Articles | Volume 17, issue 5
https://doi.org/10.5194/acp-17-3401-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-3401-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
09 Mar 2017
Research article |
| 09 Mar 2017
Bromine atom production and chain propagation during springtime Arctic ozone depletion events in Barrow, Alaska
Chelsea R. Thompson
CORRESPONDING AUTHOR
Department of Chemistry, Purdue University, West Lafayette, IN, USA
now at: Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
now at: Chemical Sciences Division, NOAA Earth System Research
Laboratory, Boulder, CO, USA
Paul B. Shepson
Department of Chemistry, Purdue University, West Lafayette, IN, USA
Department of Earth and Atmospheric Sciences and Purdue Climate Change
Research Center, Purdue University, West Lafayette, IN, USA
Jin Liao
School of Earth and Atmospheric Sciences, Georgia Institute of
Technology, Atlanta, GA, USA
now at: Atmospheric Chemistry and Dynamics Laboratory, NASA Goddard
Space Flight Center, Greenbelt, MD, USA
now at: Universities Space Research Association, Columbia, MD, USA
L. Greg Huey
School of Earth and Atmospheric Sciences, Georgia Institute of
Technology, Atlanta, GA, USA
Chris Cantrell
National Center for Atmospheric Research, Boulder, CO, USA
now at: Department of Atmospheric and Ocean Sciences, University of
Colorado Boulder, Boulder, CO, USA
Frank Flocke
National Center for Atmospheric Research, Boulder, CO, USA
John Orlando
National Center for Atmospheric Research, Boulder, CO, USA
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The first comprehensive dataset of tropospheric ozone over oceans/polar regions is presented, including 77 ship/buoy and 48 aircraft campaign observations (1977–2022, 0–5000 m altitude), supplemented by ozonesonde and surface data. Air masses isolated from land for 72+ hours are systematically selected as essentially oceanic. Among the 11 global regions, they show daytime decreases of 10–16% in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
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
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This study showed that the springtime O3 depletion plays a critical role in driving the surface O3 seasonal cycle in Central Arctic. The O3 depletion events, while occurring most notably within the lowest few hundred metres above the Arctic Ocean, can induce a 5–7 % of loss in the pan-Arctic tropospheric O3 burden during springtime. The study also found an enhancement in O3 and NOy (mostly PAN) concentrations in the Arctic due to northern boreal wildfires, particularly at altitudes.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
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.
Jin Liao, Glenn M. Wolfe, Alexander E. Kotsakis, Julie M. Nicely, Jason M. St. Clair, Thomas F. Hanisco, Gonzalo González Abad, Caroline R. Nowlan, Zolal Ayazpour, Isabelle De Smedt, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Meas. Tech., 18, 1–16, https://doi.org/10.5194/amt-18-1-2025, https://doi.org/10.5194/amt-18-1-2025, 2025
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Validation of satellite HCHO over the remote marine regions is relatively low, and modeled HCHO in these regions is usually added as a global satellite HCHO background. This paper intercompares three satellite HCHO retrievals and validates them against in situ observations from the NASA ATom mission. All retrievals are correlated with ATom-integrated columns over remote oceans, with OMI SAO (v004) showing the best agreement. A persistent low bias is found in all retrievals at high latitudes.
Sachiko Okamoto, Juan Cuesta, Gaëlle Dufour, Maxmim Eremenko, Kazuyuki Miyazaki, Cathy Boonne, Hiroshi Tanimoto, Jeff Peischl, and Chelsea Thompson
EGUsphere, https://doi.org/10.5194/egusphere-2024-3758, https://doi.org/10.5194/egusphere-2024-3758, 2024
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We analyse the distribution of tropospheric ozone over the South and Tropical Atlantic during February 2017 using a multispectral satellite approach called IASI+GOME2, three chemistry reanalysis products and in situ airborne measurements. It reveals that a significant overestimation of three chemistry reanalysis products of lowermost troposphere ozone over the Atlantic in the Northern Hemisphere due to the overestimations of ozone precursors from anthropogenic sources from North America.
Wendell W. Walters, Masayuki Takeuchi, Danielle E. Blum, Gamze Eris, David Tanner, Weiqi Xu, Jean Rivera-Rios, Fobang Liu, Tianchang Xu, Greg Huey, Justin B. Min, Rodney Weber, Nga L. Ng, and Meredith G. Hastings
EGUsphere, https://doi.org/10.5194/egusphere-2024-3860, https://doi.org/10.5194/egusphere-2024-3860, 2024
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We studied how chemicals released from plants and pollution interact in the atmosphere, affecting air quality and climate. By combining laboratory experiments and chemistry models, we tracked unique chemical fingerprints to understand how nitrogen compounds transform to form particles in the air. Our findings help explain the role of these reactions in pollution and provide tools to improve predictions for cleaner air and better climate policies.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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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.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
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.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Audrey Gaudel, Ilann Bourgeois, Meng Li, Kai-Lan Chang, Jerald Ziemke, Bastien Sauvage, Ryan M. Stauffer, Anne M. Thompson, Debra E. Kollonige, Nadia Smith, Daan Hubert, Arno Keppens, Juan Cuesta, Klaus-Peter Heue, Pepijn Veefkind, Kenneth Aikin, Jeff Peischl, Chelsea R. Thompson, Thomas B. Ryerson, Gregory J. Frost, Brian C. McDonald, and Owen R. Cooper
Atmos. Chem. Phys., 24, 9975–10000, https://doi.org/10.5194/acp-24-9975-2024, https://doi.org/10.5194/acp-24-9975-2024, 2024
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The study examines tropical tropospheric ozone changes. In situ data from 1994–2019 display increased ozone, notably over India, Southeast Asia, and Malaysia and Indonesia. Sparse in situ data limit trend detection for the 15-year period. In situ and satellite data, with limited sampling, struggle to consistently detect trends. Continuous observations are vital over the tropical Pacific Ocean, Indian Ocean, western Africa, and South Asia for accurate ozone trend estimation in these regions.
Ludovico Di Antonio, Matthias Beekmann, Guillaume Siour, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Joel F. de Brito, Paola Formenti, Cecile Gaimoz, Olivier Garret, Aline Gratien, Valérie Gros, Martial Haeffelin, Lelia N. Hawkins, Simone Kotthaus, Gael Noyalet, Diana Pereira, Jean-Eudes Petit, Eva Drew Pronovost, Véronique Riffault, Chenjie Yu, Gilles Foret, Jean-François Doussin, and Claudia Di Biagio
EGUsphere, https://doi.org/10.5194/egusphere-2024-2175, https://doi.org/10.5194/egusphere-2024-2175, 2024
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Summer 2022 has been considered a proxy for future climate scenarios, given the registered hot and dry conditions. In this paper, we used the measurements from the ACROSS campaign, occurred over the Paris area in June–July 2022, in addition to observations from existing networks, to evaluate the WRF–CHIMERE model simulation over France and the Ile-de-France regions. Results over the Ile–de–France show to be satisfactory, allowing to explain the gas and aerosol variability at the ACROSS sites.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Ludovico Di Antonio, Claudia Di Biagio, Paola Formenti, Aline Gratien, Vincent Michoud, Christopher Cantrell, Astrid Bauville, Antonin Bergé, Mathieu Cazaunau, Servanne Chevaillier, Manuela Cirtog, Patrice Coll, Barbara D'Anna, Joel F. de Brito, David O. De Haan, Juliette R. Dignum, Shravan Deshmukh, Olivier Favez, Pierre-Marie Flaud, Cecile Gaimoz, Lelia N. Hawkins, Julien Kammer, Brigitte Language, Franck Maisonneuve, Griša Močnik, Emilie Perraudin, Jean-Eudes Petit, Prodip Acharja, Laurent Poulain, Pauline Pouyes, Eva Drew Pronovost, Véronique Riffault, Kanuri I. Roundtree, Marwa Shahin, Guillaume Siour, Eric Villenave, Pascal Zapf, Gilles Foret, Jean-François Doussin, and Matthias Beekmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2299, https://doi.org/10.5194/egusphere-2024-2299, 2024
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The spectral complex refractive index (CRI) and single scattering albedo were retrieved from submicron aerosol measurements at three sites within the greater Paris area during the ACROSS field campaign (June–July 2022). Measurements revealed the urban emission impact on the surrounding areas. The CRI full period averages at 520 nm were 1.41–0.037i (urban), 1.52–0.038i (peri-urban), 1.50−0.025i (rural). Organic aerosols dominated the aerosol mass and contributed up to 22% of absorption at 370 nm.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
David P. Edwards, Sara Martínez-Alonso, Duseong S. Jo, Ivan Ortega, Louisa K. Emmons, John J. Orlando, Helen M. Worden, Jhoon Kim, Hanlim Lee, Junsung Park, and Hyunkee Hong
Atmos. Chem. Phys., 24, 8943–8961, https://doi.org/10.5194/acp-24-8943-2024, https://doi.org/10.5194/acp-24-8943-2024, 2024
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Until recently, satellite observations of atmospheric pollutants at any location could only be obtained once a day. New geostationary satellites stare at a region of the Earth to make hourly measurements, and the Geostationary Environment Monitoring Spectrometer is the first looking at Asia. These data and model simulations show how the change seen for one important pollutant that determines air quality depends on a combination of pollution emissions, atmospheric chemistry, and meteorology.
