Articles | Volume 24, issue 16
https://doi.org/10.5194/acp-24-9615-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-9615-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
30 Aug 2024
Research article |
| 30 Aug 2024
| 30 Aug 2024
Elevated oxidized mercury in the free troposphere: analytical advances and application at a remote continental mountaintop site
Eleanor J. Derry
Chemistry Department, Reed College, Portland, OR 97202, USA
Tyler R. Elgiar
Bingham Research Center, Utah State University, Vernal, UT 84078, USA
current address: Bureau of Land Management, Vernal, UT 84078, USA
Taylor Y. Wilmot
Department of Atmospheric Sciences, University of Utah, Salt Lake City, UT 84112, USA
Nicholas W. Hoch
Environmental Studies Program, Colorado College, Colorado Springs, CO 80903, USA
current address: BBA Water Consultants, Inc., Englewood, CO 80110, USA
Noah S. Hirshorn
Department of Atmospheric Sciences, University of Utah, Salt Lake City, UT 84112, USA
current address: Ramboll, New York, NY 10119, USA
Peter Weiss-Penzias
Department of Microbiology and Environmental Toxicology, University of California, Santa Cruz, Santa Cruz, CA 95064, USA
Christopher F. Lee
Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
CIRES, University of Colorado Boulder, Boulder, CO 80309, USA
John C. Lin
Department of Atmospheric Sciences, University of Utah, Salt Lake City, UT 84112, USA
A. Gannet Hallar
Storm Peak Laboratory, Department of Atmospheric Sciences, University of Utah, Salt Lake City, UT 84112, USA
Rainer Volkamer
Department of Chemistry, University of Colorado Boulder, Boulder, CO 80309, USA
CIRES, University of Colorado Boulder, Boulder, CO 80309, USA
Seth N. Lyman
Bingham Research Center, Utah State University, Vernal, UT 84078, USA
Chemistry and Biochemistry Department, Utah State University, Logan, UT 84322, USA
Chemistry Department, Reed College, Portland, OR 97202, USA
Environmental Studies Program, Reed College, Portland, OR 97202, USA
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Allison R. Moon, Leyang Liu, Xuan Wang, Yuk-Chun Chan, Alyson Fritzmann, Ryan Pound, Amy Lees, Lewis Marden, Mat Evans, Lucy J. Carpenter, Jochen Stutz, Joel A. Thornton, Gordon Novak, Andrew Rollins, Gregory P. Schill, Xu-cheng He, Henning Finkenzeller, Margarita Reza, Rainer Volkamer, Kelvin H. Bates, Alfonso Saiz-Lopez, Anoop S. Mahajan, and Becky Alexander
EGUsphere, https://doi.org/10.5194/egusphere-2025-4725, https://doi.org/10.5194/egusphere-2025-4725, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Global chemical transport models previously treated aerosols as a sink for reactive iodine (Iy); however, aerosol iodide is also a source of Iy via heterogeneous reactions involving hypohalous acids and halogen nitrates. We implemented this chemistry into GEOS-Chem, in addition to explicitly representing three aerosol iodine types: soluble organic iodine (SOI), iodide, and iodate. We found that aerosol recycling of iodide to form Iy is more than twice as fast as the other Iy sources combined.
Larissa Lacher, A. Gannet Hallar, Ian B. McCubbin, Joey Bail, Karl D. Froyd, Justin Jacquot, Xiaoli Shen, Christopher Rapp, Ottmar Möhler, and Daniel Cziczo
EGUsphere, https://doi.org/10.5194/egusphere-2025-4492, https://doi.org/10.5194/egusphere-2025-4492, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We observe a trend of increasing ice-nucleating particle (INP) concentration in spring in the Rocky Mountains, related to regional dust emissions that may intensify with climate change. Additionally, super-micrometer particles were found as the most important contributors to the INP population. This finding was partly enabled by a novel setup of the Portable Ice Nucleation Experiment (PINE), coupled with a pumped-counterflow virtual impactor allowing for direct analysis of INP properties.
