Articles | Volume 23, issue 24
https://doi.org/10.5194/acp-23-15643-2023
© 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-23-15643-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
20 Dec 2023
Research article |
| 20 Dec 2023
| 20 Dec 2023
Characterization of water-soluble brown carbon chromophores from wildfire plumes in the western USA using size-exclusion chromatography
Lisa Azzarello
Department of Chemistry, York University, Toronto, ON M3J 1P3, Canada
Rebecca A. Washenfelder
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Michael A. Robinson
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Boulder, CO 80309, USA
Alessandro Franchin
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Boulder, CO 80309, USA
now at: National Center for Atmospheric Research, Boulder, CO 80305, USA
Caroline C. Womack
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado, Boulder, Boulder, CO 80309, USA
Christopher D. Holmes
Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, FL 32304, USA
Steven S. Brown
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
Ann Middlebrook
Chemical Sciences Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Tim Newberger
Global Monitoring Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Colm Sweeney
Global Monitoring Laboratory, National Oceanic and Atmospheric Administration, 325 Broadway, Boulder, CO 80305, USA
Department of Chemistry, York University, Toronto, ON M3J 1P3, Canada
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John W. Halfacre, Lewis Marden, Marvin D. Shaw, Lucy J. Carpenter, Emily Matthews, Thomas J. Bannan, Hugh Coe, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Patrick R. Veres, Michael A. Robinson, Steven S. Brown, and Pete M. Edwards
Atmos. Meas. Tech., 18, 3799–3818, https://doi.org/10.5194/amt-18-3799-2025, https://doi.org/10.5194/amt-18-3799-2025, 2025
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Nitryl chloride (ClNO2) is a reservoir of chlorine atoms and nitrogen oxides, both of which play important roles in atmospheric chemistry. However, all ambient ClNO2 observations so far have been made by a single technique, mass spectrometry, which needs complex calibrations. Here, we present a laser-based method that detects ClNO2 (TD-TILDAS – thermal dissociation–tunable infrared laser direct absorption spectrometry) without the need for complicated calibrations. The results show excellent agreement between these two methods from both laboratory and ambient samples.
Anam M. Khan, Olivia E. Clifton, Jesse O. Bash, Sam Bland, Nathan Booth, Philip Cheung, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christian Hogrefe, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Donna Schwede, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, Leiming Zhang, and Paul C. Stoy
Atmos. Chem. Phys., 25, 8613–8635, https://doi.org/10.5194/acp-25-8613-2025, https://doi.org/10.5194/acp-25-8613-2025, 2025
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Vegetation removes tropospheric ozone through stomatal uptake, and accurately modeling the stomatal uptake of ozone is important for modeling dry deposition and air quality. We evaluated the stomatal component of ozone dry deposition modeled by atmospheric chemistry models at six sites. We find that models and observation-based estimates agree at times during the growing season at all sites, but some models overestimated the stomatal component during the dry summers at a seasonally dry site.
Christopher D. Holmes, Joshua P. Schwarz, Charles H. Fite, Anxhelo Agastra, Holly K. Nowell, Katherine Ball, T. Paul Bui, Johnathan Dean-Day, Zachary C. J. Decker, Joshua P. DiGagni, Glenn S. Diskin, Emily M. Gargulinski, Hannah Halliday, Shobha Kondragunta, John B. Nowak, David A. Peterson, Michael A. Robinson, Amber J. Soja, Rebecca A. Washenfelder, Chuanyu Xu, and Robert J. Yokelson
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-307, https://doi.org/10.5194/essd-2025-307, 2025
Preprint under review for ESSD
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Smoke age is an important factor in the chemical and physical evolution of smoke. Two methods for determining the age of smoke are applied to the NASA-NOAA FIREX-AQ field campaign: one based on wind speed and distance, and another using an ensemble of modeled air parcel trajectories. Both methods are evaluated, with the trajectory method, which includes plume rise and uncertainty estimates, proving more accurate.
Hendrik Fuchs, Aaron Stainsby, Florian Berg, René Dubus, Michelle Färber, Andreas Hofzumahaus, Frank Holland, Kelvin H. Bates, Steven S. Brown, Matthew M. Coggon, Glenn S. Diskin, Georgios I. Gkatzelis, Christopher M. Jernigan, Jeff Peischl, Michael A. Robinson, Andrew W. Rollins, Nell B. Schafer, Rebecca H. Schwantes, Chelsea E. Stockwell, Patrick R. Veres, Carsten Warneke, Eleanor M. Waxman, Lu Xu, Kristen Zuraski, Andreas Wahner, and Anna Novelli
Atmos. Meas. Tech., 18, 881–895, https://doi.org/10.5194/amt-18-881-2025, https://doi.org/10.5194/amt-18-881-2025, 2025
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Significant improvements have been made to the instruments used to measure OH reactivity, which is equivalent to the sum of air pollutant concentrations. Accurate and precise measurements with a high time resolution have been achieved, allowing use on aircraft, as demonstrated during flights in the USA.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
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In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Fernando Chouza, Thierry Leblanc, Patrick Wang, Steven S. Brown, Kristen Zuraski, Wyndom Chace, Caroline C. Womack, Jeff Peischl, John Hair, Taylor Shingler, and John Sullivan
Atmos. Meas. Tech., 18, 405–419, https://doi.org/10.5194/amt-18-405-2025, https://doi.org/10.5194/amt-18-405-2025, 2025
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The JPL lidar group developed the SMOL (Small Mobile Ozone Lidar), an affordable ozone differential absorption lidar (DIAL) system covering all altitudes from 200 m to 10 km a.g.l. The comparison with airborne in situ and lidar measurements shows very good agreement. An additional comparison with nearby surface ozone measuring instruments indicates unbiased measurements by the SMOL lidars down to 200 m a.g.l.
Olivia G. Norman, Colette L. Heald, Solomon Bililign, Pedro Campuzano-Jost, Hugh Coe, Marc N. Fiddler, Jaime R. Green, Jose L. Jimenez, Katharina Kaiser, Jin Liao, Ann M. Middlebrook, Benjamin A. Nault, John B. Nowak, Johannes Schneider, and André Welti
Atmos. Chem. Phys., 25, 771–795, https://doi.org/10.5194/acp-25-771-2025, https://doi.org/10.5194/acp-25-771-2025, 2025
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This study finds that one component of secondary inorganic aerosols, nitrate, is greatly overestimated by a global atmospheric chemistry model compared to observations from 11 flight campaigns. None of the loss and production pathways explored can explain the nitrate bias alone. The model’s inability to capture the variability in the observations remains and requires future investigation to avoid biases in policy-related studies (i.e., air quality, health, climate impacts of these aerosols).