Stéphanie Alage, Vincent Michoud, Sergio Harb, Bénédicte Picquet-Varrault, Manuela Cirtog, Avinash Kumar, Matti Rissanen, and Christopher Cantrell
Atmos. Meas. Tech., 17, 4709–4724, https://doi.org/10.5194/amt-17-4709-2024, https://doi.org/10.5194/amt-17-4709-2024, 2024
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Calibration exercises are essential for determining the accuracy of instruments. We performed calibrations on a NO3¯ ToFCIMS instrument to determine its sensitivity and linearity for detecting various organic compounds. Our findings revealed significant variability, over several orders of magnitude, in the calibration factors obtained. The results suggest that relying on a single calibration factor from H2SO4 for the quantification of all compounds detected by this technique is not appropriate.
Chenjie Yu, Edouard Pangui, Kevin Tu, Mathieu Cazaunau, Maxime Feingesicht, Landsheere Xavier, Thierry Bourrianne, Vincent Michoud, Christopher Cantrell, Timothy B. Onasch, Andrew Freedman, and Paola Formenti
Atmos. Meas. Tech., 17, 3419–3437, https://doi.org/10.5194/amt-17-3419-2024, https://doi.org/10.5194/amt-17-3419-2024, 2024
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To meet the requirements for measuring aerosol optical properties on airborne platforms and conducting dual-wavelength measurements, we introduced A2S2, an airborne dual-wavelength cavity-attenuated phase-shift single monitor. This study reports the results in the laboratory and an aircraft campaign over Paris and its surrounding regions. The results demonstrate A2S2's reliability in measuring aerosol optical properties at both wavelengths and its suitability for future aircraft campaigns.
Alice Maison, Lya Lugon, Soo-Jin Park, Alexia Baudic, Christopher Cantrell, Florian Couvidat, Barbara D'Anna, Claudia Di Biagio, Aline Gratien, Valérie Gros, Carmen Kalalian, Julien Kammer, Vincent Michoud, Jean-Eudes Petit, Marwa Shahin, Leila Simon, Myrto Valari, Jérémy Vigneron, Andrée Tuzet, and Karine Sartelet
Atmos. Chem. Phys., 24, 6011–6046, https://doi.org/10.5194/acp-24-6011-2024, https://doi.org/10.5194/acp-24-6011-2024, 2024
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This study presents the development of a bottom-up inventory of urban tree biogenic emissions. Emissions are computed for each tree based on their location and characteristics and are integrated in the regional air quality model WRF-CHIMERE. The impact of these biogenic emissions on air quality is quantified for June–July 2022. Over Paris city, urban trees increase the concentrations of particulate organic matter by 4.6 %, of PM2.5 by 0.6 %, and of ozone by 1.0 % on average over 2 months.
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.
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.
Nathaniel Brockway, Peter K. Peterson, Katja Bigge, Kristian D. Hajny, Paul B. Shepson, Kerri A. Pratt, Jose D. Fuentes, Tim Starn, Robert Kaeser, Brian H. Stirm, and William R. Simpson
Atmos. Chem. Phys., 24, 23–40, https://doi.org/10.5194/acp-24-23-2024, https://doi.org/10.5194/acp-24-23-2024, 2024
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Bromine monoxide (BrO) strongly affects atmospheric chemistry in the springtime Arctic, yet there are still many uncertainties around its sources and recycling, particularly in the context of a rapidly changing Arctic. In this study, we observed BrO as a function of altitude above the Alaskan Arctic. We found that BrO was often most concentrated near the ground, confirming the ability of snow to produce and recycle reactive bromine, and identified four common vertical distributions of BrO.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Pamela S. Rickly, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Glenn M. Wolfe, Ryan Bennett, Ilann Bourgeois, John D. Crounse, Jack E. Dibb, Joshua P. DiGangi, Glenn S. Diskin, Maximilian Dollner, Emily M. Gargulinski, Samuel R. Hall, Hannah S. Halliday, Thomas F. Hanisco, Reem A. Hannun, Jin Liao, Richard Moore, Benjamin A. Nault, John B. Nowak, Jeff Peischl, Claire E. Robinson, Thomas Ryerson, Kevin J. Sanchez, Manuel Schöberl, Amber J. Soja, Jason M. St. Clair, Kenneth L. Thornhill, Kirk Ullmann, Paul O. Wennberg, Bernadett Weinzierl, Elizabeth B. Wiggins, Edward L. Winstead, and Andrew W. Rollins
Atmos. Chem. Phys., 22, 15603–15620, https://doi.org/10.5194/acp-22-15603-2022, https://doi.org/10.5194/acp-22-15603-2022, 2022
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Biomass burning sulfur dioxide (SO2) emission factors range from 0.27–1.1 g kg-1 C. Biomass burning SO2 can quickly form sulfate and organosulfur, but these pathways are dependent on liquid water content and pH. Hydroxymethanesulfonate (HMS) appears to be directly emitted from some fire sources but is not the sole contributor to the organosulfur signal. It is shown that HMS and organosulfur chemistry may be an important S(IV) reservoir with the fate dependent on the surrounding conditions.
Qianjie Chen, Jessica A. Mirrielees, Sham Thanekar, Nicole A. Loeb, Rachel M. Kirpes, Lucia M. Upchurch, Anna J. Barget, Nurun Nahar Lata, Angela R. W. Raso, Stephen M. McNamara, Swarup China, Patricia K. Quinn, Andrew P. Ault, Aaron Kennedy, Paul B. Shepson, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 22, 15263–15285, https://doi.org/10.5194/acp-22-15263-2022, https://doi.org/10.5194/acp-22-15263-2022, 2022
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During a spring field campaign in the coastal Arctic, ultrafine particles were enhanced during high wind speeds, and coarse-mode particles were reduced during blowing snow. Calculated periods blowing snow were overpredicted compared to observations. Sea spray aerosols produced by sea ice leads affected the composition of aerosols and snowpack. An improved understanding of aerosol emissions from leads and blowing snow is critical for predicting the future climate of the rapidly warming Arctic.
Youhua Tang, Patrick C. Campbell, Pius Lee, Rick Saylor, Fanglin Yang, Barry Baker, Daniel Tong, Ariel Stein, Jianping Huang, Ho-Chun Huang, Li Pan, Jeff McQueen, Ivanka Stajner, Jose Tirado-Delgado, Youngsun Jung, Melissa Yang, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Donald Blake, Joshua Schwarz, Jose-Luis Jimenez, James Crawford, Glenn Diskin, Richard Moore, Johnathan Hair, Greg Huey, Andrew Rollins, Jack Dibb, and Xiaoyang Zhang
Geosci. Model Dev., 15, 7977–7999, https://doi.org/10.5194/gmd-15-7977-2022, https://doi.org/10.5194/gmd-15-7977-2022, 2022
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This paper compares two meteorological datasets for driving a regional air quality model: a regional meteorological model using WRF (WRF-CMAQ) and direct interpolation from an operational global model (GFS-CMAQ). In the comparison with surface measurements and aircraft data in summer 2019, these two methods show mixed performance depending on the corresponding meteorological settings. Direct interpolation is found to be a viable method to drive air quality models.
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.
Vivienne H. Payne, Susan S. Kulawik, Emily V. Fischer, Jared F. Brewer, L. Gregory Huey, Kazuyuki Miyazaki, John R. Worden, Kevin W. Bowman, Eric J. Hintsa, Fred Moore, James W. Elkins, and Julieta Juncosa Calahorrano
Atmos. Meas. Tech., 15, 3497–3511, https://doi.org/10.5194/amt-15-3497-2022, https://doi.org/10.5194/amt-15-3497-2022, 2022
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We compare new satellite measurements of peroxyacetyl nitrate (PAN) with reference aircraft measurements from two different instruments flown on the same platform. While there is a systematic difference between the two aircraft datasets, both show the same large-scale distribution of PAN and the discrepancy between aircraft datasets is small compared to the satellite uncertainties. The satellite measurements show skill in capturing large-scale variations in PAN.
Lucien Froidevaux, Douglas E. Kinnison, Michelle L. Santee, Luis F. Millán, Nathaniel J. Livesey, William G. Read, Charles G. Bardeen, John J. Orlando, and Ryan A. Fuller
Atmos. Chem. Phys., 22, 4779–4799, https://doi.org/10.5194/acp-22-4779-2022, https://doi.org/10.5194/acp-22-4779-2022, 2022
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We analyze satellite-derived distributions of chlorine monoxide (ClO) and hypochlorous acid (HOCl) in the upper atmosphere. For 2005–2020, from 50°S to 50°N and over ~30 to 45 km, ClO and HOCl decreased by −0.7 % and −0.4 % per year, respectively. A detailed model of chemistry and dynamics agrees with the results. These decreases confirm the effectiveness of the 1987 Montreal Protocol, which limited emissions of chlorine- and bromine-containing source gases, in order to protect the ozone layer.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
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.
