Articles | Volume 21, issue 19
https://doi.org/10.5194/acp-21-15153-2021
© Author(s) 2021. 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-21-15153-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Oct 2021
Research article |
| 12 Oct 2021
| 12 Oct 2021
Temporary pause in the growth of atmospheric ethane and propane in 2015–2018
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Extreme Environments Research Laboratory, École Polytechnique
Fédérale de Lausanne (EPFL) Valais Wallis, Sion, Switzerland
Connor Davel
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Christine Wiedinmyer
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
Gabrielle Pétron
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
NOAA, Global Monitoring Laboratory (GML), Earth System Research
Laboratories, Boulder, CO, USA
Jashan Chopra
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Jacques Hueber
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Boulder A.I.R. LLC, Boulder, CO, USA
Brendan Blanchard
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Ilann Bourgeois
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
NOAA, Chemical Sciences Laboratory (CSL), Earth System Research
Laboratories, Boulder, CO, USA
Isaac Vimont
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
Stephen A. Montzka
NOAA, Global Monitoring Laboratory (GML), Earth System Research
Laboratories, Boulder, CO, USA
Ben R. Miller
Cooperative Institute for Research in Environmental Sciences,
University of Colorado Boulder, Boulder, CO, USA
NOAA, Global Monitoring Laboratory (GML), Earth System Research
Laboratories, Boulder, CO, USA
James W. Elkins
NOAA, Global Monitoring Laboratory (GML), Earth System Research
Laboratories, Boulder, CO, USA
Detlev Helmig
Institute of Arctic and Alpine Research, University of Colorado
Boulder, Boulder, CO, USA
Boulder A.I.R. LLC, Boulder, CO, USA
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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
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
John D. Patterson, Murat Aydin, Andrew M. Crotwell, Gabrielle Pétron, Jeffery P. Severinghaus, Paul B. Krummel, Ray L. Langenfelds, Vasilii V. Petrenko, and Eric S. Saltzman
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Atmospheric levels of molecular hydrogen (H2) can impact climate and air quality. Constraining past changes to atmospheric H2 is useful for understanding how H2 cycles through the Earth system and predicting the impacts of increasing anthropogenic emissions under the
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Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
EGUsphere, https://doi.org/10.5194/egusphere-2023-2625, https://doi.org/10.5194/egusphere-2023-2625, 2023
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Matthew James Rowlinson, Lucy Carpenter, Katie Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin Bates, Deltev Helmig, and Mat Evans
EGUsphere, https://doi.org/10.5194/egusphere-2023-2557, https://doi.org/10.5194/egusphere-2023-2557, 2023
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Ethane and propane are volatile organic compounds emitted during human activities which contribute to the formation of ozone, a greenhouse gas, and affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job at reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emission, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Benjamin Hmiel, Vasilii V. Petrenko, Christo Buizert, Andrew M. Smith, Michael N. Dyonisius, Philip Place, Bin Yang, Quan Hua, Ross Beaudette, Jeffrey P. Severinghaus, Christina Harth, Ray F. Weiss, Lindsey Davidge, Melisa Diaz, Matthew Pacicco, James A. Menking, Michael Kalk, Xavier Faïn, Alden Adolph, Isaac Vimont, and Lee T. Murray
The Cryosphere Discuss., https://doi.org/10.5194/tc-2023-121, https://doi.org/10.5194/tc-2023-121, 2023
Preprint under review for TC
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The main aim of this research is to improve understanding of carbon-14 that is produced by cosmic rays in ice sheets. Measurements of carbon-14 in ice cores can provide a range of useful information (age of ice, past atmospheric chemistry, past cosmic ray intensity). Our results show that almost all (approx. 95 %) of carbon-14 that is produced in the upper layer of ice sheets is rapidly lost to the atmosphere. Our results also provide better estimates of carbon-14 production rates in deeper ice.
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.
Christine Wiedinmyer, Yosuke Kimura, Elena C. McDonald-Buller, Louisa K. Emmons, Rebecca R. Buchholz, Wenfu Tang, Keenan Seto, Maxwell B. Joseph, Kelley C. Barsanti, Annmarie G. Carlton, and Robert Yokelson
Geosci. Model Dev., 16, 3873–3891, https://doi.org/10.5194/gmd-16-3873-2023, https://doi.org/10.5194/gmd-16-3873-2023, 2023
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The Fire INventory from NCAR (FINN) provides daily global estimates of emissions from open fires based on satellite detections of hot spots. This version has been updated to apply MODIS and VIIRS satellite fire detection and better represents both large and small fires. FINNv2.5 generates more emissions than FINNv1 and is in general agreement with other fire emissions inventories. The new estimates are consistent with satellite observations, but uncertainties remain regionally and by pollutant.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
EGUsphere, https://doi.org/10.5194/egusphere-2023-1133, https://doi.org/10.5194/egusphere-2023-1133, 2023
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The global budgets of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Michael N. Dyonisius, Vasilii V. Petrenko, Andrew M. Smith, Benjamin Hmiel, Peter D. Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah A. Shackleton, Christo Buizert, Philip F. Place, James A. Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi A. Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward J. Brook, Jeffrey P. Severinghaus, Ray F. Weiss, and Joseph R. McConnell
The Cryosphere, 17, 843–863, https://doi.org/10.5194/tc-17-843-2023, https://doi.org/10.5194/tc-17-843-2023, 2023
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Cosmic rays that enter the atmosphere produce secondary particles which react with surface minerals to produce radioactive nuclides. These nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with a well-known exposure history to constrain the production rates from muons. 14C production in ice is analogous to quartz, but we obtain different production rates compared to commonly used estimates.
Lei Hu, Deborah Ottinger, Stephanie Bogle, Stephen A. Montzka, Philip L. DeCola, Ed Dlugokencky, Arlyn Andrews, Kirk Thoning, Colm Sweeney, Geoff Dutton, Lauren Aepli, and Andrew Crotwell
Atmos. Chem. Phys., 23, 1437–1448, https://doi.org/10.5194/acp-23-1437-2023, https://doi.org/10.5194/acp-23-1437-2023, 2023
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Effective mitigation of greenhouse gas (GHG) emissions relies on an accurate understanding of emissions. Here we demonstrate the added value of using inventory- and atmosphere-based approaches for estimating US emissions of SF6, the most potent GHG known. The results suggest a large decline in US SF6 emissions, shed light on the possible processes causing the differences between the independent estimates, and identify opportunities for substantial additional emission reductions.
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.
Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Hélène Angot, Lauriane L. J. Quéléver, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoé Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Klenø Nøjgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petäjä, Mikko Sipilä, Julia Schmale, and Tuija Jokinen
Atmos. Chem. Phys., 23, 389–415, https://doi.org/10.5194/acp-23-389-2023, https://doi.org/10.5194/acp-23-389-2023, 2023
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The Arctic is a unique environment that is warming faster than other locations on Earth. We evaluate measurements of aerosol particles, which can influence climate, over the central Arctic Ocean for a full year and compare the data to land-based measurement stations across the Arctic. Our measurements show that the central Arctic has similarities to but also distinct differences from the stations further south. We note that this may change as the Arctic warms and sea ice continues to decline.
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.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Stijn Naus, Lucas G. Domingues, Maarten Krol, Ingrid T. Luijkx, Luciana V. Gatti, John B. Miller, Emanuel Gloor, Sourish Basu, Caio Correia, Gerbrand Koren, Helen M. Worden, Johannes Flemming, Gabrielle Pétron, and Wouter Peters
Atmos. Chem. Phys., 22, 14735–14750, https://doi.org/10.5194/acp-22-14735-2022, https://doi.org/10.5194/acp-22-14735-2022, 2022
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We assimilate MOPITT CO satellite data in the TM5-4D-Var inverse modelling framework to estimate Amazon fire CO emissions for 2003–2018. We show that fire emissions have decreased over the analysis period, coincident with a decrease in deforestation rates. However, interannual variations in fire emissions are large, and they correlate strongly with soil moisture. Our results reveal an important role for robust, top-down fire CO emissions in quantifying and attributing Amazon fire intensity.
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.
Vanessa Selimovic, Damien Ketcherside, Sreelekha Chaliyakunnel, Catherine Wielgasz, Wade Permar, Hélène Angot, Dylan B. Millet, Alan Fried, Detlev Helmig, and Lu Hu
Atmos. Chem. Phys., 22, 14037–14058, https://doi.org/10.5194/acp-22-14037-2022, https://doi.org/10.5194/acp-22-14037-2022, 2022
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Arctic warming has led to an increase in plants that emit gases in response to stress, but how these gases affect regional chemistry is largely unknown due to lack of observational data. Here we present the most comprehensive gas-phase measurements for this area to date and compare them to predictions from a global transport model. We report 78 gas-phase species and investigate their importance to atmospheric chemistry in the area, with broader implications for similar plant types.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
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The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
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.
Shang Liu, Barbara Barletta, Rebecca S. Hornbrook, Alan Fried, Jeff Peischl, Simone Meinardi, Matthew Coggon, Aaron Lamplugh, Jessica B. Gilman, Georgios I. Gkatzelis, Carsten Warneke, Eric C. Apel, Alan J. Hills, Ilann Bourgeois, James Walega, Petter Weibring, Dirk Richter, Toshihiro Kuwayama, Michael FitzGibbon, and Donald Blake
Atmos. Chem. Phys., 22, 10937–10954, https://doi.org/10.5194/acp-22-10937-2022, https://doi.org/10.5194/acp-22-10937-2022, 2022
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California’s ozone persistently exceeds the air quality standards. We studied the spatial distribution of volatile organic compounds (VOCs) that produce ozone over the most polluted regions in California using aircraft measurements. We find that the oxygenated VOCs have the highest ozone formation potential. Spatially, biogenic VOCs are important during high ozone episodes in the South Coast Air Basin, while dairy emissions may be critical for ozone production in San Joaquin Valley.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Ivo Beck, Hélène Angot, Andrea Baccarini, Lubna Dada, Lauriane Quéléver, Tuija Jokinen, Tiia Laurila, Markus Lampimäki, Nicolas Bukowiecki, Matthew Boyer, Xianda Gong, Martin Gysel-Beer, Tuukka Petäjä, Jian Wang, and Julia Schmale
Atmos. Meas. Tech., 15, 4195–4224, https://doi.org/10.5194/amt-15-4195-2022, https://doi.org/10.5194/amt-15-4195-2022, 2022
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We present the pollution detection algorithm (PDA), a new method to identify local primary pollution in remote atmospheric aerosol and trace gas time series. The PDA identifies periods of contaminated data and relies only on the target dataset itself; i.e., it is independent of ancillary data such as meteorological variables. The parameters of all pollution identification steps are adjustable so that the PDA can be tuned to different locations and situations. It is available as open-access code.
