Articles | Volume 16, issue 21
https://doi.org/10.5194/acp-16-13541-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-13541-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
01 Nov 2016
Research article |
| 01 Nov 2016
Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere–lower stratosphere
Richard J. Pope
CORRESPONDING AUTHOR
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Earth Observation, University of Leeds, Leeds, UK
Nigel A. D. Richards
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Earth Observation, University of Leeds, Leeds, UK
Martyn P. Chipperfield
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Earth Observation, University of Leeds, Leeds, UK
David P. Moore
Department of Physics and Astronomy, University of Leicester, Leicester, UK
National Centre for Earth Observation, University of Leicester, Leicester, UK
Sarah A. Monks
Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
Stephen R. Arnold
School of Earth and Environment, University of Leeds, Leeds, UK
Norbert Glatthor
Karlsruhe Institute of Technology, Institute of Meteorology and Climate Research, Karlsruhe, Germany
Michael Kiefer
Karlsruhe Institute of Technology, Institute of Meteorology and Climate Research, Karlsruhe, Germany
Tom J. Breider
School of Engineering and Applied Sciences, Harvard University, Cambridge, USA
Jeremy J. Harrison
Department of Physics and Astronomy, University of Leicester, Leicester, UK
National Centre for Earth Observation, University of Leicester, Leicester, UK
John J. Remedios
Department of Physics and Astronomy, University of Leicester, Leicester, UK
National Centre for Earth Observation, University of Leicester, Leicester, UK
Carsten Warneke
Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA
James M. Roberts
Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO, USA
Glenn S. Diskin
NASA Langley Research Center, Chemistry and Dynamics Branch, Hampton, VA, USA
Lewis G. Huey
Georgia Institute of Technology, Atlanta, GA, USA
Armin Wisthaler
University of Innsbruck, Innsbruck, Austria
University of Oslo, Oslo, Norway
Eric C. Apel
Atmospheric Chemistry Division, National Centre for Atmospheric Research, Boulder, CO, USA
Peter F. Bernath
Department of Chemistry and Biochemistry, Old Dominion University, Norfolk, VA, USA
Wuhu Feng
School of Earth and Environment, University of Leeds, Leeds, UK
National Centre for Atmospheric Science, University of Leeds, Leeds, UK
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Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
R. J. Pope, N. H. Savage, M. P. Chipperfield, C. Ordóñez, and L. S. Neal
Atmos. Chem. Phys., 15, 11201–11215, https://doi.org/10.5194/acp-15-11201-2015, https://doi.org/10.5194/acp-15-11201-2015, 2015
R. J. Pope, M. P. Chipperfield, N. H. Savage, C. Ordóñez, L. S. Neal, L. A. Lee, S. S. Dhomse, N. A. D. Richards, and T. D. Keslake
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Huisheng Bian, Mian Chin, Peter R. Colarco, Eric C. Apel, Donald R. Blake, Karl Froyd, Rebecca S. Hornbrook, Jose Jimenez, Pedro Campuzano Jost, Michael Lawler, Mingxu Liu, Marianne Tronstad Lund, Hitoshi Matsui, Benjamin A. Nault, Joyce E. Penner, Andrew W. Rollins, Gregory Schill, Ragnhild B. Skeie, Hailong Wang, Lu Xu, Kai Zhang, and Jialei Zhu
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Michael P. Cartwright, Richard J. Pope, Jeremy J. Harrison, Martyn P. Chipperfield, Chris Wilson, Wuhu Feng, David P. Moore, and Parvadha Suntharalingam
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Qian Xiao, Jiaoshi Zhang, Yang Wang, Luke D. Ziemba, Ewan Crosbie, Edward L. Winstead, Claire E. Robinson, Joshua P. DiGangi, Glenn S. Diskin, Jeffrey S. Reid, K. Sebastian Schmidt, Armin Sorooshian, Miguel Ricardo A. Hilario, Sarah Woods, Paul Lawson, Snorre A. Stamnes, and Jian Wang
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Luana S. Basso, Chris Wilson, Martyn P. Chipperfield, Graciela Tejada, Henrique L. G. Cassol, Egídio Arai, Mathew Williams, T. Luke Smallman, Wouter Peters, Stijn Naus, John B. Miller, and Manuel Gloor
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Matthew M. Coggon, Chelsea E. Stockwell, Megan S. Claflin, Eva Y. Pfannerstill, Xu Lu, Jessica B. Gilman, Julia Marcantonio, Cong Cao, Kelvin Bates, Georgios I. Gkatzelis, Aaron Lamplugh, Erin F. Katz, Caleb Arata, Eric C. Apel, Rebecca S. Hornbrook, Felix Piel, Francesca Majluf, Donald R. Blake, Armin Wisthaler, Manjula Canagaratna, Brian M. Lerner, Allen H. Goldstein, John E. Mak, and Carsten Warneke
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Preprint under review for AMT
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Armin Sorooshian, Mikhail D. Alexandrov, Adam D. Bell, Ryan Bennett, Grace Betito, Sharon P. Burton, Megan E. Buzanowicz, Brian Cairns, Eduard V. Chemyakin, Gao Chen, Yonghoon Choi, Brian L. Collister, Anthony L. Cook, Andrea F. Corral, Ewan C. Crosbie, Bastiaan van Diedenhoven, Joshua P. DiGangi, Glenn S. Diskin, Sanja Dmitrovic, Eva-Lou Edwards, Marta A. Fenn, Richard A. Ferrare, David van Gilst, Johnathan W. Hair, David B. Harper, Miguel Ricardo A. Hilario, Chris A. Hostetler, Nathan Jester, Michael Jones, Simon Kirschler, Mary M. Kleb, John M. Kusterer, Sean Leavor, Joseph W. Lee, Hongyu Liu, Kayla McCauley, Richard H. Moore, Joseph Nied, Anthony Notari, John B. Nowak, David Painemal, Kasey E. Phillips, Claire E. Robinson, Amy Jo Scarino, Joseph S. Schlosser, Shane T. Seaman, Chellappan Seethala, Taylor J. Shingler, Michael A. Shook, Kenneth A. Sinclair, William L. Smith Jr., Douglas A. Spangenberg, Snorre A. Stamnes, Kenneth L. Thornhill, Christiane Voigt, Holger Vömel, Andrzej P. Wasilewski, Hailong Wang, Edward L. Winstead, Kira Zeider, Xubin Zeng, Bo Zhang, Luke D. Ziemba, and Paquita Zuidema
Earth Syst. Sci. Data, 15, 3419–3472, https://doi.org/10.5194/essd-15-3419-2023, https://doi.org/10.5194/essd-15-3419-2023, 2023
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The NASA Aerosol Cloud meTeorology Interactions oVer the western ATlantic Experiment (ACTIVATE) produced a unique dataset for research into aerosol–cloud–meteorology interactions. HU-25 Falcon and King Air aircraft conducted systematic and spatially coordinated flights over the northwest Atlantic Ocean. This paper describes the ACTIVATE flight strategy, instrument and complementary dataset products, data access and usage details, and data application notes.
Yang Li, Wuhu Feng, Xin Zhou, Yajuan Li, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2023-1452, https://doi.org/10.5194/egusphere-2023-1452, 2023
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Tibetan Plateau (TP), the highest and largest plateau, experiences strong surface solar UV radiation, whose excess can cause harmful influences on the local biota. Hence, it is critical to study TP ozone. We find ENSO, the strongest interannual phenomenon, can induce tropospheric temperature change and thus cause tropopause movement, which in turn leads to ozone change. Our understanding implies that future more strong ENSO events will play a key role in ozone recovery and ecosystems of the TP.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Yanlin Li, Tai-Yin Huang, Julio Urbina, Fabio Vargas, and Wuhu Feng
Ann. Geophys. Discuss., https://doi.org/10.5194/angeo-2023-20, https://doi.org/10.5194/angeo-2023-20, 2023
Revised manuscript under review for ANGEO
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This work combines Lidar observation data and a new numerical sodium chemistry model, using data assimilation to study the relationship between the mesospheric sodium layer and the meteoric input function. The simulation captures the seasonal variability of sodium number density compared with lidar observations over Colorado State University lidar. The estimated global ablated meteoroid material inputs inferred from ALO and CSU observations are 116.85 t/day and 61.4 t/day, respectively.
Maya Garcia-Comas, Bernd Funke, Manuel Lopez-Puertas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Belen Martinez-Mondejar, Gabriele P. Stiller, and Thomas von Clarmann
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-119, https://doi.org/10.5194/amt-2023-119, 2023
Revised manuscript under review for AMT
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We have released version 8 of MIPAS IMK/IAA MA/UA/NLC temperatures and pointing information retrieved from MIPAS version 8.03 calibrated spectra, covering the 20–115 km altitude range. We considered non-local thermodynamic equilibrium emission explicitly for each limb scan, essential to retrieve accurate temperatures above the mid-mesosphere. The comparison of this temperature dataset with co-located SABER measurements shows an excellent agreement, even better than in previous MIPAS versions.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Georgios I. Gkatzelis, Matthew M. Coggon, Chelsea E. Stockwell, Rebecca S. Hornbrook, Hannah Allen, Eric C. Apel, Katherine Ball, 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 DiGangi, Glenn Diskin, Alan Fried, Jessica Gilman, Hongyu Guo, Johnathan W. Hair, Hannah A. Halliday, Thomas F. Hanisco, Reem Hannun, Alan Hills, 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, James A. 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 Vasquez, Patrick R. Veres, Rebecca Washenfelder, Petter Weibring, Paul O. Wennberg, Armin Wisthaler, Glenn Wolfe, Caroline Womack, Lu Xu, Robert Yokelson, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2023-1439, https://doi.org/10.5194/egusphere-2023-1439, 2023
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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.
Victoria A. Flood, Kimberly Strong, Cynthia H. Whaley, Kaley A. Walker, Thomas Blumenstock, James W. Hannigan, Johan Mellqvist, Justus Notholt, Mathias Palm, Amelie N. Röhling, Stephen Arnold, Stephen Beagley, Rong-You Chien, Jesper Christensen, Makoto Deushi, Srdjan Dobricic, Xinyi Dong, Joshua S. Fu, Michael Gauss, Wanmin Gong, Joakim Langner, Kathy S. Law, Louis Marelle, Tatsuo Onishi, Naga Oshima, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Manu A. Thomas, Svetlana Tsyro, and Steven Turnock
EGUsphere, https://doi.org/10.5194/egusphere-2023-1161, https://doi.org/10.5194/egusphere-2023-1161, 2023
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It is important to understand the composition of the Arctic atmosphere and how it is changing. Atmospheric models provide simulations that can inform policy. This study examines simulations of CH4, CO, and O3 by 11 models. Model performance is assessed by comparing results matched in space and time to measurements from five high-latitude ground-based infrared spectrometers. This work finds that models are generally underpredicting the concentrations of these gases in the Arctic troposphere.
Martyn Chipperfield and Slimane Bekki
EGUsphere, https://doi.org/10.5194/egusphere-2023-1409, https://doi.org/10.5194/egusphere-2023-1409, 2023
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We give a personal perspective on recent issues related to the depletion of stratospheric ozone and some newly emerging challenges. We first provide a brief review of historic work on understanding the ozone layer and review ozone recovery from the effects of halogenated source gases and the Montreal Protocol. We then discuss the recent observations of ozone depletion from Australian fires in early 2020 and the Hunga Tonga-Hunga Ha`apai volcano in January 2022.
Richard J. Pope, Brian J. Kerridge, Richard Siddans, Barry G. Latter, Martyn P. Chipperfield, Wuhu Feng, Matilda A. Pimlott, Sandip S. Dhomse, Christian Retscher, and Richard Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2023-1172, https://doi.org/10.5194/egusphere-2023-1172, 2023
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Ozone is a potent air pollutant and we present the first study to investigate long-term changes in lower tropospheric column ozone (LTO3) from space. We have constructed a merged LTO3 dataset from GOME-1, SCIAMACHY and OMI between 1996 and 2017. Comparing LTO3 between the 1996–2000 and 2013–2017 5-year averages, we find significant positive increases in the tropics/sub-tropics, while in the northern mid-latitudes, we find small scale differences.
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
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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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.
Norbert Glatthor, Thomas von Clarmann, Bernd Funke, Maya Garcia-Comas, Udo Grabowski, Michael Höpfner, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, Manuel Lopez-Puertas, and Gabriele P. Stiller
EGUsphere, https://doi.org/10.5194/egusphere-2023-919, https://doi.org/10.5194/egusphere-2023-919, 2023
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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We present global atmospheric methane (CH4) and nitrous oxide (N2O) distributions retrieved from measurements of the MIPAS instrument onboard the ENVIronmental SATellite (ENVISAT) during 2002 to 2012. Monitoring of these gases is of scientific interest, because both of them are strong greenhouse gases. We analyse the latest, improved version of calibrated MIPAS measurements. Further, we apply a new retrieval scheme leading to an improved CH4 and N2O data product .
Manuel López-Puertas, Maya García-Comas, Bernd Funke, Thomas von Clarmann, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Alexandra Laeng, Andrea Linden, and Gabriele P. Stiller
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-118, https://doi.org/10.5194/amt-2023-118, 2023
Revised manuscript accepted for AMT
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This paper describes a new version (V8) of O3 data from MIPAS middle atmosphere spectra. The dataset comprises high-quality O3 profiles from 20 to 100 km, with a pole-to-pole latitude coverage, day and night-time, and spanning from 2005 until 2012. An exhaustive treatment of errors has been performed. Compared to other satellite instruments, MIPAS ozone shows a positive bias of 5–8 % below 70 km. In the upper mesosphere, this new version agrees much better than previous ones (within 10 %).
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Peter Joyce, Cristina Ruiz Villena, Yahui Huang, Alex Webb, Manuel Gloor, Fabien H. Wagner, Martyn P. Chipperfield, Rocío Barrio Guilló, Chris Wilson, and Hartmut Boesch
Atmos. Meas. Tech., 16, 2627–2640, https://doi.org/10.5194/amt-16-2627-2023, https://doi.org/10.5194/amt-16-2627-2023, 2023
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Methane emissions are responsible for a lot of the warming caused by the greenhouse effect, much of which comes from a small number of point sources. We can identify methane point sources by analysing satellite data, but it requires a lot of time invested by experts and is prone to very high errors. Here, we produce a neural network that can automatically identify methane point sources and estimate the mass of methane that is being released per hour and are able to do so with far smaller errors.
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
EGUsphere, https://doi.org/10.5194/egusphere-2023-860, https://doi.org/10.5194/egusphere-2023-860, 2023
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We measured cyanogen bromide (BrCN) in the troposphere for the first time as part of a series of survey flights around the globe. BrCN is found to be a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments, and so is a previously unrecognized participant in this chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Joanna E. Dyson, Lisa K. Whalley, Eloise J. Slater, Robert Woodward-Massey, Chunxiang Ye, James D. Lee, Freya Squires, James R. Hopkins, Rachel E. Dunmore, Marvin Shaw, Jacqueline F. Hamilton, Alastair C. Lewis, Stephen D. Worrall, Asan Bacak, Archit Mehra, Thomas J. Bannan, Hugh Coe, Carl J. Percival, Bin Ouyang, C. Nicholas Hewitt, Roderic L. Jones, Leigh R. Crilley, Louisa J. Kramer, W. Joe F. Acton, William J. Bloss, Supattarachai Saksakulkrai, Jingsha Xu, Zongbo Shi, Roy M. Harrison, Simone Kotthaus, Sue Grimmond, Yele Sun, Weiqi Xu, Siyao Yue, Lianfang Wei, Pingqing Fu, Xinming Wang, Stephen R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 23, 5679–5697, https://doi.org/10.5194/acp-23-5679-2023, https://doi.org/10.5194/acp-23-5679-2023, 2023
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The hydroxyl (OH) and closely coupled hydroperoxyl (HO2) radicals are vital for their role in the removal of atmospheric pollutants. In less polluted regions, atmospheric models over-predict HO2 concentrations. In this modelling study, the impact of heterogeneous uptake of HO2 onto aerosol surfaces on radical concentrations and the ozone production regime in Beijing in the summertime is investigated, and the implications for emissions policies across China are considered.
