygroscopicity to levels more like those in continental than in polluted marine regions. Hygroscopicity changes at cloud level demonstrate how surface particles impact clouds in the region, affecting model representation of aerosol and cloud interactions in similar polluted marine regions with high organic carbon emissions.
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In order to study aerosols in environments influenced by anthropogenic and biogenic emissions, we performed analyses of samples collected during the ACROSS (Atmospheric Chemistry Of the Suburban Forest) campaign in summer 2022 in the greater Paris area. After analysis of the chemical composition by means of total carbon determination and high-resolution mass spectrometry, this work highlights the influence of anthropogenic inputs on the chemical composition of both urban and forested areas.
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Physical and chemical properties of particulate matter and concentrations of trace gases were measured in a street canyon in Helsinki, Finland, and an urban background site in January–February 2022 to investigate the effect of wintertime conditions on pollutants. State-of-the-art instruments and a mobile laboratory were used, and the measurement data were analysed further with modelling tools like positive matrix factorization and the Pollution Detection Algorithm.
Guilherme Martins Pereira, Leonardo Yoshiaki Kamigauti, Rubens Fabio Pereira, Djacinto Monteiro dos Santos, Thayná da Silva Santos, José Vinicius Martins, Célia Alves, Cátia Gonçalves, Ismael Casotti Rienda, Nora Kováts, Thiago Nogueira, Luciana Rizzo, Paulo Artaxo, Regina Maura de Miranda, Marcia Akemi Yamasoe, Edmilson Dias de Freitas, Pérola de Castro Vasconcellos, and Maria de Fatima Andrade
Atmos. Chem. Phys., 25, 4587–4616, https://doi.org/10.5194/acp-25-4587-2025, https://doi.org/10.5194/acp-25-4587-2025, 2025
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The chemical composition of fine particulate matter was studied in the megacity of São Paulo (Brazil) during a polluted period. Vehicular-related sources remain relevant; however, a high contribution of biomass burning was observed and correlated with sample ecotoxicity. Emerging biomass burning sources, such as forest fires and sugarcane-bagasse-based power plants, highlight the need for additional control measures alongside stricter rules concerning vehicular emissions.
Emmanuel Chevassus, Kirsten N. Fossum, Darius Ceburnis, Lu Lei, Chunshui Lin, Wei Xu, Colin O'Dowd, and Jurgita Ovadnevaite
Atmos. Chem. Phys., 25, 4107–4129, https://doi.org/10.5194/acp-25-4107-2025, https://doi.org/10.5194/acp-25-4107-2025, 2025
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This study presents the first source apportionment of organic aerosol at Mace Head via high-resolution mass spectrometry. Introducing transfer entropy as a novel method reveals that aged organic aerosol originates from both open-ocean ozonolysis and local peat-burning oxidation. Methanesulfonic acid and organic sea spray both mirror phytoplankton activity, with the former closely tied to coccolithophore blooms and the latter linked to diatoms, chlorophytes, and cyanobacteria.
Jia-Yuan Wang, Meng-Xue Tang, Shan Lu, Ke-Jin Tang, Xing Peng, Ling-Yan He, and Xiao-Feng Huang
EGUsphere, https://doi.org/10.5194/egusphere-2025-1034, https://doi.org/10.5194/egusphere-2025-1034, 2025
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Our study explores how secondary organic aerosols (SOA), a major component of air pollution, form in different particle sizes in a coastal city in China. We found that SOA in fine particles is mainly produced through aqueous chemical reactions, especially those involving iron. In contrast, coarse particles form SOA through reactions with ozone and gases from both fossil fuels and natural sources. These findings highlight the need for size-specific air pollution models.
Ashutosh K. Shukla, Sachchida N. Tripathi, Shamitaksha Talukdar, Vishnu Murari, Sreenivas Gaddamidi, Manousos-Ioannis Manousakas, Vipul Lalchandani, Kuldeep Dixit, Vinayak M. Ruge, Peeyush Khare, Mayank Kumar, Vikram Singh, Neeraj Rastogi, Suresh Tiwari, Atul K. Srivastava, Dilip Ganguly, Kaspar Rudolf Daellenbach, and André S. H. Prévôt
Atmos. Chem. Phys., 25, 3765–3784, https://doi.org/10.5194/acp-25-3765-2025, https://doi.org/10.5194/acp-25-3765-2025, 2025
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Our study delves into the elemental composition of aerosols at three sites across the Indo-Gangetic Plain (IGP), revealing distinct patterns during pollution episodes. We found significant increases in chlorine (Cl)-rich and solid fuel combustion (SFC) sources, indicating dynamic emission sources, agricultural burning impacts, and meteorological influences. Surges in Cl-rich particles during cold periods highlight their role in particle growth under high-relative-humidity conditions.