Kouji Adachi, Jack E. Dibb, Joseph M. Katich, Joshua P. Schwarz, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Jeff Peischl, Christopher D. Holmes, and James Crawford
Atmos. Chem. Phys., 24, 10985–11004, https://doi.org/10.5194/acp-24-10985-2024, https://doi.org/10.5194/acp-24-10985-2024, 2024
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We examined aerosol particles from wildfires and identified tarballs (TBs) from the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) campaign. This study reveals the compositions, abundance, sizes, and mixing states of TBs and shows that TBs formed as the smoke aged for up to 5 h. This study provides measurements of TBs from various biomass-burning events and ages, enhancing our knowledge of TB emissions and our understanding of their climate impact.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
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The ozone sink into oceans and marine clouds is seldom studied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure eddy covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller and spatially variable.
Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
Preprint withdrawn
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High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Edward J. Strobach, Sunil Baidar, Brian J. Carroll, Steven S. Brown, Kristen Zuraski, Matthew Coggon, Chelsea E. Stockwell, Lu Xu, Yelena L. Pichugina, W. Alan Brewer, Carsten Warneke, Jeff Peischl, Jessica Gilman, Brandi McCarty, Maxwell Holloway, and Richard Marchbanks
Atmos. Chem. Phys., 24, 9277–9307, https://doi.org/10.5194/acp-24-9277-2024, https://doi.org/10.5194/acp-24-9277-2024, 2024
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Large-scale weather patterns are isolated from local patterns to study the impact that different weather scales have on air quality measurements. While impacts from large-scale meteorology were evaluated by separating ozone (O3) exceedance (>70 ppb) and non-exceedance (<70 ppb) days, we developed a technique that allows direct comparisons of small temporal variations between chemical and dynamics measurements under rapid dynamical transitions.
Alessia A. Colussi, Daniel Persaud, Melodie Lao, Bryan K. Place, Rachel F. Hems, Susan E. Ziegler, Kate A. Edwards, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 17, 3697–3718, https://doi.org/10.5194/amt-17-3697-2024, https://doi.org/10.5194/amt-17-3697-2024, 2024
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A new modular and affordable instrument was developed to automatically collect wet deposition continuously with an off-grid solar top-up power package. Monthly collections were performed across the Newfoundland and Labrador Boreal Ecosystem Latitudinal Transect of experimental forest sites from 2015 to 2016. The proof-of-concept systems were validated with baseline measurements of pH and conductivity and then applied to dissolved organic carbon as an analyte of emerging biogeochemical interest.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
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Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Linia Tashmim, William C. Porter, Qianjie Chen, Becky Alexander, Charles H. Fite, Christopher D. Holmes, Jeffrey R. Pierce, Betty Croft, and Sakiko Ishino
Atmos. Chem. Phys., 24, 3379–3403, https://doi.org/10.5194/acp-24-3379-2024, https://doi.org/10.5194/acp-24-3379-2024, 2024
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Dimethyl sulfide (DMS) is mostly emitted from ocean surfaces and represents the largest natural source of sulfur for the atmosphere. Once in the atmosphere, DMS forms stable oxidation products such as SO2 and H2SO4, which can subsequently contribute to airborne particle formation and growth. In this study, we update the DMS oxidation mechanism in the chemical transport model GEOS-Chem and describe resulting changes in particle growth as well as the overall global sulfur budget.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Megan M. Bela, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, Pedro Campuzano-Jost, Jason M. St. Clair, James H. Crawford, John D. Crounse, Douglas A. Day, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Jessica B. Gilman, Hongyu Guo, Johnathan W. Hair, Hannah S. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, L. Gregory Huey, Jose L. Jimenez, Joseph M. Katich, Aaron Lamplugh, Young Ro Lee, Jin Liao, Jakob Lindaas, Stuart A. McKeen, Tomas Mikoviny, Benjamin A. Nault, J. Andrew Neuman, John B. Nowak, Demetrios Pagonis, Jeff Peischl, Anne E. Perring, Felix Piel, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Thomas B. Ryerson, Melinda K. Schueneman, Rebecca H. Schwantes, Joshua P. Schwarz, Kanako Sekimoto, Vanessa Selimovic, Taylor Shingler, David J. Tanner, Laura Tomsche, Krystal T. Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn M. Wolfe, Caroline C. Womack, Lu Xu, Katherine Ball, Robert J. Yokelson, and Carsten Warneke
Atmos. Chem. Phys., 24, 929–956, https://doi.org/10.5194/acp-24-929-2024, https://doi.org/10.5194/acp-24-929-2024, 2024
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This study reports emissions of gases and particles from wildfires. These emissions are related to chemical proxies that can be measured by satellite and incorporated into models to improve predictions of wildfire impacts on air quality and climate.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Paul Veers, Carlo L. Bottasso, Lance Manuel, Jonathan Naughton, Lucy Pao, Joshua Paquette, Amy Robertson, Michael Robinson, Shreyas Ananthan, Thanasis Barlas, Alessandro Bianchini, Henrik Bredmose, Sergio González Horcas, Jonathan Keller, Helge Aagaard Madsen, James Manwell, Patrick Moriarty, Stephen Nolet, and Jennifer Rinker
Wind Energ. Sci., 8, 1071–1131, https://doi.org/10.5194/wes-8-1071-2023, https://doi.org/10.5194/wes-8-1071-2023, 2023
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Critical unknowns in the design, manufacturing, and operation of future wind turbine and wind plant systems are articulated, and key research activities are recommended.
Joey C. Y. Lam, Amos P. K. Tai, Jason A. Ducker, and Christopher D. Holmes
Geosci. Model Dev., 16, 2323–2342, https://doi.org/10.5194/gmd-16-2323-2023, https://doi.org/10.5194/gmd-16-2323-2023, 2023
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We developed a new component within an atmospheric chemistry model to better simulate plant ecophysiological processes relevant for ozone air quality. We showed that it reduces simulated biases in plant uptake of ozone in prior models. The new model enables us to explore how future climatic changes affect air quality via affecting plants, examine ozone–vegetation interactions and feedbacks, and evaluate the impacts of changing atmospheric chemistry and climate on vegetation productivity.
John W. Halfacre, Jordan Stewart, Scott C. Herndon, Joseph R. Roscioli, Christoph Dyroff, Tara I. Yacovitch, Michael Flynn, Stephen J. Andrews, Steven S. Brown, Patrick R. Veres, and Pete M. Edwards
Atmos. Meas. Tech., 16, 1407–1429, https://doi.org/10.5194/amt-16-1407-2023, https://doi.org/10.5194/amt-16-1407-2023, 2023
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This study details a new sampling method for the optical detection of hydrogen chloride (HCl). HCl is an important atmospheric reservoir for chlorine atoms, which can affect nitrogen oxide cycling and the lifetimes of volatile organic compounds and ozone. However, HCl has a high affinity for interacting with surfaces, thereby preventing fast, quantitative measurements. The sampling technique in this study minimizes these surface interactions and provides a high-quality measurement of HCl.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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The investigation of the night-time oxidation of the most abundant hydrocarbon, isoprene, in chamber experiments shows the importance of reaction pathways leading to epoxy products, which could enhance particle formation, that have so far not been accounted for. The chemical lifetime of organic nitrates from isoprene is long enough for the majority to be further oxidized the next day by daytime oxidants.