Linghan Zeng, Jack Dibb, Eric Scheuer, Joseph M. Katich, Joshua P. Schwarz, Ilann Bourgeois, Jeff Peischl, Tom Ryerson, Carsten Warneke, Anne E. Perring, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Richard H. Moore, Elizabeth B. Wiggins, Demetrios Pagonis, Hongyu Guo, Pedro Campuzano-Jost, Jose L. Jimenez, Lu Xu, and Rodney J. Weber
Atmos. Chem. Phys., 22, 8009–8036, https://doi.org/10.5194/acp-22-8009-2022, https://doi.org/10.5194/acp-22-8009-2022, 2022
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Wildfires emit aerosol particles containing brown carbon material that affects visibility and global climate and is toxic. Brown carbon is poorly characterized due to measurement limitations, and its evolution in the atmosphere is not well known. We report on aircraft measurements of brown carbon from large wildfires in the western United States. We compare two methods for measuring brown carbon and study the evolution of brown carbon in the smoke as it moved away from the burning regions.
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.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
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.
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.
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.
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.
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.
Fabienne Maignan, Camille Abadie, Marine Remaud, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Róisín Commane, Richard Wehr, J. Elliott Campbell, Sauveur Belviso, Stephen A. Montzka, Nina Raoult, Ulli Seibt, Yoichi P. Shiga, Nicolas Vuichard, Mary E. Whelan, and Philippe Peylin
Biogeosciences, 18, 2917–2955, https://doi.org/10.5194/bg-18-2917-2021, https://doi.org/10.5194/bg-18-2917-2021, 2021
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The assimilation of carbonyl sulfide (COS) by continental vegetation has been proposed as a proxy for gross primary production (GPP). Using a land surface and a transport model, we compare a mechanistic representation of the plant COS uptake (Berry et al., 2013) to the classical leaf relative uptake (LRU) approach linking GPP and vegetation COS fluxes. We show that at high temporal resolutions a mechanistic approach is mandatory, but at large scales the LRU approach compares similarly.
Bradley D. Hall, Andrew M. Crotwell, Duane R. Kitzis, Thomas Mefford, Benjamin R. Miller, Michael F. Schibig, and Pieter P. Tans
Atmos. Meas. Tech., 14, 3015–3032, https://doi.org/10.5194/amt-14-3015-2021, https://doi.org/10.5194/amt-14-3015-2021, 2021
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We have recently revised the carbon dioxide calibration scale used by numerous laboratories that measure atmospheric CO2. The revision follows from an improved understanding of the manometric method used to determine the absolute amount of CO2 in an atmospheric air sample. The new scale is 0.18 μmol mol−1 (ppm) greater than the previous scale at 400 ppm CO2. While this difference is small in relative terms (0.045 %), it is significant in terms of atmospheric monitoring.
Stijn Naus, Stephen A. Montzka, Prabir K. Patra, and Maarten C. Krol
Atmos. Chem. Phys., 21, 4809–4824, https://doi.org/10.5194/acp-21-4809-2021, https://doi.org/10.5194/acp-21-4809-2021, 2021
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Following up on previous box model studies, we employ a 3D transport model to estimate variations in the hydroxyl radical (OH) from observations of methyl chloroform (MCF). We derive small interannual OH variations that are consistent with variations in the El Niño–Southern Oscillation. We also find evidence for the release of MCF from oceans in atmospheric gradients of MCF. Both findings highlight the added value of a 3D transport model since box model studies did not identify these effects.
Jin Ma, Linda M. J. Kooijmans, Ara Cho, Stephen A. Montzka, Norbert Glatthor, John R. Worden, Le Kuai, Elliot L. Atlas, and Maarten C. Krol
Atmos. Chem. Phys., 21, 3507–3529, https://doi.org/10.5194/acp-21-3507-2021, https://doi.org/10.5194/acp-21-3507-2021, 2021
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Carbonyl sulfide is an important trace gas in the atmosphere and useful to estimating gross primary productivity in ecosystems, but its sources and sinks remain highly uncertain. Therefore, we applied inverse model system TM5-4DVAR to better constrain the global budget. Our finding is in line with earlier studies, pointing to missing sources in the tropics and more uptake in high latitudes. We also stress the necessity of more ground-based observations and satellite data assimilation in future.
Reem A. Hannun, Andrew K. Swanson, Steven A. Bailey, Thomas F. Hanisco, T. Paul Bui, Ilann Bourgeois, Jeff Peischl, and Thomas B. Ryerson
Atmos. Meas. Tech., 13, 6877–6887, https://doi.org/10.5194/amt-13-6877-2020, https://doi.org/10.5194/amt-13-6877-2020, 2020
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We have developed a cavity-enhanced absorption instrument to measure ozone in the atmosphere. The detection technique enables highly sensitive measurements in fast averaging times. The compact, robust instrument is suitable for operation in varied field environments, including aboard research aircraft. We have successfully flown the instrument and demonstrated its performance capabilities with measurements of ozone deposition rates over the coastal Pacific Ocean.
Hélène Angot, Katelyn McErlean, Lu Hu, Dylan B. Millet, Jacques Hueber, Kaixin Cui, Jacob Moss, Catherine Wielgasz, Tyler Milligan, Damien Ketcherside, M. Syndonia Bret-Harte, and Detlev Helmig
Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, https://doi.org/10.5194/bg-17-6219-2020, 2020
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We report biogenic volatile organic compounds (BVOCs) ambient levels and emission rates from key vegetation species in the Alaskan arctic tundra, providing a new data set to further constrain isoprene chemistry under low NOx conditions in models. We add to the growing body of evidence that climate-induced changes in the vegetation composition will significantly affect the BVOC emission potential of the tundra, with implications for atmospheric oxidation processes and climate feedbacks.
Petter Weibring, Dirk Richter, James G. Walega, Alan Fried, Joshua DiGangi, Hannah Halliday, Yonghoon Choi, Bianca Baier, Colm Sweeney, Ben Miller, Kenneth J. Davis, Zachary Barkley, and Michael D. Obland
Atmos. Meas. Tech., 13, 6095–6112, https://doi.org/10.5194/amt-13-6095-2020, https://doi.org/10.5194/amt-13-6095-2020, 2020
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The present study describes an autonomously operated instrument for high-precision (20–40 parts per trillion in 1 s) measurements of ethane during actual airborne operations on a small aircraft platform (NASA's King Air B200). This paper discusses the dynamic nature of airborne performance due to various aircraft-induced perturbations, methods devised to identify such events, and solutions we have enacted to circumvent these perturbations.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
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Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Haeyoung Lee, Edward J. Dlugokencky, Jocelyn C. Turnbull, Sepyo Lee, Scott J. Lehman, John B. Miller, Gabrielle Pétron, Jeong-Sik Lim, Gang-Woong Lee, Sang-Sam Lee, and Young-San Park
Atmos. Chem. Phys., 20, 12033–12045, https://doi.org/10.5194/acp-20-12033-2020, https://doi.org/10.5194/acp-20-12033-2020, 2020
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To understand South Korea's CO2 emissions and sinks as well as those of the surrounding region, we used flask-air samples collected for 2 years at Anmyeondo (36.53° N, 126.32° E; 46 m a.s.l.), South Korea, for analysis of observed 14C in atmospheric CO2 as a tracer of fossil fuel CO2 contribution (Cff). Here, we showed our observation result of 14C and Cff. SF6 and CO can be good proxies of Cff in this study, and the ratio of CO to Cff was compared to a bottom-up inventory.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
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Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
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
Johannes Bieser, Hélène Angot, Franz Slemr, and Lynwill Martin
Atmos. Chem. Phys., 20, 10427–10439, https://doi.org/10.5194/acp-20-10427-2020, https://doi.org/10.5194/acp-20-10427-2020, 2020
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We use numerical models to determine the origin of air masses measured for elemental gaseous mercury (GEM) at Cape Point (CPT), South Africa. Our analysis is based on 10 years of hourly GEM measurements at CPT from 2007 to 2016. Based on GEM concentration and the origin of the air mass, we identify source and sink regions at CPT. We find, that the warm Agulhas Current to the south-east is the major Hg source and the continent the major sink.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Malte Meinshausen, Zebedee R. J. Nicholls, Jared Lewis, Matthew J. Gidden, Elisabeth Vogel, Mandy Freund, Urs Beyerle, Claudia Gessner, Alexander Nauels, Nico Bauer, Josep G. Canadell, John S. Daniel, Andrew John, Paul B. Krummel, Gunnar Luderer, Nicolai Meinshausen, Stephen A. Montzka, Peter J. Rayner, Stefan Reimann, Steven J. Smith, Marten van den Berg, Guus J. M. Velders, Martin K. Vollmer, and Ray H. J. Wang
Geosci. Model Dev., 13, 3571–3605, https://doi.org/10.5194/gmd-13-3571-2020, https://doi.org/10.5194/gmd-13-3571-2020, 2020
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This study provides the future greenhouse gas (GHG) concentrations under the new set of so-called SSP scenarios (the successors of the IPCC SRES and previous representative concentration pathway (RCP) scenarios). The projected CO2 concentrations range from 350 ppm for low-emission scenarios by 2150 to more than 2000 ppm under the high-emission scenarios. We also provide concentrations, latitudinal gradients, and seasonality for most of the other 42 considered GHGs.
Dean Howard, Yannick Agnan, Detlev Helmig, Yu Yang, and Daniel Obrist
Biogeosciences, 17, 4025–4042, https://doi.org/10.5194/bg-17-4025-2020, https://doi.org/10.5194/bg-17-4025-2020, 2020
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The Arctic tundra represents a vast store of carbon that may be broken down by microbial activity into greenhouse gases such as CO2 and CH4. Though microbes are less active in winter, the long duration of the cold season makes this period very important for carbon cycling. We show that, under conditions of warmer winter air temperatures and greater snowfall, deeper soils can remain warm enough to sustain significantly enhanced CH4 emission. This could have large implications for future climates.
Franz Slemr, Lynwill Martin, Casper Labuschagne, Thumeka Mkololo, Hélène Angot, Olivier Magand, Aurélien Dommergue, Philippe Garat, Michel Ramonet, and Johannes Bieser
Atmos. Chem. Phys., 20, 7683–7692, https://doi.org/10.5194/acp-20-7683-2020, https://doi.org/10.5194/acp-20-7683-2020, 2020
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Monitoring of atmospheric mercury (Hg) concentrations is an important part of the effectiveness evaluation of the Minamata Convention on Hg. Hg concentrations in 2012–2017 at Cape Point, South Africa, and at Amsterdam Island in the remote Indian Ocean are comparable, and no trend or a slightly downward trend was observed at both stations. Over the 2007–2017 period an upward trend was observed at CPT which was driven mainly by the 2007–2014 data. The trend and its change are discussed.
Andrew W. Rollins, Pamela S. Rickly, Ru-Shan Gao, Thomas B. Ryerson, Steven S. Brown, Jeff Peischl, and Ilann Bourgeois
Atmos. Meas. Tech., 13, 2425–2439, https://doi.org/10.5194/amt-13-2425-2020, https://doi.org/10.5194/amt-13-2425-2020, 2020
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Nitric oxide (NO) is a key atmospheric constituent controlling atmospheric oxidation chemistry and tropospheric ozone formation. Existing instrumentation capable of quantifying NO at very low mixing ratios is uncommon and typically relies on chemiluminescence. We describe and demonstrate a new laser-based technique (LIF) with significant practical and technical advantages to CL. This technique is expected to allow for advances in understanding of atmospheric radical chemistry.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
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.