Ye Kuang, Biao Luo, Shan Huang, Junwen Liu, Weiwei Hu, Yuwen Peng, Duohong Chen, Dingli Yue, Wanyun Xu, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 25, 3737–3752, https://doi.org/10.5194/acp-25-3737-2025, https://doi.org/10.5194/acp-25-3737-2025, 2025
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This research reveals the potential importance of nighttime NO3 radical chemistry and aerosol water in the rapid formation of secondary brown carbon from diluted biomass burning emissions. The findings enhance our understanding of nighttime biomass burning evolution and its implications for climate and regional air quality, especially regarding interactions with background aerosol water and water-rich fogs and clouds.
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.
Yuan Cheng, Ying-jie Zhong, Zhi-qing Zhang, Xu-bing Cao, and Jiu-meng Liu
EGUsphere, https://doi.org/10.5194/egusphere-2025-537, https://doi.org/10.5194/egusphere-2025-537, 2025
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As an emerging hotspot of atmospheric sciences, Northeast China is distinct due to the frigid winter and the strong emissions from agricultural fires. Based on field campaigns conducted in Harbin, we successively identified the analytical method that could lead to proper results of organic and elemental carbon. Our results are believed to be a support for future efforts on exploration of the PM2.5 sources in Northeast China, which are essential for further improving the regional air quality.
Ting Yang, Yu Xu, Yu-Chen Wang, Yi-Jia Ma, Hong-Wei Xiao, Hao Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 25, 2967–2978, https://doi.org/10.5194/acp-25-2967-2025, https://doi.org/10.5194/acp-25-2967-2025, 2025
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Previous measurement–model comparisons of atmospheric isoprene levels showed a significant unidentified source of isoprene in some northern Chinese cities during winter. Here, the first combination of large-scale observations and field combustion experiments provides novel insights into biomass burning emissions as a significant source of isoprene-derived organosulfates during winter in northern cities of China.
Agnesh Panta, Konrad Kandler, Kerstin Schepanski, Andres Alastuey, Pavla Dagsson Waldhauserova, Sylvain Dupont, Melanie Eknayan, Cristina González-Flórez, Adolfo González-Romero, Martina Klose, Mara Montag, Xavier Querol, Jesús Yus-Díez, and Carlos Pérez García-Pando
EGUsphere, https://doi.org/10.5194/egusphere-2025-494, https://doi.org/10.5194/egusphere-2025-494, 2025
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Iceland is among the most active dust source areas in the world. Dust properties are influenced by particle size, mineralogy, shape, and mixing state. This work characterizes freshly emitted individual aerosol particles of Icelandic dust using electron microscopy. Our study provides insights into critical particle-specific information will contribute to better constraining climate models that consider mineralogical variations in their representation of the dust cycle.
Yi-Jia Ma, Yu Xu, Ting Yang, Lin Gui, Hong-Wei Xiao, Hao Xiao, and Hua-Yun Xiao
Atmos. Chem. Phys., 25, 2763–2780, https://doi.org/10.5194/acp-25-2763-2025, https://doi.org/10.5194/acp-25-2763-2025, 2025
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The abundance, potential precursors, and main formation mechanisms of nitrogen-containing organic compounds (NOCs) in PM2.5 during winter were compared among cities with different energy consumption patterns. The aerosol NOC pollution during winter in China is closely associated with the intensity of precursor emissions and the aqueous-phase processes. Our results highlight the importance of emission reduction strategies in controlling aerosol NOCs pollution during winter in China.
Dane Blanchard, Mark Gordon, Duc Huy Dang, Paul Andrew Makar, and Julian Aherne
Atmos. Chem. Phys., 25, 2423–2442, https://doi.org/10.5194/acp-25-2423-2025, https://doi.org/10.5194/acp-25-2423-2025, 2025
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This study offers the first known evaluation of water-soluble brown carbon aerosols in the Athabasca oil sands region (AOSR), Canada. Fluorescence spectroscopy analysis of aerosol samples from five regional sites (collected during the summer of 2021) identified oil sands operations as a measurable brown carbon source. Industrial aerosol emissions were unlikely to impact regional radiative forcing. These findings show that fluorescence spectroscopy can be used to monitor brown carbon in the AOSR.