Miguel Ricardo A. Hilario, Avelino F. Arellano, Ali Behrangi, Ewan C. Crosbie, Joshua P. DiGangi, Glenn S. Diskin, Michael A. Shook, Luke D. Ziemba, and Armin Sorooshian
EGUsphere, https://doi.org/10.5194/egusphere-2023-726, https://doi.org/10.5194/egusphere-2023-726, 2023
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Wet scavenging strongly influences aerosol lifetime and interactions but is a large uncertainty in global models. We present a flexible and repeatable method to identify meteorological variables relevant for estimating wet scavenging. For the tropical West Pacific, we show frequencies of precipitation or high humidity are better scavenging indicators than accumulated precipitation. This method applicable to different regions and may be used to inform scavenging parametrization schemes in models.
Andrea Pazmino, Florence Goutail, Sophie Godin-Beekmann, Alain Hauchecorne, Jean-Pierre Pommereau, Martyn P. Chipperfield, Wuhu Feng, Franck Lefèvre, Audrey Lecouffe, Michel Van Roozendael, Nis Jepsen, Georg Hansen, Rigel Kivi, Kimberly Strong, Kaley A. Walker, and Steve Colwell
EGUsphere, https://doi.org/10.5194/egusphere-2023-788, https://doi.org/10.5194/egusphere-2023-788, 2023
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The vortex-averaged ozone loss over the last three decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from SAOZ network and MSR2 reanalysis. Three metrics were developed to compute ozone trend since 2000. The study confirms the ozone recovery in the Antarctic and shows a first quantitative detection of ozone recovery in the Arctic that needs to be robustly confirmed in the future.
Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Manuel López-Puertas, Gabriele P. Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 16, 2167–2196, https://doi.org/10.5194/amt-16-2167-2023, https://doi.org/10.5194/amt-16-2167-2023, 2023
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New global nitric oxide (NO) volume-mixing-ratio and lower-thermospheric temperature data products, retrieved from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) spectra with the IMK-IAA MIPAS data processor, have been released. The dataset covers the entire Envisat mission lifetime and includes retrieval results from all MIPAS observation modes. The data are based on ESA version 8 calibration and were processed using an improved retrieval approach.
Antonio G. Bruno, Jeremy J. Harrison, Martyn P. Chipperfield, David P. Moore, Richard J. Pope, Christopher Wilson, Emmanuel Mahieu, and Justus Notholt
Atmos. Chem. Phys., 23, 4849–4861, https://doi.org/10.5194/acp-23-4849-2023, https://doi.org/10.5194/acp-23-4849-2023, 2023
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A 3-D chemical transport model, TOMCAT; satellite data; and ground-based observations have been used to investigate hydrogen cyanide (HCN) variability. We found that the oxidation by O(1D) drives the HCN loss in the middle stratosphere and the currently JPL-recommended OH reaction rate overestimates HCN atmospheric loss. We also evaluated two different ocean uptake schemes. We found them to be unrealistic, and we need to scale these schemes to obtain good agreement with HCN observations.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2023-496, https://doi.org/10.5194/egusphere-2023-496, 2023
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We quantify, for the first time, the time-varying impact of uncontrolled emissions of chlorinated very short-lived substances (Cl-VSLS) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLS are already having a non-negligible impact on stratospheric ozone, including a 6 DU reduction of Artic ozone in the cold winter of 2019/20, and any so future growth in emissions will continue to offset some of the benefits of the Montreal Protocol.
Michael Kiefer, Dale F. Hurst, Gabriele P. Stiller, Stefan Lossow, Holger Vömel, John Anderson, Faiza Azam, Jean-Loup Bertaux, Laurent Blanot, Klaus Bramstedt, John P. Burrows, Robert Damadeo, Bianca Maria Dinelli, Patrick Eriksson, Maya García-Comas, John C. Gille, Mark Hervig, Yasuko Kasai, Farahnaz Khosrawi, Donal Murtagh, Gerald E. Nedoluha, Stefan Noël, Piera Raspollini, William G. Read, Karen H. Rosenlof, Alexei Rozanov, Christopher E. Sioris, Takafumi Sugita, Thomas von Clarmann, Kaley A. Walker, and Katja Weigel
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-86, https://doi.org/10.5194/amt-2023-86, 2023
Revised manuscript accepted for AMT
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We quantify biases and drifts (and their uncertainties) between the stratospheric water vapor measurement records of 15 satellite-based instruments (SATs, with 31 different retrievals) and balloon-borne frost point hygrometers (FPs) launched at 27 globally distributed stations. These comparisons of measurements during the period 2000-2016 are made using robust, consistent statistical methods. With some exceptions, the biases and drifts determined for most SAT-FP pairs are < 10 % and < 1 % yr−1.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
EGUsphere, https://doi.org/10.5194/egusphere-2023-591, https://doi.org/10.5194/egusphere-2023-591, 2023
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For the first time a regularised multivariate regression model is used to estimate stratospheric ozone trends. Regularised regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite and chemical model-based ozone trends highlighting large uncertainties in our understanding about ozone variability, and we argue that a caution is needed while interpreting results with different methods and data sets.
Viktoria F. Sofieva, Monika Szelag, Johanna Tamminen, Carlo Arosio, Alexei Rozanov, Mark Weber, Doug Degenstein, Adam Bourassa, Daniel Zawada, Michael Kiefer, Alexandra Laeng, Kaley A. Walker, Patrick Sheese, Daan Hubert, Michel van Roozendael, Christian Retscher, Robert Damadeo, and Jerry D. Lumpe
Atmos. Meas. Tech., 16, 1881–1899, https://doi.org/10.5194/amt-16-1881-2023, https://doi.org/10.5194/amt-16-1881-2023, 2023
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The paper presents the updated SAGE-CCI-OMPS+ climate data record of monthly zonal mean ozone profiles. This dataset covers the stratosphere and combines measurements by nine limb and occultation satellite instruments (SAGE II, OSIRIS, MIPAS, SCIAMACHY, GOMOS, ACE-FTS, OMPS-LP, POAM III, and SAGE III/ISS). The update includes new versions of MIPAS, ACE-FTS, and OSIRIS datasets and introduces data from additional sensors (POAM III and SAGE III/ISS) and retrieval processors (OMPS-LP).
Ailish Melissa Graham, Richard J. Pope, Martyn P. Chipperfield, Sandip S. Dhomse, Matila Pimlott, Wuhu Feng, Vikas Singh, Ying Chen, Oliver Wild, Ranjeet Sokhi, and Gufran Beig
EGUsphere, https://doi.org/10.5194/egusphere-2023-382, https://doi.org/10.5194/egusphere-2023-382, 2023
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Our manuscript makes use of novel satellite data sets and high-resolution emissions datasets alongside a back trajectory model to investigate the balance of local and external sources influencing NOx air pollution changes in Delhi, with a focus on different emission sectors. We find that in the post-monsoon, NOx, which is mostly from the transport sector, is imported into Delhi. Therefore air quality mitigation strategies in Delhi and the surrounding regions to successfully control this issue.
Sandip S. Dhomse and Martyn P. Chipperfield
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-47, https://doi.org/10.5194/essd-2023-47, 2023
Revised manuscript accepted for ESSD
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There are no long-term stratospheric profile data set for two very important greenhouse gases : Methane (CH4) and Nitrous oxide (N2O). Along with radiative feeback, they also play key species that play an important role in controlling ozone loss in the stratosphere. Here, we use machine learning to fuse satellite and chemical model to construct long term gap free profile data sets for CH4 and N2O.
Michael Kiefer, Thomas von Clarmann, Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Michael Höpfner, Sylvia Kellmann, Alexandra Laeng, Andrea Linden, Manuel López-Puertas, and Gabriele P. Stiller
Atmos. Meas. Tech., 16, 1443–1460, https://doi.org/10.5194/amt-16-1443-2023, https://doi.org/10.5194/amt-16-1443-2023, 2023
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A new ozone data set, derived from radiation measurements of the space-borne instrument MIPAS, is presented. It consists of more than 2 million single ozone profiles from 2002–2012, covering virtually all latitudes and altitudes between 5 and 70 km. Progress in data calibration and processing methods allowed for significant improvement of the data quality, compared to previous data versions. Hence, the data set will help to better understand e.g. the time evolution of ozone in the stratosphere.
Laura Tomsche, Felix Piel, Tomas Mikoviny, Claus J. Nielsen, Hongyu Guo, Pedro Campuzano-Jost, Benjamin A. Nault, Melinda K. Schueneman, Jose L. Jimenez, Hannah Halliday, Glenn Diskin, Joshua P. DiGangi, John B. Nowak, Elizabeth B. Wiggins, Emily Gargulinski, Amber J. Soja, and Armin Wisthaler
Atmos. Chem. Phys., 23, 2331–2343, https://doi.org/10.5194/acp-23-2331-2023, https://doi.org/10.5194/acp-23-2331-2023, 2023
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Ammonia (NH3) is an important trace gas in the atmosphere and fires are among the poorly investigated sources. During the 2019 Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) aircraft campaign, we measured gaseous NH3 and particulate ammonium (NH4+) in smoke plumes emitted from 6 wildfires in the Western US and 66 small agricultural fires in the Southeastern US. We herein present a comprehensive set of emission factors of NH3 and NHx, where NHx = NH3 + NH4+.
Richard J. Pope, Brian J. Kerridge, Martyn P. Chipperfield, Richard Siddans, Barry G. Latter, Lucy J. Ventress, Matilda A. Pimlott, Wuhu Feng, Edward Comyn-Platt, Garry D. Hayman, Stephen R. Arnold, and Ailish M. Graham
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-827, https://doi.org/10.5194/acp-2022-827, 2023
Revised manuscript accepted for ACP
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In the summer of 2018, Europe experienced several persistent large-scale ozone (O3) pollution episodes. Satellite tropospheric O3 and surface O3 data recorded substantial enhancements in 2018 relative to other years. Targeted model simulations showed that meteorological processes and emissions controlled the elevated surface O3, while mid-tropospheric O3 enhancements were dominated by stratospheric O3 intrusion and advection of North Atlantic O3-rich air masses into Europe.
Cynthia H. Whaley, Kathy S. Law, Jens Liengaard Hjorth, Henrik Skov, Stephen R. Arnold, Joakim Langner, Jakob Boyd Pernov, Garance Bergeron, Ilann Bourgeois, Jesper H. Christensen, Rong-You Chien, Makoto Deushi, Xinyi Dong, Peter Effertz, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Greg Huey, Ulas Im, Rigel Kivi, Louis Marelle, Tatsuo Onishi, Naga Oshima, Irina Petropavlovskikh, Jeff Peischl, David A. Plummer, Luca Pozzoli, Jean-Christophe Raut, Tom Ryerson, Ragnhild Skeie, Sverre Solberg, Manu A. Thomas, Chelsea Thompson, Kostas Tsigaridis, Svetlana Tsyro, Steven T. Turnock, Knut von Salzen, and David W. Tarasick
Atmos. Chem. Phys., 23, 637–661, https://doi.org/10.5194/acp-23-637-2023, https://doi.org/10.5194/acp-23-637-2023, 2023
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This study summarizes recent research on ozone in the Arctic, a sensitive and rapidly warming region. We find that the seasonal cycles of near-surface atmospheric ozone are variable depending on whether they are near the coast, inland, or at high altitude. Several global model simulations were evaluated, and we found that because models lack some of the ozone chemistry that is important for the coastal Arctic locations, they do not accurately simulate ozone there.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven C. Wofsy
Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, https://doi.org/10.5194/acp-23-99-2023, 2023
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We have prepared a unique and unusual result from the recent ATom aircraft mission: a measurement-based derivation of the production and loss rates of ozone and methane over the ocean basins. These are the key products of chemistry models used in assessments but have thus far lacked observational metrics. It also shows the scales of variability of atmospheric chemical rates and provides a major challenge to the atmospheric models.
Lu Xu, Matthew M. Coggon, Chelsea E. Stockwell, Jessica B. Gilman, Michael A. Robinson, Martin Breitenlechner, Aaron Lamplugh, John D. Crounse, Paul O. Wennberg, J. Andrew Neuman, Gordon A. Novak, Patrick R. Veres, Steven S. Brown, and Carsten Warneke
Atmos. Meas. Tech., 15, 7353–7373, https://doi.org/10.5194/amt-15-7353-2022, https://doi.org/10.5194/amt-15-7353-2022, 2022
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We describe the development and operation of a chemical ionization mass spectrometer using an ammonium–water cluster (NH4+·H2O) as a reagent ion. NH4+·H2O is a highly versatile reagent ion for measurements of a wide range of oxygenated organic compounds. The major product ion is the cluster with NH4+ produced via ligand-switching reactions. The instrumental sensitivities of analytes depend on the binding energy of the analyte–NH4+ cluster; sensitivities can be estimated using voltage scanning.
Robert J. Parker, Chris Wilson, Edward Comyn-Platt, Garry Hayman, Toby R. Marthews, A. Anthony Bloom, Mark F. Lunt, Nicola Gedney, Simon J. Dadson, Joe McNorton, Neil Humpage, Hartmut Boesch, Martyn P. Chipperfield, Paul I. Palmer, and Dai Yamazaki
Biogeosciences, 19, 5779–5805, https://doi.org/10.5194/bg-19-5779-2022, https://doi.org/10.5194/bg-19-5779-2022, 2022
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Wetlands are the largest natural source of methane, one of the most important climate gases. The JULES land surface model simulates these emissions. We use satellite data to evaluate how well JULES reproduces the methane seasonal cycle over different tropical wetlands. It performs well for most regions; however, it struggles for some African wetlands influenced heavily by river flooding. We explain the reasons for these deficiencies and highlight how future development will improve these areas.
Ewa M. Bednarz, Ryan Hossaini, Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2022-215, https://doi.org/10.5194/gmd-2022-215, 2022
Revised manuscript accepted for GMD
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Development and performance of the new DEST chemistry scheme of UM-UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled very short-lived substances. It will hence aid studies in support of future WMO Ozone Assessment reports.
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.
Thomas von Clarmann, Norbert Glatthor, Udo Grabowski, Bernd Funke, Michael Kiefer, Anne Kleinert, Gabriele P. Stiller, Andrea Linden, and Sylvia Kellmann
Atmos. Meas. Tech., 15, 6991–7018, https://doi.org/10.5194/amt-15-6991-2022, https://doi.org/10.5194/amt-15-6991-2022, 2022
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Errors of profiles of temperature and mixing ratios retrieved from spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding are estimated. All known and quantified sources of uncertainty are considered. Some ongoing uncertaities contribute to both the random and to the systematic errors. In some cases, one source of uncertainty propagates onto the error budget via multiple pathways. Problems arise when the correlations of errors to be propagated are unknown.
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.
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.
Ewan Crosbie, Luke D. Ziemba, Michael A. Shook, Claire E. Robinson, Edward L. Winstead, K. Lee Thornhill, Rachel A. Braun, Alexander B. MacDonald, Connor Stahl, Armin Sorooshian, Susan C. van den Heever, Joshua P. DiGangi, Glenn S. Diskin, Sarah Woods, Paola Bañaga, Matthew D. Brown, Francesca Gallo, Miguel Ricardo A. Hilario, Carolyn E. Jordan, Gabrielle R. Leung, Richard H. Moore, Kevin J. Sanchez, Taylor J. Shingler, and Elizabeth B. Wiggins
Atmos. Chem. Phys., 22, 13269–13302, https://doi.org/10.5194/acp-22-13269-2022, https://doi.org/10.5194/acp-22-13269-2022, 2022
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The linkage between cloud droplet and aerosol particle chemical composition was analyzed using samples collected in a polluted tropical marine environment. Variations in the droplet composition were related to physical and dynamical processes in clouds to assess their relative significance across three cases that spanned a range of rainfall amounts. In spite of the pollution, sea salt still remained a major contributor to the droplet composition and was preferentially enhanced in rainwater.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Bingkun Yu, Xianghui Xue, Christopher J. Scott, Mingjiao Jia, Wuhu Feng, John M. C. Plane, Daniel R. Marsh, Jonas Hedin, Jörg Gumbel, and Xiankang Dou
Atmos. Chem. Phys., 22, 11485–11504, https://doi.org/10.5194/acp-22-11485-2022, https://doi.org/10.5194/acp-22-11485-2022, 2022
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We present a study on the climatology of the metal sodium layer in the upper atmosphere from the ground-based measurements obtained from a lidar network, the Odin satellite measurements, and a global model of meteoric sodium in the atmosphere. Comprehensively, comparisons show good agreement and some discrepancies between ground-based observations, satellite measurements, and global model simulations.