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.
Eric J. Hintsa, Fred L. Moore, Dale F. Hurst, Geoff S. Dutton, Bradley D. Hall, J. David Nance, Ben R. Miller, Stephen A. Montzka, Laura P. Wolton, Audra McClure-Begley, James W. Elkins, Emrys G. Hall, Allen F. Jordan, Andrew W. Rollins, Troy D. Thornberry, Laurel A. Watts, Chelsea R. Thompson, Jeff Peischl, Ilann Bourgeois, Thomas B. Ryerson, Bruce C. Daube, Yenny Gonzalez Ramos, Roisin Commane, Gregory W. Santoni, Jasna V. Pittman, Steven C. Wofsy, Eric Kort, Glenn S. Diskin, and T. Paul Bui
Atmos. Meas. Tech., 14, 6795–6819, https://doi.org/10.5194/amt-14-6795-2021, https://doi.org/10.5194/amt-14-6795-2021, 2021
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We built UCATS to study atmospheric chemistry and transport. It has measured trace gases including CFCs, N2O, SF6, CH4, CO, and H2 with gas chromatography, as well as ozone and water vapor. UCATS has been part of missions to study the tropical tropopause; transport of air into the stratosphere; greenhouse gases, transport, and chemistry in the troposphere; and ozone chemistry, on both piloted and unmanned aircraft. Its design, capabilities, and some results are shown and described here.
Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
Geosci. Model Dev., 14, 6309–6329, https://doi.org/10.5194/gmd-14-6309-2021, https://doi.org/10.5194/gmd-14-6309-2021, 2021
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Over the past decade, understanding of isoprene oxidation has improved, and proper representation of isoprene oxidation and isoprene-derived SOA (iSOA) formation in canopy–chemistry models is now recognized to be important for an accurate understanding of forest–atmosphere exchange. The updated FORCAsT version 2.0 improves the estimation of some isoprene oxidation products and is one of the few canopy models currently capable of simulating SOA formation from monoterpenes and isoprene.
Charles A. Brock, Karl D. Froyd, Maximilian Dollner, Christina J. Williamson, Gregory Schill, Daniel M. Murphy, Nicholas J. Wagner, Agnieszka Kupc, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Jason C. Schroder, Douglas A. Day, Derek J. Price, Bernadett Weinzierl, Joshua P. Schwarz, Joseph M. Katich, Siyuan Wang, Linghan Zeng, Rodney Weber, Jack Dibb, Eric Scheuer, Glenn S. Diskin, Joshua P. DiGangi, ThaoPaul Bui, Jonathan M. Dean-Day, Chelsea R. Thompson, Jeff Peischl, Thomas B. Ryerson, Ilann Bourgeois, Bruce C. Daube, Róisín Commane, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 15023–15063, https://doi.org/10.5194/acp-21-15023-2021, https://doi.org/10.5194/acp-21-15023-2021, 2021
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The Atmospheric Tomography Mission was an airborne study that mapped the chemical composition of the remote atmosphere. From this, we developed a comprehensive description of aerosol properties that provides a unique, global-scale dataset against which models can be compared. The data show the polluted nature of the remote atmosphere in the Northern Hemisphere and quantify the contributions of sea salt, dust, soot, biomass burning particles, and pollution particles to the haziness of the sky.
Zhe Peng, Julia Lee-Taylor, Harald Stark, John J. Orlando, Bernard Aumont, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 14649–14669, https://doi.org/10.5194/acp-21-14649-2021, https://doi.org/10.5194/acp-21-14649-2021, 2021
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We use the fully explicit GECKO-A model to study the OH reactivity (OHR) evolution in the NO-free photooxidation of several volatile organic compounds. Oxidation progressively produces more saturated and functionalized species, then breaks them into small species. OHR per C atom evolution is similar for different precursors once saturated multifunctional species are formed. We also find that partitioning of these species to chamber walls leads to large deviations in chambers from the atmosphere.
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 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Taylor S. Jones, Jonathan E. Franklin, Jia Chen, Florian Dietrich, Kristian D. Hajny, Johannes C. Paetzold, Adrian Wenzel, Conor Gately, Elaine Gottlieb, Harrison Parker, Manvendra Dubey, Frank Hase, Paul B. Shepson, Levi H. Mielke, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 13131–13147, https://doi.org/10.5194/acp-21-13131-2021, https://doi.org/10.5194/acp-21-13131-2021, 2021
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Methane emissions from leaks in natural gas pipes are often a large source in urban areas, but they are difficult to measure on a city-wide scale. Here we use an array of innovative methane sensors distributed around the city of Indianapolis and a new method of combining their data with an atmospheric model to accurately determine the magnitude of these emissions, which are about 70 % larger than predicted. This method can serve as a framework for cities trying to account for their emissions.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Christina J. Williamson, Agnieszka Kupc, Andrew Rollins, Jan Kazil, Karl D. Froyd, Eric A. Ray, Daniel M. Murphy, Gregory P. Schill, Jeff Peischl, Chelsea Thompson, Ilann Bourgeois, Thomas B. Ryerson, Glenn S. Diskin, Joshua P. DiGangi, Donald R. Blake, Thao Paul V. Bui, Maximilian Dollner, Bernadett Weinzierl, and Charles A. Brock
Atmos. Chem. Phys., 21, 9065–9088, https://doi.org/10.5194/acp-21-9065-2021, https://doi.org/10.5194/acp-21-9065-2021, 2021
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Aerosols in the stratosphere influence climate by scattering and absorbing sunlight and through chemical reactions occurring on the particles’ surfaces. We observed more nucleation mode aerosols (small aerosols, with diameters below 12 nm) in the mid- and high-latitude lowermost stratosphere (8–13 km) in the Northern Hemisphere (NH) than in the Southern Hemisphere. The most likely cause of this is aircraft emissions, which are concentrated in the NH at similar altitudes to our observations.
Daniel M. Murphy, Karl D. Froyd, Ilann Bourgeois, Charles A. Brock, Agnieszka Kupc, Jeff Peischl, Gregory P. Schill, Chelsea R. Thompson, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 21, 8915–8932, https://doi.org/10.5194/acp-21-8915-2021, https://doi.org/10.5194/acp-21-8915-2021, 2021
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New measurements in the lower stratosphere highlight differences between particles that originated in the troposphere or the stratosphere. The stratospheric-origin particles have relatively large radiative effects because they are at nearly the optimum diameter for light scattering. The tropospheric particles contribute significantly to surface area. These and other chemical and physical properties are then extended to study the implications if material were to be added to the stratosphere.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145, https://doi.org/10.5194/acp-21-129-2021, https://doi.org/10.5194/acp-21-129-2021, 2021
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Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
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.
Wayne M. Angevine, Jeff Peischl, Alice Crawford, Christopher P. Loughner, Ilana B. Pollack, and Chelsea R. Thompson
Atmos. Chem. Phys., 20, 11855–11868, https://doi.org/10.5194/acp-20-11855-2020, https://doi.org/10.5194/acp-20-11855-2020, 2020
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Emissions of air pollutants must be known for a wide variety of applications. Different methods of estimating emissions often disagree substantially. In this study, we apply standard methods to a well-known source, a power plant. We explore the uncertainty implied by the different answers that come from the different methods, different samples taken over several years, and different pollutants. We find that the overall uncertainty of emissions estimates is about 30 %.
Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Kenneth C. Aikin, Teresa Campos, Hannah Clark, Róisín Commane, Bruce Daube, Glenn W. Diskin, James W. Elkins, Ru-Shan Gao, Audrey Gaudel, Eric J. Hintsa, Bryan J. Johnson, Rigel Kivi, Kathryn McKain, Fred L. Moore, David D. Parrish, Richard Querel, Eric Ray, Ricardo Sánchez, Colm Sweeney, David W. Tarasick, Anne M. Thompson, Valérie Thouret, Jacquelyn C. Witte, Steve C. Wofsy, and Thomas B. Ryerson
Atmos. Chem. Phys., 20, 10611–10635, https://doi.org/10.5194/acp-20-10611-2020, https://doi.org/10.5194/acp-20-10611-2020, 2020
Jianghanyang Li, Xuan Zhang, John Orlando, Geoffrey Tyndall, and Greg Michalski
Atmos. Chem. Phys., 20, 9805–9819, https://doi.org/10.5194/acp-20-9805-2020, https://doi.org/10.5194/acp-20-9805-2020, 2020
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Nitrogen isotopic compositions of atmospheric reactive nitrogen are widely used to infer their sources. However, the reactions between NO and NO2 strongly impact their isotopes, which was not well understood. We conducted a series of experiments in an atmospheric simulation chamber to determine the isotopic effects of (1) direct isotopic exchange between NO and NO2 and (2) the isotopic fractionations during NOx photochemistry, then developed an equation to quantify the overall isotopic effect.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Yi Ji, L. Gregory Huey, David J. Tanner, Young Ro Lee, Patrick R. Veres, J. Andrew Neuman, Yuhang Wang, and Xinming Wang
Atmos. Meas. Tech., 13, 3683–3696, https://doi.org/10.5194/amt-13-3683-2020, https://doi.org/10.5194/amt-13-3683-2020, 2020
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A common way of measuring trace gases in the atmosphere is chemical ionization mass spectrometry. One large drawback of these instruments is that they require radioactive ion sources. In this work we demonstrate a simple ion source that uses a small krypton lamp that can be used to replace a radioactive source.