Kira Zeider, Kayla McCauley, Sanja Dmitrovic, Leong Wai Siu, Yonghoon Choi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Simon Kirschler, John B. Nowak, Michael A. Shook, Kenneth L. Thornhill, Christiane Voigt, Edward L. Winstead, Luke D. Ziemba, Paquita Zuidema, and Armin Sorooshian
Atmos. Chem. Phys., 25, 2407–2422, https://doi.org/10.5194/acp-25-2407-2025, https://doi.org/10.5194/acp-25-2407-2025, 2025
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In situ aircraft data collected over the northwest Atlantic Ocean are utilized to compare aerosol conditions and turbulence between near-surface and below-cloud-base altitudes for different regimes of coupling strength between those two levels, along with how cloud microphysical properties vary across those regimes. Stronger coupling yields more homogenous aerosol structure vertically along with higher cloud drop concentrations and sea salt influence in clouds.
Junke Zhang, Xinyi Fu, Chunying Chen, Yunfei Su, Siyu Liu, Luyao Chen, Yubao Chen, Gehui Wang, and Andre S. H. Prevot
EGUsphere, https://doi.org/10.5194/egusphere-2025-92, https://doi.org/10.5194/egusphere-2025-92, 2025
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The 125 organic aerosol (OA) compounds in PM2.5 in winter in Chengdu were measured at the molecular level. OA was dominated by fatty acids, phthalate esters, and anhydrosugars, and were deeply influenced by anthropogenic sources. As pollution worsens: secondary inorganic species and secondary organic carbon (OC) dominated the increase in PM2.5; fatty acids and anhydrosugars dominated the increase in OA; and the contribution of secondary formation and biomass burning to OC increased markedly.
Amie Dobracki, Ernie R. Lewis, Arthur J. Sedlacek III, Tyler Tatro, Maria A. Zawadowicz, and Paquita Zuidema
Atmos. Chem. Phys., 25, 2333–2363, https://doi.org/10.5194/acp-25-2333-2025, https://doi.org/10.5194/acp-25-2333-2025, 2025
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Biomass-burning aerosol is commonly present in the marine boundary layer over the southeast Atlantic Ocean between June and October. Our research indicates that burning conditions, aerosol transport pathways, and prolonged oxidation processes (heterogeneous and aqueous phases) determine the chemical, microphysical, and optical properties of the boundary layer aerosol. Notably, we find that the aerosol optical properties can be estimated from the chemical properties alone.
Benjamin Heutte, Nora Bergner, Hélène Angot, Jakob B. Pernov, Lubna Dada, Jessica A. Mirrielees, Ivo Beck, Andrea Baccarini, Matthew Boyer, Jessie M. Creamean, Kaspar R. Daellenbach, Imad El Haddad, Markus M. Frey, Silvia Henning, Tiia Laurila, Vaios Moschos, Tuukka Petäjä, Kerri A. Pratt, Lauriane L. J. Quéléver, Matthew D. Shupe, Paul Zieger, Tuija Jokinen, and Julia Schmale
Atmos. Chem. Phys., 25, 2207–2241, https://doi.org/10.5194/acp-25-2207-2025, https://doi.org/10.5194/acp-25-2207-2025, 2025
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Limited aerosol measurements in the central Arctic hinder our understanding of aerosol–climate interactions in the region. Our year-long observations of aerosol physicochemical properties during the MOSAiC expedition reveal strong seasonal variations in aerosol chemical composition, where the short-term variability is heavily affected by storms in the Arctic. Local wind-generated particles are shown to be an important source of cloud seeds, especially in autumn.
Feng Jiang, Harald Saathoff, Uzoamaka Ezenobi, Junwei Song, Hengheng Zhang, Linyu Gao, and Thomas Leisner
Atmos. Chem. Phys., 25, 1917–1930, https://doi.org/10.5194/acp-25-1917-2025, https://doi.org/10.5194/acp-25-1917-2025, 2025
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The chemical composition of brown carbon in the particle and gas phase was determined by mass spectrometry. BrC in the gas phase was mainly controlled by secondary formation and particle-to-gas partitioning. BrC in the particle phase was mainly from secondary formation. This work helps to get a better understanding of diurnal variations and the sources of brown carbon aerosol at a rural location in central Europe.