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.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Andreas Chrysanthou, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 22, 10635–10656, https://doi.org/10.5194/acp-22-10635-2022, https://doi.org/10.5194/acp-22-10635-2022, 2022
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Chemical transport models forced with (re)analysis meteorological fields are ideally suited for interpreting the influence of important physical processes on the ozone variability. We use TOMCAT forced by ECMWF ERA-Interim and ERA5 reanalysis data sets to investigate the effects of reanalysis forcing fields on ozone changes. Our results show that models forced by ERA5 reanalyses may not yet be capable of reproducing observed changes in stratospheric ozone, particularly in the lower stratosphere.
Matilda A. Pimlott, Richard J. Pope, Brian J. Kerridge, Barry G. Latter, Diane S. Knappett, Dwayne E. Heard, Lucy J. Ventress, Richard Siddans, Wuhu Feng, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 10467–10488, https://doi.org/10.5194/acp-22-10467-2022, https://doi.org/10.5194/acp-22-10467-2022, 2022
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We present a new method to derive global information of the hydroxyl radical (OH), an important atmospheric oxidant. OH controls the lifetime of trace gases important to air quality and climate. We use satellite observations of ozone, carbon monoxide, methane and water vapour in a simple expression to derive OH around 3–4 km altitude. The derived OH compares well to model and aircraft OH data. We then apply the method to 10 years of satellite data to study the inter-annual variability of OH.
Michael A. Robinson, J. Andrew Neuman, L. Gregory Huey, James M. Roberts, Steven S. Brown, and Patrick R. Veres
Atmos. Meas. Tech., 15, 4295–4305, https://doi.org/10.5194/amt-15-4295-2022, https://doi.org/10.5194/amt-15-4295-2022, 2022
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Iodide chemical ionization mass spectrometry (CIMS) is commonly used in atmospheric chemistry laboratory studies and field campaigns. Deployment of the NOAA iodide CIMS instrument in the summer of 2021 indicated a significant and overlooked temperature dependence of the instrument sensitivity. This work explores which analytes are influenced by this phenomena. Additionally, we recommend controls to reduce this effect for future field deployments.
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.
William G. Read, Gabriele Stiller, Stefan Lossow, Michael Kiefer, Farahnaz Khosrawi, Dale Hurst, Holger Vömel, Karen Rosenlof, Bianca M. Dinelli, Piera Raspollini, Gerald E. Nedoluha, John C. Gille, Yasuko Kasai, Patrick Eriksson, Christopher E. Sioris, Kaley A. Walker, Katja Weigel, John P. Burrows, and Alexei Rozanov
Atmos. Meas. Tech., 15, 3377–3400, https://doi.org/10.5194/amt-15-3377-2022, https://doi.org/10.5194/amt-15-3377-2022, 2022
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This paper attempts to provide an assessment of the accuracy of 21 satellite-based instruments that remotely measure atmospheric humidity in the upper troposphere of the Earth's atmosphere. The instruments made their measurements from 1984 to the present time; however, most of these instruments began operations after 2000, and only a few are still operational. The objective of this study is to quantify the accuracy of each satellite humidity data set.
Tianlang Zhao, Jingqiu Mao, William R. Simpson, Isabelle De Smedt, Lei Zhu, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Gonzalo González Abad, Caroline R. Nowlan, Barbara Barletta, Simone Meinardi, Donald R. Blake, Eric C. Apel, and Rebecca S. Hornbrook
Atmos. Chem. Phys., 22, 7163–7178, https://doi.org/10.5194/acp-22-7163-2022, https://doi.org/10.5194/acp-22-7163-2022, 2022
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Monitoring formaldehyde (HCHO) can help us understand Arctic vegetation change. Here, we compare satellite data and model and show that Alaska summertime HCHO is largely dominated by a background from methane oxidation during mild wildfire years and is dominated by wildfire (largely from direct emission of fire) during strong fire years. Consequently, it is challenging to use satellite HCHO to study vegetation change in the Arctic region.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Hannah Walker, Daniel Stone, Trevor Ingham, Sina Hackenberg, Danny Cryer, Shalini Punjabi, Katie Read, James Lee, Lisa Whalley, Dominick V. Spracklen, Lucy J. Carpenter, Steve R. Arnold, and Dwayne E. Heard
Atmos. Chem. Phys., 22, 5535–5557, https://doi.org/10.5194/acp-22-5535-2022, https://doi.org/10.5194/acp-22-5535-2022, 2022
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Glyoxal is a ubiquitous reactive organic compound in the atmosphere, which may form organic aerosol and impact the atmosphere's oxidising capacity. There are limited measurements of glyoxal's abundance in the remote marine atmosphere. We made new measurements of glyoxal using a highly sensitive technique over two 4-week periods in the tropical Atlantic atmosphere. We show that daytime measurements are mostly consistent with our chemical understanding but a potential missing source at night.
Merritt Deeter, Gene Francis, John Gille, Debbie Mao, Sara Martínez-Alonso, Helen Worden, Dan Ziskin, James Drummond, Róisín Commane, Glenn Diskin, and Kathryn McKain
Atmos. Meas. Tech., 15, 2325–2344, https://doi.org/10.5194/amt-15-2325-2022, https://doi.org/10.5194/amt-15-2325-2022, 2022
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The MOPITT (Measurements of Pollution in the Troposphere) satellite instrument uses remote sensing to obtain retrievals (measurements) of carbon monoxide (CO) in the atmosphere. This paper describes the latest MOPITT data product, Version 9. Globally, the number of daytime MOPITT retrievals over land has increased by 30 %–40 % compared to the previous product. The reported improvements in the MOPITT product should benefit a wide variety of applications including studies of pollution sources.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Richard J. Pope, Rebecca Kelly, Eloise A. Marais, Ailish M. Graham, Chris Wilson, Jeremy J. Harrison, Savio J. A. Moniz, Mohamed Ghalaieny, Steve R. Arnold, and Martyn P. Chipperfield
Atmos. Chem. Phys., 22, 4323–4338, https://doi.org/10.5194/acp-22-4323-2022, https://doi.org/10.5194/acp-22-4323-2022, 2022
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Nitrogen oxides (NOx) are potent air pollutants which directly impact on human health. In this study, we use satellite nitrogen dioxide (NO2) data to evaluate the spatial distribution and temporal evolution of the UK official NOx emissions inventory, with reasonable agreement. We also derived satellite-based NOx emissions for several UK cities. In the case of London and Birmingham, the NAEI NOx emissions are potentially too low by >50%.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Piera Raspollini, Enrico Arnone, Flavio Barbara, Massimo Bianchini, Bruno Carli, Simone Ceccherini, Martyn P. Chipperfield, Angelika Dehn, Stefano Della Fera, Bianca Maria Dinelli, Anu Dudhia, Jean-Marie Flaud, Marco Gai, Michael Kiefer, Manuel López-Puertas, David P. Moore, Alessandro Piro, John J. Remedios, Marco Ridolfi, Harjinder Sembhi, Luca Sgheri, and Nicola Zoppetti
Atmos. Meas. Tech., 15, 1871–1901, https://doi.org/10.5194/amt-15-1871-2022, https://doi.org/10.5194/amt-15-1871-2022, 2022
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The MIPAS instrument onboard the ENVISAT satellite provided 10 years of measurements of the atmospheric emission al limb that allow for the retrieval of latitude- and altitude-resolved atmospheric composition. We describe the improvements implemented in the retrieval algorithm used for the full mission reanalysis, which allows for the generation of the global distributions of 21 atmospheric constituents plus temperature with increased accuracy with respect to previously generated data.
Sören Johansson, Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Michael Höpfner, Anne Kleinert, Tom Neubert, Björn-Martin Sinnhuber, and Jörn Ungermann
Atmos. Chem. Phys., 22, 3675–3691, https://doi.org/10.5194/acp-22-3675-2022, https://doi.org/10.5194/acp-22-3675-2022, 2022
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We present GLORIA airborne cross sections of PAN, C2H6, HCOOH, CH3OH, and C2H4 in the South Atlantic UTLS in September/October 2019. Filamentary structures and a large plume were observed. Backward trajectories indicate that measured pollutants come from South America and central Africa. Comparisons to CAMS show structural agreement of the measured distributions. PAN absolute VMRs agree with the GLORIA measurements, C2H6 and HCOOH are simulated too low, and CH3OH and C2H4 are too high.
Davide Zanchettin, Claudia Timmreck, Myriam Khodri, Anja Schmidt, Matthew Toohey, Manabu Abe, Slimane Bekki, Jason Cole, Shih-Wei Fang, Wuhu Feng, Gabriele Hegerl, Ben Johnson, Nicolas Lebas, Allegra N. LeGrande, Graham W. Mann, Lauren Marshall, Landon Rieger, Alan Robock, Sara Rubinetti, Kostas Tsigaridis, and Helen Weierbach
Geosci. Model Dev., 15, 2265–2292, https://doi.org/10.5194/gmd-15-2265-2022, https://doi.org/10.5194/gmd-15-2265-2022, 2022
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This paper provides metadata and first analyses of the volc-pinatubo-full experiment of CMIP6-VolMIP. Results from six Earth system models reveal significant differences in radiative flux anomalies that trace back to different implementations of volcanic forcing. Surface responses are in contrast overall consistent across models, reflecting the large spread due to internal variability. A second phase of VolMIP shall consider both aspects toward improved protocol for volc-pinatubo-full.
Michael T. Kiefer, Warren E. Heilman, Shiyuan Zhong, Joseph J. Charney, Xindi Bian, Nicholas S. Skowronski, Kenneth L. Clark, Michael R. Gallagher, John L. Hom, and Matthew Patterson
Geosci. Model Dev., 15, 1713–1734, https://doi.org/10.5194/gmd-15-1713-2022, https://doi.org/10.5194/gmd-15-1713-2022, 2022
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We examine methods used to represent wildland fire sensible heat release in atmospheric models. A set of simulations are evaluated using observations from a low-intensity prescribed fire in the New Jersey Pine Barrens. The comparison is motivated by the need for guidance regarding the representation of low-intensity fire sensible heating in atmospheric models. Such fires are prevalent during prescribed fire operations and can impact the health and safety of fire personnel and the public.
Ka Ming Fung, Colette L. Heald, Jesse H. Kroll, Siyuan Wang, Duseong S. Jo, Andrew Gettelman, Zheng Lu, Xiaohong Liu, Rahul A. Zaveri, Eric C. Apel, Donald R. Blake, Jose-Luis Jimenez, Pedro Campuzano-Jost, Patrick R. Veres, Timothy S. Bates, John E. Shilling, and Maria Zawadowicz
Atmos. Chem. Phys., 22, 1549–1573, https://doi.org/10.5194/acp-22-1549-2022, https://doi.org/10.5194/acp-22-1549-2022, 2022
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Understanding the natural aerosol burden in the preindustrial era is crucial for us to assess how atmospheric aerosols affect the Earth's radiative budgets. Our study explores how a detailed description of dimethyl sulfide (DMS) oxidation (implemented in the Community Atmospheric Model version 6 with chemistry, CAM6-chem) could help us better estimate the present-day and preindustrial concentrations of sulfate and other relevant chemicals, as well as the resulting aerosol radiative impacts.
Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Ryan Hossaini, Graham W. Mann, Michelle L. Santee, and Mark Weber
Atmos. Chem. Phys., 22, 903–916, https://doi.org/10.5194/acp-22-903-2022, https://doi.org/10.5194/acp-22-903-2022, 2022
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Solar flux variations associated with 11-year sunspot cycle is believed to exert important external climate forcing. As largest variations occur at shorter wavelengths such as ultra-violet part of the solar spectrum, associated changes in stratospheric ozone are thought to provide direct evidence for solar climate interaction. Until now, most of the studies reported double-peak structured solar cycle signal (SCS), but relatively new satellite data suggest only single-peak-structured SCS.
Dongwook Kim, Changmin Cho, Seokhan Jeong, Soojin Lee, Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Jose L. Jimenez, Rainer Volkamer, Donald R. Blake, Armin Wisthaler, Alan Fried, Joshua P. DiGangi, Glenn S. Diskin, Sally E. Pusede, Samuel R. Hall, Kirk Ullmann, L. Gregory Huey, David J. Tanner, Jack Dibb, Christoph J. Knote, and Kyung-Eun Min
Atmos. Chem. Phys., 22, 805–821, https://doi.org/10.5194/acp-22-805-2022, https://doi.org/10.5194/acp-22-805-2022, 2022
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CHOCHO was simulated using a 0-D box model constrained by measurements during the KORUS-AQ mission. CHOCHO concentration was high in large cities, aromatics being the most important precursors. Loss path to aerosol was the highest sink, contributing to ~ 20 % of secondary organic aerosol formation. Our work highlights that simple CHOCHO surface uptake approach is valid only for low aerosol conditions and more work is required to understand CHOCHO solubility in high-aerosol conditions.
Bianca Maria Dinelli, Piera Raspollini, Marco Gai, Luca Sgheri, Marco Ridolfi, Simone Ceccherini, Flavio Barbara, Nicola Zoppetti, Elisa Castelli, Enzo Papandrea, Paolo Pettinari, Angelika Dehn, Anu Dudhia, Michael Kiefer, Alessandro Piro, Jean-Marie Flaud, Manuel López-Puertas, David Moore, John Remedios, and Massimo Bianchini
Atmos. Meas. Tech., 14, 7975–7998, https://doi.org/10.5194/amt-14-7975-2021, https://doi.org/10.5194/amt-14-7975-2021, 2021
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The level-2 v8 database from the measurements of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), aboard the European Space Agency Envisat satellite, containing atmospheric fields of pressure, temperature, and volume mixing ratio of 21 trace gases, is described in this paper. The database covers all the measurements acquired by MIPAS (from July 2002 to April 2012). The number of species included makes it of particular importance for the studies of stratospheric chemistry.
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.
Catherine Hardacre, Jane P. Mulcahy, Richard J. Pope, Colin G. Jones, Steven T. Rumbold, Can Li, Colin Johnson, and Steven T. Turnock
Atmos. Chem. Phys., 21, 18465–18497, https://doi.org/10.5194/acp-21-18465-2021, https://doi.org/10.5194/acp-21-18465-2021, 2021
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We investigate UKESM1's ability to represent the sulfur (S) cycle in the recent historical period. The S cycle is a key driver of historical radiative forcing. Earth system models such as UKESM1 should represent the S cycle well so that we can have confidence in their projections of future climate. We compare UKESM1 to observations of sulfur compounds, finding that the model generally performs well. We also identify areas for UKESM1’s development, focussing on how SO2 is removed from the air.
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.
Sandip S. Dhomse, Carlo Arosio, Wuhu Feng, Alexei Rozanov, Mark Weber, and Martyn P. Chipperfield
Earth Syst. Sci. Data, 13, 5711–5729, https://doi.org/10.5194/essd-13-5711-2021, https://doi.org/10.5194/essd-13-5711-2021, 2021
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High-quality long-term ozone profile data sets are key to estimating short- and long-term ozone variability. Almost all the satellite (and chemical model) data sets show some kind of bias with respect to each other. This is because of differences in measurement methodologies as well as simplified processes in the models. We use satellite data sets and chemical model output to generate 42 years of ozone profile data sets using a random-forest machine-learning algorithm that is named ML-TOMCAT.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
James M. Roberts
Atmos. Chem. Phys., 21, 16793–16795, https://doi.org/10.5194/acp-21-16793-2021, https://doi.org/10.5194/acp-21-16793-2021, 2021
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This comment provides evidence that recently reported measurements of the isotope composition of wildfire-derived oxides of nitrogen have a significant interference from other nitrogen compounds. In addition, the conceptual model used to interpret the results was missing several key reactions.