Teles C. Furlani, RenXi Ye, Jordan Stewart, Leigh R. Crilley, Peter M. Edwards, Tara F. Kahan, and Cora J. Young
Atmos. Meas. Tech., 16, 181–193, https://doi.org/10.5194/amt-16-181-2023, https://doi.org/10.5194/amt-16-181-2023, 2023
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This study describes a new technique to measure total gaseous chlorine, which is the sum of gas-phase chlorine-containing chemicals. The method converts any chlorine-containing molecule to hydrogen chloride that can be detected in real time using a cavity ring-down spectrometer. The new method was validated through laboratory experiments, as well as by making measurements of ambient outdoor air and indoor air during cleaning with a chlorine-based cleaner.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Caroline C. Womack, Steven S. Brown, Steven J. Ciciora, Ru-Shan Gao, Richard J. McLaughlin, Michael A. Robinson, Yinon Rudich, and Rebecca A. Washenfelder
Atmos. Meas. Tech., 15, 6643–6652, https://doi.org/10.5194/amt-15-6643-2022, https://doi.org/10.5194/amt-15-6643-2022, 2022
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We present a new miniature instrument to measure nitrogen dioxide (NO2) using cavity-enhanced spectroscopy. NO2 contributes to the formation of pollutants such as ozone and particulate matter, and its concentration can vary widely near sources. We developed this lightweight (3.05 kg) low-power (<35 W) instrument to measure NO2 on uncrewed aircraft vehicles (UAVs) and demonstrate that it has the accuracy and precision needed for atmospheric field measurements.
William F. Swanson, Chris D. Holmes, William R. Simpson, Kaitlyn Confer, Louis Marelle, Jennie L. Thomas, Lyatt Jaeglé, Becky Alexander, Shuting Zhai, Qianjie Chen, Xuan Wang, and Tomás Sherwen
Atmos. Chem. Phys., 22, 14467–14488, https://doi.org/10.5194/acp-22-14467-2022, https://doi.org/10.5194/acp-22-14467-2022, 2022
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Radical bromine molecules are seen at higher concentrations during the Arctic spring. We use the global model GEOS-Chem to test whether snowpack and wind-blown snow sources can explain high bromine concentrations. We run this model for the entire year of 2015 and compare results to observations of bromine from floating platforms on the Arctic Ocean and at Utqiaġvik. We find that the model performs best when both sources are enabled but may overestimate bromine production in summer and fall.
Ilann Bourgeois, Jeff Peischl, J. Andrew Neuman, Steven S. Brown, Hannah M. Allen, Pedro Campuzano-Jost, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Jessica B. Gilman, Georgios I. Gkatzelis, Hongyu Guo, Hannah A. Halliday, Thomas F. Hanisco, Christopher D. Holmes, L. Gregory Huey, Jose L. Jimenez, Aaron D. Lamplugh, Young Ro Lee, Jakob Lindaas, Richard H. Moore, Benjamin A. Nault, John B. Nowak, Demetrios Pagonis, Pamela S. Rickly, Michael A. Robinson, Andrew W. Rollins, Vanessa Selimovic, Jason M. St. Clair, David Tanner, Krystal T. Vasquez, Patrick R. Veres, Carsten Warneke, Paul O. Wennberg, Rebecca A. Washenfelder, Elizabeth B. Wiggins, Caroline C. Womack, Lu Xu, Kyle J. Zarzana, and Thomas B. Ryerson
Atmos. Meas. Tech., 15, 4901–4930, https://doi.org/10.5194/amt-15-4901-2022, https://doi.org/10.5194/amt-15-4901-2022, 2022
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Understanding fire emission impacts on the atmosphere is key to effective air quality management and requires accurate measurements. We present a comparison of airborne measurements of key atmospheric species in ambient air and in fire smoke. We show that most instruments performed within instrument uncertainties. In some cases, further work is needed to fully characterize instrument performance. Comparing independent measurements using different techniques is important to assess their accuracy.
Michael A. Robinson, J. Andrew Neuman, L. Gregory Huey, James M. Roberts, Steven S. Brown, and Patrick R. Veres
Atmos. Meas. Tech., 15, 4295–4305, https://doi.org/10.5194/amt-15-4295-2022, https://doi.org/10.5194/amt-15-4295-2022, 2022
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Iodide chemical ionization mass spectrometry (CIMS) is commonly used in atmospheric chemistry laboratory studies and field campaigns. Deployment of the NOAA iodide CIMS instrument in the summer of 2021 indicated a significant and overlooked temperature dependence of the instrument sensitivity. This work explores which analytes are influenced by this phenomena. Additionally, we recommend controls to reduce this effect for future field deployments.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
Shihan Sun, Amos P. K. Tai, David H. Y. Yung, Anthony Y. H. Wong, Jason A. Ducker, and Christopher D. Holmes
Biogeosciences, 19, 1753–1776, https://doi.org/10.5194/bg-19-1753-2022, https://doi.org/10.5194/bg-19-1753-2022, 2022
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We developed and used a terrestrial biosphere model to compare and evaluate widely used empirical dry deposition schemes with different stomatal approaches and found that using photosynthesis-based stomatal approaches can reduce biases in modeled dry deposition velocities in current chemical transport models. Our study shows systematic errors in current dry deposition schemes and the importance of representing plant ecophysiological processes in models under a changing climate.
Andrew O. Langford, Christoph J. Senff, Raul J. Alvarez II, Ken C. Aikin, Sunil Baidar, Timothy A. Bonin, W. Alan Brewer, Jerome Brioude, Steven S. Brown, Joel D. Burley, Dani J. Caputi, Stephen A. Conley, Patrick D. Cullis, Zachary C. J. Decker, Stéphanie Evan, Guillaume Kirgis, Meiyun Lin, Mariusz Pagowski, Jeff Peischl, Irina Petropavlovskikh, R. Bradley Pierce, Thomas B. Ryerson, Scott P. Sandberg, Chance W. Sterling, Ann M. Weickmann, and Li Zhang
Atmos. Chem. Phys., 22, 1707–1737, https://doi.org/10.5194/acp-22-1707-2022, https://doi.org/10.5194/acp-22-1707-2022, 2022
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The Fires, Asian, and Stratospheric Transport–Las Vegas Ozone Study (FAST-LVOS) combined lidar, aircraft, and in situ measurements with global models to investigate the contributions of stratospheric intrusions, regional and Asian pollution, and wildfires to background ozone in the southwestern US during May and June 2017 and demonstrated that these processes contributed to background ozone levels that exceeded 70 % of the US National Ambient Air Quality Standard during the 6-week campaign.