Therese S. Carter, Colette L. Heald, Jose L. Jimenez, Pedro Campuzano-Jost, Yutaka Kondo, Nobuhiro Moteki, Joshua P. Schwarz, Christine Wiedinmyer, Anton S. Darmenov, Arlindo M. da Silva, and Johannes W. Kaiser
Atmos. Chem. Phys., 20, 2073–2097, https://doi.org/10.5194/acp-20-2073-2020, https://doi.org/10.5194/acp-20-2073-2020, 2020
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Fires and the smoke they emit impact air quality, health, and climate, but the abundance and properties of smoke remain uncertain and poorly constrained. To explore this, we compare model simulations driven by four commonly-used fire emission inventories with surface, aloft, and satellite observations. We show that across inventories smoke emissions differ by factors of 4 to 7 over North America, challenging our ability to accurately characterize the impact of smoke on air quality and climate.
Detlev Helmig, Daniel Liptzin, Jacques Hueber, and Joel Savarino
The Cryosphere, 14, 199–209, https://doi.org/10.5194/tc-14-199-2020, https://doi.org/10.5194/tc-14-199-2020, 2020
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We present 15 months of trace gas observations from air withdrawn within the snowpack and from above the snow at Concordia Station in Antarctica. The data show occasional positive spikes, indicative of pollution from the station generator. The pollution signal can be seen in snowpack air shortly after it is observed above the snow surface, and lasting for up to several days, much longer than above the surface.
Chi-Tsan Wang, Christine Wiedinmyer, Kirsti Ashworth, Peter C. Harley, John Ortega, Quazi Z. Rasool, and William Vizuete
Atmos. Chem. Phys., 19, 13973–13987, https://doi.org/10.5194/acp-19-13973-2019, https://doi.org/10.5194/acp-19-13973-2019, 2019
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The legal commercialization of cannabis has created a new and almost unregulated industry. Here we present the first inventory of volatile organic compound emissions from cannabis cultivation facilities (CCFs) for Colorado. When applied within a regulatory air quality model to predict regional ozone impacts, our inventory results in net ozone formation near CCFs with the largest increases in Denver County. However, our inventory is highly uncertain and we identify future critical data needs.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339, https://doi.org/10.5194/acp-19-13325-2019, https://doi.org/10.5194/acp-19-13325-2019, 2019
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The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Martin Jiskra, Jeroen E. Sonke, Yannick Agnan, Detlev Helmig, and Daniel Obrist
Biogeosciences, 16, 4051–4064, https://doi.org/10.5194/bg-16-4051-2019, https://doi.org/10.5194/bg-16-4051-2019, 2019
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The tundra plays a pivotal role in Arctic mercury cycling by storing atmospheric mercury deposition and shuttling it to the Arctic Ocean. We used the isotopic fingerprint of mercury to investigate the processes controlling atmospheric mercury deposition. We found that the uptake of atmospheric mercury by vegetation was the major deposition source. Direct deposition to snow or soils only played a minor role. These results improve our understanding of Arctic mercury cycling.
Fang Li, Maria Val Martin, Meinrat O. Andreae, Almut Arneth, Stijn Hantson, Johannes W. Kaiser, Gitta Lasslop, Chao Yue, Dominique Bachelet, Matthew Forrest, Erik Kluzek, Xiaohong Liu, Stephane Mangeon, Joe R. Melton, Daniel S. Ward, Anton Darmenov, Thomas Hickler, Charles Ichoku, Brian I. Magi, Stephen Sitch, Guido R. van der Werf, Christine Wiedinmyer, and Sam S. Rabin
Atmos. Chem. Phys., 19, 12545–12567, https://doi.org/10.5194/acp-19-12545-2019, https://doi.org/10.5194/acp-19-12545-2019, 2019
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Fire emissions are critical for atmospheric composition, climate, carbon cycle, and air quality. We provide the first global multi-model fire emission reconstructions for 1700–2012, including carbon and 33 species of trace gases and aerosols, based on the nine state-of-the-art global fire models that participated in FireMIP. We also provide information on the recent status and limitations of the model-based reconstructions and identify the main uncertainty sources in their long-term changes.
Laura Kiely, Dominick V. Spracklen, Christine Wiedinmyer, Luke Conibear, Carly L. Reddington, Scott Archer-Nicholls, Douglas Lowe, Stephen R. Arnold, Christoph Knote, Md Firoz Khan, Mohd Talib Latif, Mikinori Kuwata, Sri Hapsari Budisulistiorini, and Lailan Syaufina
Atmos. Chem. Phys., 19, 11105–11121, https://doi.org/10.5194/acp-19-11105-2019, https://doi.org/10.5194/acp-19-11105-2019, 2019
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In 2015, a large fire episode occurred in Indonesia, reducing air quality. Fires occurred predominantly on peatland, where large uncertainties are associated with emissions. Current fire emissions datasets underestimate peat fire emissions. We created new fire emissions data, with data specific to Indonesian peat fires. Using these emissions in simulations of particulate matter and aerosol optical depth shows an improvement over simulations using current data, when compared with observations.
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.
Bradley D. Hall, Andrew M. Crotwell, Benjamin R. Miller, Michael Schibig, and James W. Elkins
Atmos. Meas. Tech., 12, 517–524, https://doi.org/10.5194/amt-12-517-2019, https://doi.org/10.5194/amt-12-517-2019, 2019
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We have used a one-step method for gravimetric preparation of CO2-in-air standards in aluminum cylinders. We consider both adsorption to stainless steel surfaces used in the transfer of highly pure CO2 and adsorption of CO2 to cylinder walls. This work compliments ongoing efforts to support atmospheric monitoring of CO2.
Pingyang Li, Jens Mühle, Stephen A. Montzka, David E. Oram, Benjamin R. Miller, Ray F. Weiss, Paul J. Fraser, and Toste Tanhua
Ocean Sci., 15, 33–60, https://doi.org/10.5194/os-15-33-2019, https://doi.org/10.5194/os-15-33-2019, 2019
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Use of CFCs as oceanic transient tracers is difficult for recently ventilated water masses as their atmospheric mole fractions have been decreasing. To explore novel tracers, we synthesized consistent annual mean atmospheric histories of HCFC-22, HCFC-141b, HCFC-142b, HFC-134a, HFC-125, HFC-23, PFC-14 (CF4) and PFC-116 in both hemispheres and reconstructed their solubility functions in water and seawater. This work is also potentially useful for tracer studies in a range of natural waters.
Stijn Naus, Stephen A. Montzka, Sudhanshu Pandey, Sourish Basu, Ed J. Dlugokencky, and Maarten Krol
Atmos. Chem. Phys., 19, 407–424, https://doi.org/10.5194/acp-19-407-2019, https://doi.org/10.5194/acp-19-407-2019, 2019
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We investigate how the use of a two-box model to describe the troposphere can impact derived results, relative to more complex models. For this, we use a 3-D transport model to tune a two-box model of OH, CH4, and MCF. By comparing the tuned two-box model with a standard model run, we can diagnose and quantify biases inherent to a two-box model. We find strong biases, but these have only a small impact on our final conclusions. However, it is not obvious that this should hold for future studies.
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Robyn Butler, Paul I. Palmer, Liang Feng, Stephen J. Andrews, Elliot L. Atlas, Lucy J. Carpenter, Valeria Donets, Neil R. P. Harris, Stephen A. Montzka, Laura L. Pan, Ross J. Salawitch, and Sue M. Schauffler
Atmos. Chem. Phys., 18, 13135–13153, https://doi.org/10.5194/acp-18-13135-2018, https://doi.org/10.5194/acp-18-13135-2018, 2018
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Natural sources of short-lived bromoform and dibromomethane are important for determining the inorganic bromine budget in the stratosphere that drives ozone loss. Two new modelling techniques describe how different geographical source regions influence their atmospheric variability over the western Pacific. We find that it is driven primarily by open ocean sources, and we use atmospheric observations to help estimate their contributions to the upper tropospheric inorganic bromine budget.
Mary E. Whelan, Sinikka T. Lennartz, Teresa E. Gimeno, Richard Wehr, Georg Wohlfahrt, Yuting Wang, Linda M. J. Kooijmans, Timothy W. Hilton, Sauveur Belviso, Philippe Peylin, Róisín Commane, Wu Sun, Huilin Chen, Le Kuai, Ivan Mammarella, Kadmiel Maseyk, Max Berkelhammer, King-Fai Li, Dan Yakir, Andrew Zumkehr, Yoko Katayama, Jérôme Ogée, Felix M. Spielmann, Florian Kitz, Bharat Rastogi, Jürgen Kesselmeier, Julia Marshall, Kukka-Maaria Erkkilä, Lisa Wingate, Laura K. Meredith, Wei He, Rüdiger Bunk, Thomas Launois, Timo Vesala, Johan A. Schmidt, Cédric G. Fichot, Ulli Seibt, Scott Saleska, Eric S. Saltzman, Stephen A. Montzka, Joseph A. Berry, and J. Elliott Campbell
Biogeosciences, 15, 3625–3657, https://doi.org/10.5194/bg-15-3625-2018, https://doi.org/10.5194/bg-15-3625-2018, 2018
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Measurements of the trace gas carbonyl sulfide (OCS) are helpful in quantifying photosynthesis at previously unknowable temporal and spatial scales. While CO2 is both consumed and produced within ecosystems, OCS is mostly produced in the oceans or from specific industries, and destroyed in plant leaves in proportion to CO2. This review summarizes the advancements we have made in the understanding of OCS exchange and applications to vital ecosystem water and carbon cycle questions.
Yannick Agnan, Thomas A. Douglas, Detlev Helmig, Jacques Hueber, and Daniel Obrist
The Cryosphere, 12, 1939–1956, https://doi.org/10.5194/tc-12-1939-2018, https://doi.org/10.5194/tc-12-1939-2018, 2018
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In this study, we investigated mercury dynamics in an interior arctic tundra at Toolik Field Station (200 km from the Arctic Ocean) during two full snow seasons. We continuously measured atmospheric, snow gas phase, and soil pores mercury concentrations. We observed consistent concentration declines from the atmosphere to snowpack to soils, indicating that soils are continuous sinks of mercury. We suggest that interior arctic snowpacks may be negligible sources of mercury.
Felicia Kolonjari, David A. Plummer, Kaley A. Walker, Chris D. Boone, James W. Elkins, Michaela I. Hegglin, Gloria L. Manney, Fred L. Moore, Diane Pendlebury, Eric A. Ray, Karen H. Rosenlof, and Gabriele P. Stiller
Atmos. Chem. Phys., 18, 6801–6828, https://doi.org/10.5194/acp-18-6801-2018, https://doi.org/10.5194/acp-18-6801-2018, 2018
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We used satellite observations and model simulations of CFC-11, CFC-12, and N2O to investigate stratospheric transport, which is important for predicting the recovery of the ozone layer and future climate. We found that sampling can impact results and that the model consistently overestimates concentrations of these gases in the lower stratosphere, consistent with a too rapid Brewer–Dobson circulation. An issue with mixing in the tropical lower stratosphere in June–July–August was also found.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Yaoxian Huang, Shiliang Wu, Louisa J. Kramer, Detlev Helmig, and Richard E. Honrath
Atmos. Chem. Phys., 17, 14661–14674, https://doi.org/10.5194/acp-17-14661-2017, https://doi.org/10.5194/acp-17-14661-2017, 2017
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A global chemical transport model (GEOS-Chem) was employed to simulate surface ozone and its precursors at Summit, Greenland in the Arctic and compare them with 2-year in situ surface observations. The model performed well in simulating certain species (such as carbon monoxide and propane), but some significant discrepancies were identified for other species (e.g., nitrogen oxides, ethane, PAN, and ozone). We further investigated the exact causes for model–data biases.