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.
Jianfei Wu, Wuhu Feng, Han-Li Liu, Xianghui Xue, Daniel Robert Marsh, and John Maurice Campbell Plane
Atmos. Chem. Phys., 21, 15619–15630, https://doi.org/10.5194/acp-21-15619-2021, https://doi.org/10.5194/acp-21-15619-2021, 2021
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Metal layers occur in the MLT region (80–120 km) from the ablation of cosmic dust. The latest lidar observations show these metals can reach a height approaching 200 km, which is challenging to explain. We have developed the first global simulation incorporating the full life cycle of metal atoms and ions. The model results compare well with lidar and satellite observations of the seasonal and diurnal variation of the metals and demonstrate the importance of ion mass and ion-neutral coupling.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
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.
Jayanarayanan Kuttippurath, Wuhu Feng, Rolf Müller, Pankaj Kumar, Sarath Raj, Gopalakrishna Pillai Gopikrishnan, and Raina Roy
Atmos. Chem. Phys., 21, 14019–14037, https://doi.org/10.5194/acp-21-14019-2021, https://doi.org/10.5194/acp-21-14019-2021, 2021
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The Arctic winter/spring 2020 was one of the coldest with a strong and long-lasting vortex, high chlorine activation, severe denitrification, and unprecedented ozone loss. The loss was even equal to the levels of some of the warm Antarctic winters. Total column ozone values below 220 DU for several weeks and ozone loss saturation were observed during the period. These results show an unusual meteorology and warrant dedicated studies on the impact of climate change on ozone loss.
Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Halogen radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a new mechanistic description and comprehensive simulation of tropospheric halogens in a global 3-D model and compare the model results with surface and aircraft measurements. We find that halogen chemistry decreases the global tropospheric burden of ozone by 11 %, NOx by 6 %, and OH by 4 %.
Hao Guo, Clare M. Flynn, Michael J. Prather, Sarah A. Strode, Stephen D. Steenrod, Louisa Emmons, Forrest Lacey, Jean-Francois Lamarque, Arlene M. Fiore, Gus Correa, Lee T. Murray, Glenn M. Wolfe, Jason M. St. Clair, Michelle Kim, John Crounse, Glenn Diskin, Joshua DiGangi, Bruce C. Daube, Roisin Commane, Kathryn McKain, Jeff Peischl, Thomas B. Ryerson, Chelsea Thompson, Thomas F. Hanisco, Donald Blake, Nicola J. Blake, Eric C. Apel, Rebecca S. Hornbrook, James W. Elkins, Eric J. Hintsa, Fred L. Moore, and Steven Wofsy
Atmos. Chem. Phys., 21, 13729–13746, https://doi.org/10.5194/acp-21-13729-2021, https://doi.org/10.5194/acp-21-13729-2021, 2021
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The NASA Atmospheric Tomography (ATom) mission built a climatology of the chemical composition of tropospheric air parcels throughout the middle of the Pacific and Atlantic oceans. The level of detail allows us to reconstruct the photochemical budgets of O3 and CH4 over these vast, remote regions. We find that most of the chemical heterogeneity is captured at the resolution used in current global chemistry models and that the majority of reactivity occurs in the
hottest20 % of parcels.
Jessica L. McCarty, Juha Aalto, Ville-Veikko Paunu, Steve R. Arnold, Sabine Eckhardt, Zbigniew Klimont, Justin J. Fain, Nikolaos Evangeliou, Ari Venäläinen, Nadezhda M. Tchebakova, Elena I. Parfenova, Kaarle Kupiainen, Amber J. Soja, Lin Huang, and Simon Wilson
Biogeosciences, 18, 5053–5083, https://doi.org/10.5194/bg-18-5053-2021, https://doi.org/10.5194/bg-18-5053-2021, 2021
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Fires, including extreme fire seasons, and fire emissions are more common in the Arctic. A review and synthesis of current scientific literature find climate change and human activity in the north are fuelling an emerging Arctic fire regime, causing more black carbon and methane emissions within the Arctic. Uncertainties persist in characterizing future fire landscapes, and thus emissions, as well as policy-relevant challenges in understanding, monitoring, and managing Arctic fire regimes.
Francesco Grieco, Kristell Pérot, Donal Murtagh, Patrick Eriksson, Bengt Rydberg, Michael Kiefer, Maya Garcia-Comas, Alyn Lambert, and Kaley A. Walker
Atmos. Meas. Tech., 14, 5823–5857, https://doi.org/10.5194/amt-14-5823-2021, https://doi.org/10.5194/amt-14-5823-2021, 2021
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We present improved Odin/SMR mesospheric H2O concentration and temperature data sets, reprocessed assuming a bigger sideband leakage of the instrument. The validation study shows how the improved SMR data sets agree better with other instruments' observations than the old SMR version did. Given their unique time extension and geographical coverage, and H2O being a good tracer of mesospheric circulation, the new data sets are valuable for the study of dynamical processes and multi-year trends.
Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Yenny Gonzalez, Róisín Commane, Ethan Manninen, Bruce C. Daube, Luke D. Schiferl, J. Barry McManus, Kathryn McKain, Eric J. Hintsa, James W. Elkins, Stephen A. Montzka, Colm Sweeney, Fred Moore, Jose L. Jimenez, Pedro Campuzano Jost, Thomas B. Ryerson, Ilann Bourgeois, Jeff Peischl, Chelsea R. Thompson, Eric Ray, Paul O. Wennberg, John Crounse, Michelle Kim, Hannah M. Allen, Paul A. Newman, Britton B. Stephens, Eric C. Apel, Rebecca S. Hornbrook, Benjamin A. Nault, Eric Morgan, and Steven C. Wofsy
Atmos. Chem. Phys., 21, 11113–11132, https://doi.org/10.5194/acp-21-11113-2021, https://doi.org/10.5194/acp-21-11113-2021, 2021
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Vertical profiles of N2O and a variety of chemical species and aerosols were collected nearly from pole to pole over the oceans during the NASA Atmospheric Tomography mission. We observed that tropospheric N2O variability is strongly driven by the influence of stratospheric air depleted in N2O, especially at middle and high latitudes. We also traced the origins of biomass burning and industrial emissions and investigated their impact on the variability of tropospheric N2O.
Johannes de Leeuw, Anja Schmidt, Claire S. Witham, Nicolas Theys, Isabelle A. Taylor, Roy G. Grainger, Richard J. Pope, Jim Haywood, Martin Osborne, and Nina I. Kristiansen
Atmos. Chem. Phys., 21, 10851–10879, https://doi.org/10.5194/acp-21-10851-2021, https://doi.org/10.5194/acp-21-10851-2021, 2021
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Using the NAME dispersion model in combination with high-resolution SO2 satellite data from TROPOMI, we investigate the dispersion of volcanic SO2 from the 2019 Raikoke eruption. NAME accurately simulates the dispersion of SO2 during the first 2–3 weeks after the eruption and illustrates the potential of using high-resolution satellite data to identify potential limitations in dispersion models, which will ultimately help to improve efforts to forecast the dispersion of volcanic clouds.
Chris Wilson, Martyn P. Chipperfield, Manuel Gloor, Robert J. Parker, Hartmut Boesch, Joey McNorton, Luciana V. Gatti, John B. Miller, Luana S. Basso, and Sarah A. Monks
Atmos. Chem. Phys., 21, 10643–10669, https://doi.org/10.5194/acp-21-10643-2021, https://doi.org/10.5194/acp-21-10643-2021, 2021
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Methane (CH4) is an important greenhouse gas emitted from wetlands like those found in the basin of the Amazon River. Using an atmospheric model and observations from GOSAT, we quantified CH4 emissions from Amazonia during the previous decade. We found that the largest emissions came from a region in the eastern basin and that emissions there were rising faster than in other areas of South America. This finding was supported by CH4 observations made on aircraft within the basin.
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.
Thomas von Clarmann, Udo Grabowski, Gabriele P. Stiller, Beatriz M. Monge-Sanz, Norbert Glatthor, and Sylvia Kellmann
Atmos. Chem. Phys., 21, 8823–8843, https://doi.org/10.5194/acp-21-8823-2021, https://doi.org/10.5194/acp-21-8823-2021, 2021
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Measurements of long-lived trace gases (SF6, CFC-11, CFC-12, HCFC-12, CCl4, N2O, CH4, H2O, and CO) performed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) have been used to infer the stratospheric and mesospheric meridional circulation. The MIPAS data set covers the time period from July 2002 to April 2012. The method used for this purpose was the direct inversion of the two-dimensional continuity equation. Multiannual monthly mean circulation fields are presented.
Michael Kiefer, Thomas von Clarmann, Bernd Funke, Maya García-Comas, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Anne Kleinert, Alexandra Laeng, Andrea Linden, Manuel López-Puertas, Daniel R. Marsh, and Gabriele P. Stiller
Atmos. Meas. Tech., 14, 4111–4138, https://doi.org/10.5194/amt-14-4111-2021, https://doi.org/10.5194/amt-14-4111-2021, 2021
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An improved dataset of vertical temperature profiles of the Earth's atmosphere in the altitude range 5–70 km is presented. These profiles are derived from measurements of the MIPAS instrument onboard ESA's Envisat satellite. The overall improvements are based on upgrades in the input data and several improvements in the data processing approach. Both of these are discussed, and an extensive error discussion is included. Enhancements of the new dataset are demonstrated by means of examples.
Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Jens-Uwe Grooß, Thomas Gulde, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Erik Kretschmer, Guido Maucher, Hans Nordmeyer, Hermann Oelhaf, Johannes Orphal, Christof Piesch, Björn-Martin Sinnhuber, Jörn Ungermann, and Bärbel Vogel
Atmos. Chem. Phys., 21, 8213–8232, https://doi.org/10.5194/acp-21-8213-2021, https://doi.org/10.5194/acp-21-8213-2021, 2021
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Measurements of the pollutants C2H6, C2H2, HCOOH, and PAN were performed in the North Atlantic UTLS region with the airborne limb imager GLORIA in 2017. Enhanced amounts of these species were detected in the upper troposphere and even in the lowermost stratosphere (PAN). Main sources of these gases are forest fires in North America and anthropogenic pollution in South Asia. Simulations of EMAC and CAMS are qualitatively able to reproduce the measured data but underestimate the absolute amounts.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Joanna E. Dyson, Graham A. Boustead, Lauren T. Fleming, Mark Blitz, Daniel Stone, Stephen R. Arnold, Lisa K. Whalley, and Dwayne E. Heard
Atmos. Chem. Phys., 21, 5755–5775, https://doi.org/10.5194/acp-21-5755-2021, https://doi.org/10.5194/acp-21-5755-2021, 2021
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The hydroxyl radical (OH) dominates the removal of atmospheric pollutants, with nitrous acid (HONO) recognised as a major OH source. For remote regions HONO production through the action of sunlight on aerosol surfaces can provide a source of nitrogen oxides. In this study, HONO production rates at illuminated aerosol surfaces are measured under atmospheric conditions, a model consistent with the data is developed and aerosol production of HONO in the atmosphere is shown to be significant.
Akash Biswal, Vikas Singh, Shweta Singh, Amit P. Kesarkar, Khaiwal Ravindra, Ranjeet S. Sokhi, Martyn P. Chipperfield, Sandip S. Dhomse, Richard J. Pope, Tanbir Singh, and Suman Mor
Atmos. Chem. Phys., 21, 5235–5251, https://doi.org/10.5194/acp-21-5235-2021, https://doi.org/10.5194/acp-21-5235-2021, 2021
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Satellite and surface observations show a reduction in NO2 levels over India during the lockdown compared to business-as-usual years. A substantial reduction, proportional to the population, was observed over the urban areas. The changes in NO2 levels at the surface during the lockdown appear to be present in the satellite observations. However, TROPOMI showed a better correlation with surface NO2 and was more sensitive to the changes than OMI because of the finer resolution.
Thomas Thorp, Stephen R. Arnold, Richard J. Pope, Dominick V. Spracklen, Luke Conibear, Christoph Knote, Mikhail Arshinov, Boris Belan, Eija Asmi, Tuomas Laurila, Andrei I. Skorokhod, Tuomo Nieminen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 4677–4697, https://doi.org/10.5194/acp-21-4677-2021, https://doi.org/10.5194/acp-21-4677-2021, 2021
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We compare modelled near-surface pollutants with surface and satellite observations to better understand the controls on the regional concentrations of pollution in western Siberia for late spring and summer in 2011. We find two commonly used emission inventories underestimate human emissions when compared to observations. Transport emissions are the main source of pollutants within the region during this period, whilst fire emissions peak during June and are only significant south of 60° N.
Bingkun Yu, Xianghui Xue, Christopher J. Scott, Jianfei Wu, Xinan Yue, Wuhu Feng, Yutian Chi, Daniel R. Marsh, Hanli Liu, Xiankang Dou, and John M. C. Plane
Atmos. Chem. Phys., 21, 4219–4230, https://doi.org/10.5194/acp-21-4219-2021, https://doi.org/10.5194/acp-21-4219-2021, 2021
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A long-standing mystery of metal ions within Es layers in the Earth's upper atmosphere is the marked seasonal dependence, with a summer maximum and a winter minimum. We report a large-scale winter-to-summer transport of metal ions from 6-year multi-satellite observations and worldwide ground-based stations. A global atmospheric circulation is responsible for the phenomenon. Our results emphasise the effect of this atmospheric circulation on the transport of composition in the upper atmosphere.
Miguel Ricardo A. Hilario, Ewan Crosbie, Michael Shook, Jeffrey S. Reid, Maria Obiminda L. Cambaliza, James Bernard B. Simpas, Luke Ziemba, Joshua P. DiGangi, Glenn S. Diskin, Phu Nguyen, F. Joseph Turk, Edward Winstead, Claire E. Robinson, Jian Wang, Jiaoshi Zhang, Yang Wang, Subin Yoon, James Flynn, Sergio L. Alvarez, Ali Behrangi, and Armin Sorooshian
Atmos. Chem. Phys., 21, 3777–3802, https://doi.org/10.5194/acp-21-3777-2021, https://doi.org/10.5194/acp-21-3777-2021, 2021
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This study characterizes long-range transport from major Asian pollution sources into the tropical northwest Pacific and the impact of scavenging on these air masses. We combined aircraft observations, HYSPLIT trajectories, reanalysis, and satellite retrievals to reveal distinct composition and size distribution profiles associated with specific emission sources and wet scavenging. The results of this work have implications for international policymaking related to climate and health.