Yugo Kanaya, Roberto Sommariva, Alfonso Saiz-Lopez, Andrea Mazzeo, Theodore K. Koenig, Kaori Kawana, James E. Johnson, Aurélie Colomb, Pierre Tulet, Suzie Molloy, Ian E. Galbally, Rainer Volkamer, Anoop Mahajan, John W. Halfacre, Paul B. Shepson, Julia Schmale, Hélène Angot, Byron Blomquist, Matthew D. Shupe, Detlev Helmig, Junsu Gil, Meehye Lee, Sean C. Coburn, Ivan Ortega, Gao Chen, James Lee, Kenneth C. Aikin, David D. Parrish, John S. Holloway, Thomas B. Ryerson, Ilana B. Pollack, Eric J. Williams, Brian M. Lerner, Andrew J. Weinheimer, Teresa Campos, Frank M. Flocke, J. Ryan Spackman, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Ralf M. Staebler, Amir A. Aliabadi, Wanmin Gong, Roeland Van Malderen, Anne M. Thompson, Ryan M. Stauffer, Debra E. Kollonige, Juan Carlos Gómez Martin, Masatomo Fujiwara, Katie Read, Matthew Rowlinson, Keiichi Sato, Junichi Kurokawa, Yoko Iwamoto, Fumikazu Taketani, Hisahiro Takashima, Mónica Navarro-Comas, Marios Panagi, and Martin G. Schultz
Earth Syst. Sci. Data, 17, 4901–4932, https://doi.org/10.5194/essd-17-4901-2025, https://doi.org/10.5194/essd-17-4901-2025, 2025
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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 11–16 % in the tropics, while near-zero depletions are rare, unlike in the Arctic, implying different mechanisms.
Marc L. Mansfield and Seth N. Lyman
Atmos. Chem. Phys., 25, 11261–11274, https://doi.org/10.5194/acp-25-11261-2025, https://doi.org/10.5194/acp-25-11261-2025, 2025
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Precursor compounds must be present in the lower atmosphere for ozone to form. Ozone abatement strategies focus on reducing such precursors, but measuring and modeling are necessary to determine the most efficient way to do this. We show that the sensitivity of ozone to various precursors changes over the course of the winter. We also argue that similar seasonal changes probably occur in many regions of the Northern Hemisphere.
Neil M. Donahue, Victoria Hofbauer, Henning Finkenzeller, Dominik Stolzenburg, Paulus S. Bauer, Randall Chiu, Lubna Dada, Jonathan Duplissy, Xu-Cheng He, Martin Heinritzi, Christopher R. Hoyle, Andreas Kürten, Aleksandr Kvashnin, Katrianne Lehtipalo, Naser Mahfouz, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Mario Simon, Andrea C. Wagner, Mingyi Wang, Chao Yan, Penglin Ye, Ilona Riipinen, Hamish Gordon, Joachim Curtius, Armin Hansel, Imad El Haddad, Markku Kulmala, Douglas R. Worsnop, Rainer Volkamer, Paul M. Winkler, Jasper Kirkby, and Richard Flagan
EGUsphere, https://doi.org/10.5194/egusphere-2025-2412, https://doi.org/10.5194/egusphere-2025-2412, 2025
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We describe accurate measurement of particle formation and growth in the CERN CLOUD chamber, using a suite of gas- and particle-phase instruments. The interconnected measurements establish high accuracy in key particle properties and critically important gas-phase sulfuric acid. This is a template for accurate calibration of similar experiments and thus accurate determination of aerosol nucleation and growth rates, which are an important source of uncertainty in climate science.