Stephen Conley, Ian Faloona, Shobhit Mehrotra, Maxime Suard, Donald H. Lenschow, Colm Sweeney, Scott Herndon, Stefan Schwietzke, Gabrielle Pétron, Justin Pifer, Eric A. Kort, and Russell Schnell
Atmos. Meas. Tech., 10, 3345–3358, https://doi.org/10.5194/amt-10-3345-2017, https://doi.org/10.5194/amt-10-3345-2017, 2017
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This paper describes a new method of quantifying surface trace gas emissions (e.g. methane) from small aircraft (e.g. Mooney, Cessna) in about 30 min. This technique greatly enhances our ability to rapidly respond in the event of catastrophic failures such as Aliso Canyon and Deep Water Horizon.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Mike J. Newland, Patricia Martinerie, Emmanuel Witrant, Detlev Helmig, David R. Worton, Chris Hogan, William T. Sturges, and Claire E. Reeves
Atmos. Chem. Phys., 17, 8269–8283, https://doi.org/10.5194/acp-17-8269-2017, https://doi.org/10.5194/acp-17-8269-2017, 2017
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We report increasing levels of alkyl nitrates in the Northern Hemisphere atmosphere between 1960 and the mid-1990s. These increases are symptomatic of large-scale changes to the chemical composition of the atmosphere, particularly with regards to the amounts of short-lived, reactive species. The observed increases are likely driven by increasing levels of nitrogen oxides. These changes have direct implications for the lifetimes of climate-relevant species in the atmosphere, such as methane.
Malte Meinshausen, Elisabeth Vogel, Alexander Nauels, Katja Lorbacher, Nicolai Meinshausen, David M. Etheridge, Paul J. Fraser, Stephen A. Montzka, Peter J. Rayner, Cathy M. Trudinger, Paul B. Krummel, Urs Beyerle, Josep G. Canadell, John S. Daniel, Ian G. Enting, Rachel M. Law, Chris R. Lunder, Simon O'Doherty, Ron G. Prinn, Stefan Reimann, Mauro Rubino, Guus J. M. Velders, Martin K. Vollmer, Ray H. J. Wang, and Ray Weiss
Geosci. Model Dev., 10, 2057–2116, https://doi.org/10.5194/gmd-10-2057-2017, https://doi.org/10.5194/gmd-10-2057-2017, 2017
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Climate change is primarily driven by human-induced increases of greenhouse gas (GHG) concentrations. Based on ongoing community efforts (e.g. AGAGE and NOAA networks, ice cores), this study presents historical concentrations of CO2, CH4, N2O and 40 other GHGs from year 0 to year 2014. The data is recommended as input for climate models for pre-industrial, historical runs under CMIP6. Global means, but also latitudinal by monthly surface concentration fields are provided.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Linda M. J. Kooijmans, Nelly A. M. Uitslag, Mark S. Zahniser, David D. Nelson, Stephen A. Montzka, and Huilin Chen
Atmos. Meas. Tech., 9, 5293–5314, https://doi.org/10.5194/amt-9-5293-2016, https://doi.org/10.5194/amt-9-5293-2016, 2016
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The accuracy of carbon models, used for the prediction of global climate change, is limited by the knowledge of the uptake of carbon by plants through photosynthesis. Carbonyl sulfide (COS) has been suggested as a tracer for this process. To be able to further explore and verify the application of this novel tracer we have tested a laser spectrometer for its suitability to obtain accurate and high precision measurements of COS and CO2 with both laboratory experiments and field measurements.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Francesco Carbone, Sergio Cinnirella, Valentino Mannarino, Matthew Landis, Ralf Ebinghaus, Andreas Weigelt, Ernst-Günther Brunke, Casper Labuschagne, Lynwill Martin, John Munthe, Ingvar Wängberg, Paulo Artaxo, Fernando Morais, Henrique de Melo Jorge Barbosa, Joel Brito, Warren Cairns, Carlo Barbante, María del Carmen Diéguez, Patricia Elizabeth Garcia, Aurélien Dommergue, Helene Angot, Olivier Magand, Henrik Skov, Milena Horvat, Jože Kotnik, Katie Alana Read, Luis Mendes Neves, Bernd Manfred Gawlik, Fabrizio Sena, Nikolay Mashyanov, Vladimir Obolkin, Dennis Wip, Xin Bin Feng, Hui Zhang, Xuewu Fu, Ramesh Ramachandran, Daniel Cossa, Joël Knoery, Nicolas Marusczak, Michelle Nerentorp, and Claus Norstrom
Atmos. Chem. Phys., 16, 11915–11935, https://doi.org/10.5194/acp-16-11915-2016, https://doi.org/10.5194/acp-16-11915-2016, 2016
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This work presents atmospheric Hg concentrations recorded within the GMOS global network analyzing Hg measurement results in terms of temporal trends, seasonality and comparability within the network. The over-arching benefit of this coordinated Hg monitoring network would clearly be the production of high-quality measurement datasets on a global scale useful in developing and validating models on different spatial and temporal scales.
James H. Butler, Shari A. Yvon-Lewis, Jurgen M. Lobert, Daniel B. King, Stephen A. Montzka, John L. Bullister, Valentin Koropalov, James W. Elkins, Bradley D. Hall, Lei Hu, and Yina Liu
Atmos. Chem. Phys., 16, 10899–10910, https://doi.org/10.5194/acp-16-10899-2016, https://doi.org/10.5194/acp-16-10899-2016, 2016
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This study was conducted to understand the influence of the ocean on the lifetime of atmospheric carbon tetrachloride, a strong, ozone-depleting gas. Data from 16 research cruises conducted between 1987 and 2010 show that, unlike the unreactive chlorofluorocarbons, carbon tetrachloride is undersaturated in surface waters regardless of temperature, wind, or biological regime, but with larger undersaturations with upwelling. Results suggest that the ocean consumes about 18 % of atmospheric CCl4.
Maite Bauwens, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Michel Van Roozendael, Guido R. van der Werf, Christine Wiedinmyer, Johannes W. Kaiser, Katerina Sindelarova, and Alex Guenther
Atmos. Chem. Phys., 16, 10133–10158, https://doi.org/10.5194/acp-16-10133-2016, https://doi.org/10.5194/acp-16-10133-2016, 2016
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Relying on a 9-year record of satellite observations of formaldehyde, we use inverse techniques to derive global top–down hydrocarbon fluxes over 2005–2013, infer seasonal and interannual variability, and detect emission trends. Our results suggest changes in fire seasonal patterns, a stronger contribution of agricultural burning, overestimated isoprene flux rates in the tropics, overly decreased isoprene emissions due to soil moisture stress in arid areas, and enhanced isoprene trends.
E. Eckert, A. Laeng, S. Lossow, S. Kellmann, G. Stiller, T. von Clarmann, N. Glatthor, M. Höpfner, M. Kiefer, H. Oelhaf, J. Orphal, B. Funke, U. Grabowski, F. Haenel, A. Linden, G. Wetzel, W. Woiwode, P. F. Bernath, C. Boone, G. S. Dutton, J. W. Elkins, A. Engel, J. C. Gille, F. Kolonjari, T. Sugita, G. C. Toon, and K. A. Walker
Atmos. Meas. Tech., 9, 3355–3389, https://doi.org/10.5194/amt-9-3355-2016, https://doi.org/10.5194/amt-9-3355-2016, 2016
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We investigate the accuracy, precision and long-term stability of the MIPAS Envisat IMK/IAA CFC-11 (CCl3F) and CFC-12 (CCl2F2) products.
For comparisons we use several data products from satellite, airplane and balloon-borne instruments as well as ground-based data.
MIPAS Envisat CFC-11 has a slight high bias at the lower end of the profile.
CFC-12 agrees well with other data products.
The temporal stability is good up to ~ 30 km, but still leaves room for improvement.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Hélène Angot, Olivier Magand, Detlev Helmig, Philippe Ricaud, Boris Quennehen, Hubert Gallée, Massimo Del Guasta, Francesca Sprovieri, Nicola Pirrone, Joël Savarino, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8249–8264, https://doi.org/10.5194/acp-16-8249-2016, https://doi.org/10.5194/acp-16-8249-2016, 2016
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While the Arctic has been extensively monitored, there is still much to be learned from the Antarctic continent regarding the processes that govern the budget of atmospheric mercury species. We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. The striking reactivity observed on the Antarctic plateau most likely influences the cycle of atmospheric mercury on a continental scale.
Hélène Angot, Iris Dion, Nicolas Vogel, Michel Legrand, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8265–8279, https://doi.org/10.5194/acp-16-8265-2016, https://doi.org/10.5194/acp-16-8265-2016, 2016
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This paper presents a multi-year record of atmospheric gaseous elemental mercury (Hg(0)) at Dumont d’Urville (DDU) on the East Antarctic coast. This record reveals particularities that are not seen at other coastal Antarctic sites, likely due to the more frequent arrival of inland air masses at DDU than at other coastal sites, and to the influence of oceanic air masses. This study confirms the influence of processes observed inland on the cycle of atmospheric mercury at a continental scale.
Michel Legrand, Susanne Preunkert, Joël Savarino, Markus M. Frey, Alexandre Kukui, Detlev Helmig, Bruno Jourdain, Anna E. Jones, Rolf Weller, Neil Brough, and Hubert Gallée
Atmos. Chem. Phys., 16, 8053–8069, https://doi.org/10.5194/acp-16-8053-2016, https://doi.org/10.5194/acp-16-8053-2016, 2016
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Surface ozone, the most abundant atmospheric oxidant, has been measured since 2004 at the coastal East Antarctic site of Dumont d’Urville, and since 2007 at the Concordia station located on the high East Antarctic plateau. Long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites are discussed. Influences like sea ice extent and outflow from inland Antarctica are discussed.
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
John K. Kodros, Rachel Cucinotta, David A. Ridley, Christine Wiedinmyer, and Jeffrey R. Pierce
Atmos. Chem. Phys., 16, 6771–6784, https://doi.org/10.5194/acp-16-6771-2016, https://doi.org/10.5194/acp-16-6771-2016, 2016
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We provide a first estimate of the aerosol radiative effects from open, uncontrolled combustion of domestic waste. We find the direct and cloud-albedo indirect radiative effects are predominantly negative (cooling tendency) with regional forcings exceeding −0.4 W m−2; however, the magnitude of these effects depends on the assumed emitted aerosol size, mass, and optical properties.