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.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Betty Croft, Randall V. Martin, Richard H. Moore, Luke D. Ziemba, Ewan C. Crosbie, Hongyu Liu, Lynn M. Russell, Georges Saliba, Armin Wisthaler, Markus Müller, Arne Schiller, Martí Galí, Rachel Y.-W. Chang, Erin E. McDuffie, Kelsey R. Bilsback, and Jeffrey R. Pierce
Atmos. Chem. Phys., 21, 1889–1916, https://doi.org/10.5194/acp-21-1889-2021, https://doi.org/10.5194/acp-21-1889-2021, 2021
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North Atlantic Aerosols and Marine Ecosystems Study measurements combined with GEOS-Chem-TOMAS modeling suggest that several not-well-understood key factors control northwest Atlantic aerosol number and size. These synergetic and climate-relevant factors include particle formation near and above the marine boundary layer top, particle growth by marine secondary organic aerosol on descent, particle formation/growth related to dimethyl sulfide, sea spray aerosol, and ship emissions.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Sören Johansson, Michael Höpfner, Oliver Kirner, Ingo Wohltmann, Silvia Bucci, Bernard Legras, Felix Friedl-Vallon, Norbert Glatthor, Erik Kretschmer, Jörn Ungermann, and Gerald Wetzel
Atmos. Chem. Phys., 20, 14695–14715, https://doi.org/10.5194/acp-20-14695-2020, https://doi.org/10.5194/acp-20-14695-2020, 2020
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We present high-resolution measurements of pollutant trace gases (PAN, C2H2, and HCOOH) in the Asian monsoon UTLS from the airborne limb imager GLORIA during StratoClim 2017. Enhancements are observed up to 16 km altitude, and PAN and C2H2 even up to 18 km. Two atmospheric models, CAMS and EMAC, reproduce the pollutant's large-scale structures but not finer structures. Convection is investigated using backward trajectories of the models ATLAS and TRACZILLA with advanced detection of convection.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Robert J. Parker, Chris Wilson, A. Anthony Bloom, Edward Comyn-Platt, Garry Hayman, Joe McNorton, Hartmut Boesch, and Martyn P. Chipperfield
Biogeosciences, 17, 5669–5691, https://doi.org/10.5194/bg-17-5669-2020, https://doi.org/10.5194/bg-17-5669-2020, 2020
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Wetlands contribute the largest uncertainty to the atmospheric methane budget. WetCHARTs is a simple, data-driven model that estimates wetland emissions using observations of precipitation and temperature. We perform the first detailed evaluation of WetCHARTs against satellite data and find it performs well in reproducing the observed wetland methane seasonal cycle for the majority of wetland regions. In regions where it performs poorly, we highlight incorrect wetland extent as a key reason.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Benjamin Birner, Martyn P. Chipperfield, Eric J. Morgan, Britton B. Stephens, Marianna Linz, Wuhu Feng, Chris Wilson, Jonathan D. Bent, Steven C. Wofsy, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Chem. Phys., 20, 12391–12408, https://doi.org/10.5194/acp-20-12391-2020, https://doi.org/10.5194/acp-20-12391-2020, 2020
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With new high-precision observations from nine aircraft campaigns and 3-D chemical transport modeling, we show that the argon-to-nitrogen ratio (Ar / N2) in the lowermost stratosphere provides a useful constraint on the “age of air” (the time elapsed since entry of an air parcel into the stratosphere). Therefore, Ar / N2 in combination with traditional age-of-air indicators, such as CO2 and N2O, could provide new insights into atmospheric mixing and transport.
Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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We develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns. The platform offers an alternative way to quickly assess systematic biases in HCHO satellite products over large domains and long periods, facilitating optimization of retrieval settings and the minimization of retrieval biases. Application to the NASA operational HCHO product indicates that relative biases range from −44.5 % to +112.1 % depending on locations and seasons.
Ben Silver, Luke Conibear, Carly L. Reddington, Christoph Knote, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 20, 11683–11695, https://doi.org/10.5194/acp-20-11683-2020, https://doi.org/10.5194/acp-20-11683-2020, 2020
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China suffers from serious air pollution, which is thought to cause millions of early deaths each year. Measurements on the ground show that overall air quality is improving. Air quality is also affected by weather conditions, which can vary from year to year. We conduct computer simulations to show it is the reduction of the amount of pollution emitted, rather than weather conditions, which caused air quality to improve during 2015–2017. We then estimate that 150 000 fewer people die early.
Hirofumi Ohyama, Isamu Morino, Voltaire A. Velazco, Theresa Klausner, Gerry Bagtasa, Matthäus Kiel, Matthias Frey, Akihiro Hori, Osamu Uchino, Tsuneo Matsunaga, Nicholas M. Deutscher, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Sally E. Pusede, Alina Fiehn, Anke Roiger, Michael Lichtenstern, Hans Schlager, Pao K. Wang, Charles C.-K. Chou, Maria Dolores Andrés-Hernández, and John P. Burrows
Atmos. Meas. Tech., 13, 5149–5163, https://doi.org/10.5194/amt-13-5149-2020, https://doi.org/10.5194/amt-13-5149-2020, 2020
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Column-averaged dry-air mole fractions of CO2 and CH4 measured by a solar viewing portable Fourier transform spectrometer (EM27/SUN) were validated with in situ profile data obtained during the transfer flights of two aircraft campaigns. Atmospheric dynamical properties based on ERA5 and WRF-Chem were used as criteria for selecting the best aircraft profiles for the validation. The resulting air-mass-independent correction factors for the EM27/SUN data were 0.9878 for CO2 and 0.9829 for CH4.
Matthew J. Rowlinson, Alexandru Rap, Douglas S. Hamilton, Richard J. Pope, Stijn Hantson, Steve R. Arnold, Jed O. Kaplan, Almut Arneth, Martyn P. Chipperfield, Piers M. Forster, and Lars Nieradzik
Atmos. Chem. Phys., 20, 10937–10951, https://doi.org/10.5194/acp-20-10937-2020, https://doi.org/10.5194/acp-20-10937-2020, 2020
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Tropospheric ozone is an important greenhouse gas which contributes to anthropogenic climate change; however, the effect of human emissions is uncertain because pre-industrial ozone concentrations are not well understood. We use revised inventories of pre-industrial natural emissions to estimate the human contribution to changes in tropospheric ozone. We find that tropospheric ozone radiative forcing is up to 34 % lower when using improved pre-industrial biomass burning and vegetation emissions.
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
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
James M. Roberts, Chelsea E. Stockwell, Robert J. Yokelson, Joost de Gouw, Yong Liu, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, Kyle J. Zarzana, Steven S. Brown, Cristina Santin, Stefan H. Doerr, and Carsten Warneke
Atmos. Chem. Phys., 20, 8807–8826, https://doi.org/10.5194/acp-20-8807-2020, https://doi.org/10.5194/acp-20-8807-2020, 2020
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We measured total reactive nitrogen, Nr, in lab fires from western North American fuels, along with measurements of individual nitrogen compounds. We measured the amount of N that gets converted to inactive compounds (avg. 70 %), and the amount that is accounted for by individual species (85 % of remaining N). We provide guidelines for how the reactive nitrogen is distributed among individual compounds such as NOx and ammonia. This will help estimates and predictions of wildfire emissions.
Yajuan Li, Martyn P. Chipperfield, Wuhu Feng, Sandip S. Dhomse, Richard J. Pope, Faquan Li, and Dong Guo
Atmos. Chem. Phys., 20, 8627–8639, https://doi.org/10.5194/acp-20-8627-2020, https://doi.org/10.5194/acp-20-8627-2020, 2020
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The Tibetan Plateau (TP) exerts important thermal and dynamical effects on atmospheric circulation, climate change as well as the ozone distribution. In this study, we use updated observations and model simulations to investigate the ozone trends and variations over the TP. Wintertime TP ozone variations are largely controlled by tropical to high-latitude transport processes, whereas summertime concentrations are a combined effect of photochemical decay and tropical processes.
Christopher D. Cappa, Christopher Y. Lim, David H. Hagan, Matthew Coggon, Abigail Koss, Kanako Sekimoto, Joost de Gouw, Timothy B. Onasch, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 8511–8532, https://doi.org/10.5194/acp-20-8511-2020, https://doi.org/10.5194/acp-20-8511-2020, 2020
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Smoke from combustion of a wide range of biomass fuels (e.g., leaves, twigs, logs, peat, and dung) was photochemically aged in a small chamber for up to 8 d of equivalent atmospheric aging. Upon aging, the particle chemical composition and ability to absorb sunlight changed owing to reactions in both the gas and particulate phases. We developed a model to explain the observations and used this to derive insights into the aging of smoke in the atmosphere.
Ifayoyinsola Ibikunle, Andreas Beyersdorf, Pedro Campuzano-Jost, Chelsea Corr, John D. Crounse, Jack Dibb, Glenn Diskin, Greg Huey, Jose-Luis Jimenez, Michelle J. Kim, Benjamin A. Nault, Eric Scheuer, Alex Teng, Paul O. Wennberg, Bruce Anderson, James Crawford, Rodney Weber, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-501, https://doi.org/10.5194/acp-2020-501, 2020
Publication in ACP not foreseen
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Analysis of observations over South Korea during the NASA/NIER
KORUS-AQ field campaign show that aerosol is fairly acidic (mean pH 2.43 ± 0.68). Aerosol formation is always sensitive to HNO3 levels, especially in highly polluted regions, while it is only exclusively sensitive to NH3 in some rural/remote regions. Nitrate levels accumulate because dry deposition velocity is low. HNO3 reductions achieved by NOx controls can be the most effective PM reduction strategy for all conditions observed.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Yi Ji, L. Gregory Huey, David J. Tanner, Young Ro Lee, Patrick R. Veres, J. Andrew Neuman, Yuhang Wang, and Xinming Wang
Atmos. Meas. Tech., 13, 3683–3696, https://doi.org/10.5194/amt-13-3683-2020, https://doi.org/10.5194/amt-13-3683-2020, 2020
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A common way of measuring trace gases in the atmosphere is chemical ionization mass spectrometry. One large drawback of these instruments is that they require radioactive ion sources. In this work we demonstrate a simple ion source that uses a small krypton lamp that can be used to replace a radioactive source.
Katherine R. Travis, Colette L. Heald, Hannah M. Allen, Eric C. Apel, Stephen R. Arnold, Donald R. Blake, William H. Brune, Xin Chen, Róisín Commane, John D. Crounse, Bruce C. Daube, Glenn S. Diskin, James W. Elkins, Mathew J. Evans, Samuel R. Hall, Eric J. Hintsa, Rebecca S. Hornbrook, Prasad S. Kasibhatla, Michelle J. Kim, Gan Luo, Kathryn McKain, Dylan B. Millet, Fred L. Moore, Jeffrey Peischl, Thomas B. Ryerson, Tomás Sherwen, Alexander B. Thames, Kirk Ullmann, Xuan Wang, Paul O. Wennberg, Glenn M. Wolfe, and Fangqun Yu
Atmos. Chem. Phys., 20, 7753–7781, https://doi.org/10.5194/acp-20-7753-2020, https://doi.org/10.5194/acp-20-7753-2020, 2020
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Atmospheric models overestimate the rate of removal of trace gases by the hydroxyl radical (OH). This is a concern for studies of the climate and air quality impacts of human activities. Here, we evaluate the performance of a commonly used model of atmospheric chemistry against data from the NASA Atmospheric Tomography Mission (ATom) over the remote oceans where models have received little validation. The model is generally successful, suggesting that biases in OH may be a concern over land.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
Preprint withdrawn
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
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The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Pablo E. Saide, Meng Gao, Zifeng Lu, Daniel L. Goldberg, David G. Streets, Jung-Hun Woo, Andreas Beyersdorf, Chelsea A. Corr, Kenneth L. Thornhill, Bruce Anderson, Johnathan W. Hair, Amin R. Nehrir, Glenn S. Diskin, Jose L. Jimenez, Benjamin A. Nault, Pedro Campuzano-Jost, Jack Dibb, Eric Heim, Kara D. Lamb, Joshua P. Schwarz, Anne E. Perring, Jhoon Kim, Myungje Choi, Brent Holben, Gabriele Pfister, Alma Hodzic, Gregory R. Carmichael, Louisa Emmons, and James H. Crawford
Atmos. Chem. Phys., 20, 6455–6478, https://doi.org/10.5194/acp-20-6455-2020, https://doi.org/10.5194/acp-20-6455-2020, 2020
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Air quality forecasts over the Korean Peninsula captured aerosol optical depth but largely overpredicted surface PM during a Chinese haze transport event. Model deficiency was related to the calculation of optical properties. In order to improve it, aerosol size representation needs to be refined in the calculations, and the representation of aerosol properties, such as size distribution, chemical composition, refractive index, hygroscopicity parameter, and density, needs to be improved.
Young Ro Lee, Yi Ji, David J. Tanner, and L. Gregory Huey
Atmos. Meas. Tech., 13, 2473–2480, https://doi.org/10.5194/amt-13-2473-2020, https://doi.org/10.5194/amt-13-2473-2020, 2020
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In this work we show how to construct a radioactive ion source for a chemical ionization mass spectrometer (CIMS) from commercially available components. The source is low activity and can be shipped with a minimum of complications. This facilitates the deployment of CIMS to measure atmospheric pollutants at remote ground sites.
Andreas Chrysanthou, Amanda C. Maycock, and Martyn P. Chipperfield
Weather Clim. Dynam., 1, 155–174, https://doi.org/10.5194/wcd-1-155-2020, https://doi.org/10.5194/wcd-1-155-2020, 2020
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We perform 50-year-long time-slice experiments using the Met Office HadGEM3 global climate model in order to decompose the Brewer–Dobson circulation (BDC) response to an abrupt quadrupling of CO2 in three distinct components, (a) the rapid adjustment, associated with CO2 radiative effects; (b) a global uniform sea surface temperature warming; and (c) sea surface temperature patterns. This demonstrates a potential for fast and slow timescales of the response of the BDC to greenhouse gas forcing.
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.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
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Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Rebecca H. Schwantes, Louisa K. Emmons, John J. Orlando, Mary C. Barth, Geoffrey S. Tyndall, Samuel R. Hall, Kirk Ullmann, Jason M. St. Clair, Donald R. Blake, Armin Wisthaler, and Thao Paul V. Bui
Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, https://doi.org/10.5194/acp-20-3739-2020, 2020
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Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Here adding more complex and updated chemistry for isoprene and terpenes, which are biogenic hydrocarbons emitted from trees and vegetation, into an earth system model greatly reduces the simulated surface ozone bias compared to aircraft and monitoring station data.
Wenfu Tang, Helen M. Worden, Merritt N. Deeter, David P. Edwards, Louisa K. Emmons, Sara Martínez-Alonso, Benjamin Gaubert, Rebecca R. Buchholz, Glenn S. Diskin, Russell R. Dickerson, Xinrong Ren, Hao He, and Yutaka Kondo
Atmos. Meas. Tech., 13, 1337–1356, https://doi.org/10.5194/amt-13-1337-2020, https://doi.org/10.5194/amt-13-1337-2020, 2020
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
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Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
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We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Kanako Sekimoto, Bin Yuan, Jessica B. Gilman, David H. Hagan, Vanessa Selimovic, Kyle J. Zarzana, Steven S. Brown, James M. Roberts, Markus Müller, Robert Yokelson, Armin Wisthaler, Jordan E. Krechmer, Jose L. Jimenez, Christopher Cappa, Jesse H. Kroll, Joost de Gouw, and Carsten Warneke
Atmos. Chem. Phys., 19, 14875–14899, https://doi.org/10.5194/acp-19-14875-2019, https://doi.org/10.5194/acp-19-14875-2019, 2019
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Wildfire emissions significantly contribute to adverse air quality; however, the chemical processes that lead to hazardous pollutants, such as ozone, are not fully understood. In this study, we describe laboratory experiments where we simulate the atmospheric chemistry of smoke emitted from a range of biomass fuels. We show that certain understudied compounds, such as furans and phenolic compounds, are significant contributors to pollutants formed as a result of typical atmospheric oxidation.
Jiajue Chai, David J. Miller, Eric Scheuer, Jack Dibb, Vanessa Selimovic, Robert Yokelson, Kyle J. Zarzana, Steven S. Brown, Abigail R. Koss, Carsten Warneke, and Meredith Hastings
Atmos. Meas. Tech., 12, 6303–6317, https://doi.org/10.5194/amt-12-6303-2019, https://doi.org/10.5194/amt-12-6303-2019, 2019
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Isotopic analysis offers a potential tool to distinguish between sources and interpret transformation pathways of atmospheric species. We applied recently developed techniques in our lab to characterize the isotopic composition of reactive nitrogen species (NOx, HONO, HNO3, pNO3-) in fresh biomass burning emissions. Intercomparison with other techniques confirms the suitability of our methods, allowing for future applications of our techniques in a variety of environments.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Ingo Wohltmann, Ralph Lehmann, Georg A. Gottwald, Karsten Peters, Alain Protat, Valentin Louf, Christopher Williams, Wuhu Feng, and Markus Rex
Geosci. Model Dev., 12, 4387–4407, https://doi.org/10.5194/gmd-12-4387-2019, https://doi.org/10.5194/gmd-12-4387-2019, 2019
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We present a trajectory-based model for simulating the transport of air parcels by convection. Our model extends the approach of existing models by explicitly simulating vertical updraft velocities inside the clouds and the time that an air parcel spends inside the convective event.