Max R. McGillen, William P. L. Carter, Abdelwahid Mellouki, John J. Orlando, Bénédicte Picquet-Varrault, and Timothy J. Wallington
Earth Syst. Sci. Data, 12, 1203–1216, https://doi.org/10.5194/essd-12-1203-2020, https://doi.org/10.5194/essd-12-1203-2020, 2020
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The gas-phase reactions of organic compounds in the atmosphere are a crucial step in the degradation of anthropogenic and biogenic emissions and the formation of secondary pollutants. This work is an attempt to produce a dataset that is as comprehensive as possible regarding the multitude of chemicals that react in the atmosphere. We find that we are able to make substantial improvements upon previous compendia and that this progress will help improve our understanding of atmospheric chemistry.
Camille Mouchel-Vallon, Julia Lee-Taylor, Alma Hodzic, Paulo Artaxo, Bernard Aumont, Marie Camredon, David Gurarie, Jose-Luis Jimenez, Donald H. Lenschow, Scot T. Martin, Janaina Nascimento, John J. Orlando, Brett B. Palm, John E. Shilling, Manish Shrivastava, and Sasha Madronich
Atmos. Chem. Phys., 20, 5995–6014, https://doi.org/10.5194/acp-20-5995-2020, https://doi.org/10.5194/acp-20-5995-2020, 2020
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The GoAmazon 2014/5 field campaign took place near the city of Manaus, Brazil, isolated in the Amazon rainforest, to study the impacts of urban pollution on natural air masses. We simulated this campaign with an extremely detailed organic chemistry model to understand how the city would affect the growth and composition of natural aerosol particles. Discrepancies between the model and the measurements indicate that the chemistry of naturally emitted organic compounds is still poorly understood.
Young Ro Lee, Yi Ji, David J. Tanner, and L. Gregory Huey
Atmos. Meas. Tech., 13, 2473–2480, https://doi.org/10.5194/amt-13-2473-2020, https://doi.org/10.5194/amt-13-2473-2020, 2020
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In this work we show how to construct a radioactive ion source for a chemical ionization mass spectrometer (CIMS) from commercially available components. The source is low activity and can be shipped with a minimum of complications. This facilitates the deployment of CIMS to measure atmospheric pollutants at remote ground sites.
Alexander B. Thames, William H. Brune, David O. Miller, Hannah M. Allen, Eric C. Apel, Donald R. Blake, T. Paul Bui, Roisin Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, Joshua P. DiGangi, James W. Elkins, Samuel R. Hall, Thomas F. Hanisco, Reem A. Hannun, Eric Hintsa, Rebecca S. Hornbrook, Michelle J. Kim, Kathryn McKain, Fred L. Moore, Julie M. Nicely, Jeffrey Peischl, Thomas B. Ryerson, Jason M. St. Clair, Colm Sweeney, Alex Teng, Chelsea R. Thompson, Kirk Ullmann, Paul O. Wennberg, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 4013–4029, https://doi.org/10.5194/acp-20-4013-2020, https://doi.org/10.5194/acp-20-4013-2020, 2020
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Oceans and the atmosphere exchange volatile gases that react with the hydroxyl radical (OH). During a NASA airborne study, measurements of the total frequency of OH reactions, called the OH reactivity, were made in the marine boundary layer of the Atlantic and Pacific oceans. The measured OH reactivity often exceeded the OH reactivity calculated from measured chemical species. This missing OH reactivity appears to be from unmeasured volatile organic compounds coming out of the ocean.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Xuan Zhang, Haofei Zhang, Wen Xu, Xiaokang Wu, Geoffrey S. Tyndall, John J. Orlando, John T. Jayne, Douglas R. Worsnop, and Manjula R. Canagaratna
Atmos. Meas. Tech., 12, 5535–5545, https://doi.org/10.5194/amt-12-5535-2019, https://doi.org/10.5194/amt-12-5535-2019, 2019
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We develop a new technique to characterize organic nitrates as intact molecules in atmospheric aerosols, and we apply this technique to identify hydroxy nitrates in secondary organic aerosols produced from the photochemical oxidation of isoprene.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Olivia E. Salmon, Lisa R. Welp, Michael E. Baldwin, Kristian D. Hajny, Brian H. Stirm, and Paul B. Shepson
Atmos. Chem. Phys., 19, 11525–11543, https://doi.org/10.5194/acp-19-11525-2019, https://doi.org/10.5194/acp-19-11525-2019, 2019
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We conducted airborne vertical profile measurements of water vapor stable isotopes to examine how boundary layer, cloud, and mixing processes influence the vertical structure of deuterium excess in the lower troposphere. We discuss reasons our observations are consistent with water vapor isotope theory on some days and not others. Deuterium excess may be useful for understanding complex processes occurring at the top of the boundary layer, including cloud formation, evaporation, and air mixing.
Xin Chen, Dylan B. Millet, Hanwant B. Singh, Armin Wisthaler, Eric C. Apel, Elliot L. Atlas, Donald R. Blake, Ilann Bourgeois, Steven S. Brown, John D. Crounse, Joost A. de Gouw, Frank M. Flocke, Alan Fried, Brian G. Heikes, Rebecca S. Hornbrook, Tomas Mikoviny, Kyung-Eun Min, Markus Müller, J. Andrew Neuman, Daniel W. O'Sullivan, Jeff Peischl, Gabriele G. Pfister, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Stephen R. Shertz, Chelsea R. Thompson, Victoria Treadaway, Patrick R. Veres, James Walega, Carsten Warneke, Rebecca A. Washenfelder, Petter Weibring, and Bin Yuan
Atmos. Chem. Phys., 19, 9097–9123, https://doi.org/10.5194/acp-19-9097-2019, https://doi.org/10.5194/acp-19-9097-2019, 2019
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Volatile organic compounds (VOCs) affect air quality and modify the lifetimes of other pollutants. We combine a high-resolution 3-D atmospheric model with an ensemble of aircraft observations to perform an integrated analysis of the VOC budget over North America. We find that biogenic emissions provide the main source of VOC reactivity even in most major cities. Our findings point to key gaps in current models related to oxygenated VOCs and to the distribution of VOCs in the free troposphere.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
John W. Halfacre, Paul B. Shepson, and Kerri A. Pratt
Atmos. Chem. Phys., 19, 4917–4931, https://doi.org/10.5194/acp-19-4917-2019, https://doi.org/10.5194/acp-19-4917-2019, 2019
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In this study, we found that a chemical called hydroxyl radical can help create chlorine, bromine, and iodine (i.e., halogens) from acidic frozen imitation seawater. Even more halogens are created if we also add ozone. This result helps our understanding of how halogens are released from the frozen Arctic ice and snow into the atmosphere, where they alter the atmosphere's oxidation ability.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Shino Toma, Steve Bertman, Christopher Groff, Fulizi Xiong, Paul B. Shepson, Paul Romer, Kaitlin Duffey, Paul Wooldridge, Ronald Cohen, Karsten Baumann, Eric Edgerton, Abigail R. Koss, Joost de Gouw, Allen Goldstein, Weiwei Hu, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 1867–1880, https://doi.org/10.5194/acp-19-1867-2019, https://doi.org/10.5194/acp-19-1867-2019, 2019
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Acyl peroxy nitrates (APN) were measured near the ground in Alabama using GC in summer 2013 to study biosphere–atmosphere interactions. APN were lower than measured in the SE USA over the past 2 decades. Historical data showed APN in 2013 was limited by NOx and production was dominated by biogenic precursors more than in the past. Isoprene-derived MPAN correlated with isoprene hydroxynitrates as NOx-dependent products. MPAN varied with aerosol growth, but not with N-containing particles.