Theresa Mathes, Heather Guy, John Prytherch, Julia Kojoj, Ian Brooks, Sonja Murto, Paul Zieger, Birgit Wehner, Michael Tjernström, and Andreas Held
EGUsphere, https://doi.org/10.5194/egusphere-2025-183, https://doi.org/10.5194/egusphere-2025-183, 2025
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The Arctic is warming faster than the global average and aerosol-cloud-sea-ice interactions are crucial for studying its climate system. During the ARTofMELT Expedition 2023, particle and sensible heat fluxes were measured over multiple surfaces. Wide lead surfaces acted as particle sources with the strongest sensible heat fluxes, while closed ice surfaces acted as a particle sink. This study improves methods to measure these interactions, enhancing our understanding of Arctic climate processes.
Vikram Pratap, Christopher J. Hennigan, Bastian Stieger, Andreas Tilgner, Laurent Poulain, Dominik van Pinxteren, Gerald Spindler, and Hartmut Herrmann
EGUsphere, https://doi.org/10.5194/egusphere-2025-457, https://doi.org/10.5194/egusphere-2025-457, 2025
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In this work, we characterize trends in aerosol pH and its controlling factors over the period of 2010 – 2019 at the Melpitz research station in eastern Germany. We find strong trends in aerosol pH and major inorganic species in response to changing emissions. We conduct a detailed thermodynamic analysis of the aerosol system and discuss implications for controlling PM2.5 in the region.
Rui Li, Yubing Shen, Yumeng Shao, Yining Gao, Ziwei Yao, Qian Liu, Xing Liu, and Guitao Shi
EGUsphere, https://doi.org/10.5194/egusphere-2024-3740, https://doi.org/10.5194/egusphere-2024-3740, 2025
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It is the first time to reveal the global variations of PAHs derivatives in the marine air. We found that marine aerosols in East China Sea (ECS) and Western Pacific (WP) were significantly affected by coal and engine combustion, while those in Bismarck Sea (BS) and East Australian Sea (EAS) were mainly influenced by wildfire and coal combustion. Antarctic Ocean (AO) was dominated by biomass burning and local shipping emissions. This finding help elucidate the mechanism of global PAH cycle.
James Brean, David C. S. Beddows, Eija Asmi, Aki 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, Rolf Weller, Giselle L. Marincovich, Gabriela C. Mulena, Roy M. Harrison, and Manuel Dall'Osto
Atmos. Chem. Phys., 25, 1145–1162, https://doi.org/10.5194/acp-25-1145-2025, https://doi.org/10.5194/acp-25-1145-2025, 2025
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Our results emphasise how understanding the geographical variation in surface types across the Antarctic is key to understanding secondary aerosol sources.
Adam E. Thomas, Hayley S. Glicker, Alex B. Guenther, Roger Seco, Oscar Vega Bustillos, Julio Tota, Rodrigo A. F. Souza, and James N. Smith
Atmos. Chem. Phys., 25, 959–977, https://doi.org/10.5194/acp-25-959-2025, https://doi.org/10.5194/acp-25-959-2025, 2025
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We present measurements of the organic composition of ultrafine particles collected from the eastern Amazon, an understudied region that is subjected to increasing human influence. We find that while isoprene chemistry is likely significant for ultrafine-particle growth throughout the year, compounds related to other sources, such as biological-spore emissions and biomass burning, exhibit striking seasonal differences, implying extensive variation in regional ultrafine-particle sources.
Xiufeng Lian, Yongjiang Xu, Fengxian Liu, Long Peng, Xiaodong Hu, Guigang Tang, Xu Dao, Hui Guo, Liwei Wang, Bo Huang, Chunlei Cheng, Lei Li, Guohua Zhang, Xinhui Bi, Xiaofei Wang, Zhen Zhou, and Mei Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-3469, https://doi.org/10.5194/egusphere-2024-3469, 2025
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In this study, we analyzed the mixing state and atmospheric chemical processes of Pb-rich single particles in Beijing. Then, we focused on analyzing the differences in Pb-rich particles between the heating period and non-heating period, as well as the formation mechanism of lead nitrate after coal-to-gas conversion. Our results highlighted the improvement of coal-to-gas conversion on Pb in the particulate.