Jin Liao, Glenn M. Wolfe, Reem A. Hannun, Jason M. St. Clair, Thomas F. Hanisco, Jessica B. Gilman, Aaron Lamplugh, Vanessa Selimovic, Glenn S. Diskin, John B. Nowak, Hannah S. Halliday, Joshua P. DiGangi, Samuel R. Hall, Kirk Ullmann, Christopher D. Holmes, Charles H. Fite, Anxhelo Agastra, Thomas B. Ryerson, Jeff Peischl, Ilann Bourgeois, Carsten Warneke, Matthew M. Coggon, Georgios I. Gkatzelis, Kanako Sekimoto, Alan Fried, Dirk Richter, Petter Weibring, Eric C. Apel, Rebecca S. Hornbrook, Steven S. Brown, Caroline C. Womack, Michael A. Robinson, Rebecca A. Washenfelder, Patrick R. Veres, and J. Andrew Neuman
Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, https://doi.org/10.5194/acp-21-18319-2021, 2021
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Formaldehyde (HCHO) is an important oxidant precursor and affects the formation of O3 and other secondary pollutants in wildfire plumes. We disentangle the processes controlling HCHO evolution from wildfire plumes sampled by NASA DC-8 during FIREX-AQ. We find that OH abundance rather than normalized OH reactivity is the main driver of fire-to-fire variability in HCHO secondary production and estimate an effective HCHO yield per volatile organic compound molecule oxidized in wildfire plumes.
Nicole Jacobs, William R. Simpson, Kelly A. Graham, Christopher Holmes, Frank Hase, Thomas Blumenstock, Qiansi Tu, Matthias Frey, Manvendra K. Dubey, Harrison A. Parker, Debra Wunch, Rigel Kivi, Pauli Heikkinen, Justus Notholt, Christof Petri, and Thorsten Warneke
Atmos. Chem. Phys., 21, 16661–16687, https://doi.org/10.5194/acp-21-16661-2021, https://doi.org/10.5194/acp-21-16661-2021, 2021
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Spatial patterns of carbon dioxide seasonal cycle amplitude and summer drawdown timing derived from the OCO-2 satellite over northern high latitudes agree well with corresponding estimates from two models. The Asian boreal forest is anomalous with the largest amplitude and earliest seasonal drawdown. Modeled land contact tracers suggest that accumulated CO2 exchanges during atmospheric transport play a major role in shaping carbon dioxide seasonality in northern high-latitude regions.
Zachary C. J. Decker, Michael A. Robinson, Kelley C. Barsanti, Ilann Bourgeois, Matthew M. Coggon, Joshua P. DiGangi, Glenn S. Diskin, Frank M. Flocke, Alessandro Franchin, Carley D. Fredrickson, Georgios I. Gkatzelis, Samuel R. Hall, Hannah Halliday, Christopher D. Holmes, L. Gregory Huey, Young Ro Lee, Jakob Lindaas, Ann M. Middlebrook, Denise D. Montzka, Richard Moore, J. Andrew Neuman, John B. Nowak, Brett B. Palm, Jeff Peischl, Felix Piel, Pamela S. Rickly, Andrew W. Rollins, Thomas B. Ryerson, Rebecca H. Schwantes, Kanako Sekimoto, Lee Thornhill, Joel A. Thornton, Geoffrey S. Tyndall, Kirk Ullmann, Paul Van Rooy, Patrick R. Veres, Carsten Warneke, Rebecca A. Washenfelder, Andrew J. Weinheimer, Elizabeth Wiggins, Edward Winstead, Armin Wisthaler, Caroline Womack, and Steven S. Brown
Atmos. Chem. Phys., 21, 16293–16317, https://doi.org/10.5194/acp-21-16293-2021, https://doi.org/10.5194/acp-21-16293-2021, 2021
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To understand air quality impacts from wildfires, we need an accurate picture of how wildfire smoke changes chemically both day and night as sunlight changes the chemistry of smoke. We present a chemical analysis of wildfire smoke as it changes from midday through the night. We use aircraft observations from the FIREX-AQ field campaign with a chemical box model. We find that even under sunlight typical
nighttimechemistry thrives and controls the fate of key smoke plume chemical processes.
Stefano Galmarini, Paul Makar, Olivia E. Clifton, Christian Hogrefe, Jesse O. Bash, Roberto Bellasio, Roberto Bianconi, Johannes Bieser, Tim Butler, Jason Ducker, Johannes Flemming, Alma Hodzic, Christopher D. Holmes, Ioannis Kioutsioukis, Richard Kranenburg, Aurelia Lupascu, Juan Luis Perez-Camanyo, Jonathan Pleim, Young-Hee Ryu, Roberto San Jose, Donna Schwede, Sam Silva, and Ralf Wolke
Atmos. Chem. Phys., 21, 15663–15697, https://doi.org/10.5194/acp-21-15663-2021, https://doi.org/10.5194/acp-21-15663-2021, 2021
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This technical note presents the research protocols for phase 4 of the Air Quality Model Evaluation International Initiative (AQMEII4). This initiative has three goals: (i) to define the state of wet and dry deposition in regional models, (ii) to evaluate how dry deposition influences air concentration and flux predictions, and (iii) to identify the causes for prediction differences. The evaluation compares LULC-specific dry deposition and effective conductances and fluxes.
Quanfu He, Zheng Fang, Ofir Shoshanim, Steven S. Brown, and Yinon Rudich
Atmos. Chem. Phys., 21, 14927–14940, https://doi.org/10.5194/acp-21-14927-2021, https://doi.org/10.5194/acp-21-14927-2021, 2021
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Rayleigh scattering and absorption cross sections for CO2, N2O, SF6, O2, and CH4 were measured between 307 and 725 nm. New dispersion relations for N2O, SF6, and CH4 in the UV–vis range were derived. This study provides refractive index dispersion relations, scattering, and absorption cross sections which are highly needed for accurate instrument calibration and for improved accuracy of Rayleigh scattering parameterizations for major greenhouse gases in Earth's atmosphere.