M. Chirkov, G. P. Stiller, A. Laeng, S. Kellmann, T. von Clarmann, C. D. Boone, J. W. Elkins, A. Engel, N. Glatthor, U. Grabowski, C. M. Harth, M. Kiefer, F. Kolonjari, P. B. Krummel, A. Linden, C. R. Lunder, B. R. Miller, S. A. Montzka, J. Mühle, S. O'Doherty, J. Orphal, R. G. Prinn, G. Toon, M. K. Vollmer, K. A. Walker, R. F. Weiss, A. Wiegele, and D. Young
Atmos. Chem. Phys., 16, 3345–3368, https://doi.org/10.5194/acp-16-3345-2016, https://doi.org/10.5194/acp-16-3345-2016, 2016
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HCFC-22 global distributions from MIPAS measurements for 2005 to 2012 are presented. Tropospheric trends are in good agreement with ground-based observations. A layer of enhanced HCFC-22 in the upper tropospheric tropics and northern subtropics is identified to come from Asian sources uplifted in the Asian monsoon. Stratospheric distributions provide show seasonal, semi-annual, and QBO-related variations. Hemispheric asymmetries of trends hint towards a change in the stratospheric circulation.
Johannes Plieninger, Alexandra Laeng, Stefan Lossow, Thomas von Clarmann, Gabriele P. Stiller, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Kaley A. Walker, Stefan Noël, Mark E. Hervig, Martin McHugh, Alyn Lambert, Joachim Urban, James W. Elkins, and Donal Murtagh
Atmos. Meas. Tech., 9, 765–779, https://doi.org/10.5194/amt-9-765-2016, https://doi.org/10.5194/amt-9-765-2016, 2016
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We compare concentration profiles of methane and nitrous oxide measured from MIPAS-ENVISAT and derived with a new retrieval setup to those measured by other satellite instruments and to surface measurements. For methane we use profiles measured by ACE-FTS, HALOE and SCIAMACHY; for nitrous oxide we use profiles measured by ACE-FTS, Aura-MLS and Odin-SMR for the comparisons. We give a quantitative bias estimation and compare the estimated errors provided by the instruments.
R. Gonzalez-Abraham, S. H. Chung, J. Avise, B. Lamb, E. P. Salathé Jr., C. G. Nolte, D. Loughlin, A. Guenther, C. Wiedinmyer, T. Duhl, Y. Zhang, and D. G. Streets
Atmos. Chem. Phys., 15, 12645–12665, https://doi.org/10.5194/acp-15-12645-2015, https://doi.org/10.5194/acp-15-12645-2015, 2015
S. T. Lennartz, G. Krysztofiak, C. A. Marandino, B.-M. Sinnhuber, S. Tegtmeier, F. Ziska, R. Hossaini, K. Krüger, S. A. Montzka, E. Atlas, D. E. Oram, T. Keber, H. Bönisch, and B. Quack
Atmos. Chem. Phys., 15, 11753–11772, https://doi.org/10.5194/acp-15-11753-2015, https://doi.org/10.5194/acp-15-11753-2015, 2015
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Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
S. Song, N. E. Selin, A. L. Soerensen, H. Angot, R. Artz, S. Brooks, E.-G. Brunke, G. Conley, A. Dommergue, R. Ebinghaus, T. M. Holsen, D. A. Jaffe, S. Kang, P. Kelley, W. T. Luke, O. Magand, K. Marumoto, K. A. Pfaffhuber, X. Ren, G.-R. Sheu, F. Slemr, T. Warneke, A. Weigelt, P. Weiss-Penzias, D. C. Wip, and Q. Zhang
Atmos. Chem. Phys., 15, 7103–7125, https://doi.org/10.5194/acp-15-7103-2015, https://doi.org/10.5194/acp-15-7103-2015, 2015
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A better knowledge of mercury (Hg) emission fluxes into the global atmosphere is important for assessing its human health impacts and evaluating the effectiveness of corresponding policy actions. We for the first time apply a top-down approach at a global scale to quantitatively estimate present-day mercury emission sources as well as key parameters in a chemical transport model, in order to better constrain the global biogeochemical cycle of mercury.
L. J. Kramer, D. Helmig, J. F. Burkhart, A. Stohl, S. Oltmans, and R. E. Honrath
Atmos. Chem. Phys., 15, 6827–6849, https://doi.org/10.5194/acp-15-6827-2015, https://doi.org/10.5194/acp-15-6827-2015, 2015
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.
S. Preunkert, M. Legrand, M. M. Frey, A. Kukui, J. Savarino, H. Gallée, M. King, B. Jourdain, W. Vicars, and D. Helmig
Atmos. Chem. Phys., 15, 6689–6705, https://doi.org/10.5194/acp-15-6689-2015, https://doi.org/10.5194/acp-15-6689-2015, 2015
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During two austral summers HCHO was investigated in air, snow, and interstitial air at the Concordia site located on the East Antarctic Plateau. Snow emission fluxes were estimated to be around 1 to 2 and 3 to 5 x 10^12 molecules m-2 s-1 at night and at noon, respectively. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible. The mean HCHO level of 130pptv observed at 1m above the surface is quite well reproduced by 1-D simulations.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
K. Dzepina, C. Mazzoleni, P. Fialho, S. China, B. Zhang, R. C. Owen, D. Helmig, J. Hueber, S. Kumar, J. A. Perlinger, L. J. Kramer, M. P. Dziobak, M. T. Ampadu, S. Olsen, D. J. Wuebbles, and L. R. Mazzoleni
Atmos. Chem. Phys., 15, 5047–5068, https://doi.org/10.5194/acp-15-5047-2015, https://doi.org/10.5194/acp-15-5047-2015, 2015
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Aerosol was sampled at the Pico Mountain Observatory located at 2.2km amsl on Pico Island of the North Atlantic Azores archipelago. Two aerosol samples characterized by ultrahigh resolution mass spectrometry had biomass burning and marine emissions origins, as corroborated by collocated gas- and particle-phase measurements, air masses analyses and satellites. The paper presents the first molecular characterization of aged and processed aerosol intercepted at a remote lower free troposphere
F. Slemr, H. Angot, A. Dommergue, O. Magand, M. Barret, A. Weigelt, R. Ebinghaus, E.-G. Brunke, K. A. Pfaffhuber, G. Edwards, D. Howard, J. Powell, M. Keywood, and F. Wang
Atmos. Chem. Phys., 15, 3125–3133, https://doi.org/10.5194/acp-15-3125-2015, https://doi.org/10.5194/acp-15-3125-2015, 2015
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• Longer-term mercury measurement in the Southern Hemisphere is compared.
• Mercury, in terms of monthly and annual medians and averages, is more evenly distributed than hitherto believed.
• Consequently, trends observed at one or a few sites are likely to be representative of the whole hemisphere, and smaller trends can be detected in shorter time periods.
• We report a change in the trend sign at Cape Point from decreasing mercury concentrations in 1996-2004 to increasing ones since 2007.
B. de Foy, Y. Y. Cui, J. J. Schauer, M. Janssen, J. R. Turner, and C. Wiedinmyer
Atmos. Chem. Phys., 15, 2405–2427, https://doi.org/10.5194/acp-15-2405-2015, https://doi.org/10.5194/acp-15-2405-2015, 2015
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Elemental carbon and organic carbon are components of fine particulate matter that are harmful to health. We use computer simulations of wind patterns and pollution dispersion to analyze a year-long time series of hourly measurements made at the St. Louis-Midwest supersite. The inverse method produced improved estimates of emissions of these pollutants by different types of sources such as on-road and off-road emissions and open burning.
Emma C. Leedham Elvidge, D. E. Oram, J. C. Laube, A. K. Baker, S. A. Montzka, S. Humphrey, D. A. O'Sullivan, and C. A. M. Brenninkmeijer
Atmos. Chem. Phys., 15, 1939–1958, https://doi.org/10.5194/acp-15-1939-2015, https://doi.org/10.5194/acp-15-1939-2015, 2015
S. Kulkarni, N. Sobhani, J. P. Miller-Schulze, M. M. Shafer, J. J. Schauer, P. A. Solomon, P. E. Saide, S. N. Spak, Y. F. Cheng, H. A. C. Denier van der Gon, Z. Lu, D. G. Streets, G. Janssens-Maenhout, C. Wiedinmyer, J. Lantz, M. Artamonova, B. Chen, S. Imashev, L. Sverdlik, J. T. Deminter, B. Adhikary, A. D'Allura, C. Wei, and G. R. Carmichael
Atmos. Chem. Phys., 15, 1683–1705, https://doi.org/10.5194/acp-15-1683-2015, https://doi.org/10.5194/acp-15-1683-2015, 2015
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This study presents a regional-scale modeling analysis of aerosols in the Central Asia region including detailed characterization of seasonal source region and sector contributions along with the predicted changes in distribution of aerosols using 2030 future emission scenarios. The influence of long transport and impact of varied emission sources including dust, biomass burning, and anthropogenic sources on the regional aerosol distributions and the associated transport pathways are discussed.