Chiara Giorio, Anne Monod, Valerio Di Marco, Pierre Herckes, Denise Napolitano, Amy Sullivan, Gautier Landrot, Daniel Warnes, Marika Nasti, Sara D'Aronco, Agathe Gérardin, Nicolas Brun, Karine Desboeufs, Sylvain Triquet, Servanne Chevaillier, Claudia Di Biagio, Francesco Battaglia, Frédéric Burnet, Stuart J. Piketh, Andreas Namwoonde, Jean-François Doussin, and Paola Formenti
EGUsphere, https://doi.org/10.5194/egusphere-2024-4140, https://doi.org/10.5194/egusphere-2024-4140, 2025
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A comparison between the solubility of trace metals in pairs of total suspended particulate (TSP) and fog water samples collected in Henties Bay, Namibia, during the AEROCLO-sA field campaign is presented. We found enhanced solubility of metals in fog samples which we attributed to metal-ligand complexes formation in the early stages of particle activation into droplets which can then remain in a kinetically stable form in fog or lead to the formation of colloidal nanoparticles.
Xu Yu, Min Zhou, Shuhui Zhu, Liping Qiao, Jinjian Li, Yingge Ma, Zijing Zhang, Kezheng Liao, Hongli Wang, and Jian Zhen Yu
EGUsphere, https://doi.org/10.5194/egusphere-2024-4103, https://doi.org/10.5194/egusphere-2024-4103, 2025
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Online measurements of bulk aerosol organic nitrogen (ON), in conjunction with a comprehensive array of source markers, have revealed five emission sources and five potentially significant formation processes of nitrogenous organic aerosols. This study provides first quantitative source analysis of ON aerosol and valuable observational evidence on secondary ON aerosol formation through NH3 and NOx chemistries.
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, Moe Kadota, Akane Tsushima, Naoko Nagatsuka, and Teruo Aoki
Atmos. Chem. Phys., 25, 657–683, https://doi.org/10.5194/acp-25-657-2025, https://doi.org/10.5194/acp-25-657-2025, 2025
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Monthly ice core records spanning 350 years from Greenland show trends in refractory black carbon (rBC) concentrations and sizes. rBC levels have increased since the 1870s due to the inflow of anthropogenic rBC, with larger diameters than those from biomass burning (BB) rBC. High summer BB rBC peaks may reduce the ice sheet albedo, but BB rBC showed no increase until the early 2000s. These results are vital for validating aerosol and climate models.
Petr Vodička, Kimitaka Kawamura, Bhagawati Kunwar, Lin Huang, Dhananjay K. Deshmukh, Md. Mozammel Haque, Sangeeta Sharma, and Leonard Barrie
EGUsphere, https://doi.org/10.5194/egusphere-2024-3656, https://doi.org/10.5194/egusphere-2024-3656, 2025
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Carbonate carbon (CC) is not negligible in Arctic total suspended particles (TSP). If not considered, CC biases the contribution of elemental and organic carbon. CC content in TSP was strongly reflected in the δ13C values of total carbon (TC). Carbon contribution from CaCO3 supports strong dependence of CC and δ13C on Ca. Finally, two hypothetical CC sources were identified based on the analysis of air mass back trajectories – dust resuspension and marine microorganisms.
Mingjie Kang, Mengying Bao, Wenhuai Song, Aduburexiati Abulimiti, Changliu Wu, Fang Cao, Sönke Szidat, and Yanlin Zhang
Atmos. Chem. Phys., 25, 73–91, https://doi.org/10.5194/acp-25-73-2025, https://doi.org/10.5194/acp-25-73-2025, 2025
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Reports on molecular-level knowledge of high-temporal-resolution particulate matter ≤2.5 µm in diameter (PM2.5) on hazy days are limited. We investigated various PM2.5 species and their sources. The results show biomass burning (BB) was the main source of organic carbon. Moreover, BB enhanced fungal spore emissions and secondary aerosol formation. The contribution of non-fossil sources increased with increasing haze pollution, suggesting BB may be an important driver of haze events in winter.
Gregory P. Schill, Karl D. Froyd, Daniel M. Murphy, Christina J. Williamson, Charles A. Brock, Tomás Sherwen, Mat J. Evans, Eric A. Ray, Eric C. Apel, Rebecca S. Hornbrook, Alan J. Hills, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Ilann Bourgeois, Donald R. Blake, Joshua P. DiGangi, and Glenn S. Diskin
Atmos. Chem. Phys., 25, 45–71, https://doi.org/10.5194/acp-25-45-2025, https://doi.org/10.5194/acp-25-45-2025, 2025
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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.