Daun Jeong, Roger Seco, Dasa Gu, Youngro Lee, Benjamin A. Nault, Christoph J. Knote, Tom Mcgee, John T. Sullivan, Jose L. Jimenez, Pedro Campuzano-Jost, Donald R. Blake, Dianne Sanchez, Alex B. Guenther, David Tanner, L. Gregory Huey, Russell Long, Bruce E. Anderson, Samuel R. Hall, Kirk Ullmann, Hye-jung Shin, Scott C. Herndon, Youngjae Lee, Danbi Kim, Joonyoung Ahn, and Saewung Kim
Atmos. Chem. Phys., 19, 12779–12795, https://doi.org/10.5194/acp-19-12779-2019, https://doi.org/10.5194/acp-19-12779-2019, 2019
Christopher Y. Lim, David H. Hagan, Matthew M. Coggon, Abigail R. Koss, Kanako Sekimoto, Joost de Gouw, Carsten Warneke, Christopher D. Cappa, and Jesse H. Kroll
Atmos. Chem. Phys., 19, 12797–12809, https://doi.org/10.5194/acp-19-12797-2019, https://doi.org/10.5194/acp-19-12797-2019, 2019
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Wildfires are a large source of gases and particles to the atmosphere, both of which impact human health and climate. The amount and composition of particles from wildfires can change with time in the atmosphere; however, the impact of aging is not well understood. In a series of controlled laboratory experiments, we show that the particles are oxidized and a significant fraction of the gas-phase carbon (24 %–56 %) is converted to particle mass over the course of several days in the atmosphere.
Thomas von Clarmann and Norbert Glatthor
Atmos. Meas. Tech., 12, 5155–5160, https://doi.org/10.5194/amt-12-5155-2019, https://doi.org/10.5194/amt-12-5155-2019, 2019
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To avoid unnecessary data traffic it is sometimes desirable to apply mean averaging kernels to mean profiles of atmospheric state variables. Unfortunately, the application of individual averaging kernels to individual profiles and subsequent averaging will, in general, lead to different results than averaging of the original profiles prior to the application of the mean averaging kernels. This effect is investigated and a correction scheme is proposed.
Carly L. Reddington, Luke Conibear, Christoph Knote, Ben J. Silver, Yong J. Li, Chak K. Chan, Steve R. Arnold, and Dominick V. Spracklen
Atmos. Chem. Phys., 19, 11887–11910, https://doi.org/10.5194/acp-19-11887-2019, https://doi.org/10.5194/acp-19-11887-2019, 2019
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We use a high-resolution model over South and East Asia to explore air quality and human health benefits of eliminating emissions from six man-made pollution sources. We find that preventing emissions from either residential energy use, industry, or open biomass burning yields the largest reductions in ground-level particulate matter pollution and its associated disease burden over this region. We also summarize previous estimates of the source-specific disease burden in China and India.
Andreas Chrysanthou, Amanda C. Maycock, Martyn P. Chipperfield, Sandip Dhomse, Hella Garny, Douglas Kinnison, Hideharu Akiyoshi, Makoto Deushi, Rolando R. Garcia, Patrick Jöckel, Oliver Kirner, Giovanni Pitari, David A. Plummer, Laura Revell, Eugene Rozanov, Andrea Stenke, Taichu Y. Tanaka, Daniele Visioni, and Yousuke Yamashita
Atmos. Chem. Phys., 19, 11559–11586, https://doi.org/10.5194/acp-19-11559-2019, https://doi.org/10.5194/acp-19-11559-2019, 2019
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We perform the first multi-model comparison of the impact of nudged meteorology on the stratospheric residual circulation (RC) in chemistry–climate models. Nudging meteorology does not constrain the mean strength of RC compared to free-running simulations, and despite the lack of agreement in the mean circulation, nudging tightly constrains the inter-annual variability in the tropical upward mass flux in the lower stratosphere. In summary, nudging strongly affects the representation of RC.
Jeffrey S. Reid, Derek J. Posselt, Kathleen Kaku, Robert A. Holz, Gao Chen, Edwin W. Eloranta, Ralph E. Kuehn, Sarah Woods, Jianglong Zhang, Bruce Anderson, T. Paul Bui, Glenn S. Diskin, Patrick Minnis, Michael J. Newchurch, Simone Tanelli, Charles R. Trepte, K. Lee Thornhill, and Luke D. Ziemba
Atmos. Chem. Phys., 19, 11413–11442, https://doi.org/10.5194/acp-19-11413-2019, https://doi.org/10.5194/acp-19-11413-2019, 2019
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The scientific community often focuses on the vertical transport of pollutants by clouds for those with bases at the planetary boundary layer (such as typical fair-weather cumulus) and the outflow from thunderstorms at their tops. We demonstrate complex aerosol and cloud features formed in mid-level thunderstorm outflow. These layers have strong relationships to mid-level tropospheric clouds, an important but difficult to model or monitor cloud regime for climate studies.
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.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
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In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
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.
Matthew J. Rowlinson, Alexandru Rap, Stephen R. Arnold, Richard J. Pope, Martyn P. Chipperfield, Joe McNorton, Piers Forster, Hamish Gordon, Kirsty J. Pringle, Wuhu Feng, Brian J. Kerridge, Barry L. Latter, and Richard Siddans
Atmos. Chem. Phys., 19, 8669–8686, https://doi.org/10.5194/acp-19-8669-2019, https://doi.org/10.5194/acp-19-8669-2019, 2019
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Wildfires and meteorology have a substantial effect on atmospheric concentrations of greenhouse gases such as methane and ozone. During the 1997 El Niño event, unusually large fire emissions indirectly increased global methane through carbon monoxide emission, which decreased the oxidation capacity of the atmosphere. There were also large regional changes to tropospheric ozone concentrations, but contrasting effects of fire and meteorology resulted in a small change to global radiative forcing.
Xiaoxi Liu, Benjamin Deming, Demetrios Pagonis, Douglas A. Day, Brett B. Palm, Ranajit Talukdar, James M. Roberts, Patrick R. Veres, Jordan E. Krechmer, Joel A. Thornton, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 12, 3137–3149, https://doi.org/10.5194/amt-12-3137-2019, https://doi.org/10.5194/amt-12-3137-2019, 2019
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Delays or losses of gases in sampling tubing and instrumental surfaces due to surface interactions can lead to inaccurate quantification. By sampling with several chemical ionization mass spectrometers and six tubing materials, we quantify delays of semivolatile organic compounds and small polar gases. Delay times generally increase with decreasing volatility or increasing polarity and also depend on materials. The method and results will inform inlet material selection and instrumental design.
Lei Zhu, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Xuan Wang, Tomás Sherwen, Mat J. Evans, Qianjie Chen, Becky Alexander, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Michael Le Breton, Thomas J. Bannan, and Carl J. Percival
Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, https://doi.org/10.5194/acp-19-6497-2019, 2019
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We quantify the effect of sea salt aerosol on tropospheric bromine chemistry with a new mechanistic description of the halogen chemistry in a global atmospheric chemistry model. For the first time, we are able to reproduce the observed levels of bromide activation from the sea salt aerosol in a manner consistent with bromine oxide radical measured from various platforms. Sea salt aerosol plays a far more complex role in global tropospheric chemistry than previously recognized.
Stefan Lossow, Farahnaz Khosrawi, Michael Kiefer, Kaley A. Walker, Jean-Loup Bertaux, Laurent Blanot, James M. Russell, Ellis E. Remsberg, John C. Gille, Takafumi Sugita, Christopher E. Sioris, Bianca M. Dinelli, Enzo Papandrea, Piera Raspollini, Maya García-Comas, Gabriele P. Stiller, Thomas von Clarmann, Anu Dudhia, William G. Read, Gerald E. Nedoluha, Robert P. Damadeo, Joseph M. Zawodny, Katja Weigel, Alexei Rozanov, Faiza Azam, Klaus Bramstedt, Stefan Noël, John P. Burrows, Hideo Sagawa, Yasuko Kasai, Joachim Urban, Patrick Eriksson, Donal P. Murtagh, Mark E. Hervig, Charlotta Högberg, Dale F. Hurst, and Karen H. Rosenlof
Atmos. Meas. Tech., 12, 2693–2732, https://doi.org/10.5194/amt-12-2693-2019, https://doi.org/10.5194/amt-12-2693-2019, 2019
James M. Roberts and Yong Liu
Atmos. Chem. Phys., 19, 4419–4437, https://doi.org/10.5194/acp-19-4419-2019, https://doi.org/10.5194/acp-19-4419-2019, 2019
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Condensed-phase reactions are important removal processes for reduced nitrogen species, isocyanic acid (HNCO), methyl isocyanate (CH3NCO), and cyanogen halides (XCN, X = Cl, Br, I). This chemistry is not well understood, so we measured aqueous-phase solubilities and reaction rates under a range of temperatures and conditions and in n-octanol, a proxy for non-polar media and biological membranes. The results were used to estimate atmospheric removal rates and fates of these nitrogen compounds.
Daniel M. Murphy, Karl D. Froyd, Huisheng Bian, Charles A. Brock, Jack E. Dibb, Joshua P. DiGangi, Glenn Diskin, Maximillian Dollner, Agnieszka Kupc, Eric M. Scheuer, Gregory P. Schill, Bernadett Weinzierl, Christina J. Williamson, and Pengfei Yu
Atmos. Chem. Phys., 19, 4093–4104, https://doi.org/10.5194/acp-19-4093-2019, https://doi.org/10.5194/acp-19-4093-2019, 2019
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We present the first data on the concentration of sea-salt aerosol throughout most of the depth of the troposphere and a wide range of latitudes. Sea-salt concentrations in the upper troposphere are very small. This puts stringent limits on how sea-salt aerosol affects halogen and nitric acid chemistry there. With a widely distributed source, sea-salt aerosol provides an excellent test of wet scavenging and vertical transport of aerosols in chemical transport models.
Xuan Wang, Daniel J. Jacob, Sebastian D. Eastham, Melissa P. Sulprizio, Lei Zhu, Qianjie Chen, Becky Alexander, Tomás Sherwen, Mathew J. Evans, Ben H. Lee, Jessica D. Haskins, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Gregory L. Huey, and Hong Liao
Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, https://doi.org/10.5194/acp-19-3981-2019, 2019
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Chlorine radicals have a broad range of implications for tropospheric chemistry, air quality, and climate. We present a comprehensive simulation of tropospheric chlorine in a global 3-D model, which includes explicit accounting of chloride mobilization from sea salt aerosol. We find the chlorine chemistry contributes 1.0 % of the global oxidation of methane and decreases global burdens of tropospheric ozone by 7 % and OH by 3 % through the associated bromine radical chemistry.
Tao Yuan, Wuhu Feng, John M. C. Plane, and Daniel R. Marsh
Atmos. Chem. Phys., 19, 3769–3777, https://doi.org/10.5194/acp-19-3769-2019, https://doi.org/10.5194/acp-19-3769-2019, 2019
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The Na layer in the upper atmosphere is very sensitive to solar radiation and varies considerably during sunrise and sunset. In this paper, we use the lidar observations and an advanced model to investigate this process. We found that the variation is mostly due to the changes in several photochemical reactions involving Na compounds, especially NaHCO3. We also reveal that the Fe layer in the same region changes more quickly than the Na layer due to a faster reaction rate of FeOH to sunlight.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Jin Liao, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Jose L. Jimenez, Pedro Campuzano-Jost, Benjamin A. Nault, Alan Fried, Eloise A. Marais, Gonzalo Gonzalez Abad, Kelly Chance, Hiren T. Jethva, Thomas B. Ryerson, Carsten Warneke, and Armin Wisthaler
Atmos. Chem. Phys., 19, 2765–2785, https://doi.org/10.5194/acp-19-2765-2019, https://doi.org/10.5194/acp-19-2765-2019, 2019
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Organic aerosol (OA) intimately links natural and anthropogenic emissions with air quality and climate. Direct OA measurements from space are currently not possible. This paper describes a new method to estimate OA by combining satellite HCHO and in situ OA and HCHO. The OA estimate is validated with the ground network. This new method has a potential for mapping observation-based global OA estimate.
Evgenia Galytska, Alexey Rozanov, Martyn P. Chipperfield, Sandip. S. Dhomse, Mark Weber, Carlo Arosio, Wuhu Feng, and John P. Burrows
Atmos. Chem. Phys., 19, 767–783, https://doi.org/10.5194/acp-19-767-2019, https://doi.org/10.5194/acp-19-767-2019, 2019
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In this study we analysed ozone changes in the tropical mid-stratosphere as observed by the SCIAMACHY instrument during 2004–2012. We used simulations from TOMCAT model with different chemical and dynamical forcings to reveal primary causes of ozone changes. We also considered measured NO2 and modelled NOx, NOx, and N2O data. With modelled AoA data we identified seasonal changes in the upwelling speed and explained how those changes affect N2O chemistry which leads to observed ozone changes.
Debora Griffin, Kaley A. Walker, Ingo Wohltmann, Sandip S. Dhomse, Markus Rex, Martyn P. Chipperfield, Wuhu Feng, Gloria L. Manney, Jane Liu, and David Tarasick
Atmos. Chem. Phys., 19, 577–601, https://doi.org/10.5194/acp-19-577-2019, https://doi.org/10.5194/acp-19-577-2019, 2019
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Ozone in the stratosphere is important to protect the Earth from UV radiation. Using measurements taken by the Atmospheric Chemistry Experiment satellite between 2005 and 2013, we examine different methods to calculate the ozone loss in the high Arctic and establish the altitude at which most of the ozone is destroyed. Our results show that the different methods agree within the uncertainties. Recommendations are made on which methods are most appropriate to use.
Joe McNorton, Chris Wilson, Manuel Gloor, Rob J. Parker, Hartmut Boesch, Wuhu Feng, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 18149–18168, https://doi.org/10.5194/acp-18-18149-2018, https://doi.org/10.5194/acp-18-18149-2018, 2018
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Since 2007 atmospheric methane (CH4) has been unexpectedly increasing following a 6-year hiatus. We have used an atmospheric model to attribute regional sources and global sinks of CH4 using observations for the 2003–2015 period. Model results show the renewed growth is best explained by decreased atmospheric removal, decreased biomass burning emissions, and an increased energy sector (mainly from Africa–Middle East and Southern Asia–Oceania) and wetland emissions (mainly from northern Eurasia).
Tommaso Galeazzo, Slimane Bekki, Erwan Martin, Joël Savarino, and Stephen R. Arnold
Atmos. Chem. Phys., 18, 17909–17931, https://doi.org/10.5194/acp-18-17909-2018, https://doi.org/10.5194/acp-18-17909-2018, 2018
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Volcanic sulfur can have climatic impacts for the planet via sulfate aerosol formation, leading also to pollution events. We provide model constraints on tropospheric volcanic sulfate formation, with implications for its lifetime and impacts on regional air quality. Oxygen isotope investigations from our model suggest that in the poor tropospheric plumes of halogens, the O2/TMI sulfur oxidation pathway might significantly control sulfate production. The produced sulfate has no isotopic anomaly.
Benjamin A. Nault, Pedro Campuzano-Jost, Douglas A. Day, Jason C. Schroder, Bruce Anderson, Andreas J. Beyersdorf, Donald R. Blake, William H. Brune, Yonghoon Choi, Chelsea A. Corr, Joost A. de Gouw, Jack Dibb, Joshua P. DiGangi, Glenn S. Diskin, Alan Fried, L. Gregory Huey, Michelle J. Kim, Christoph J. Knote, Kara D. Lamb, Taehyoung Lee, Taehyun Park, Sally E. Pusede, Eric Scheuer, Kenneth L. Thornhill, Jung-Hun Woo, and Jose L. Jimenez
Atmos. Chem. Phys., 18, 17769–17800, https://doi.org/10.5194/acp-18-17769-2018, https://doi.org/10.5194/acp-18-17769-2018, 2018
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Aerosol impacts visibility and human health in large cities. Sources of aerosols are still highly uncertain, especially for cities surrounded by numerous other cities. We use observations collected during the Korea–United States Air Quality study to determine sources of organic aerosol (OA). We find that secondary OA (SOA) is rapidly produced over Seoul, South Korea, and that the sources of the SOA originate from short-lived hydrocarbons, which originate from local emissions.