Linghan Zeng, Amy P. Sullivan, Rebecca A. Washenfelder, Jack Dibb, Eric Scheuer, Teresa L. Campos, Joseph M. Katich, Ezra Levin, Michael A. Robinson, and Rodney J. Weber
Atmos. Meas. Tech., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, https://doi.org/10.5194/amt-14-6357-2021, 2021
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Three online systems for measuring water-soluble brown carbon are compared. A mist chamber and two different particle-into-liquid samplers were deployed on separate research aircraft targeting wildfires and followed a similar detection method using a long-path liquid waveguide with a spectrometer to measure the light absorption from 300 to 700 nm. Detection limits, signal hysteresis and other sampling issues are compared, and further improvements of these liquid-based systems are provided.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 13537–13551, https://doi.org/10.5194/acp-21-13537-2021, https://doi.org/10.5194/acp-21-13537-2021, 2021
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Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources that are formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report on their atmospheric degradation through reaction with NO3, which is useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Teles C. Furlani, Patrick R. Veres, Kathryn E. R. Dawe, J. Andrew Neuman, Steven S. Brown, Trevor C. VandenBoer, and Cora J. Young
Atmos. Meas. Tech., 14, 5859–5871, https://doi.org/10.5194/amt-14-5859-2021, https://doi.org/10.5194/amt-14-5859-2021, 2021
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This study characterized and validated a commercial spectroscopic instrument for the measurement of hydrogen chloride (HCl) in the atmosphere. Near the Earth’s surface, HCl acts as the dominant reservoir for other chlorine-containing reactive chemicals that play an important role in atmospheric chemistry. The properties of HCl make it challenging to measure. This instrument can overcome many of these challenges, enabling reliable HCl measurements.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Caroline C. Womack, Katherine M. Manfred, Nicholas L. Wagner, Gabriela Adler, Alessandro Franchin, Kara D. Lamb, Ann M. Middlebrook, Joshua P. Schwarz, Charles A. Brock, Steven S. Brown, and Rebecca A. Washenfelder
Atmos. Chem. Phys., 21, 7235–7252, https://doi.org/10.5194/acp-21-7235-2021, https://doi.org/10.5194/acp-21-7235-2021, 2021
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Microscopic particles interact with sunlight and affect the earth's climate in ways that are not fully understood. Aerosols from wildfire smoke present particular challenges due to their complexity in shape and composition. We demonstrate that we can experimentally measure aerosol optical properties for many types of smoke particles, using measurements of smoke from controlled burns, but that the method does not work well for smoke with high soot content.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
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Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Aikaterini Bougiatioti, Athanasios Nenes, Jack J. Lin, Charles A. Brock, Joost A. de Gouw, Jin Liao, Ann M. Middlebrook, and André Welti
Atmos. Chem. Phys., 20, 12163–12176, https://doi.org/10.5194/acp-20-12163-2020, https://doi.org/10.5194/acp-20-12163-2020, 2020
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The number concentration of droplets in clouds in the summertime in the southeastern United States is influenced by aerosol variations but limited by the strong competition for supersaturated water vapor. Concurrent variations in vertical velocity magnify the response of cloud droplet number to aerosol increases by up to a factor of 5. Omitting the covariance of vertical velocity with aerosol number may therefore bias estimates of the cloud albedo effect from aerosols.
Li Zhang, Meiyun Lin, Andrew O. Langford, Larry W. Horowitz, Christoph J. Senff, Elizabeth Klovenski, Yuxuan Wang, Raul J. Alvarez II, Irina Petropavlovskikh, Patrick Cullis, Chance W. Sterling, Jeff Peischl, Thomas B. Ryerson, Steven S. Brown, Zachary C. J. Decker, Guillaume Kirgis, and Stephen Conley
Atmos. Chem. Phys., 20, 10379–10400, https://doi.org/10.5194/acp-20-10379-2020, https://doi.org/10.5194/acp-20-10379-2020, 2020
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Measuring and quantifying the sources of elevated springtime ozone in the southwestern US is challenging but relevant to the implications for control policy. Here we use intensive field measurements and two global models to study ozone sources in the region. We find that ozone from the stratosphere, wildfires, and Asia is an important source of high-ozone events in the region. Our analysis also helps understand the uncertainties in ozone simulations with individual models.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Cited articles
Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, https://doi.org/10.5194/acp-6-3131-2006, 2006.
Bateman, A. P., Walser, M. L., Desyaterik, Y., Laskin, J., Laskin, A., and Nizkorodov, S. A.: The effect of solvent on the analysis of secondary organic aerosol using electrospray ionization mass spectrometry, Environ. Sci. Technol., 42, 7341–7346, https://doi.org/10.1021/es801226w, 2008.
Bluvshtein, N., Lin, P., Flores, M., Segev, L., Mazar, Y., Tas, E., Snider, G., Weagle, C., Brown, S., Laskin, A., and Rudich, Y.: Broadband optical properties of biomass burning aerosol and identification of brown carbon chromophores, J. Geophys. Res.-Atmos., 122, 5441–5456, https://doi.org/10.1002/2016JD026230, 2017.
Bond, T. C., Streets, D. G., Yarber, K. F., Nelson, S. M., Woo, J.-H., and Klimont, Z.: A technology-based global inventory of black and organic carbon emissions from combustion, J. Geophys. Res.-Atmos., 109, D14203, https://doi.org/10.1029/2003JD003697, 2004.
Boucher, O., Randall, D., Artaxo, P., Bretherton, C., Feingold, G., Forster, P., Kerminen, V. M., Kondo, Y., Liao, H., Lohmann, U., Rasch, P., Satheesh, S. K., Sherwood, S., Stevens, B., and Zhang, X. Y.: Clouds and Aerosols, in: Climate Change 2013: The Physical Science Basis. Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, Cambridge University Press, New York, NY, https://doi.org/10.1017/CBO9781107415324.016, 2013.
Buis, A.: The climate connections of a record fire year in the U.S. West – climate change vital Signs of the planet, https://climate.nasa.gov/blog/3066/the-climate-connections-of-a-record-fire-year-in-the-us-west/ (last access: 10 October 2023), 2021.
Chen, K., Raeofy, N., Lum, M., Mayorga, R., Woods, M., Bahreini, R., Zhang, H., and Lin, Y.-H.: Solvent effects on chemical composition and optical properties of extracted secondary brown carbon constituents, Aerosol Sci. Tech., 56, 917–930, https://doi.org/10.1080/02786826.2022.2100734, 2022.
Crosson, E. R.: A cavity ring-down analyzer for measuring atmospheric levels of methane, carbon dioxide, and water vapor, Appl. Phys. B, 92, 403–408, https://doi.org/10.1007/s00340-008-3135-y, 2008.
Dalton, A. B., Le, S. M., Karimova, N. V., Gerber, R. B., and Nizkorodov, S. A.: Influence of solvent on the electronic structure and the photochemistry of nitrophenols, Environ. Sci.-Atmos., 3, 257–267, https://doi.org/10.1039/D2EA00144F, 2023.
De Haan, D. O., Tapavicza, E., Riva, M., Cui, T., Surratt, J. D., Smith, A. C., Jordan, M.-C., Nilakantan, S., Almodovar, M., Stewart, T. N., de Loera, A., De Haan, A. C., Cazaunau, M., Gratien, A., Pangui, E., and Doussin, J.-F.: Nitrogen-containing, light-absorbing oligomers produced in aerosol particles exposed to methylglyoxal, photolysis, and cloud cycling, Environ. Sci. Technol., 52, 4061–4071, https://doi.org/10.1021/acs.est.7b06105, 2018.
Di Lorenzo, R. A. and Young, C. J.: Size separation method for absorption characterization in brown carbon: Application to an aged biomass burning sample, Geophys. Res. Lett., 43, 458–465, https://doi.org/10.1002/2015GL066954, 2016.