Zhe Peng, Julia Lee-Taylor, John J. Orlando, Geoffrey S. Tyndall, and Jose L. Jimenez
Atmos. Chem. Phys., 19, 813–834, https://doi.org/10.5194/acp-19-813-2019, https://doi.org/10.5194/acp-19-813-2019, 2019
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The use of oxidation flow reactors (OFRs) has been rapidly increasing. We investigate organic peroxy radical (RO2) chemistry in OFRs by kinetic modeling. It is found that, at low NO, UV intensity should be limited to avoid high radical levels leading to significant reaction of RO2 with OH and negligible RO2 isomerization, both of which are atmospherically irrelevant. We also develop two RO2 fate estimators (for general use and for OFRs) to aid experiment design and interpretation.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Maryam Abdi-Oskouei, Gabriele Pfister, Frank Flocke, Negin Sobhani, Pablo Saide, Alan Fried, Dirk Richter, Petter Weibring, James Walega, and Gregory Carmichael
Atmos. Chem. Phys., 18, 16863–16883, https://doi.org/10.5194/acp-18-16863-2018, https://doi.org/10.5194/acp-18-16863-2018, 2018
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This study presents a quantification of model uncertainties due to configurations and errors in the emission inventories. The analysis includes performing simulations with different configurations and comparisons with airborne and ground-based observations with a focus on capturing transport and emissions from the oil and gas sector. The presented results reflect the challenges that one may face when attempting to improve emission inventories by contrasting measured with modeled concentrations.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Chunxiang Ye, Xianliang Zhou, Dennis Pu, Jochen Stutz, James Festa, Max Spolaor, Catalina Tsai, Christopher Cantrell, Roy L. Mauldin III, Andrew Weinheimer, Rebecca S. Hornbrook, Eric C. Apel, Alex Guenther, Lisa Kaser, Bin Yuan, Thomas Karl, Julie Haggerty, Samuel Hall, Kirk Ullmann, James Smith, and John Ortega
Atmos. Chem. Phys., 18, 9107–9120, https://doi.org/10.5194/acp-18-9107-2018, https://doi.org/10.5194/acp-18-9107-2018, 2018
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Substantial levels of HONO existed during the day throughout the troposphere over the southeastern US during NOMADSS 2013. Particulate nitrate photolysis appeared to be the major volume HONO source, while NOx was an important HONO precursor only in industrial and urban plumes. HONO was not a significant OH radical precursor in the rural troposphere away from the ground surface; however, its production from particulate nitrate photolysis was an important renoxification pathway.
Roya Bahreini, Ravan Ahmadov, Stu A. McKeen, Kennedy T. Vu, Justin H. Dingle, Eric C. Apel, Donald R. Blake, Nicola Blake, Teresa L. Campos, Chris Cantrell, Frank Flocke, Alan Fried, Jessica B. Gilman, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Brian M. Lerner, Roy L. Mauldin, Simone Meinardi, Denise D. Montzka, Dirk Richter, Jason R. Schroeder, Meghan Stell, David Tanner, James Walega, Peter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 18, 8293–8312, https://doi.org/10.5194/acp-18-8293-2018, https://doi.org/10.5194/acp-18-8293-2018, 2018
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We measured organic aerosol (OA) and relevant trace gases during FRAPPÉ in the Colorado Front Range, with the goal of characterizing summertime OA formation. Our results indicate a significant production of secondary OA (SOA) in this region. About 2 μg m−3 of OA was present at background CO levels, suggesting contribution of non-combustion sources to SOA. Contribution of oil- and gas-related activities to anthropogenic SOA was modeled to be ~38 %. Biogenic SOA contributed to >40 % of OA.
Martin G. Schultz, Scarlet Stadtler, Sabine Schröder, Domenico Taraborrelli, Bruno Franco, Jonathan Krefting, Alexandra Henrot, Sylvaine Ferrachat, Ulrike Lohmann, David Neubauer, Colombe Siegenthaler-Le Drian, Sebastian Wahl, Harri Kokkola, Thomas Kühn, Sebastian Rast, Hauke Schmidt, Philip Stier, Doug Kinnison, Geoffrey S. Tyndall, John J. Orlando, and Catherine Wespes
Geosci. Model Dev., 11, 1695–1723, https://doi.org/10.5194/gmd-11-1695-2018, https://doi.org/10.5194/gmd-11-1695-2018, 2018
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The chemistry–climate model ECHAM-HAMMOZ contains a detailed representation of tropospheric and stratospheric reactive chemistry and state-of-the-art parameterizations of aerosols. It thus allows for detailed investigations of chemical processes in the climate system. Evaluation of the model with various observational data yields good results, but the model has a tendency to produce too much OH in the tropics. This highlights the important interplay between atmospheric chemistry and dynamics.
Xuan Zhang, John Ortega, Yuanlong Huang, Stephen Shertz, Geoffrey S. Tyndall, and John J. Orlando
Atmos. Meas. Tech., 11, 2537–2551, https://doi.org/10.5194/amt-11-2537-2018, https://doi.org/10.5194/amt-11-2537-2018, 2018
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We present the development and characterization of the NCAR Atmospheric Simulation Chamber, which is operated in steady state continuous
flow mode for simulating atmospheric daytime and nighttime chemistry over chemical regimes not accessible in traditional static chamber
experiments. We focus on establishing an
intermediate NOregime characterized by a constant steady-state NO level ranging from tens of ppt to a few ppb in the chamber.
Emily V. Fischer, Liye Zhu, Vivienne H. Payne, John R. Worden, Zhe Jiang, Susan S. Kulawik, Steven Brey, Arsineh Hecobian, Daniel Gombos, Karen Cady-Pereira, and Frank Flocke
Atmos. Chem. Phys., 18, 5639–5653, https://doi.org/10.5194/acp-18-5639-2018, https://doi.org/10.5194/acp-18-5639-2018, 2018
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PAN is an atmospheric reservoir for nitrogen oxide radicals, and it plays a lead role in their redistribution in the troposphere. We analyze new Tropospheric Emission Spectrometer (TES) PAN observations over North America during July 2006 to 2009. We identify smoke-impacted TES PAN retrievals by co-location with NOAA Hazard Mapping System (HMS) smoke plumes. Depending on the year, 15–32 % of cases where elevated PAN is identified in TES observations overlap with smoke plumes.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Jin Liao, Charles A. Brock, Daniel M. Murphy, Donna T. Sueper, André Welti, and Ann M. Middlebrook
Atmos. Meas. Tech., 10, 3801–3820, https://doi.org/10.5194/amt-10-3801-2017, https://doi.org/10.5194/amt-10-3801-2017, 2017
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The Aerodyne aerosol mass spectrometer (AMS) has emerged as a widely used method for measuring the real-time, submicron, nonrefractory aerosol composition. A large uncertainty in accurate measurements with the AMS (the collection efficiency due to particle bounce) is evaluated in this paper using in situ measurements of particle light scattering. Current calculations of the collection efficiency reasonably predict this effect in acidic environments, resulting in more confidence for AMS results.
Bianca C. Baier, William H. Brune, David O. Miller, Donald Blake, Russell Long, Armin Wisthaler, Christopher Cantrell, Alan Fried, Brian Heikes, Steven Brown, Erin McDuffie, Frank Flocke, Eric Apel, Lisa Kaser, and Andrew Weinheimer
Atmos. Chem. Phys., 17, 11273–11292, https://doi.org/10.5194/acp-17-11273-2017, https://doi.org/10.5194/acp-17-11273-2017, 2017
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Ozone production rates were measured using the Measurement of Ozone Production Sensor (MOPS). Measurements are compared to modeled ozone production rates using two different chemical mechanisms. At high nitric oxide levels, observed rates are higher than those modeled, prompting the need to revisit current model photochemistry. These direct measurements can add to our understanding of the ozone chemistry within air quality models and can be used to guide government regulatory strategies.
Jakob Lindaas, Delphine K. Farmer, Ilana B. Pollack, Andrew Abeleira, Frank Flocke, Rob Roscioli, Scott Herndon, and Emily V. Fischer
Atmos. Chem. Phys., 17, 10691–10707, https://doi.org/10.5194/acp-17-10691-2017, https://doi.org/10.5194/acp-17-10691-2017, 2017
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Wildfire smoke is becoming increasingly important for air quality in the US. We used measurements taken during the summer 2015 near Denver, CO, to provide a case study of how wildfire smoke can impact air quality, specifically ozone, which is harmful to humans. Wildfire smoke during this time period was associated with about 15 % more ozone than we would expect under normal conditions. This smoke came from fires in the Pacific Northwest and likely impacted much of the central and western US.
Carlena J. Ebben, Tamara L. Sparks, Paul J. Wooldridge, Teresa L. Campos, Christopher A. Cantrell, Roy L. Mauldin, Andrew J. Weinheimer, and Ronald C. Cohen
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-671, https://doi.org/10.5194/acp-2017-671, 2017
Revised manuscript has not been submitted
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We use observations from the FRAPPÉ campaign to examine the evolution of reactive nitrogen as it is transported from Denver. We provide estimates for dilution rates, chemical lifetimes, and deposition rates. While dilution is the primary loss process in the immediate outflow from Denver, chemically, a majority of NOx is converted to HNO3 and is subsequently deposited. Understanding the evolution of reactive nitrogen informs how urban emissions affect air quality in the surrounding regions.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
William R. Simpson, Peter K. Peterson, Udo Frieß, Holger Sihler, Johannes Lampel, Ulrich Platt, Chris Moore, Kerri Pratt, Paul Shepson, John Halfacre, and Son V. Nghiem
Atmos. Chem. Phys., 17, 9291–9309, https://doi.org/10.5194/acp-17-9291-2017, https://doi.org/10.5194/acp-17-9291-2017, 2017
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We investigated Arctic atmospheric bromine chemistry during March–April 2012 to improve understanding of the role of sea ice and cracks in sea ice (leads) in this phenomenon. We find that leads vertically redistribute reactive bromine but that open/re-freezing leads are not major direct reactive halogen sources. Surface ozone depletion affects the vertical distribution and amount of reactive halogens, and aerosol particles are necessary but not sufficient to maintain reactive bromine aloft.