Kyle J. Zarzana, Vanessa Selimovic, Abigail R. Koss, Kanako Sekimoto, Matthew M. Coggon, Bin Yuan, William P. Dubé, Robert J. Yokelson, Carsten Warneke, Joost A. de Gouw, James M. Roberts, and Steven S. Brown
Atmos. Chem. Phys., 18, 15451–15470, https://doi.org/10.5194/acp-18-15451-2018, https://doi.org/10.5194/acp-18-15451-2018, 2018
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Emissions of glyoxal and methylglyoxal from fuels common to the western United States were measured using cavity-enhanced spectroscopy, which provides a more selective measurement of those compounds than was previously available. Primary emissions of glyoxal were lower than previously reported and showed variability between the different fuel groups. However, emissions of glyoxal relative to formaldehyde were constant across almost all the fuel groups at 6 %–7 %.
Jeremy J. Harrison
Atmos. Meas. Tech., 11, 5827–5836, https://doi.org/10.5194/amt-11-5827-2018, https://doi.org/10.5194/amt-11-5827-2018, 2018
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CFC-11 is a stratospheric-ozone-depleting molecule which is banned under the Montreal Protocol but still present in the atmosphere due to its long lifetime. Using infrared limb sounders on satellite platforms to monitor its concentration crucially requires accurate laboratory spectroscopic data. This paper describes a new high-resolution infrared absorption cross-section dataset for remote-sensing purposes; this improves upon the one currently available in the HITRAN and GEISA databases.
John M. C. Plane, Wuhu Feng, Juan Carlos Gómez Martín, Michael Gerding, and Shikha Raizada
Atmos. Chem. Phys., 18, 14799–14811, https://doi.org/10.5194/acp-18-14799-2018, https://doi.org/10.5194/acp-18-14799-2018, 2018
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Meteoric ablation creates layers of metal atoms in the atmosphere around 90 km. Although Ca and Na have similar elemental abundances in most minerals found in the solar system, surprisingly the Ca abundance in the atmosphere is less than 1 % that of Na. This study uses a detailed chemistry model of Ca, largely based on laboratory kinetics measurements, in a whole-atmosphere model to show that the depletion is caused by inefficient ablation of Ca and the formation of stable molecular reservoirs.
William H. Brune, Xinrong Ren, Li Zhang, Jingqiu Mao, David O. Miller, Bruce E. Anderson, Donald R. Blake, Ronald C. Cohen, Glenn S. Diskin, Samuel R. Hall, Thomas F. Hanisco, L. Gregory Huey, Benjamin A. Nault, Jeff Peischl, Ilana Pollack, Thomas B. Ryerson, Taylor Shingler, Armin Sorooshian, Kirk Ullmann, Armin Wisthaler, and Paul J. Wooldridge
Atmos. Chem. Phys., 18, 14493–14510, https://doi.org/10.5194/acp-18-14493-2018, https://doi.org/10.5194/acp-18-14493-2018, 2018
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Thunderstorms pull in polluted air from near the ground, transport it up through clouds containing lightning, and deposit it at altitudes where airplanes fly. The resulting chemical mixture in this air reacts to form ozone and particles, which affect climate. In this study, aircraft observations of the reactive gases responsible for this chemistry generally agree with modeled values, even in ice clouds. Thus, atmospheric oxidation chemistry appears to be mostly understood for this environment.
Theodora Nah, Yi Ji, David J. Tanner, Hongyu Guo, Amy P. Sullivan, Nga Lee Ng, Rodney J. Weber, and L. Gregory Huey
Atmos. Meas. Tech., 11, 5087–5104, https://doi.org/10.5194/amt-11-5087-2018, https://doi.org/10.5194/amt-11-5087-2018, 2018
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The sources and atmospheric chemistry of gas-phase organic acids are currently poorly understood, due in part to the limited range of measurement techniques available. We evaluated the use of SF6− as a sensitive and selective chemical ionization reagent ion for real-time measurements of gas-phase organic acids at a rural site in Yorkville, Georgia. We found that ambient concentrations of organic acids ranged from a few ppt to several ppb, and are dependent on ambient temperature.
Paul I. Palmer, Simon O'Doherty, Grant Allen, Keith Bower, Hartmut Bösch, Martyn P. Chipperfield, Sarah Connors, Sandip Dhomse, Liang Feng, Douglas P. Finch, Martin W. Gallagher, Emanuel Gloor, Siegfried Gonzi, Neil R. P. Harris, Carole Helfter, Neil Humpage, Brian Kerridge, Diane Knappett, Roderic L. Jones, Michael Le Breton, Mark F. Lunt, Alistair J. Manning, Stephan Matthiesen, Jennifer B. A. Muller, Neil Mullinger, Eiko Nemitz, Sebastian O'Shea, Robert J. Parker, Carl J. Percival, Joseph Pitt, Stuart N. Riddick, Matthew Rigby, Harjinder Sembhi, Richard Siddans, Robert L. Skelton, Paul Smith, Hannah Sonderfeld, Kieran Stanley, Ann R. Stavert, Angelina Wenger, Emily White, Christopher Wilson, and Dickon Young
Atmos. Chem. Phys., 18, 11753–11777, https://doi.org/10.5194/acp-18-11753-2018, https://doi.org/10.5194/acp-18-11753-2018, 2018
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This paper provides an overview of the Greenhouse gAs Uk and Global Emissions (GAUGE) experiment. GAUGE was designed to quantify nationwide GHG emissions of the UK, bringing together measurements and atmospheric transport models. This novel experiment is the first of its kind. We anticipate it will inform the blueprint for countries that are building a measurement infrastructure in preparation for global stocktakes, which are a key part of the Paris Agreement.
Tao Li, Chao Ban, Xin Fang, Jing Li, Zhaopeng Wu, Wuhu Feng, John M. C. Plane, Jiangang Xiong, Daniel R. Marsh, Michael J. Mills, and Xiankang Dou
Atmos. Chem. Phys., 18, 11683–11695, https://doi.org/10.5194/acp-18-11683-2018, https://doi.org/10.5194/acp-18-11683-2018, 2018
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A total of 154 nights of observations by the USTC Na temperature and wind lidar (32° N, 117° E) suggest significant seasonal variability in the mesopause. Chemistry plays an important role in Na atom formation. More than half of the observed gravity wave (GW) momentum flux (MF), whose divergence determines the GW forcing, is induced by short-period (10 min–2 h) waves. The anticorrelation between MF and zonal wind (U) suggests strong filtering of short-period GWs by semiannual oscillation U.
Juliane L. Fry, Steven S. Brown, Ann M. Middlebrook, Peter M. Edwards, Pedro Campuzano-Jost, Douglas A. Day, José L. Jimenez, Hannah M. Allen, Thomas B. Ryerson, Ilana Pollack, Martin Graus, Carsten Warneke, Joost A. de Gouw, Charles A. Brock, Jessica Gilman, Brian M. Lerner, William P. Dubé, Jin Liao, and André Welti
Atmos. Chem. Phys., 18, 11663–11682, https://doi.org/10.5194/acp-18-11663-2018, https://doi.org/10.5194/acp-18-11663-2018, 2018
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This paper uses measurements made during research aircraft flights through power plant smokestack emissions plumes as a natural laboratory in the field experiment. We investigated a specific source of airborne particulate matter from the combination of human-produced NOx pollutant emissions (the smokestack plumes) with isoprene emitted by naturally by trees in the southeastern United States. These field-based yields appear to be higher than those typically measured in chamber studies.
Birgit Hassler, Stefanie Kremser, Greg E. Bodeker, Jared Lewis, Kage Nesbit, Sean M. Davis, Martyn P. Chipperfield, Sandip S. Dhomse, and Martin Dameris
Earth Syst. Sci. Data, 10, 1473–1490, https://doi.org/10.5194/essd-10-1473-2018, https://doi.org/10.5194/essd-10-1473-2018, 2018
Theodora Nah, Hongyu Guo, Amy P. Sullivan, Yunle Chen, David J. Tanner, Athanasios Nenes, Armistead Russell, Nga Lee Ng, L. Gregory Huey, and Rodney J. Weber
Atmos. Chem. Phys., 18, 11471–11491, https://doi.org/10.5194/acp-18-11471-2018, https://doi.org/10.5194/acp-18-11471-2018, 2018
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We present measurements from a field study conducted in an agriculturally intensive region in the southeastern US during the fall of 2016 to investigate how NH3 affects particle acidity and SOA formation via gas–particle partitioning of semi-volatile organic acids. For this study, higher NH3 concentrations relative to what has been measured in the region in previous studies had minor effects on PM1 organic acids and their influence on the overall organic aerosol and PM1 mass concentrations.
Norbert Glatthor, Thomas von Clarmann, Gabriele P. Stiller, Michael Kiefer, Alexandra Laeng, Bianca M. Dinelli, Gerald Wetzel, and Johannes Orphal
Atmos. Meas. Tech., 11, 4707–4723, https://doi.org/10.5194/amt-11-4707-2018, https://doi.org/10.5194/amt-11-4707-2018, 2018
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We report differences in ozone retrievals in channels A and AB of the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), which amount to up to 8 %. We provide strong evidence that the bias is caused by inconsistencies in different spectroscopic databases (MIPAS, HITRAN, GEISA). We show that a major part of the differences can be attributed to inconsistent air-broadening coefficients of the ozone lines contained in the databases.
Alexandra Laeng, Ellen Eckert, Thomas von Clarmann, Michael Kiefer, Daan Hubert, Gabriele Stiller, Norbert Glatthor, Manuel López-Puertas, Bernd Funke, Udo Grabowski, Johannes Plieninger, Sylvia Kellmann, Andrea Linden, Stefan Lossow, Arne Babenhauserheide, Lucien Froidevaux, and Kaley Walker
Atmos. Meas. Tech., 11, 4693–4705, https://doi.org/10.5194/amt-11-4693-2018, https://doi.org/10.5194/amt-11-4693-2018, 2018
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MIPAS was an IR limb emission spectrometer on the Envisat platform. From 2002 to 2012, it performed pole-to-pole measurements of ozone during day and night. ESA recently released the new version 7 of Level 1 MIPAS spectra, which is expected to reduce the long-term drift of the MIPAS Level 2 data. We evaluate the long-term stability of ozone Level 2 data from the KIT IMK processor. Our results indicate that MIPAS data are now even more suited for trend studies, alone or as part of merged data.
Wenfu Tang, Avelino F. Arellano, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Anna Agustí-Panareda, Mark Parrington, Sebastien Massart, Benjamin Gaubert, Youngjae Lee, Danbi Kim, Jinsang Jung, Jinkyu Hong, Je-Woo Hong, Yugo Kanaya, Mindo Lee, Ryan M. Stauffer, Anne M. Thompson, James H. Flynn, and Jung-Hun Woo
Atmos. Chem. Phys., 18, 11007–11030, https://doi.org/10.5194/acp-18-11007-2018, https://doi.org/10.5194/acp-18-11007-2018, 2018
Maarten Krol, Marco de Bruine, Lars Killaars, Huug Ouwersloot, Andrea Pozzer, Yi Yin, Frederic Chevallier, Philippe Bousquet, Prabir Patra, Dmitry Belikov, Shamil Maksyutov, Sandip Dhomse, Wuhu Feng, and Martyn P. Chipperfield
Geosci. Model Dev., 11, 3109–3130, https://doi.org/10.5194/gmd-11-3109-2018, https://doi.org/10.5194/gmd-11-3109-2018, 2018
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The TransCom inter-comparison project regularly carries out studies to quantify errors in simulated atmospheric transport. This paper presents the first results of an age of air (AoA) inter-comparison of six global transport models. Following a protocol, six models simulated five tracers from which atmospheric transport times can easily be deduced. Results highlight that inter-model differences associated with atmospheric transport are still large and require further analysis.
Farahnaz Khosrawi, Stefan Lossow, Gabriele P. Stiller, Karen H. Rosenlof, Joachim Urban, John P. Burrows, Robert P. Damadeo, Patrick Eriksson, Maya García-Comas, John C. Gille, Yasuko Kasai, Michael Kiefer, Gerald E. Nedoluha, Stefan Noël, Piera Raspollini, William G. Read, Alexei Rozanov, Christopher E. Sioris, Kaley A. Walker, and Katja Weigel
Atmos. Meas. Tech., 11, 4435–4463, https://doi.org/10.5194/amt-11-4435-2018, https://doi.org/10.5194/amt-11-4435-2018, 2018
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Time series of stratospheric and lower mesospheric water vapour using 33 data sets from 15 satellite instruments were compared in the framework of the second SPARC water vapour assessment. We find that most data sets can be considered in observational and modelling studies addressing, e.g. stratospheric and lower mesospheric water vapour variability and trends if data-set-specific characteristics (e.g. a drift) and restrictions (e.g. temporal and spatial coverage) are taken into account.
Kanako Sekimoto, Abigail R. Koss, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Carsten Warneke, Robert J. Yokelson, James M. Roberts, and Joost de Gouw
Atmos. Chem. Phys., 18, 9263–9281, https://doi.org/10.5194/acp-18-9263-2018, https://doi.org/10.5194/acp-18-9263-2018, 2018
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We found that on average 85 % of the VOC emissions from biomass burning across various fuels representative of the western US (including various coniferous and chaparral fuels) can be explained using only two emission profiles: (i) a high-temperature pyrolysis profile and (ii) a low-temperature pyrolysis profile. The high-temperature profile is quantitatively similar between different fuel types (r2 > 0.84), and likewise for the low-temperature profile.
Chunxiang Ye, Xianliang Zhou, Dennis Pu, Jochen Stutz, James Festa, Max Spolaor, Catalina Tsai, Christopher Cantrell, Roy L. Mauldin III, Andrew Weinheimer, Rebecca S. Hornbrook, Eric C. Apel, Alex Guenther, Lisa Kaser, Bin Yuan, Thomas Karl, Julie Haggerty, Samuel Hall, Kirk Ullmann, James Smith, and John Ortega
Atmos. Chem. Phys., 18, 9107–9120, https://doi.org/10.5194/acp-18-9107-2018, https://doi.org/10.5194/acp-18-9107-2018, 2018
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Substantial levels of HONO existed during the day throughout the troposphere over the southeastern US during NOMADSS 2013. Particulate nitrate photolysis appeared to be the major volume HONO source, while NOx was an important HONO precursor only in industrial and urban plumes. HONO was not a significant OH radical precursor in the rural troposphere away from the ground surface; however, its production from particulate nitrate photolysis was an important renoxification pathway.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
Richard J. Pope, Martyn P. Chipperfield, Stephen R. Arnold, Norbert Glatthor, Wuhu Feng, Sandip S. Dhomse, Brian J. Kerridge, Barry G. Latter, and Richard Siddans
Atmos. Chem. Phys., 18, 8389–8408, https://doi.org/10.5194/acp-18-8389-2018, https://doi.org/10.5194/acp-18-8389-2018, 2018
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Roya Bahreini, Ravan Ahmadov, Stu A. McKeen, Kennedy T. Vu, Justin H. Dingle, Eric C. Apel, Donald R. Blake, Nicola Blake, Teresa L. Campos, Chris Cantrell, Frank Flocke, Alan Fried, Jessica B. Gilman, Alan J. Hills, Rebecca S. Hornbrook, Greg Huey, Lisa Kaser, Brian M. Lerner, Roy L. Mauldin, Simone Meinardi, Denise D. Montzka, Dirk Richter, Jason R. Schroeder, Meghan Stell, David Tanner, James Walega, Peter Weibring, and Andrew Weinheimer
Atmos. Chem. Phys., 18, 8293–8312, https://doi.org/10.5194/acp-18-8293-2018, https://doi.org/10.5194/acp-18-8293-2018, 2018
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We measured organic aerosol (OA) and relevant trace gases during FRAPPÉ in the Colorado Front Range, with the goal of characterizing summertime OA formation. Our results indicate a significant production of secondary OA (SOA) in this region. About 2 μg m−3 of OA was present at background CO levels, suggesting contribution of non-combustion sources to SOA. Contribution of oil- and gas-related activities to anthropogenic SOA was modeled to be ~38 %. Biogenic SOA contributed to >40 % of OA.