Di Lorenzo, R. A., Washenfelder, R. A., Attwood, A. R., Guo, H., Xu, L., Ng, N. L., Weber, R. J., Baumann, K., Edgerton, E., and Young, C. J.: Molecular-size-separated brown carbon absorption for biomass-burning aerosol at multiple field sites, Environ. Sci. Technol., 51, 3128–3137, https://doi.org/10.1021/acs.est.6b06160, 2017.
Di Lorenzo, R. A., Place, B. K., VandenBoer, T. C., and Young, C. J.: Composition of Size-Resolved Aged Boreal Fire Aerosols: Brown Carbon, Biomass Burning Tracers, and Reduced Nitrogen, ACS Earth and Space Chemistry, 2, 278–285, https://doi.org/10.1021/acsearthspacechem.7b00137, 2018.
Feng, Y., Ramanathan, V., and Kotamarthi, V. R.: Brown carbon: a significant atmospheric absorber of solar radiation?, Atmos. Chem. Phys., 13, 8607–8621, https://doi.org/10.5194/acp-13-8607-2013, 2013.
Finewax, Z., de Gouw, J. A., and Ziemann, P. J.: Identification and quantification of 4-nitrocatechol formed from OH and NO3 radical-initiated reactions of catechol in air in the presence of NOx: implications for secondary organic aerosol formation from biomass burning, Environ. Sci. Technol., 52, 1981–1989, https://doi.org/10.1021/acs.est.7b05864, 2018.
FIREX-AQ Platform: NOAA-CHEM Twin Otter Data Download, https://csl.noaa.gov/groups/csl7/measurements/2019firex-aq/TwinOtter/DataDownload/, last access: 18 December 2023.
Fleming, L. T., Lin, P., Roberts, J. M., Selimovic, V., Yokelson, R., Laskin, J., Laskin, A., and Nizkorodov, S. A.: Molecular composition and photochemical lifetimes of brown carbon chromophores in biomass burning organic aerosol, Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, 2020.
Forrister, H., Liu, J., Scheuer, E., Dibb, J., Ziemba, L., Thornhill, K. L., Anderson, B., Diskin, G., Perring, A. E., Schwarz, J. P., Campuzano-Jost, P., Day, D. A., Palm, B. B., Jimenez, J. L., Nenes, A., and Weber, R. J.: Evolution of brown carbon in wildfire plumes, Geophys. Res. Lett., 42, 4623–4630, https://doi.org/10.1002/2015GL063897, 2015.
Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R. , Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in atmospheric constituents and in radiative forcing, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L., Cambridge University Press: Cambridge, United Kingdom and New York, NY, 129-−243, ISBN: 9780521880091, 2007.
Gorkowski, K., Benedict, K. B., Carrico, C. M., and Dubey, M. K.: Complexities in Modeling Organic Aerosol Light Absorption, J. Phys. Chem. A, 126, 4827–4833, https://doi.org/10.1021/acs.jpca.2c02236, 2022.
Harrison, M. A. J., Barra, S., Borghesi, D., Vione, D., Arsene, C., and Olariu, R. I.: Nitrated phenols in the atmosphere: a review, Atmos. Environ., 39, 231–248, https://doi.org/10.1016/j.atmosenv.2004.09.044, 2005.
Hems, R. F., Schnitzler, E. G., Liu-Kang, C., Cappa, C. D., and Abbatt, J. P. D.: Aging of atmospheric brown carbon aerosol, ACS Earth and Space Chemistry, 5, 722–748, https://doi.org/10.1021/acsearthspacechem.0c00346, 2021.
Hettiyadura, A. P. S., Garcia, V., Li, C., West, C. P., Tomlin, J., He, Q., Rudich, Y., and Laskin, A.: Chemical composition and molecular-specific optical properties of atmospheric brown carbon associated with biomass burning, Environ. Sci. Technol., 55, 2511–2521, https://doi.org/10.1021/acs.est.0c05883, 2021.
Hinrichs, R. Z., Buczek, P., and Trivedi, J. J.: Solar absorption by aerosol-bound nitrophenols compared to aqueous and gaseous nitrophenols, Environ. Sci. Technol., 50, 5661–5667, https://doi.org/10.1021/acs.est.6b00302, 2016.
Hong, P., Koza, S., and Bouvier, E. S. P.: a review size-exclusion chromatography for the analysis of protein biotherapeutics and their aggregates, J. Liq. Chromatogr. R. T., 35, 2923–2950, https://doi.org/10.1080/10826076.2012.743724, 2012.
Ji, Y., Shi, Q., Ma, X., Gao, L., Wang, J., Li, Y., Gao, Y., Li, G., Zhang, R., and An, T.: Elucidating the critical oligomeric steps in secondary organic aerosol and brown carbon formation, Atmos. Chem. Phys., 22, 7259–7271, https://doi.org/10.5194/acp-22-7259-2022, 2022.
Karion, A., Sweeney, C., Wolter, S., Newberger, T., Chen, H., Andrews, A., Kofler, J., Neff, D., and Tans, P.: Long-term greenhouse gas measurements from aircraft, Atmos. Meas. Tech., 6, 511–526, https://doi.org/10.5194/amt-6-511-2013, 2013.
Laskin, A., Laskin, J., and Nizkorodov, S. A.: Chemistry of Atmospheric Brown Carbon, Chem. Rev., 115, 4335–4382, https://doi.org/10.1021/cr5006167, 2015.
Liao, J., Wolfe, G. M., Hannun, R. A., St. Clair, J. M., Hanisco, T. F., Gilman, J. B., Lamplugh, A., Selimovic, V., Diskin, G. S., Nowak, J. B., Halliday, H. S., DiGangi, J. P., Hall, S. R., Ullmann, K., Holmes, C. D., Fite, C. H., Agastra, A., Ryerson, T. B., Peischl, J., Bourgeois, I., Warneke, C., Coggon, M. M., Gkatzelis, G. I., Sekimoto, K., Fried, A., Richter, D., Weibring, P., Apel, E. C., Hornbrook, R. S., Brown, S. S., Womack, C. C., Robinson, M. A., Washenfelder, R. A., Veres, P. R., and Neuman, J. A.: Formaldehyde evolution in US wildfire plumes during the Fire Influence on Regional to Global Environments and Air Quality experiment (FIREX-AQ), Atmos. Chem. Phys., 21, 18319–18331, https://doi.org/10.5194/acp-21-18319-2021, 2021.
Lignell, H., Hinks, M. L., and Nizkorodov, S. A.: Exploring matrix effects on photochemistry of organic aerosols, P. Natl. Acad. Sci. USA, 111, 13780–13785, https://doi.org/10.1073/pnas.1322106111, 2014.