Capucine Camin, François Lacan, Catherine Pradoux, Marie Labatut, Anne Johansen, and James W. Murray
EGUsphere, https://doi.org/10.5194/egusphere-2024-3777, https://doi.org/10.5194/egusphere-2024-3777, 2024
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This manuscript presents the chemical composition of aerosols (> 1µm) over the Equatorial and Tropical Pacific Ocean, presenting the first measurements of iron isotopes in aerosols from this region. Iron concentrations and isotopes were determined using a Neptune MC-ICPMS. Our data analysis reveals that a significant portion of the aerosols undergo dissolution and removal during atmospheric transport. These findings contribute to original conclusions about the chemistry and physics of aerosols.
Andreas Aktypis, Dontavious J. Sippial, Christina N. Vasilakopoulou, Angeliki Matrali, Christos Kaltsonoudis, Andrea Simonati, Marco Paglione, Matteo Rinaldi, Stefano Decesari, and Spyros N. Pandis
Atmos. Chem. Phys., 24, 13769–13791, https://doi.org/10.5194/acp-24-13769-2024, https://doi.org/10.5194/acp-24-13769-2024, 2024
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A dual-chamber system was deployed in two different environments (Po Valley, Italy, and Pertouli forest, Greece) to study the potential of ambient air directly injected into the chambers, to form secondary organic aerosol (SOA). In the Po Valley, the system reacts rapidly, forming large amounts of SOA, while in Pertouli the SOA formation chemistry appears to have been practically terminated before the beginning of most experiments, so there is little additional SOA formation potential left.
Amna Ijaz, Brice Temime-Roussel, Benjamin Chazeau, Sarah Albertin, Stephen R. Arnold, Brice Barrett, Slimane Bekki, Natalie Brett, Meeta Cesler-Maloney, Elsa Dieudonne, Kayane K. Dingilian, Javier G. Fochesatto, Jingqiu Mao, Allison Moon, Joel Savarino, William Simpson, Rodney J. Weber, Kathy S. Law, and Barbara D'Anna
EGUsphere, https://doi.org/10.5194/egusphere-2024-3789, https://doi.org/10.5194/egusphere-2024-3789, 2024
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Fairbanks is among the most polluted cities with the highest particulate matter (PM) levels in the US during winters. Highly time-resolved measurements of the sub-micron PM elucidated residential heating with wood and oil and hydrocarbon-like organics from traffic, as well as sulphur-containing organic aerosol, to be the key pollution sources. Remarkable differences existed between complementary instruments, warranting the deployment of multiple tools at sites with wide-ranging influences.
Fredrik Mattsson, Almuth Neuberger, Liine Heikkinen, Yvette Gramlich, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Paul Zieger, Ilona Riipinen, and Claudia Mohr
EGUsphere, https://doi.org/10.5194/egusphere-2024-3629, https://doi.org/10.5194/egusphere-2024-3629, 2024
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This study investigated aerosol-cloud interactions, focusing on organic nitrogen (ON) formation in the aqueous phase. Measurements were conducted in wintertime Italian Po Valley, using aerosol mass spectrometry. The fog was enriched in more hygroscopic inorganic compounds and ON, containing e.g. imidazoles. The formation of imidazole by aerosol-fog interactions could be confirmed for the first time in atmospheric observations. Findings highlight the role of fog in nitrogen aerosol formation.
Jie Zhang, Tianyu Zhu, Alexandra Catena, Yaowei Li, Margaret J. Schwab, Pengfei Liu, Akua Asa-Awuku, and James Schwab
Atmos. Chem. Phys., 24, 13445–13456, https://doi.org/10.5194/acp-24-13445-2024, https://doi.org/10.5194/acp-24-13445-2024, 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), when the aerosol chemical composition is already known.
Wei Yuan, Ru-Jin Huang, Chao Luo, Lu Yang, Wenjuan Cao, Jie Guo, and Huinan Yang
Atmos. Chem. Phys., 24, 13219–13230, https://doi.org/10.5194/acp-24-13219-2024, https://doi.org/10.5194/acp-24-13219-2024, 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 dithiothreitol (DTTv) in the north was comparable to that in the south, while the mass-normalized dithiothreitol (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 to DTTv in the north.