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
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Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
H. Angot, M. Barret, O. Magand, M. Ramonet, and A. Dommergue
Atmos. Chem. Phys., 14, 11461–11473, https://doi.org/10.5194/acp-14-11461-2014, https://doi.org/10.5194/acp-14-11461-2014, 2014
M. Maione, F. Graziosi, J. Arduini, F. Furlani, U. Giostra, D. R. Blake, P. Bonasoni, X. Fang, S. A. Montzka, S. J. O'Doherty, S. Reimann, A. Stohl, and M. K. Vollmer
Atmos. Chem. Phys., 14, 9755–9770, https://doi.org/10.5194/acp-14-9755-2014, https://doi.org/10.5194/acp-14-9755-2014, 2014
S. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20117-2014, https://doi.org/10.5194/acpd-14-20117-2014, 2014
Revised manuscript not accepted
G. W. Santoni, B. C. Daube, E. A. Kort, R. Jiménez, S. Park, J. V. Pittman, E. Gottlieb, B. Xiang, M. S. Zahniser, D. D. Nelson, J. B. McManus, J. Peischl, T. B. Ryerson, J. S. Holloway, A. E. Andrews, C. Sweeney, B. Hall, E. J. Hintsa, F. L. Moore, J. W. Elkins, D. F. Hurst, B. B. Stephens, J. Bent, and S. C. Wofsy
Atmos. Meas. Tech., 7, 1509–1526, https://doi.org/10.5194/amt-7-1509-2014, https://doi.org/10.5194/amt-7-1509-2014, 2014
E. Saikawa, R. G. Prinn, E. Dlugokencky, K. Ishijima, G. S. Dutton, B. D. Hall, R. Langenfelds, Y. Tohjima, T. Machida, M. Manizza, M. Rigby, S. O'Doherty, P. K. Patra, C. M. Harth, R. F. Weiss, P. B. Krummel, M. van der Schoot, P. J. Fraser, L. P. Steele, S. Aoki, T. Nakazawa, and J. W. Elkins
Atmos. Chem. Phys., 14, 4617–4641, https://doi.org/10.5194/acp-14-4617-2014, https://doi.org/10.5194/acp-14-4617-2014, 2014
P. Boylan, D. Helmig, and J.-H. Park
Atmos. Meas. Tech., 7, 1231–1244, https://doi.org/10.5194/amt-7-1231-2014, https://doi.org/10.5194/amt-7-1231-2014, 2014
B. Zhang, R. C. Owen, J. A. Perlinger, A. Kumar, S. Wu, M. Val Martin, L. Kramer, D. Helmig, and R. E. Honrath
Atmos. Chem. Phys., 14, 2267–2287, https://doi.org/10.5194/acp-14-2267-2014, https://doi.org/10.5194/acp-14-2267-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
B. D. Hall, A. Engel, J. Mühle, J. W. Elkins, F. Artuso, E. Atlas, M. Aydin, D. Blake, E.-G. Brunke, S. Chiavarini, P. J. Fraser, J. Happell, P. B. Krummel, I. Levin, M. Loewenstein, M. Maione, S. A. Montzka, S. O'Doherty, S. Reimann, G. Rhoderick, E. S. Saltzman, H. E. Scheel, L. P. Steele, M. K. Vollmer, R. F. Weiss, D. Worthy, and Y. Yokouchi
Atmos. Meas. Tech., 7, 469–490, https://doi.org/10.5194/amt-7-469-2014, https://doi.org/10.5194/amt-7-469-2014, 2014
L. Kuai, J. Worden, S. S. Kulawik, S. A. Montzka, and J. Liu
Atmos. Meas. Tech., 7, 163–172, https://doi.org/10.5194/amt-7-163-2014, https://doi.org/10.5194/amt-7-163-2014, 2014
C. Cressot, F. Chevallier, P. Bousquet, C. Crevoisier, E. J. Dlugokencky, A. Fortems-Cheiney, C. Frankenberg, R. Parker, I. Pison, R. A. Scheepmaker, S. A. Montzka, P. B. Krummel, L. P. Steele, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 577–592, https://doi.org/10.5194/acp-14-577-2014, https://doi.org/10.5194/acp-14-577-2014, 2014
A. Kumar, S. Wu, M. F. Weise, R. Honrath, R. C. Owen, D. Helmig, L. Kramer, M. Val Martin, and Q. Li
Atmos. Chem. Phys., 13, 12537–12547, https://doi.org/10.5194/acp-13-12537-2013, https://doi.org/10.5194/acp-13-12537-2013, 2013
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, and T. P. Guilderson
Atmos. Chem. Phys., 13, 11101–11120, https://doi.org/10.5194/acp-13-11101-2013, https://doi.org/10.5194/acp-13-11101-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
X. Jiang, M. C. Barth, C. Wiedinmyer, and S. T. Massie
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-21383-2013, https://doi.org/10.5194/acpd-13-21383-2013, 2013
Revised manuscript not accepted
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
M. Val Martin, C. L. Heald, B. Ford, A. J. Prenni, and C. Wiedinmyer
Atmos. Chem. Phys., 13, 7429–7439, https://doi.org/10.5194/acp-13-7429-2013, https://doi.org/10.5194/acp-13-7429-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
L. Hu, D. B. Millet, S. Y. Kim, K. C. Wells, T. J. Griffis, E. V. Fischer, D. Helmig, J. Hueber, and A. J. Curtis
Atmos. Chem. Phys., 13, 3379–3392, https://doi.org/10.5194/acp-13-3379-2013, https://doi.org/10.5194/acp-13-3379-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Contribution of cooking emissions to the urban volatile organic compounds in Las Vegas, NV
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A large role of missing volatile organic compound reactivity from anthropogenic emissions in ozone pollution regulation
Measurement report: Insights into the chemical composition and origin of molecular clusters and potential precursor molecules present in the free troposphere over the southern Indian Ocean: observations from the Maïdo Observatory (2150 m a.s.l., Réunion)
Production of oxygenated volatile organic compounds from the ozonolysis of coastal seawater
Comment on “Transport of substantial stratospheric ozone to the surface by a dying typhoon and shallow convection” by Chen et al. (2022)
Observations of cyanogen bromide (BrCN) in the global troposphere and their relation to polar surface O3 destruction
Individual coal mine methane emissions constrained by eddy covariance measurements: low bias and missing sources
Measurement report: Observations of ground-level ozone concentration gradients perpendicular to the Lake Ontario shoreline
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Quantifying SO2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation
Influences of downward transport and photochemistry on surface ozone over East Antarctica during austral summer: in situ observations and model simulations
Iodine oxoacids and their roles in sub-3 nm particle growth in polluted urban environments
Intensive photochemical oxidation in the marine atmosphere: evidence from direct radical measurements
Diurnal variations in oxygen and nitrogen isotopes of atmospheric nitrogen dioxide and nitrate: implications for tracing NOx oxidation pathways and emission sources
Measurement report: Method for evaluating CO2 emissions from a cement plant using atmospheric δ(O2 ∕ N2) and CO2 measurements and its implication for future detection of CO2 capture signals
Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the southern North Sea
Parameterizations of US wildfire and prescribed fire emission ratios and emission factors based on FIREX-AQ aircraft measurements
Measurement report: Atmospheric nitrate radical chemistry in the South China Sea influenced by the urban outflow of the Pearl River Delta
The interhemispheric gradient of SF6 in the upper troposphere
Weather regimes and the related atmospheric composition at a Pyrenean observatory characterized by hierarchical clustering of a 5-year data set
Tropospheric bromine monoxide vertical profiles retrieved across the Alaskan Arctic in springtime
Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures
Measurement report: Exchange fluxes of HONO over agricultural fields in the North China Plain
HONO chemistry at a suburban site during the EXPLORE-YRD campaign in 2018: formation mechanisms and impacts on O3 production
Evaluation of modelled climatologies of O3, CO, water vapour and NOy in the upper troposphere–lower stratosphere using regular in situ observations by passenger aircraft
Photochemical ageing of aerosols contributes significantly to the production of atmospheric formic acid
Nitrous acid budgets in the coastal atmosphere: potential daytime marine sources
Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany
Undetected biogenic volatile organic compounds from Norway spruce drive total ozone reactivity measurements
Quantification of fossil fuel CO2 from combined CO, δ13CO2 and Δ14CO2 observations
Radical chemistry and ozone production at a UK coastal receptor site
Sources and long-term variability of carbon monoxide at Mount Kenya and in Nairobi
Shipping and algae emissions have a major impact on ambient air mixing ratios of NMHCs and methanethiol on Utö island in the Baltic Sea
Opinion: Strengthening Research in the Global South: Atmospheric Science Opportunities in South America and Africa
Measurement report: Airborne measurements of NOx fluxes over Los Angeles during the RECAP-CA 2021 campaign
Influence of anthropogenic emissions on the composition of highly oxygenated organic molecules in Helsinki: a street canyon and urban background station comparison
Changes in surface ozone in South Korea on diurnal to decadal timescales for the period of 2001–2021
Characterization of the nitrogen stable isotope composition (δ15N) of ship-emitted NOx
Volatile organic compound fluxes in the agricultural San Joaquin Valley – spatial distribution, source attribution, and inventory comparison
Exploring the amplified role of HCHO in the formation of HMS and O3 during the co-occurring PM2.5 and O3 pollution in a coastal city of southeast China
High potential for CH4 emission mitigation from oil infrastructure in one of EU's major production regions
Measurement report: Source apportionment and environmental impacts of volatile organic compounds (VOCs) in Lhasa, a highland city in China
OH, HO2, and RO2 radical chemistry in a rural forest environment: measurements, model comparisons, and evidence of a missing radical sink
The atmospheric fate of 1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane (TBECH): spatial patterns, seasonal variability, and deposition to Canadian coastal regions
A single-point modeling approach for the intercomparison and evaluation of ozone dry deposition across chemical transport models (Activity 2 of AQMEII4)
Direct observations of NOx emissions over the San Joaquin Valley using airborne flux measurements during RECAP-CA 2021 field campaign
Surface snow bromide and nitrate at Eureka, Canada in early spring and implications for polar boundary layer chemistry
Trends and seasonal variability in ammonia across major biomes in western and central Africa inferred from long-term series of ground-based and satellite measurements
A rise in HFC-23 emissions from eastern Asia since 2015
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Fabien Paulot, Gabrielle Pétron, Andrew M. Crotwell, and Matteo B. Bertagni
Atmos. Chem. Phys., 24, 4217–4229, https://doi.org/10.5194/acp-24-4217-2024, https://doi.org/10.5194/acp-24-4217-2024, 2024
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New data from the National Oceanic and Atmospheric Administration show that hydrogen (H2) concentrations increased from 2010 to 2019, which is consistent with the simulated increase in H2 photochemical production (mainly from methane). But this cannot be reconciled with the expected decrease (increase) in H2 anthropogenic emissions (soil deposition) in the same period. This shows gaps in our knowledge of the H2 biogeochemical cycle that must be resolved to quantify the impact of higher H2 usage.
Wenjie Wang, Bin Yuan, Hang Su, Yafang Cheng, Jipeng Qi, Sihang Wang, Wei Song, Xinming Wang, Chaoyang Xue, Chaoqun Ma, Fengxia Bao, Hongli Wang, Shengrong Lou, and Min Shao
Atmos. Chem. Phys., 24, 4017–4027, https://doi.org/10.5194/acp-24-4017-2024, https://doi.org/10.5194/acp-24-4017-2024, 2024
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This study investigates the important role of unmeasured volatile organic compounds (VOCs) in ozone formation. Based on results in a megacity of China, we show that unmeasured VOCs can contribute significantly to ozone fomation and also influence the determination of ozone control strategy. Our results show that these unmeasured VOCs are mainly from human sources.
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
Atmos. Chem. Phys., 24, 3729–3742, https://doi.org/10.5194/acp-24-3729-2024, https://doi.org/10.5194/acp-24-3729-2024, 2024
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOCs generated by the ozonolysis of surface seawater are competitive with biological VOC production and emission.
Xiangdong Zheng, Wen Yang, Yuting Sun, Chunmei Geng, Yingying Liu, and Xiaobin Xu
Atmos. Chem. Phys., 24, 3759–3768, https://doi.org/10.5194/acp-24-3759-2024, https://doi.org/10.5194/acp-24-3759-2024, 2024
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Chen et al. (2022) attributed the nocturnal ozone enhancement (NOE) during the night of 31 July 2021 in the North China Plain (NCP) to "the direct stratospheric intrusion to reach the surface". We analyzed in situ data from the NCP. Our results do not suggest that there was a significant impact from the stratosphere on surface ozone during the NOE. We argue that the NOE was not caused by stratospheric intrusion but originated from fresh photochemical production in the lower troposphere.
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.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
Atmos. Chem. Phys., 24, 3009–3028, https://doi.org/10.5194/acp-24-3009-2024, https://doi.org/10.5194/acp-24-3009-2024, 2024
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We compute CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned mines. Mine-by-mine gas and flux data and 30 min observations from a flux tower located next to a mine shaft are integrated. The observed variability and bias correction are propagated over the emissions dataset, demonstrating that daily observations may not cover the range of variability. Comparisons show both an emissions magnitude and spatial mismatch with current inventories.