Lin, P., Bluvshtein, N., Rudich, Y., Nizkorodov, S. A., Laskin, J., and Laskin, A.: Molecular chemistry of atmospheric brown carbon inferred from a nationwide biomass burning event, Environ. Sci. Technol., 51, 11561–11570, https://doi.org/10.1021/acs.est.7b02276, 2017.
Liu, J., Lin, P., Laskin, A., Laskin, J., Kathmann, S. M., Wise, M., Caylor, R., Imholt, F., Selimovic, V., and Shilling, J. E.: Optical properties and aging of light-absorbing secondary organic aerosol, Atmos. Chem. Phys., 16, 12815–12827, https://doi.org/10.5194/acp-16-12815-2016, 2016.
Lyu, M., Thompson, D. K., Zhang, N., Cuss, C. W., Young, C. J., and Styler, S. A.: Unraveling the complexity of atmospheric brown carbon produced by smoldering boreal peat using size-exclusion chromatography with selective mobile phases, Environ. Sci.-Atmos., 1, 241–252, https://doi.org/10.1039/D1EA00011J, 2021.
Marlon, J. R., Bartlein, P. J., Gavin, D. G., Long, C. J., Anderson, R. S., Briles, C. E., Brown, K. J., Colombaroli, D., Hallett, D. J., Power, M. J., Scharf, E. A., and Walsh, M. K.: Long-term perspective on wildfires in the western USA, P. Natl. Acad. Sci. USA, 109, E535–E543, https://doi.org/10.1073/pnas.1112839109, 2012.
Marrero-Ortiz, W., Hu, M., Du, Z., Ji, Y., Wang, Y., Guo, S., Lin, Y., Gomez-Hermandez, M., Peng, J., Li, Y., Secrest, J., Zamora, M. L., Wang, Y., An, T., and Zhang, R.: Formation and optical properties of brown carbon from small α-dicarbonyls and amines, Environ. Sci. Technol., 53, 117–126, https://doi.org/10.1021/acs.est.8b03995, 2019.
Mo, Y., Li, J., Liu, J., Zhong, G., Cheng, Z., Tian, C., Chen, Y., and Zhang, G.: The influence of solvent and pH on determination of the light absorption properties of water-soluble brown carbon, Atmos. Environ., 161, 90–98, https://doi.org/10.1016/j.atmosenv.2017.04.037, 2017.
Parks, S. A. and Abatzoglou, J. T.: Warmer and Drier Fire Seasons Contribute to Increases in Area Burned at High Severity in Western US Forests From 1985 to 2017, Geophys. Res. Lett., 47, e2020GL089858, https://doi.org/10.1029/2020GL089858, 2020.
Phillips, S. M., Bellcross, A. D., and Smith, G. D.: Light Absorption by Brown Carbon in the Southeastern United States is pH-dependent, Environ. Sci. Technol., 51, 6782–6790, https://doi.org/10.1021/acs.est.7b01116, 2017.
Powelson, M. H., Espelien, B. M., Hawkins, L. N., Galloway, M. M., and De Haan, D. O.: Brown Carbon Formation by Aqueous-Phase Carbonyl Compound Reactions with Amines and Ammonium Sulfate, Environ. Sci. Technol., 48, 985–993, https://doi.org/10.1021/es4038325, 2014.
Ramanathan, V. and Carmichael, G.: Global and regional climate changes due to black carbon, Nat. Geosci., 1, 221–227, https://doi.org/10.1038/ngeo156, 2008.
Resch, J., Wolfer, K., Barth, A., and Kalberer, M.: Effects of storage conditions on the molecular-level composition of organic aerosol particles, Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, 2023.
Seinfeld, J. H. and Pankow, J. F.: Organic Atmospheric Particulate Material, Annu. Rev. Phys. Chem., 54, 121–140, https://doi.org/10.1146/annurev.physchem.54.011002.103756, 2003.
Simoneit, B. R. T.: Biomass burning – a review of organic tracers for smoke from incomplete combustion, Appl. Geochem., 17, 129–162, https://doi.org/10.1016/S0883-2927(01)00061-0, 2002.
Smith, J. D., Sio, V., Yu, L., Zhang, Q., and Anastasio, C.: Secondary organic aerosol production from aqueous reactions of atmospheric phenols with an organic triplet excited state, Environ. Sci. Technol., 48, 1049–1057, https://doi.org/10.1021/es4045715, 2014.
Sullivan, A. P., Pokhrel, R. P., Shen, Y., Murphy, S. M., Toohey, D. W., Campos, T., Lindaas, J., Fischer, E. V., and Collett Jr., J. L.: Examination of brown carbon absorption from wildfires in the western US during the WE-CAN study, Atmos. Chem. Phys., 22, 13389–13406, https://doi.org/10.5194/acp-22-13389-2022, 2022.
Turpin, B. J., Cary, R. A., and Huntzicker, J. J.: An in situ, time-resolved analyzer for aerosol organic and elemental carbon, Aerosol Sci. Tech., 12, 161–171, https://doi.org/10.1080/02786829008959336, 1990.
van der Werf, G. R., Randerson, J. T., Giglio, L., Collatz, G. J., Mu, M., Kasibhatla, P. S., Morton, D. C., DeFries, R. S., Jin, Y., and van Leeuwen, T. T.: Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997–2009), Atmos. Chem. Phys., 10, 11707–11735, https://doi.org/10.5194/acp-10-11707-2010, 2010.
Walser, M. L., Desyaterik, Y., Laskin, J., Laskin, A., and Nizkorodov, S. A.: High-resolution mass spectrometric analysis of secondary organic aerosol produced by ozonation of limonene, Phys. Chem. Chem. Phys., 10, 1009–1022, https://doi.org/10.1039/B712620D, 2008.
Warneke, C., Schwarz, J. P., Dibb, J., Kalashnikova, O., Frost, G., Al-Saad, J., Brown, S. S., Brewer, Wm. A., Soja, A., Seidel, F. C., Washenfelder, R. A., Wiggins, E. B., Moore, R. H., Anderson, B. E., Jordan, C., Yacovitch, T. I., Herndon, S. C., Liu, S., Kuwayama, T., Jaffe, D., Johnston, N., Selimovic, V., Yokelson, R., Giles, D. M., Holben, B. N., Goloub, P., Popovici, I., Trainer, M., Kumar, A., Pierce, R. B., Fahey, D., Roberts, J., Gargulinski, E. M., Peterson, D. A., Ye, X., Thapa, L. H., Saide, P. E., Fite, C. H., Holmes, C. D., Wang, S., Coggon, M. M., Decker, Z. C. J., Stockwell, C. E., Xu, L., Gkatzelis, G., Aikin, K., Lefer, B., Kaspari, J., Griffin, D., Zeng, L., Weber, R., Hastings, M., Chai, J., Wolfe, G. M., Hanisco, T. F., Liao, J., Campuzano Jost, P., Guo, H., Jimenez, J. L., Crawford, J., and the FIREX-AQ Science Team: Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ), J. Geophys. Res.-Atmos., 128, e2022JD037758, https://doi.org/10.1029/2022JD037758, 2023.