Jonathan H. Slade, Chloé de Perre, Linda Lee, and Paul B. Shepson
Atmos. Chem. Phys., 17, 8635–8650, https://doi.org/10.5194/acp-17-8635-2017, https://doi.org/10.5194/acp-17-8635-2017, 2017
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This study provides new insight into the oxidation of polyolefinic monoterpenes and the dependence of the formation and yields of organic nitrates (ON) and secondary organic aerosol (SOA) on hydrocarbon structure. Here we have elucidated the ON, hydroxy nitrate, and SOA yields from the NO3 oxidation of γ-terpinene, a potentially relevant nighttime ON precursor in the Midwestern US. The results advance our understanding of the chemistry that influences NOx, O3 production, and aerosol formation.
Peter K. Peterson, Denis Pöhler, Holger Sihler, Johannes Zielcke, Stephan General, Udo Frieß, Ulrich Platt, William R. Simpson, Son V. Nghiem, Paul B. Shepson, Brian H. Stirm, Suresh Dhaniyala, Thomas Wagner, Dana R. Caulton, Jose D. Fuentes, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 7567–7579, https://doi.org/10.5194/acp-17-7567-2017, https://doi.org/10.5194/acp-17-7567-2017, 2017
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High-spatial-resolution aircraft measurements in the Arctic showed the sustained transport of reactive bromine in a lofted layer via heterogeneous reactions on aerosol particles. This process provides an explanation for free tropospheric reactive bromine and the significant spatial extent of satellite-observed bromine monoxide. The knowledge gained herein improves our understanding of the fate and transport of atmospheric pollutants in the Arctic.
Lindsay E. Hatch, Robert J. Yokelson, Chelsea E. Stockwell, Patrick R. Veres, Isobel J. Simpson, Donald R. Blake, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 17, 1471–1489, https://doi.org/10.5194/acp-17-1471-2017, https://doi.org/10.5194/acp-17-1471-2017, 2017
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The most comprehensive database of gaseous biomass burning emissions to date was compiled. Four complementary instruments were deployed together during laboratory fires. The results generally compared within experimental uncertainty and highlighted that a range of measurement approaches are required for adequate characterization of smoke composition. Observed compounds were binned based on volatility, and priority recommendations were made to improve secondary organic aerosol predictions.
Joel D. Rindelaub, Carlos H. Borca, Matthew A. Hostetler, Jonathan H. Slade, Mark A. Lipton, Lyudmila V. Slipchenko, and Paul B. Shepson
Atmos. Chem. Phys., 16, 15425–15432, https://doi.org/10.5194/acp-16-15425-2016, https://doi.org/10.5194/acp-16-15425-2016, 2016
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This study provides new insight into the hydrolysis reaction mechanism, which was elucidated for atmospherically relevant organic nitrates using kinetic measurements, product identification, and theoretical calculations. The results help broaden our knowledge of the organic chemistry that impacts the fate of NOx, ozone production, aerosol phase processing, and aerosol composition.
Richard J. Pope, Nigel A. D. Richards, Martyn P. Chipperfield, David P. Moore, Sarah A. Monks, Stephen R. Arnold, Norbert Glatthor, Michael Kiefer, Tom J. Breider, Jeremy J. Harrison, John J. Remedios, Carsten Warneke, James M. Roberts, Glenn S. Diskin, Lewis G. Huey, Armin Wisthaler, Eric C. Apel, Peter F. Bernath, and Wuhu Feng
Atmos. Chem. Phys., 16, 13541–13559, https://doi.org/10.5194/acp-16-13541-2016, https://doi.org/10.5194/acp-16-13541-2016, 2016
Amelia F. Longo, David J. Vine, Laura E. King, Michelle Oakes, Rodney J. Weber, Lewis Gregory Huey, Armistead G. Russell, and Ellery D. Ingall
Atmos. Chem. Phys., 16, 13389–13398, https://doi.org/10.5194/acp-16-13389-2016, https://doi.org/10.5194/acp-16-13389-2016, 2016
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New synchrotron-based techniques were applied to characterize the oxidation state and composition of sulfur in ambient aerosol and emission sources. Individual particles were found to contain surprisingly high levels of elemental sulfur, a form of sulfur found in only one of the emission sources analyzed. We also show metal sulfates as a key component of urban aerosols. These metal sulfate phases are highly soluble and are indicative of acidic processes transforming metals in the environment.
Kennedy T. Vu, Justin H. Dingle, Roya Bahreini, Patrick J. Reddy, Eric C. Apel, Teresa L. Campos, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, Scott C. Herndon, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Denise D. Montzka, John B. Nowak, Sally E. Pusede, Dirk Richter, Joseph R. Roscioli, Glen W. Sachse, Stephen Shertz, Meghan Stell, David Tanner, Geoffrey S. Tyndall, James Walega, Peter Weibring, Andrew J. Weinheimer, Gabriele Pfister, and Frank Flocke
Atmos. Chem. Phys., 16, 12039–12058, https://doi.org/10.5194/acp-16-12039-2016, https://doi.org/10.5194/acp-16-12039-2016, 2016
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In this manuscript, we report on airborne measurements of non-refractory composition and optical extinction along with relevant trace gases during a unique surface mesoscale circulation event, namely the Denver Cyclone, in Colorado, USA, during in July–August 2014. The focus of this paper is to investigate how meteorological conditions associated with the Denver Cyclone impacted air quality of the Colorado Front Range.
Glenn M. Wolfe, Margaret R. Marvin, Sandra J. Roberts, Katherine R. Travis, and Jin Liao
Geosci. Model Dev., 9, 3309–3319, https://doi.org/10.5194/gmd-9-3309-2016, https://doi.org/10.5194/gmd-9-3309-2016, 2016
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The Framework for 0-D Atmospheric Modeling (F0AM) is a new, user-friendly platform for simulation of atmospheric chemistry systems. It incorporates a suite of commonly used mechanisms and is adaptable to photochemical chambers, Lagrangian plumes, and steady-state or time-varying diurnal cycles. We provide a detailed model description, demonstrate several common applications, and highlight some of the advantages and challenges of the 0-D box modeling approach.
Justin H. Dingle, Kennedy Vu, Roya Bahreini, Eric C. Apel, Teresa L. Campos, Frank Flocke, Alan Fried, Scott Herndon, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Denise D. Montzka, John B. Nowak, Mike Reeves, Dirk Richter, Joseph R. Roscioli, Stephen Shertz, Meghan Stell, David Tanner, Geoff Tyndall, James Walega, Petter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 16, 11207–11217, https://doi.org/10.5194/acp-16-11207-2016, https://doi.org/10.5194/acp-16-11207-2016, 2016
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The focus of this paper was to use gas-phase tracers and aerosol composition to characterize the influence of the different sources on optical extinction (RH = 22 %) and summertime visibility in the Colorado Front Range. Our analysis indicates that aerosol nitrate contributed significantly to optical extinction in agriculturally influenced air masses, while in other plumes, organics could explain most of the observed variability in optical extinction.
Javier Sanchez, David J. Tanner, Dexian Chen, L. Gregory Huey, and Nga L. Ng
Atmos. Meas. Tech., 9, 3851–3861, https://doi.org/10.5194/amt-9-3851-2016, https://doi.org/10.5194/amt-9-3851-2016, 2016
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HO2 radicals play an important role in tropospheric chemistry. Here we propose a new direct method for measuring HO2 radicals in the atmosphere using bromide anion chemical ionization mass spectrometry. Ambient measurements in Atlanta are presented. Instrument performance parameters: sensitivity, lower detection limit, and time resolution are discussed. We demonstrate that the technique provides excellent selectivity and is suitable for in situ ground-based HO2 measurements.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Jenny A. Fisher, Daniel J. Jacob, Katherine R. Travis, Patrick S. Kim, Eloise A. Marais, Christopher Chan Miller, Karen Yu, Lei Zhu, Robert M. Yantosca, Melissa P. Sulprizio, Jingqiu Mao, Paul O. Wennberg, John D. Crounse, Alex P. Teng, Tran B. Nguyen, Jason M. St. Clair, Ronald C. Cohen, Paul Romer, Benjamin A. Nault, Paul J. Wooldridge, Jose L. Jimenez, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Paul B. Shepson, Fulizi Xiong, Donald R. Blake, Allen H. Goldstein, Pawel K. Misztal, Thomas F. Hanisco, Glenn M. Wolfe, Thomas B. Ryerson, Armin Wisthaler, and Tomas Mikoviny
Atmos. Chem. Phys., 16, 5969–5991, https://doi.org/10.5194/acp-16-5969-2016, https://doi.org/10.5194/acp-16-5969-2016, 2016
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We use new airborne and ground-based observations from two summer 2013 campaigns in the southeastern US, interpreted with a chemical transport model, to understand the impact of isoprene and monoterpene chemistry on the atmospheric NOx budget via production of organic nitrates (RONO2). We find that a diversity of species contribute to observed RONO2. Our work implies that the NOx sink to RONO2 production is only sensitive to NOx emissions in regions where they are already low.