Yao Yan Huang and D. James Donaldson
Atmos. Chem. Phys., 24, 2387–2398, https://doi.org/10.5194/acp-24-2387-2024, https://doi.org/10.5194/acp-24-2387-2024, 2024
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Ground-level ozone interacts at the lake–land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are more greatly affected seasonally.
Katrin Müller, Jordis S. Tradowsky, Peter von der Gathen, Christoph Ritter, Sharon Patris, Justus Notholt, and Markus Rex
Atmos. Chem. Phys., 24, 2169–2193, https://doi.org/10.5194/acp-24-2169-2024, https://doi.org/10.5194/acp-24-2169-2024, 2024
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The Palau Atmospheric Observatory is introduced as an ideal site to detect changes in atmospheric composition and dynamics above the remote tropical western Pacific. We focus on the ozone sounding program from 2016–2021, including El Niño 2016. The year-round high convective activity is reflected in dominant low tropospheric ozone and high relative humidity. Their seasonal distributions are unique compared to other tropical sites and are modulated by the Intertropical Convergence Zone.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
Atmos. Chem. Phys., 24, 2195–2205, https://doi.org/10.5194/acp-24-2195-2024, https://doi.org/10.5194/acp-24-2195-2024, 2024
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The formation of secondary sulfate needs to be further explored. In this work, we simultaneously measured sulfur and oxygen isotopic compositions to gain an increased understanding of specific sulfate formation processes. The results indicated that secondary sulfate was mainly ascribed to SO2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H2O2 and Fe3+ / O2. This study is favourable for deeply investigating the sulfur cycle in the atmosphere.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Ying Zhang, Duzitian Li, Xu-Cheng He, Wei Nie, Chenjuan Deng, Runlong Cai, Yuliang Liu, Yishuo Guo, Chong Liu, Yiran Li, Liangduo Chen, Yuanyuan Li, Chenjie Hua, Tingyu Liu, Zongcheng Wang, Jiali Xie, Lei Wang, Tuukka Petäjä, Federico Bianchi, Ximeng Qi, Xuguang Chi, Pauli Paasonen, Yongchun Liu, Chao Yan, Jingkun Jiang, Aijun Ding, and Markku Kulmala
Atmos. Chem. Phys., 24, 1873–1893, https://doi.org/10.5194/acp-24-1873-2024, https://doi.org/10.5194/acp-24-1873-2024, 2024
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This study conducts a long-term observation of gaseous iodine oxoacids in two Chinese megacities, revealing their ubiquitous presence with peak concentrations (up to 0.1 pptv) in summer. Our analysis suggests a mix of terrestrial and marine sources for iodine. Additionally, iodic acid is identified as a notable contributor to sub-3 nm particle growth and particle survival probability.
Guoxian Zhang, Renzhi Hu, Pinhua Xie, Changjin Hu, Xiaoyan Liu, Liujun Zhong, Haotian Cai, Bo Zhu, Shiyong Xia, Xiaofeng Huang, Xin Li, and Wenqing Liu
Atmos. Chem. Phys., 24, 1825–1839, https://doi.org/10.5194/acp-24-1825-2024, https://doi.org/10.5194/acp-24-1825-2024, 2024
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Comprehensive observation of HOx radicals was conducted at a coastal site in the Pearl River Delta. Radical chemistry was influenced by different air masses in a time-dependent way. Land mass promotes a more active photochemical process, with daily averages of 7.1 × 106 and 5.2 × 108 cm−3 for OH and HO2 respectively. The rapid oxidation process was accompanied by a higher diurnal HONO concentration, which influences the ozone-sensitive system and eventually magnifies the background ozone.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Shigeyuki Ishidoya, Kazuhiro Tsuboi, Hiroaki Kondo, Kentaro Ishijima, Nobuyuki Aoki, Hidekazu Matsueda, and Kazuyuki Saito
Atmos. Chem. Phys., 24, 1059–1077, https://doi.org/10.5194/acp-24-1059-2024, https://doi.org/10.5194/acp-24-1059-2024, 2024
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A method evaluating techniques for carbon neutrality, such as carbon capture and storage (CCS), is important. This study presents a method to evaluate CO2 emissions from a cement plant based on atmospheric O2 and CO2 measurements. The method will also be useful for evaluating CO2 capture from flue gas at CCS plants, since the plants remove CO2 from the atmosphere without causing any O2 changes, just as cement plants do, differing only in the direction of CO2 exchange with the atmosphere.
Magdalena Pühl, Anke Roiger, Alina Fiehn, Alan M. Gorchov Negron, Eric A. Kort, Stefan Schwietzke, Ignacio Pisso, Amy Foulds, James Lee, James L. France, Anna E. Jones, Dave Lowry, Rebecca E. Fisher, Langwen Huang, Jacob Shaw, Prudence Bateson, Stephen Andrews, Stuart Young, Pamela Dominutti, Tom Lachlan-Cope, Alexandra Weiss, and Grant Allen
Atmos. Chem. Phys., 24, 1005–1024, https://doi.org/10.5194/acp-24-1005-2024, https://doi.org/10.5194/acp-24-1005-2024, 2024
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In April–May 2019 we carried out an airborne field campaign in the southern North Sea with the aim of studying methane emissions of offshore gas installations. We determined methane emissions from elevated methane measured downstream of the sampled installations. We compare our measured methane emissions with estimated methane emissions from national and global annual inventories. As a result, we find inconsistencies of inventories and large discrepancies between measurements and inventories.
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.
Jie Wang, Haichao Wang, Yee Jun Tham, Lili Ming, Zelong Zheng, Guizhen Fang, Cuizhi Sun, Zhenhao Ling, Jun Zhao, and Shaojia Fan
Atmos. Chem. Phys., 24, 977–992, https://doi.org/10.5194/acp-24-977-2024, https://doi.org/10.5194/acp-24-977-2024, 2024
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Many works report NO3 chemistry in inland regions while less target marine regions. We measured N2O5 and related species on a typical island and found intensive nighttime chemistry and rapid NO3 loss. NO contributed significantly to NO3 loss despite its sub-ppbv level, suggesting nocturnal NO3 reactions would be largely enhanced once free from NO emissions in the open ocean. This highlights the strong influences of urban outflow on downward marine areas in terms of nighttime chemistry.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Jérémy Gueffier, François Gheusi, Marie Lothon, Véronique Pont, Alban Philibert, Fabienne Lohou, Solène Derrien, Yannick Bezombes, Gilles Athier, Yves Meyerfeld, Antoine Vial, and Emmanuel Leclerc
Atmos. Chem. Phys., 24, 287–316, https://doi.org/10.5194/acp-24-287-2024, https://doi.org/10.5194/acp-24-287-2024, 2024
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This study investigates the link between weather regime and atmospheric composition at a Pyrenean observatory. Five years of meteorological data were synchronized on a daily basis and then, using a clustering method, separated into six groups of observation days, with most showing marked characteristics of different weather regimes (fair and disturbed weather, winter windstorms, foehn). Statistical differences in gas and particle concentrations appeared between the groups and are discussed.
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.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
Yifei Song, Chaoyang Xue, Yuanyuan Zhang, Pengfei Liu, Fengxia Bao, Xuran Li, and Yujing Mu
Atmos. Chem. Phys., 23, 15733–15747, https://doi.org/10.5194/acp-23-15733-2023, https://doi.org/10.5194/acp-23-15733-2023, 2023
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We present measurements of HONO flux and related parameters over an agricultural field during a whole growing season of summer maize. This dataset allows studies on the characteristics and influencing factors of soil HONO emissions, determination of HONO emission factors, estimation of total HONO emissions at a national scale, and the discussion on future environmental policies in terms of mitigating regional air pollution.
Can Ye, Keding Lu, Xuefei Ma, Wanyi Qiu, Shule Li, Xinping Yang, Chaoyang Xue, Tianyu Zhai, Yuhan Liu, Xuan Li, Yang Li, Haichao Wang, Zhaofeng Tan, Xiaorui Chen, Huabin Dong, Limin Zeng, Min Hu, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 15455–15472, https://doi.org/10.5194/acp-23-15455-2023, https://doi.org/10.5194/acp-23-15455-2023, 2023
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In this study, combining comprehensive field measurements and a box model, we found NO2 conversion on the ground surface was the most important source for HONO production among the proposed heterogeneous and gas-phase HONO sources. In addition, HONO was found to evidently enhance O3 production and aggravate O3 pollution in summer in China. Our study improved our understanding of the relative importance of different HONO sources and the crucial role of HONO in O3 formation in polluted areas.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Yifan Jiang, Men Xia, Zhe Wang, Penggang Zheng, Yi Chen, and Tao Wang
Atmos. Chem. Phys., 23, 14813–14828, https://doi.org/10.5194/acp-23-14813-2023, https://doi.org/10.5194/acp-23-14813-2023, 2023
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This study provides the first estimate of high rates of formic acid (HCOOH) production from the photochemical aging of real ambient particles and demonstrates the potential importance of this pathway in the formation of HCOOH under ambient conditions. Incorporating this pathway significantly improved the performance of a widely used chemical model. Our solution irradiation experiments demonstrated the importance of nitrate photolysis in HCOOH production via the production of oxidants.
Xuelian Zhong, Hengqing Shen, Min Zhao, Ji Zhang, Yue Sun, Yuhong Liu, Yingnan Zhang, Ye Shan, Hongyong Li, Jiangshan Mu, Yu Yang, Yanqiu Nie, Jinghao Tang, Can Dong, Xinfeng Wang, Yujiao Zhu, Mingzhi Guo, Wenxing Wang, and Likun Xue
Atmos. Chem. Phys., 23, 14761–14778, https://doi.org/10.5194/acp-23-14761-2023, https://doi.org/10.5194/acp-23-14761-2023, 2023
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Nitrous acid (HONO) is vital for atmospheric oxidation. In research at Mount Lao, China, models revealed a significant unidentified marine HONO source. Overlooking this could skew our understanding of air quality and climate change. This finding emphasizes HONO’s importance in the coastal atmosphere, uncovering previously unnoticed interactions.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
EGUsphere, https://doi.org/10.5194/egusphere-2023-2255, https://doi.org/10.5194/egusphere-2023-2255, 2023
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This study presents the concurrent online measurements of organic gas and particles (VOCs and OA) at a forest site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contribute significantly to nighttime particle growth. The results help to understand the causes of nighttime particle growth regularly observed in summer in the central European rural forested environments.