Dongwook Kim, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Da Yang, Suresh Dhaniyala, Leah Williams, Philip Croteau, John Jayne, Douglas Worsnop, Rainer Volkamer, and Jose L. Jimenez
Aerosol Research, 3, 371–404, https://doi.org/10.5194/ar-3-371-2025, https://doi.org/10.5194/ar-3-371-2025, 2025
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Quantitative real-time aerosol sampling on board aircraft platforms is challenging, especially at higher altitudes. Herein, we present comprehensive analyses of a new aircraft inlet system and tools for aerosol beam diagnostics for aerosol mass spectrometers (AMSs). The beam focusing of aerodynamic lenses and the thermal decomposition on the vaporizer were investigated. The new inlet system can be operated at higher altitudes while sampling aerosols over a broader size range than previous versions.
Tyler R. Elgiar, Lynne Gratz, A. Gannet Hallar, Rainer Volkamer, and Seth N. Lyman
EGUsphere, https://doi.org/10.5194/egusphere-2025-977, https://doi.org/10.5194/egusphere-2025-977, 2025
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This manuscript compares verified atmospheric mercury measurements against output from the GEOS-Chem 3D photochemical transport model. It shows that the model is unable to reproduce measured atmospheric oxidized mercury concentrations, even in several cases where oxidation rates in the model are enhanced.
Paul J. DeMott, Jessica A. Mirrielees, Sarah Suda Petters, Daniel J. Cziczo, Markus D. Petters, Heinz G. Bingemer, Thomas C. J. Hill, Karl Froyd, Sarvesh Garimella, A. Gannet Hallar, Ezra J. T. Levin, Ian B. McCubbin, Anne E. Perring, Christopher N. Rapp, Thea Schiebel, Jann Schrod, Kaitlyn J. Suski, Daniel Weber, Martin J. Wolf, Maria Zawadowicz, Jake Zenker, Ottmar Möhler, and Sarah D. Brooks
Atmos. Meas. Tech., 18, 639–672, https://doi.org/10.5194/amt-18-639-2025, https://doi.org/10.5194/amt-18-639-2025, 2025
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The Fifth International Ice Nucleation Workshop Phase 3 (FIN-03) compared the ambient atmospheric performance of ice-nucleating particle (INP) measuring systems and explored general methods for discerning atmospheric INP compositions. Mirroring laboratory results, INP concentrations agreed within 5–10 factors. Measurements of total aerosol properties and investigations of INP compositions supported a dominant role of soil and plant organic aerosol elements as INPs during the study.
Livia Lown, Sarrah M. Dunham-Cheatham, Seth N. Lyman, and Mae S. Gustin
Atmos. Meas. Tech., 17, 6397–6413, https://doi.org/10.5194/amt-17-6397-2024, https://doi.org/10.5194/amt-17-6397-2024, 2024
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New sorbent materials are needed to preconcentrate atmospheric oxidized mercury for analysis by developing mass spectrometry methods. Chitosan, α-Al2O3, and γ-Al2O3 were tested for quantitative gaseous oxidized mercury sorption in ambient air under laboratory and field conditions. Although these materials sorbed gaseous oxidized mercury without sorbing elemental mercury in the laboratory, less oxidized mercury was recovered from these materials compared to cation exchange membranes in the field.
Theodore K. Koenig, François Hendrick, Douglas Kinnison, Christopher F. Lee, Michel Van Roozendael, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5911–5934, https://doi.org/10.5194/amt-17-5911-2024, https://doi.org/10.5194/amt-17-5911-2024, 2024
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Atmospheric bromine destroys ozone, impacts oxidation capacity, and oxidizes mercury into its toxic form. We constrain bromine by remote sensing of BrO from a mountaintop. Previous measurements retrieved two to three pieces of information vertically; we apply new methods to get five and a half vertically and two more in time. We compare with aircraft measurements to validate the methods and look at variations in BrO over the Pacific.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
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The ozone sink into oceans and marine clouds is seldom studied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure eddy covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller and spatially variable.
Da Yang, Emmanuel Assaf, Roy Mauldin, Suresh Dhaniyala, and Rainer Volkamer
EGUsphere, https://doi.org/10.5194/egusphere-2024-2390, https://doi.org/10.5194/egusphere-2024-2390, 2024
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Sulfuric acid forms particles in the atmosphere, but the airborne sampling faces challenges due to vapor losses in inlet lines. An innovative aircraft sampling system to sample sulfuric acid from the sea surface into the lower stratosphere (0–15 km) is described and characterized. Our results challenge the widely held view that laminar core sampling is the best strategy to sample condensable vapors, and identify better strategies to sample condensable vapors.