Fulizi Xiong, Carlos H. Borca, Lyudmila V. Slipchenko, and Paul B. Shepson
Atmos. Chem. Phys., 16, 5595–5610, https://doi.org/10.5194/acp-16-5595-2016, https://doi.org/10.5194/acp-16-5595-2016, 2016
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Here we report on a detailed study of the photochemistry and fate of a nitrooxy enal that is produced from the reaction of NO3 with isoprene. We synthesized the 4,1-nitrooxy enal, purified it, and measured the O3 and OH reaction rate constants, and determined the atmospheric photodissociation rate constant for specified radiation conditions. The determined fast photolysis rate and high reactivity toward OH lead to a lifetime of less than 1 hour, with photolysis being a dominant daytime sink.
V. Shah, L. Jaeglé, L. E. Gratz, J. L. Ambrose, D. A. Jaffe, N. E. Selin, S. Song, T. L. Campos, F. M. Flocke, M. Reeves, D. Stechman, M. Stell, J. Festa, J. Stutz, A. J. Weinheimer, D. J. Knapp, D. D. Montzka, G. S. Tyndall, E. C. Apel, R. S. Hornbrook, A. J. Hills, D. D. Riemer, N. J. Blake, C. A. Cantrell, and R. L. Mauldin III
Atmos. Chem. Phys., 16, 1511–1530, https://doi.org/10.5194/acp-16-1511-2016, https://doi.org/10.5194/acp-16-1511-2016, 2016
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We present airborne observations of mercury over the southeastern USA during summer. Higher concentrations of oxidized mercury were observed in clean, dry air masses descending in the subtropical anti-cyclones. We used an atmospheric model to simulate the chemistry and transport of mercury. We found reasonable agreement with the observations when the modeled oxidation of elemental mercury was increased, suggesting fast cycling between elemental and oxidized mercury.
F. Xiong, K. M. McAvey, K. A. Pratt, C. J. Groff, M. A. Hostetler, M. A. Lipton, T. K. Starn, J. V. Seeley, S. B. Bertman, A. P. Teng, J. D. Crounse, T. B. Nguyen, P. O. Wennberg, P. K. Misztal, A. H. Goldstein, A. B. Guenther, A. R. Koss, K. F. Olson, J. A. de Gouw, K. Baumann, E. S. Edgerton, P. A. Feiner, L. Zhang, D. O. Miller, W. H. Brune, and P. B. Shepson
Atmos. Chem. Phys., 15, 11257–11272, https://doi.org/10.5194/acp-15-11257-2015, https://doi.org/10.5194/acp-15-11257-2015, 2015
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Hydroxynitrates from isoprene oxidation were quantified both in the laboratory and through field studies. The yield of hydroxynitrates 9(+4/-3)% derived from chamber experiments was applied in a zero-dimensional model to simulate the production and loss of isoprene hydroxynitrates in an ambient environment during the 2013 Southern Oxidant and Aerosol Study (SOAS). NOx was determined to be the limiting factor for the formation of isoprene hydroxynitrates during SOAS.
K. D. Custard, C. R. Thompson, K. A. Pratt, P B. Shepson, J. Liao, L. G. Huey, J. J. Orlando, A. J. Weinheimer, E. Apel, S. R. Hall, F. Flocke, L. Mauldin, R. S. Hornbrook, D. Pöhler, S. General, J. Zielcke, W. R. Simpson, U. Platt, A. Fried, P. Weibring, B. C. Sive, K. Ullmann, C. Cantrell, D. J. Knapp, and D. D. Montzka
Atmos. Chem. Phys., 15, 10799–10809, https://doi.org/10.5194/acp-15-10799-2015, https://doi.org/10.5194/acp-15-10799-2015, 2015
C. R. Thompson, P. B. Shepson, J. Liao, L. G. Huey, E. C. Apel, C. A. Cantrell, F. Flocke, J. Orlando, A. Fried, S. R. Hall, R. S. Hornbrook, D. J. Knapp, R. L. Mauldin III, D. D. Montzka, B. C. Sive, K. Ullmann, P. Weibring, and A. Weinheimer
Atmos. Chem. Phys., 15, 9651–9679, https://doi.org/10.5194/acp-15-9651-2015, https://doi.org/10.5194/acp-15-9651-2015, 2015
A. Hodzic, S. Madronich, P. S. Kasibhatla, G. Tyndall, B. Aumont, J. L. Jimenez, J. Lee-Taylor, and J. Orlando
Atmos. Chem. Phys., 15, 9253–9269, https://doi.org/10.5194/acp-15-9253-2015, https://doi.org/10.5194/acp-15-9253-2015, 2015
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Our study combines process and global chemistry modeling to investigate the potential effect of gas- and particle-phase organic photolysis reactions on the formation and lifetime of secondary organic aerosols (SOAs). Photolysis of the oxidation intermediates that partition between gas and particle phases to form SOA is not included in 3D models. Our results suggest that exposure to UV light can suppress the formation of SOA or even lead to its substantial loss (comparable to wet deposition).
N. L. Wagner, C. A. Brock, W. M. Angevine, A. Beyersdorf, P. Campuzano-Jost, D. Day, J. A. de Gouw, G. S. Diskin, T. D. Gordon, M. G. Graus, J. S. Holloway, G. Huey, J. L. Jimenez, D. A. Lack, J. Liao, X. Liu, M. Z. Markovic, A. M. Middlebrook, T. Mikoviny, J. Peischl, A. E. Perring, M. S. Richardson, T. B. Ryerson, J. P. Schwarz, C. Warneke, A. Welti, A. Wisthaler, L. D. Ziemba, and D. M. Murphy
Atmos. Chem. Phys., 15, 7085–7102, https://doi.org/10.5194/acp-15-7085-2015, https://doi.org/10.5194/acp-15-7085-2015, 2015
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This paper investigates the summertime vertical profile of aerosol over the southeastern US using in situ measurements collected from aircraft. We use a vertical mixing model and measurements of CO to predict the vertical profile of aerosol that we would expect from vertical mixing alone and compare with the observed aerosol profile. We found a modest enhancement of aerosol in the cloudy transition layer during shallow cumulus convection and attribute the enhancement to local aerosol formation.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
R. Thalman, M. T. Baeza-Romero, S. M. Ball, E. Borrás, M. J. S. Daniels, I. C. A. Goodall, S. B. Henry, T. Karl, F. N. Keutsch, S. Kim, J. Mak, P. S. Monks, A. Muñoz, J. Orlando, S. Peppe, A. R. Rickard, M. Ródenas, P. Sánchez, R. Seco, L. Su, G. Tyndall, M. Vázquez, T. Vera, E. Waxman, and R. Volkamer
Atmos. Meas. Tech., 8, 1835–1862, https://doi.org/10.5194/amt-8-1835-2015, https://doi.org/10.5194/amt-8-1835-2015, 2015
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Measurements of α-dicarbonyl compounds, like glyoxal (CHOCHO) and methyl glyoxal (CH3C(O)CHO), are informative about the rate of hydrocarbon oxidation, oxidative capacity, and secondary organic aerosol (SOA) formation in the atmosphere. We have compared nine instruments and seven techniques to measure α-dicarbonyl, using simulation chamber facilities in the US and Europe. We assess our understanding of calibration, precision, accuracy and detection limits, as well as possible sampling biases.
P. K. Peterson, W. R. Simpson, K. A. Pratt, P. B. Shepson, U. Frieß, J. Zielcke, U. Platt, S. J. Walsh, and S. V. Nghiem
Atmos. Chem. Phys., 15, 2119–2137, https://doi.org/10.5194/acp-15-2119-2015, https://doi.org/10.5194/acp-15-2119-2015, 2015
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We developed methods to measure the vertical distribution of bromine monoxide, a gas that oxidizes pollutants, above sea ice based upon MAX-DOAS observations from Barrow, Alaska, and find that atmospheric stability exerts a strong control on BrO's vertical distribution. Specifically, more stable (temperature inversion) situations result in BrO being closer to the ground while more neutral (not inverted) atmospheres allow BrO to ascend further aloft and grow to larger column abundance.