Steven Job Thomas, Toni Tykkä, Heidi Hellén, Federico Bianchi, and Arnaud P. Praplan
Atmos. Chem. Phys., 23, 14627–14642, https://doi.org/10.5194/acp-23-14627-2023, https://doi.org/10.5194/acp-23-14627-2023, 2023
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The study employed total ozone reactivity to demonstrate how emissions of Norway spruce readily react with ozone and could be a major ozone sink, particularly under stress. Additionally, this approach provided insight into the limitations of current analytical techniques that measure the compounds present or emitted into the atmosphere. The study shows how the technique used was not enough to measure all compounds emitted, and this could potentially underestimate various atmospheric processes.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Robert Woodward-Massey, Roberto Sommariva, Lisa K. Whalley, Danny R. Cryer, Trevor Ingham, William J. Bloss, Stephen M. Ball, Sam Cox, James D. Lee, Chris P. Reed, Leigh R. Crilley, Louisa J. Kramer, Brian J. Bandy, Grant L. Forster, Claire E. Reeves, Paul S. Monks, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 14393–14424, https://doi.org/10.5194/acp-23-14393-2023, https://doi.org/10.5194/acp-23-14393-2023, 2023
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Measurements of OH, HO2 and RO2 radicals and also OH reactivity were made at a UK coastal site and compared to calculations from a constrained box model utilising the Master Chemical Mechanism. The model agreement displayed a strong dependence on the NO concentration. An experimental budget analysis for OH, HO2, RO2 and total ROx demonstrated significant imbalances between HO2 and RO2 production rates. Ozone production rates were calculated from measured radicals and compared to modelled values.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Heidi Hellén, Rostislav Kouznetsov, Kaisa Kraft, Jukka Seppälä, Mika Vestenius, Jukka-Pekka Jalkanen, Lauri Laakso, and Hannele Hakola
EGUsphere, https://doi.org/10.5194/egusphere-2023-2323, https://doi.org/10.5194/egusphere-2023-2323, 2023
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Mixing ratios of C2-C5 NMHCs and methanethiol were measured on an island in Baltic Sea using an in-situ gas chromatograph. Shipping emissions were found to be an important source of ethene, ethyne, propene and benzene. High summertime mixing ratios of methanethiol and dependence of mixing ratios on sea water temperature and height indicated the biogenic origin possibly from phytoplankton or macroalgae. These emissions may have strong impacts on SO2 production and new particle formation.
Rebecca M. Garland, Katye E. Altieri, Laura Dawidowski, Laura Gallardo, Aderiana Mbandi, Nestor Y. Rojas, and N'datchoh E. Touré
EGUsphere, https://doi.org/10.5194/egusphere-2023-2566, https://doi.org/10.5194/egusphere-2023-2566, 2023
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In this opinion, we focus on two geographical areas in the Global South to discuss some common challenges and constraints, with a focus on our strengths in atmospheric science research. It is these strengths, we believe, that highlight the critical role of Global South researchers in the future of atmospheric science research.
Clara M. Nussbaumer, Bryan K. Place, Qindan Zhu, Eva Y. Pfannerstill, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Ryan Ward, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 13015–13028, https://doi.org/10.5194/acp-23-13015-2023, https://doi.org/10.5194/acp-23-13015-2023, 2023
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NOx is a precursor to hazardous tropospheric ozone and can be emitted from various anthropogenic sources. It is important to quantify NOx emissions in urban environments to improve the local air quality, which still remains a challenge, as sources are heterogeneous in space and time. In this study, we calculate NOx emissions over Los Angeles, based on aircraft measurements in June 2021, and compare them to a local emission inventory, which we find mostly overpredicts the measured values.
Magdalena Okuljar, Olga Garmash, Miska Olin, Joni Kalliokoski, Hilkka Timonen, Jarkko V. Niemi, Pauli Paasonen, Jenni Kontkanen, Yanjun Zhang, Heidi Hellén, Heino Kuuluvainen, Minna Aurela, Hanna E. Manninen, Mikko Sipilä, Topi Rönkkö, Tuukka Petäjä, Markku Kulmala, Miikka Dal Maso, and Mikael Ehn
Atmos. Chem. Phys., 23, 12965–12983, https://doi.org/10.5194/acp-23-12965-2023, https://doi.org/10.5194/acp-23-12965-2023, 2023
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Highly oxygenated organic molecules (HOMs) form secondary organic aerosol that affects air quality and health. In this study, we demonstrate that in a moderately polluted city with abundant vegetation, the composition of HOMs is largely controlled by the effect of NOx on the biogenic volatile organic compound oxidation. Comparing the results from two nearby stations, we show that HOM composition and formation pathways can change considerably within small distances in urban environments.
Si-Wan Kim, Kyoung-Min Kim, Yujoo Jeong, Seunghwan Seo, Yeonsu Park, and Jeongyeon Kim
Atmos. Chem. Phys., 23, 12867–12886, https://doi.org/10.5194/acp-23-12867-2023, https://doi.org/10.5194/acp-23-12867-2023, 2023
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Surface ozone is a pollutant regulated for public health. This study derived surface ozone trends over South Korea from 2001 to 2021 and highlighted that South Korea has been a nonattainment area since 2010, based on the US EPA standard. However, the occurrences of high ozone condition decreased in spring during the COVID-19 pandemic, partly due to large reductions of ozone precursor concentrations in China and South Korea.
Zeyu Sun, Zheng Zong, Yang Tan, Chongguo Tian, Zeyu Liu, Fan Zhang, Rong Sun, Yingjun Chen, Jun Li, and Gan Zhang
Atmos. Chem. Phys., 23, 12851–12865, https://doi.org/10.5194/acp-23-12851-2023, https://doi.org/10.5194/acp-23-12851-2023, 2023
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This is the first report of ship-emitted nitrogen stable isotope composition (δ15N) of nitrogen oxides (NOx). The results showed that δ15N–NOx from ships was −18.5 ± 10.9 ‰ and increased monotonically with tightening emission regulations. The selective catalytic reduction system was the most vital factor. The temporal variation in δ15N–NOx was evaluated and can be used to select suitable δ15N–NOx for a more accurate assessment of the contribution of ship-emitted exhaust to atmospheric NOx.
Eva Y. Pfannerstill, Caleb Arata, Qindan Zhu, Benjamin C. Schulze, Roy Woods, John H. Seinfeld, Anthony Bucholtz, Ronald C. Cohen, and Allen H. Goldstein
Atmos. Chem. Phys., 23, 12753–12780, https://doi.org/10.5194/acp-23-12753-2023, https://doi.org/10.5194/acp-23-12753-2023, 2023
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The San Joaquin Valley is an agricultural area with poor air quality. Organic gases drive the formation of hazardous air pollutants. Agricultural emissions of these gases are not well understood and have rarely been quantified at landscape scale. By combining aircraft-based emission measurements with land cover information, we found mis- or unrepresented emission sources. Our results help in understanding of pollution sources and in improving predictions of air quality in agricultural regions.
Youwei Hong, Keran Zhang, Dan Liao, Gaojie Chen, Min Zhao, Yiling Lin, Xiaoting Ji, Ke Xu, Yu Wu, Ruilian Yu, Gongren Hu, Sung-Deuk Choi, Likun Xue, and Jinsheng Chen
Atmos. Chem. Phys., 23, 10795–10807, https://doi.org/10.5194/acp-23-10795-2023, https://doi.org/10.5194/acp-23-10795-2023, 2023
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Particle uptakes of HCHO and the impacts on PM2.5 and O3 production remain highly uncertain. Based on the investigation of co-occurring wintertime O3 and PM2.5 pollution in a coastal city of southeast China, we found enhanced heterogeneous formation of hydroxymethanesulfonate (HMS) and increased ROx concentrations and net O3 production rates. The findings of this study are helpful to better explore the mechanisms of key precursors for co-occurring PM2.5 and O3 pollution.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Chunxiang Ye, Shuzheng Guo, Weili Lin, Fangjie Tian, Jianshu Wang, Chong Zhang, Suzhen Chi, Yi Chen, Yingjie Zhang, Limin Zeng, Xin Li, Duo Bu, Jiacheng Zhou, and Weixiong Zhao
Atmos. Chem. Phys., 23, 10383–10397, https://doi.org/10.5194/acp-23-10383-2023, https://doi.org/10.5194/acp-23-10383-2023, 2023
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Online volatile organic compound (VOC) measurements by gas chromatography–mass spectrometry, with other O3 precursors, were used to identify key VOC and other key sources in Lhasa. Total VOCs (TVOCs), alkanes, and aromatics are half as abundant as in Beijing. Oxygenated VOCs (OVOCs) consist of 52 % of the TVOCs. Alkenes and OVOCs account for 80 % of the ozone formation potential. Aromatics dominate secondary organic aerosol potential. Positive matrix factorization decomposed residential sources.
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.
Jenny Oh, Chubashini Shunthirasingham, Ying Duan Lei, Faqiang Zhan, Yuening Li, Abigaëlle Dalpé Castilloux, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Sabine Eckhardt, Nick Alexandrou, Hayley Hung, and Frank Wania
Atmos. Chem. Phys., 23, 10191–10205, https://doi.org/10.5194/acp-23-10191-2023, https://doi.org/10.5194/acp-23-10191-2023, 2023
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An emerging brominated flame retardant (BFR) called TBECH (1,2-dibromo-4-(1,2-dibromoethyl)cyclohexane) has never been produced or imported for use in Canada yet is found to be one of the most abundant gaseous BFRs in the Canadian atmosphere. The recorded spatial and temporal variability of TBECH suggest that the release from imported consumer products containing TBECH is the most likely explanation for its environmental occurrence in Canada.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Qindan Zhu, Bryan Place, Eva Y. Pfannerstill, Sha Tong, Huanxin Zhang, Jun Wang, Clara M. Nussbaumer, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Allen H. Goldstein, and Ronald C. Cohen
Atmos. Chem. Phys., 23, 9669–9683, https://doi.org/10.5194/acp-23-9669-2023, https://doi.org/10.5194/acp-23-9669-2023, 2023
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Nitrogen oxide (NOx) is a hazardous air pollutant, and it is the precursor of short-lived climate forcers like tropospheric ozone and aerosol particles. While NOx emissions from transportation has been strictly regulated, soil NOx emissions are overlooked. We use the airborne flux measurements to observe NOx emissions from highways and urban and cultivated soil land cover types. We show non-negligible soil NOx emissions, which are significantly underestimated in current model simulations.
Xin Yang, Kimberly Strong, Alison Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley Walker, Sara Morris, and Peter Effertz
EGUsphere, https://doi.org/10.5194/egusphere-2023-1446, https://doi.org/10.5194/egusphere-2023-1446, 2023
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This study uses in-situ field data collected from a Canadian high Arctic site to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. In addition, surface snow bromide and nitrate are significantly correlated, one molecule bromide deposited is accompanied by 4–7 molecules nitrate, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. This is the first time such an effect was seen in snow chemistry on a time scale of one day.
Money Ossohou, Jonathan Edward Hickman, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, Marcellin Adon, Véronique Yoboué, Eric Gardrat, Maria Dias Alvès, and Corinne Galy-Lacaux
Atmos. Chem. Phys., 23, 9473–9494, https://doi.org/10.5194/acp-23-9473-2023, https://doi.org/10.5194/acp-23-9473-2023, 2023
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The updated analyses of ground-based concentrations and satellite total vertical columns of atmospheric ammonia help us to better understand 21st century ammonia dynamics in sub-Saharan Africa. We conclude that the drivers of trends are agriculture in the dry savanna of Katibougou, Mali; air temperature and agriculture in the wet savanna of Djougou, Benin, and Lamto, Côte d'Ivoire; and leaf area index, air temperature, residential, and agriculture in forests of Bomassa, Republic of Congo.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
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Short summary
After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors...
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