Murat Aydin, Melinda R. Nicewonger, Gregory L. Britten, Dominic Winski, Mary Whelan, John D. Patterson, Erich Osterberg, Christopher F. Lee, Tara Harder, Kyle J. Callahan, David Ferris, and Eric S. Saltzman
Clim. Past, 20, 1885–1917, https://doi.org/10.5194/cp-20-1885-2024, https://doi.org/10.5194/cp-20-1885-2024, 2024
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We present a new ice core carbonyl sulfide (COS) record from the South Pole, Antarctica, yielding a 52 000-year atmospheric record after correction for production in the ice sheet. The results display a large increase in atmospheric COS concurrent with the last deglaciation. The deglacial COS rise results from an overall strengthening of atmospheric COS sources, implying a large increase in ocean sulfur gas emissions. Atmospheric sulfur gases have negative climate feedbacks.
Da Yang, Margarita Reza, Roy Mauldin, Rainer Volkamer, and Suresh Dhaniyala
Atmos. Meas. Tech., 17, 1463–1474, https://doi.org/10.5194/amt-17-1463-2024, https://doi.org/10.5194/amt-17-1463-2024, 2024
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This paper evaluates the performance of an aircraft gas inlet. Here, we use computational fluid dynamics (CFD) and experiments to demonstrate the role of turbulence in determining sampling performance of a gas inlet and identify ideal conditions for inlet operation to minimize gas loss. Experiments conducted in a high-speed wind tunnel under near-aircraft speeds validated numerical results. We believe that the results obtained from this work will greatly inform future gas inlet studies.
Dien Wu, Joshua L. Laughner, Junjie Liu, Paul I. Palmer, John C. Lin, and Paul O. Wennberg
Geosci. Model Dev., 16, 6161–6185, https://doi.org/10.5194/gmd-16-6161-2023, https://doi.org/10.5194/gmd-16-6161-2023, 2023
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To balance computational expenses and chemical complexity in extracting emission signals from tropospheric NO2 columns, we propose a simplified non-linear Lagrangian chemistry transport model and assess its performance against TROPOMI v2 over power plants and cities. Using this model, we then discuss how NOx chemistry affects the relationship between NOx and CO2 emissions and how studying NO2 columns helps quantify modeled biases in wind directions and prior emissions.
Tobias Borsdorff, Teresa Campos, Natalie Kille, Kyle J. Zarzana, Rainer Volkamer, and Jochen Landgraf
Atmos. Meas. Tech., 16, 3027–3038, https://doi.org/10.5194/amt-16-3027-2023, https://doi.org/10.5194/amt-16-3027-2023, 2023
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ECMWF plans to assimilate TROPOMI CO with their CAMS-IFS model. This will constrain the total column and the vertical CO distribution of the model. To show this, we combine individual TROPOMI CO column retrievals with different vertical sensitivities and obtain a vertical CO concentration profile. We test the approach on three CO pollution events in comparison with CAMS-IFS simulations that do not assimilate TROPOMI CO data and in situ airborne measurements of the BB-FLUX campaign.
Noah S. Hirshorn, Lauren M. Zuromski, Christopher Rapp, Ian McCubbin, Gerardo Carrillo-Cardenas, Fangqun Yu, and A. Gannet Hallar
Atmos. Chem. Phys., 22, 15909–15924, https://doi.org/10.5194/acp-22-15909-2022, https://doi.org/10.5194/acp-22-15909-2022, 2022
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New particle formation (NPF) is a source of atmospheric aerosol number concentration that can impact climate by growing to larger sizes and under proper conditions form cloud condensation nuclei (CCN). Using novel methods, we find that at Storm Peak Laboratory, a remote, mountaintop site in Colorado, NPF is observed to enhance CCN concentrations in the spring by a factor of 1.54 and in the winter by a factor of 1.36 which can occur on a regional scale having important climate implications.