Washenfelder, R., Attwood, A., Brock, C., Guo, H., Xu, L., Weber, R., Ng, N., Allen, H., Ayres, B., Baumann, K., Cohen, R., Draper, D., Duffey, K., Edgerton, E., Fry, J., Hu, W., Jimenez, J., Palm, B., Romer, P., and Brown, S.: Biomass burning dominates brown carbon absorption in the rural southeastern United States, Geophys. Res. Lett., 42, 653–664, https://doi.org/10.1002/2014GL062444, 2015.
Washenfelder, R. A., Azzarello, L., Ball, K., Brown, S. S., Decker, Z. C. J., Franchin, A., Fredrickson, C. D., Hayden, K., Holmes, C. D., Middlebrook, A. M., Palm, B. B., Pierce, R. B., Price, D. J., Roberts, J. M., Robinson, M. A., Thornton, J. A., Womack, C. C., and Young, C. J.: Complexity in the evolution, composition, and spectroscopy of brown carbon in aircraft measurements of wildfire plumes, Geophys. Res. Lett., 49, e2022GL098951, https://doi.org/10.1029/2022GL098951, 2022.
Weber, R. J., Orsini, D., Daun, Y., Lee, Y.-N., Klotz, P. J., and Brechtel, F.: A particle-into-liquid collector for rapid measurement of aerosol bulk chemical composition, Aerosol Sci. Tech., 35, 718–727, https://doi.org/10.1080/02786820152546761, 2001.
Wong, J. P. S., Nenes, A., and Weber, R. J.: Changes in light absorptivity of molecular weight separated brown carbon due to photolytic aging, Environ. Sci. Technol., 51, 8414–8421, https://doi.org/10.1021/acs.est.7b01739, 2017.
Wong, J. P. S., Tsagkaraki, M., Tsiodra, I., Mihalopoulos, N., Violaki, K., Kanakidou, M., Sciare, J., Nenes, A., and Weber, R. J.: Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning, Atmos. Chem. Phys., 19, 7319–7334, https://doi.org/10.5194/acp-19-7319-2019, 2019.
Xie, M., Chen, X., Hays, M. D., Lewandowski, M., Offenberg, J., Kleindienst, T. E., and Holder, A. L.: Light Absorption of secondary organic aerosol: composition and contribution of nitroaromatic compounds, Environ. Sci. Technol., 51, 11607–11616, https://doi.org/10.1021/acs.est.7b03263, 2017.
Xie, M., Chen, X., Hays, M. D., and Holder, A. L.: Composition and light absorption of N-containing aromatic compounds in organic aerosols from laboratory biomass burning, Atmos. Chem. Phys., 19, 2899–2915, https://doi.org/10.5194/acp-19-2899-2019, 2019.
Yang, L., Huang, R.-J., Shen, J., Wang, T., Gong, Y., Yuan, W., Liu, Y., Huang, H., You, Q., Huang, D. D., and Huang, C.: New Insights into the Brown Carbon Chromophores and Formation Pathways for Aqueous Reactions of α-Dicarbonyls with Amines and Ammonium, Environ. Sci. Technol., 57, 12351–12361, https://doi.org/10.1021/acs.est.3c04133, 2023.
Zeng, L., Zhang, A., Wang, Y., Wagner, N. L., Katich, J. M., Schwarz, J. P., Schill, G. P., Brock, C., Froyd, K. D., Murphy, D. M., Williamson, C. J., Kupc, A., Scheuer, E., Dibb, J., and Weber, R. J.: Global Measurements of Brown Carbon and Estimated Direct Radiative Effects, Geophys. Res. Lett., 47, e2020GL088747, https://doi.org/10.1029/2020GL088747, 2020.
Zeng, L., Sullivan, A. P., Washenfelder, R. A., Dibb, J., Scheuer, E., Campos, T. L., Katich, J. M., Levin, E., Robinson, M. A., and Weber, R. J.: Assessment of online water-soluble brown carbon measuring systems for aircraft sampling, Atmos. Meas. Tech., 14, 6357–6378, https://doi.org/10.5194/amt-14-6357-2021, 2021.
Zeng, L., Dibb, J., Scheuer, E., Katich, J. M., Schwarz, J. P., Bourgeois, I., Peischl, J., Ryerson, T., Warneke, C., Perring, A. E., Diskin, G. S., DiGangi, J. P., Nowak, J. B., Moore, R. H., Wiggins, E. B., Pagonis, D., Guo, H., Campuzano-Jost, P., Jimenez, J. L., Xu, L., and Weber, R. J.: Characteristics and evolution of brown carbon in western United States wildfires, Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, 2022.
Zeng, Y., Shen, Z., Takahama, S., Zhang, L., Zhang, T., Lei, Y., Zhang, Q., Xu, H., Ning, Y., Huang, Y., Cao, J., and Rudolf, H.: Molecular absorption and evolution mechanisms of PM2.5 brown carbon revealed by electrospray ionization fourier transform–ion cyclotron resonance mass spectrometry during a severe winter pollution episode in Xi'an, China, Geophys. Res. Lett., 47, e2020GL087977, https://doi.org/10.1029/2020GL087977, 2020.
Zhang, Y., Forrister, H., Liu, J., Dibb, J., Anderson, B., Schwarz, J. P., Perring, A. E., Jimenez, J. L., Campuzano-Jost, P., Wang, Y., Nenes, A., and Weber, R. J.: Top-of-atmosphere radiative forcing affected by brown carbon in the upper troposphere, Nat. Geosci., 10, 486–489, https://doi.org/10.1038/ngeo2960, 2017.
Zhao, R., Kenseth, C. M., Huang, Y., Dalleska, N. F., Kuang, X. M., Chen, J., Paulson, S. E., and Seinfeld, J. H.: Rapid Aqueous-Phase Hydrolysis of Ester Hydroperoxides Arising from Criegee Intermediates and Organic Acids, J. Phys. Chem. A, 122, 5190–5201, https://doi.org/10.1021/acs.jpca.8b02195, 2018.
Zheng, D., Yuan, X.-A., Ma, H., Li, X., Wang, X., Liu, Z., and Ma, J.: Unexpected solvent effects on the UV/Vis absorption spectra of o-cresol in toluene and benzene: in contrast with non-aromatic solvents, Roy. Soc. Open Sci., 5, 171928, https://doi.org/10.1098/rsos.171928, 2018.
Short summary
We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on an aircraft during FIREX-AQ. The smoke plumes were aged 0 to 5 h, where absorption was dominated by small molecular weight molecules, brown carbon absorption downwind did not consistently decrease, and the measurements differed from online absorption measurements of the same samples. We show how differences between online and offline absorption could be related to different measurement conditions.
We present a molecular size-resolved offline analysis of water-soluble brown carbon collected on...
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