S. General, D. Pöhler, H. Sihler, N. Bobrowski, U. Frieß, J. Zielcke, M. Horbanski, P. B. Shepson, B. H. Stirm, W. R. Simpson, K. Weber, C. Fischer, and U. Platt
Atmos. Meas. Tech., 7, 3459–3485, https://doi.org/10.5194/amt-7-3459-2014, https://doi.org/10.5194/amt-7-3459-2014, 2014
M. O. L. Cambaliza, P. B. Shepson, D. R. Caulton, B. Stirm, D. Samarov, K. R. Gurney, J. Turnbull, K. J. Davis, A. Possolo, A. Karion, C. Sweeney, B. Moser, A. Hendricks, T. Lauvaux, K. Mays, J. Whetstone, J. Huang, I. Razlivanov, N. L. Miles, and S. J. Richardson
Atmos. Chem. Phys., 14, 9029–9050, https://doi.org/10.5194/acp-14-9029-2014, https://doi.org/10.5194/acp-14-9029-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
C. Knote, A. Hodzic, J. L. Jimenez, R. Volkamer, J. J. Orlando, S. Baidar, J. Brioude, J. Fast, D. R. Gentner, A. H. Goldstein, P. L. Hayes, W. B. Knighton, H. Oetjen, A. Setyan, H. Stark, R. Thalman, G. Tyndall, R. Washenfelder, E. Waxman, and Q. Zhang
Atmos. Chem. Phys., 14, 6213–6239, https://doi.org/10.5194/acp-14-6213-2014, https://doi.org/10.5194/acp-14-6213-2014, 2014
J. W. Halfacre, T. N. Knepp, P. B. Shepson, C. R. Thompson, K. A. Pratt, B. Li, P. K. Peterson, S. J. Walsh, W. R. Simpson, P. A. Matrai, J. W. Bottenheim, S. Netcheva, D. K. Perovich, and A. Richter
Atmos. Chem. Phys., 14, 4875–4894, https://doi.org/10.5194/acp-14-4875-2014, https://doi.org/10.5194/acp-14-4875-2014, 2014
G. M. Wolfe, C. Cantrell, S. Kim, R. L. Mauldin III, T. Karl, P. Harley, A. Turnipseed, W. Zheng, F. Flocke, E. C. Apel, R. S. Hornbrook, S. R. Hall, K. Ullmann, S. B. Henry, J. P. DiGangi, E. S. Boyle, L. Kaser, R. Schnitzhofer, A. Hansel, M. Graus, Y. Nakashima, Y. Kajii, A. Guenther, and F. N. Keutsch
Atmos. Chem. Phys., 14, 4715–4732, https://doi.org/10.5194/acp-14-4715-2014, https://doi.org/10.5194/acp-14-4715-2014, 2014
J. D. Rindelaub, K. M. McAvey, and P. B. Shepson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-3301-2014, https://doi.org/10.5194/acpd-14-3301-2014, 2014
Revised manuscript not accepted
J. L. Fry, D. C. Draper, K. J. Zarzana, P. Campuzano-Jost, D. A. Day, J. L. Jimenez, S. S. Brown, R. C. Cohen, L. Kaser, A. Hansel, L. Cappellin, T. Karl, A. Hodzic Roux, A. Turnipseed, C. Cantrell, B. L. Lefer, and N. Grossberg
Atmos. Chem. Phys., 13, 8585–8605, https://doi.org/10.5194/acp-13-8585-2013, https://doi.org/10.5194/acp-13-8585-2013, 2013
S. M. Griffith, R. F. Hansen, S. Dusanter, P. S. Stevens, M. Alaghmand, S. B. Bertman, M. A. Carroll, M. Erickson, M. Galloway, N. Grossberg, J. Hottle, J. Hou, B. T. Jobson, A. Kammrath, F. N. Keutsch, B. L. Lefer, L. H. Mielke, A. O'Brien, P. B. Shepson, M. Thurlow, W. Wallace, N. Zhang, and X. L. Zhou
Atmos. Chem. Phys., 13, 5403–5423, https://doi.org/10.5194/acp-13-5403-2013, https://doi.org/10.5194/acp-13-5403-2013, 2013
E. C. Browne, K.-E. Min, P. J. Wooldridge, E. Apel, D. R. Blake, W. H. Brune, C. A. Cantrell, M. J. Cubison, G. S. Diskin, J. L. Jimenez, A. J. Weinheimer, P. O. Wennberg, A. Wisthaler, and R. C. Cohen
Atmos. Chem. Phys., 13, 4543–4562, https://doi.org/10.5194/acp-13-4543-2013, https://doi.org/10.5194/acp-13-4543-2013, 2013
L. Kaser, T. Karl, R. Schnitzhofer, M. Graus, I. S. Herdlinger-Blatt, J. P. DiGangi, B. Sive, A. Turnipseed, R. S. Hornbrook, W. Zheng, F. M. Flocke, A. Guenther, F. N. Keutsch, E. Apel, and A. Hansel
Atmos. Chem. Phys., 13, 2893–2906, https://doi.org/10.5194/acp-13-2893-2013, https://doi.org/10.5194/acp-13-2893-2013, 2013
M. Huang, G. R. Carmichael, T. Chai, R. B. Pierce, S. J. Oltmans, D. A. Jaffe, K. W. Bowman, A. Kaduwela, C. Cai, S. N. Spak, A. J. Weinheimer, L. G. Huey, and G. S. Diskin
Atmos. Chem. Phys., 13, 359–391, https://doi.org/10.5194/acp-13-359-2013, https://doi.org/10.5194/acp-13-359-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Surface ozone trend variability across the United States and the impact of heatwaves (1990–2023)
Opinion: Challenges and needs of tropospheric chemical mechanism development
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Tropospheric ozone precursors: global and regional distributions, trends, and variability
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Local and transboundary contributions to nitrogen loadings across East Asia using CMAQ-ISAM and GEMS-informed emissions inventory during the winter-spring transition
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Revisiting the high tropospheric ozone over Southern Africa: overestimated biomass burning and underestimated anthropogenic emissions
Source contribution to ozone pollution during June 2021 in Arizona: Insights from WRF-Chem tagged O3 and CO
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Estimating the variability of NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations: a case study of the 2019 Raikoke eruption
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over South and East Asia
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
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Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
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We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
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Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
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Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
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We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
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The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
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This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
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We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonné, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
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Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching −35°C are required to reproduce observed NOx.
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.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
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Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
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The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
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In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
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Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
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This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
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Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
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Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
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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.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Kai-Lan Chang, Brian C. McDonald, and Owen R. Cooper
EGUsphere, https://doi.org/10.5194/egusphere-2024-3674, https://doi.org/10.5194/egusphere-2024-3674, 2024
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Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over 1990–2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heatwave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
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Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O.T. Pye
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
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We develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
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Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 2024
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We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to explain the weaker hourly variation in NO2 columns than at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
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We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
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Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 2024
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Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 2024
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We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show that SF6 emissions are decreasing in the USA and in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
EGUsphere, https://doi.org/10.5194/egusphere-2024-3464, https://doi.org/10.5194/egusphere-2024-3464, 2024
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We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants, which may influence future approaches to modeling climate.
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3079, https://doi.org/10.5194/egusphere-2024-3079, 2024
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Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs for different amounts of leakages, where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
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We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
EGUsphere, https://doi.org/10.5194/egusphere-2024-3312, https://doi.org/10.5194/egusphere-2024-3312, 2024
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We investigated NOx emissions’ contributions to nitrogen loadings across five regions of East Asia during the 2022 winter-spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
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In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
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This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
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Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
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Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
EGUsphere, https://doi.org/10.5194/egusphere-2024-2912, https://doi.org/10.5194/egusphere-2024-2912, 2024
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Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimise these natural emissions over Africa in 2019. Our approach led to an increase in natural emissions that is supported by independent data showing that current estimates are underestimated.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
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Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2576, https://doi.org/10.5194/egusphere-2024-2576, 2024
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The impact of biomass burning and anthropogenic emissions on high tropospheric ozone was not well studied in Southern Africa. We combined the model simulation with recent observations at the surface and from space to quantify tropospheric ozone and its main drivers in Southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in Southern Africa.
Yafang Guo, Mohammad Amin Mirrezaei, Armin Sorooshian, and Avelino F. Arellano
EGUsphere, https://doi.org/10.5194/egusphere-2024-2617, https://doi.org/10.5194/egusphere-2024-2617, 2024
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We assess the contributions of fire and anthropogenic emissions to O3 levels in Phoenix Arizona during a period of intense heat and drought conditions. We find that fire exacerbates O3 pollution and that interactions between weather, climate, and air chemistry are important to consider. This has implications to activities related to formulating emission reduction strategies in areas that are currently under-studied yet becoming relevant due to reports of increasing global aridity.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2500, https://doi.org/10.5194/egusphere-2024-2500, 2024
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Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of ozone and large-scale circulations such as atmospheric blocking. In addition to local heatwave effects, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation play in regional air quality.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
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Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
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Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2596, https://doi.org/10.5194/egusphere-2024-2596, 2024
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We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
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Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
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The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
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Domine, F., Bock, J., Voisin, D., and Donaldson, D. J.: Can We Model Snow Photochemistry? Problems with the Current Approaches, J. Phys. Chem., A, 117, 4733–4749, https://doi.org/10.1021/jp3123314, 2013.
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Short summary
The generally accepted mechanism leading to ozone depletion events in the Arctic assumes efficient gas-phase recycling of bromine atoms, such that the rate of ozone depletion has often been estimated as the rate that Br atoms regenerate through gas-phase BrO + BrO and BrO + ClO reactions. Using a large suite of data from the OASIS2009 campaign, our modeling results show that the gas-phase regeneration of Br is less efficient than expected and that heterogeneous recycling on surfaces is critical.
The generally accepted mechanism leading to ozone depletion events in the Arctic assumes...
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