Anna L. Hodshire, Ezra J. T. Levin, A. Gannet Hallar, Christopher N. Rapp, Dan R. Gilchrist, Ian McCubbin, and Gavin R. McMeeking
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-216, https://doi.org/10.5194/amt-2022-216, 2022
Publication in AMT not foreseen
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The new Continuous Flow Diffusion Chamber-Ice Activation Spectrometer collected 4 months of ice nucleating particle (INP) measurements at a 5-minute resolution at the mountainside Storm Peak Laboratory. Most long-term INP measurements are at a time resolution of a day or longer: our instrument is a promising advance towards high-resolution long-term INP measurements. We observe higher peak INP concentrations than previous mountain studies, possibly due to the higher time resolution of our data.
Libby Koolik, Michael Roesch, Carmen Dameto de Espana, Christopher Nathan Rapp, Lesly J. Franco Deloya, Chuanyang Shen, A. Gannet Hallar, Ian B. McCubbin, and Daniel J. Cziczo
Atmos. Meas. Tech., 15, 3213–3222, https://doi.org/10.5194/amt-15-3213-2022, https://doi.org/10.5194/amt-15-3213-2022, 2022
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A new inlet for studying the small particles, droplets, and ice crystals that constitute mixed-phase clouds has been constructed and is described here. This new inlet was tested in the laboratory. We present the performance of the new inlet to demonstrate its capability of separating ice, droplets, and small particles.
Dustin Roten, John C. Lin, Lewis Kunik, Derek Mallia, Dien Wu, Tomohiro Oda, and Eric A. Kort
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-315, https://doi.org/10.5194/acp-2022-315, 2022
Revised manuscript not accepted
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The systems used to monitor carbon dioxide (CO2) emissions from urban areas provides a means to observe and quantify emissions reductions from policy-related reduction efforts. Space-based instruments, such as NASA's Orbiting Carbon Observatory-3 (OCO-3), provides detailed "snapshots" of CO2 emissions from many megacities around the world. This work quantifies the amount of emission "information" contained in these snapshots and uses this information to update previous estimates of urban CO2.
Anna L. Hodshire, Ezra J. T. Levin, A. Gannet Hallar, Christopher N. Rapp, Dan R. Gilchrist, Ian McCubbin, and Gavin R. McMeeking
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-29, https://doi.org/10.5194/acp-2022-29, 2022
Preprint withdrawn
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The new Continuous Flow Diffusion Chamber-Ice Activation Spectrometer collected 4 months of ice nucleating particle (INP) measurements at a 5-minute resolution at the mountainside Storm Peak Laboratory. Most long-term INP measurements are at a time resolution of a day or longer: our instrument is a promising advance towards high-resolution long-term INP measurements. We observe higher peak INP concentrations than previous mountain studies, possibly due to the higher time resolution of our data.
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.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Debora Griffin, Chris A. McLinden, Enrico Dammers, Cristen Adams, Chelsea E. Stockwell, Carsten Warneke, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Kyle J. Zarzana, Jake P. Rowe, Rainer Volkamer, Christoph Knote, Natalie Kille, Theodore K. Koenig, Christopher F. Lee, Drew Rollins, Pamela S. Rickly, Jack Chen, Lukas Fehr, Adam Bourassa, Doug Degenstein, Katherine Hayden, Cristian Mihele, Sumi N. Wren, John Liggio, Ayodeji Akingunola, and Paul Makar
Atmos. Meas. Tech., 14, 7929–7957, https://doi.org/10.5194/amt-14-7929-2021, https://doi.org/10.5194/amt-14-7929-2021, 2021
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Satellite-derived NOx emissions from biomass burning are estimated with TROPOMI observations. Two common emission estimation methods are applied, and sensitivity tests with model output were performed to determine the accuracy of these methods. The effect of smoke aerosols on TROPOMI NO2 columns is estimated and compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
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Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Sharmine Akter Simu, Yuzo Miyazaki, Eri Tachibana, Henning Finkenzeller, Jérôme Brioude, Aurélie Colomb, Olivier Magand, Bert Verreyken, Stephanie Evan, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 21, 17017–17029, https://doi.org/10.5194/acp-21-17017-2021, https://doi.org/10.5194/acp-21-17017-2021, 2021
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The tropical Indian Ocean (IO) is expected to be a significant source of water-soluble organic carbon (WSOC), which is relevant to cloud formation. Our study showed that marine secondary organic formation dominantly contributed to the aerosol WSOC mass at the high-altitude observatory in the southwest IO in the wet season in both marine boundary layer and free troposphere (FT). This suggests that the effect of marine secondary sources is important up to FT, a process missing in climate models.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
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 %.