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, Baoling Liang, Qibin Sun, Jun Zhao, Duohong Chen, Jiaren Sun, Zhiyong Yang, and Min Shao
Atmos. Chem. Phys., 24, 13065–13079, https://doi.org/10.5194/acp-24-13065-2024, https://doi.org/10.5194/acp-24-13065-2024, 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. A 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.
Qingxiao Meng, Yunjiang Zhang, Sheng Zhong, Jie Fang, Lili Tang, Yongcai Rao, Minfeng Zhou, Jian Qiu, Xiaofeng Xu, Jean-Eudes Petit, Olivier Favez, and Xinlei Ge
EGUsphere, https://doi.org/10.5194/egusphere-2024-2776, https://doi.org/10.5194/egusphere-2024-2776, 2024
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We developed a new method to reconstruct missing elemental carbon (EC) data in four Chinese cities from 2013 to 2023. Using machine learning, we accurately filled data gaps and introduced a new approach to analyze EC trends. Our findings reveal a significant decline in EC due to stricter pollution controls, though this slowed after 2020. This study provides a versatile framework for addressing data gaps and supports strategies to reduce urban air pollution and its climate impacts.
Yingjie Shen, Rudra P. Pokhrel, Amy P. Sullivan, Ezra J. T. Levin, Lauren A. Garofalo, Delphine K. Farmer, Wade Permar, Lu Hu, Darin W. Toohey, Teresa Campos, Emily V. Fischer, and Shane M. Murphy
Atmos. Chem. Phys., 24, 12881–12901, https://doi.org/10.5194/acp-24-12881-2024, https://doi.org/10.5194/acp-24-12881-2024, 2024
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The magnitude and evolution of brown carbon (BrC) absorption remain unclear, with uncertainty in climate models. Data from the WE-CAN airborne experiment show that model parameterizations overestimate the mass absorption cross section (MAC) of BrC. Observed decreases in BrC absorption with chemical markers are due to decreasing organic aerosol (OA) mass rather than a decreasing BrC MAC, which is currently implemented in models. Water-soluble BrC contributes 23 % of total absorption at 660 nm.
Qun He, Zhaowen Wang, Houfeng Liu, Pengju Xu, Rongbao Duan, Caihong Xu, Jianmin Chen, and Min Wei
Atmos. Chem. Phys., 24, 12775–12792, https://doi.org/10.5194/acp-24-12775-2024, https://doi.org/10.5194/acp-24-12775-2024, 2024
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Coastal environments provide an ideal setting for investigating the intermixing of terrestrial and marine aerosols. Terrestrial air mass constituted a larger number of microbes from anthropogenic and soil emissions, whereas saprophytic and gut microbes were predominant in marine samples. Mixed air masses indicated a fusion of marine and terrestrial aerosols, characterized by alterations in the ratio of pathogenic and saprophytic microbes when compared to either terrestrial or marine samples.
Rime El Asmar, Zongrun Li, David J. Tanner, Yongtao Hu, Susan O'Neill, L. Gregory Huey, M. Talat Odman, and Rodney J. Weber
Atmos. Chem. Phys., 24, 12749–12773, https://doi.org/10.5194/acp-24-12749-2024, https://doi.org/10.5194/acp-24-12749-2024, 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 2 different years, we characterize emissions and evolutions of up to 8 h of PM2.5 mass, black carbon (BC), and brown carbon (BrC) in smoke from burning of forested lands in the southeastern USA.
Matthew Boyer, Diego Aliaga, Lauriane L. J. Quéléver, Silvia Bucci, Hélène Angot, Lubna Dada, Benjamin Heutte, Lisa Beck, Marina Duetsch, Andreas Stohl, Ivo Beck, Tiia Laurila, Nina Sarnela, Roseline C. Thakur, Branka Miljevic, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 24, 12595–12621, https://doi.org/10.5194/acp-24-12595-2024, https://doi.org/10.5194/acp-24-12595-2024, 2024
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We analyze the seasonal cycle and sources of gases that are relevant for the formation of aerosol particles in the central Arctic. Since theses gases can form new particles, they can influence Arctic climate. We show that the sources of these gases are associated with changes in the Arctic environment during the year, especially with respect to sea ice. Therefore, the concentration of these gases will likely change in the future as the Arctic continues to warm.
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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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