Dien Wu, John C. Lin, Henrique F. Duarte, Vineet Yadav, Nicholas C. Parazoo, Tomohiro Oda, and Eric A. Kort
Geosci. Model Dev., 14, 3633–3661, https://doi.org/10.5194/gmd-14-3633-2021, https://doi.org/10.5194/gmd-14-3633-2021, 2021
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A model (SMUrF) is presented that estimates biogenic CO2 fluxes over cities around the globe to separate out biogenic fluxes from anthropogenic emissions. The model leverages satellite-based solar-induced fluorescence data and a machine-learning technique. We evaluate the biogenic fluxes against flux observations and show contrasts between biogenic and anthropogenic fluxes over cities, revealing urban–rural flux gradients, diurnal cycles, and the resulting imprints on atmospheric-column CO2.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Amy Hrdina, Jennifer G. Murphy, Anna Gannet Hallar, John C. Lin, Alexander Moravek, Ryan Bares, Ross C. Petersen, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Munkh Baasandorj, and Steven S. Brown
Atmos. Chem. Phys., 21, 8111–8126, https://doi.org/10.5194/acp-21-8111-2021, https://doi.org/10.5194/acp-21-8111-2021, 2021
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Wintertime air pollution in the Salt Lake Valley is primarily composed of ammonium nitrate, which is formed when gas-phase ammonia and nitric acid react. The major point in this work is that the chemical composition of snow tells a very different story to what we measured in the atmosphere. With the dust–sea salt cations observed in PM2.5 and particle sizing data, we can estimate how much nitric acid may be lost to dust–sea salt that is not accounted for and how much more PM2.5 this could form.
Bert Verreyken, Crist Amelynck, Jérôme Brioude, Jean-François Müller, Niels Schoon, Nicolas Kumps, Aurélie Colomb, Jean-Marc Metzger, Christopher F. Lee, Theodore K. Koenig, Rainer Volkamer, and Trissevgeni Stavrakou
Atmos. Chem. Phys., 20, 14821–14845, https://doi.org/10.5194/acp-20-14821-2020, https://doi.org/10.5194/acp-20-14821-2020, 2020
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Biomass burning (BB) plumes arriving at the Maïdo observatory located in the south-west Indian Ocean during August 2018 and August 2019 are studied using trace gas measurements, Lagrangian transport models and the CAMS near-real-time atmospheric composition service. We investigate (i) secondary production of volatile organic compounds during transport, (ii) efficacy of the CAMS model to reproduce the chemical makeup of BB plumes and (iii) the impact of BB on the remote marine boundary layer.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
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Short summary
Mercury (Hg) is a globally distributed neurotoxic pollutant. Atmospheric deposition is the main source of Hg in ecosystems. However, measurement biases hinder understanding of the origins and abundance of the more bioavailable oxidized form. We used an improved, calibrated measurement system to study air mass composition and transport of atmospheric Hg at a remote mountaintop site in the central US. Oxidized Hg originated upwind in the low to middle free troposphere under clean, dry conditions.
Mercury (Hg) is a globally distributed neurotoxic pollutant. Atmospheric deposition is the main...
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