Si-Wan Kim, Vijay Natraj, Seoyoung Lee, Hyeong-Ahn Kwon, Rokjin Park, Joost de Gouw, Gregory Frost, Jhoon Kim, Jochen Stutz, Michael Trainer, Catalina Tsai, and Carsten Warneke
Atmos. Chem. Phys., 18, 7639–7655, https://doi.org/10.5194/acp-18-7639-2018, https://doi.org/10.5194/acp-18-7639-2018, 2018
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Formaldehyde (HCHO) is a hazardous air pollutant and is associated with tropospheric ozone production. HCHO has been monitored from space. In this study, to acquire high-quality satellite-based HCHO observations, we utilize fine-resolution atmospheric chemistry model results as an input to the computer code for satellite retrievals over the Los Angeles Basin. Our study indicates that the use of fine-resolution profile shapes helps to identify HCHO plumes from space.
Chelsea E. Stockwell, Agnieszka Kupc, Bartłomiej Witkowski, Ranajit K. Talukdar, Yong Liu, Vanessa Selimovic, Kyle J. Zarzana, Kanako Sekimoto, Carsten Warneke, Rebecca A. Washenfelder, Robert J. Yokelson, Ann M. Middlebrook, and James M. Roberts
Atmos. Meas. Tech., 11, 2749–2768, https://doi.org/10.5194/amt-11-2749-2018, https://doi.org/10.5194/amt-11-2749-2018, 2018
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This work investigates the total conversion of particle-bound nitrogen and organic carbon across platinum and molybdenum catalysts followed by NO–O3 chemiluminescence and nondispersive infrared CO2 detection. We show the instrument is an accurate particle mass measurement method and demonstrate its ability to calibrate particle mass measurement instrumentation through comparisons with a calibrated particle-into-liquid sampler coupled to an electrospray ionization source of a mass spectrometer.
Young-Suk Oh, S. Takele Kenea, Tae-Young Goo, Kyu-Sun Chung, Jae-Sang Rhee, Mi-Lim Ou, Young-Hwa Byun, Paul O. Wennberg, Matthäus Kiel, Joshua P. DiGangi, Glenn S. Diskin, Voltaire A. Velazco, and David W. T. Griffith
Atmos. Meas. Tech., 11, 2361–2374, https://doi.org/10.5194/amt-11-2361-2018, https://doi.org/10.5194/amt-11-2361-2018, 2018
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We focused on the measurements taken during the period of February 2014 to November 2017. The FTS instrument was stable during the whole measurement period. The g-b FTS retrieval of XCO2 and XCH4 were compared with aircraft measurements that were conducted over Anmyeondo station on 22 May 2016, 29 October, and 12 November 2017. The preliminary comparison results of XCO2 between FTS and OCO-2 were also presented over the Anmyeondo station.
Manuel López-Puertas, Maya García-Comas, Bernd Funke, Angela Gardini, Gabriele P. Stiller, Thomas von Clarmann, Norbert Glatthor, Alexandra Laeng, Martin Kaufmann, Viktoria F. Sofieva, Lucien Froidevaux, Kaley A. Walker, and Masato Shiotani
Atmos. Meas. Tech., 11, 2187–2212, https://doi.org/10.5194/amt-11-2187-2018, https://doi.org/10.5194/amt-11-2187-2018, 2018
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This paper describes the inversion of O3 data from MIPAS middle atmosphere spectra which requires non-LTE. The O3 dataset comprises from 20 to 100 km, has a pole-to-pole latitude coverage, day and nighttime, and span from 2005 until 2012. A validation of the data against other satellite measurements and an overall description of O3 is also presented. This is an important dataset for the community and describes the major characteristics of stratospheric and mesospheric O3.
Glenn M. Wolfe, S. Randy Kawa, Thomas F. Hanisco, Reem A. Hannun, Paul A. Newman, Andrew Swanson, Steve Bailey, John Barrick, K. Lee Thornhill, Glenn Diskin, Josh DiGangi, John B. Nowak, Carl Sorenson, Geoffrey Bland, James K. Yungel, and Craig A. Swenson
Atmos. Meas. Tech., 11, 1757–1776, https://doi.org/10.5194/amt-11-1757-2018, https://doi.org/10.5194/amt-11-1757-2018, 2018
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We describe a new NASA airborne system for directly observing the surface–atmosphere exchange of greenhouse gases and energy over regional scales. Such measurements are needed benchmark model and satellite products and can improve process-level understanding of greenhouse gas sources and sinks over forest, croplands, wetlands, urban areas, and other ecosystems.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
Abigail R. Koss, Kanako Sekimoto, Jessica B. Gilman, Vanessa Selimovic, Matthew M. Coggon, Kyle J. Zarzana, Bin Yuan, Brian M. Lerner, Steven S. Brown, Jose L. Jimenez, Jordan Krechmer, James M. Roberts, Carsten Warneke, Robert J. Yokelson, and Joost de Gouw
Atmos. Chem. Phys., 18, 3299–3319, https://doi.org/10.5194/acp-18-3299-2018, https://doi.org/10.5194/acp-18-3299-2018, 2018
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Non-methane organic gases (NMOGs) were detected by proton-transfer-reaction mass spectrometry (PTR-ToF) during an extensive laboratory characterization of wildfire emissions. Identifications for PTR-ToF ion masses are proposed and supported by a combination of techniques. Overall excellent agreement with other instrumentation is shown. Scalable emission factors and ratios are reported for many newly reported reactive species. An analysis of chemical characteristics is presented.
Vanessa Selimovic, Robert J. Yokelson, Carsten Warneke, James M. Roberts, Joost de Gouw, James Reardon, and David W. T. Griffith
Atmos. Chem. Phys., 18, 2929–2948, https://doi.org/10.5194/acp-18-2929-2018, https://doi.org/10.5194/acp-18-2929-2018, 2018
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We burned fuels representing western US wildfires in large-scale laboratory simulations to generate relevant emissions as confirmed by lab–field comparison. We report emission factors (EFs) for light scattering and absorption and BC along with SSA at 870 and 401 nm and AAE. We report EF for 22 trace gases that are major inorganic and organic emissions from flaming and smoldering. We report trace gas EF for species rarely (NH3) or not yet measured (e.g., HONO, acetic acid) for real US wildfires.
Jingqiu Mao, Annmarie Carlton, Ronald C. Cohen, William H. Brune, Steven S. Brown, Glenn M. Wolfe, Jose L. Jimenez, Havala O. T. Pye, Nga Lee Ng, Lu Xu, V. Faye McNeill, Kostas Tsigaridis, Brian C. McDonald, Carsten Warneke, Alex Guenther, Matthew J. Alvarado, Joost de Gouw, Loretta J. Mickley, Eric M. Leibensperger, Rohit Mathur, Christopher G. Nolte, Robert W. Portmann, Nadine Unger, Mika Tosca, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2615–2651, https://doi.org/10.5194/acp-18-2615-2018, https://doi.org/10.5194/acp-18-2615-2018, 2018
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This paper is aimed at discussing progress in evaluating, diagnosing, and improving air quality and climate modeling using comparisons to SAS observations as a guide to thinking about improvements to mechanisms and parameterizations in models.
Jingyi Li, Jingqiu Mao, Arlene M. Fiore, Ronald C. Cohen, John D. Crounse, Alex P. Teng, Paul O. Wennberg, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Jeff Peischl, Ilana B. Pollack, Thomas B. Ryerson, Patrick Veres, James M. Roberts, J. Andrew Neuman, John B. Nowak, Glenn M. Wolfe, Thomas F. Hanisco, Alan Fried, Hanwant B. Singh, Jack Dibb, Fabien Paulot, and Larry W. Horowitz
Atmos. Chem. Phys., 18, 2341–2361, https://doi.org/10.5194/acp-18-2341-2018, https://doi.org/10.5194/acp-18-2341-2018, 2018
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We present the first comprehensive model evaluation of summertime reactive oxidized nitrogen using a high-resolution chemistry–climate model with up-to-date isoprene oxidation chemistry, along with a series of observations from aircraft campaigns and ground measurement networks from 2004 to 2013 over the Southeast US. We investigate the impact of NOx emission reductions on changes in reactive nitrogen speciation and export efficiency as well as ozone in the past and future decade.
Catalina Tsai, Max Spolaor, Santo Fedele Colosimo, Olga Pikelnaya, Ross Cheung, Eric Williams, Jessica B. Gilman, Brian M. Lerner, Robert J. Zamora, Carsten Warneke, James M. Roberts, Ravan Ahmadov, Joost de Gouw, Timothy Bates, Patricia K. Quinn, and Jochen Stutz
Atmos. Chem. Phys., 18, 1977–1996, https://doi.org/10.5194/acp-18-1977-2018, https://doi.org/10.5194/acp-18-1977-2018, 2018
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Nitrous acid (HONO) photolysis is an important source of hydroxyl radicals (OH). Vertical HONO fluxes, observed in the snow-free, wintertime Uintah Basin, Utah, USA, show that chemical formation of HONO on the ground closes the HONO budget. Under high NOx conditions, HONO formation is most likely due to photo-enhanced conversion of NO2 on the ground. Under moderate to low NO2 conditions, photolysis of HNO3 on the ground seems to be the most likely source of HONO.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Hugh C. Pumphrey, Norbert Glatthor, Peter F. Bernath, Christopher D. Boone, James W. Hannigan, Ivan Ortega, Nathaniel J. Livesey, and William G. Read
Atmos. Chem. Phys., 18, 691–703, https://doi.org/10.5194/acp-18-691-2018, https://doi.org/10.5194/acp-18-691-2018, 2018
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The Microwave Limb Sounder (MLS) is a satellite instrument that has been measuring the amount of various gases in the atmosphere since 2004. In late 2015 and 2016 it observed unusual amounts of hydrogen cyanide (HCN), a gas produced when vegetation is burned. We compare the MLS observations to similar observations from other instruments. The excess HCN is shown to come from fires in Indonesia. There are more fires than usual in 2015–16 due to a drought caused by an El Niño event.
Daniel R. Moon, Giorgio S. Taverna, Clara Anduix-Canto, Trevor Ingham, Martyn P. Chipperfield, Paul W. Seakins, Maria-Teresa Baeza-Romero, and Dwayne E. Heard
Atmos. Chem. Phys., 18, 327–338, https://doi.org/10.5194/acp-18-327-2018, https://doi.org/10.5194/acp-18-327-2018, 2018
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One geoengineering mitigation strategy for global temperature rises is to inject particles into the stratosphere to scatter solar radiation back to space. However, the injection of such particles must not perturb ozone. We measured the rate of uptake of HO2 radicals, an important stratospheric intermediate, onto TiO2 particles. Using the atmospheric model TOMCAT, we showed that surface reactions between HO2 and TiO2 would have a negligible effect on stratospheric concentrations of HO2 and ozone.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Gerald E. Nedoluha, Michael Kiefer, Stefan Lossow, R. Michael Gomez, Niklaus Kämpfer, Martin Lainer, Peter Forkman, Ole Martin Christensen, Jung Jin Oh, Paul Hartogh, John Anderson, Klaus Bramstedt, Bianca M. Dinelli, Maya Garcia-Comas, Mark Hervig, Donal Murtagh, Piera Raspollini, William G. Read, Karen Rosenlof, Gabriele P. Stiller, and Kaley A. Walker
Atmos. Chem. Phys., 17, 14543–14558, https://doi.org/10.5194/acp-17-14543-2017, https://doi.org/10.5194/acp-17-14543-2017, 2017
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As part of the second SPARC (Stratosphere–troposphere Processes And their Role in Climate) water vapor assessment (WAVAS-II), we present measurements taken from or coincident with seven sites from which ground-based microwave instruments measure water vapor in the middle atmosphere. In the lower mesosphere, we quantify instrumental differences in the observed trends and annual variations at six sites. We then present a range of observed trends in water vapor over the past 20 years.
Robert C. Rhew, Malte Julian Deventer, Andrew A. Turnipseed, Carsten Warneke, John Ortega, Steve Shen, Luis Martinez, Abigail Koss, Brian M. Lerner, Jessica B. Gilman, James N. Smith, Alex B. Guenther, and Joost A. de Gouw
Atmos. Chem. Phys., 17, 13417–13438, https://doi.org/10.5194/acp-17-13417-2017, https://doi.org/10.5194/acp-17-13417-2017, 2017
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Alkenes emanate from both natural and anthropogenic sources and can contribute to atmospheric ozone production. This study measured
lightalkene (ethene, propene and butene) fluxes from a ponderosa pine forest using a novel relaxed eddy accumulation method, revealing much larger emissions than previously estimated and accounting for a significant fraction of OH reactivity. Emissions have a diurnal cycle related to sunlight and temperature, and the forest canopy appears to be the source.
Bianca C. Baier, William H. Brune, David O. Miller, Donald Blake, Russell Long, Armin Wisthaler, Christopher Cantrell, Alan Fried, Brian Heikes, Steven Brown, Erin McDuffie, Frank Flocke, Eric Apel, Lisa Kaser, and Andrew Weinheimer
Atmos. Chem. Phys., 17, 11273–11292, https://doi.org/10.5194/acp-17-11273-2017, https://doi.org/10.5194/acp-17-11273-2017, 2017
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Ozone production rates were measured using the Measurement of Ozone Production Sensor (MOPS). Measurements are compared to modeled ozone production rates using two different chemical mechanisms. At high nitric oxide levels, observed rates are higher than those modeled, prompting the need to revisit current model photochemistry. These direct measurements can add to our understanding of the ozone chemistry within air quality models and can be used to guide government regulatory strategies.
Martin P. Langowski, Christian von Savigny, John P. Burrows, Didier Fussen, Erin C. M. Dawkins, Wuhu Feng, John M. C. Plane, and Daniel R. Marsh
Atmos. Meas. Tech., 10, 2989–3006, https://doi.org/10.5194/amt-10-2989-2017, https://doi.org/10.5194/amt-10-2989-2017, 2017
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Meteoric metals form metal layers in the upper atmosphere anandplay a role in the formation of middle-atmospheric clouds and aerosols. However, the total metal influx rate is not well known. Global Na datasets from measurements and a model are available, which had not been compared yet on a global scale until this paper. Overall the agreement is good, and many differences between measurements are also found in the model simulations. However, the modeled layer altitude is too low.
Min Huang, Gregory R. Carmichael, James H. Crawford, Armin Wisthaler, Xiwu Zhan, Christopher R. Hain, Pius Lee, and Alex B. Guenther
Geosci. Model Dev., 10, 3085–3104, https://doi.org/10.5194/gmd-10-3085-2017, https://doi.org/10.5194/gmd-10-3085-2017, 2017
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Various sensitivity simulations during two airborne campaigns were performed to assess the impact of different initialization methods and model resolutions on NUWRF-modeled weather states, heat fluxes, and the follow-on MEGAN isoprene emission calculations. Proper land initialization is shown to be important to the coupled weather modeling and the follow-on emission modeling, which is also critical to accurately representing other processes in air quality modeling and data assimilation.
Sarah A. Monks, Stephen R. Arnold, Michael J. Hollaway, Richard J. Pope, Chris Wilson, Wuhu Feng, Kathryn M. Emmerson, Brian J. Kerridge, Barry L. Latter, Georgina M. Miles, Richard Siddans, and Martyn P. Chipperfield
Geosci. Model Dev., 10, 3025–3057, https://doi.org/10.5194/gmd-10-3025-2017, https://doi.org/10.5194/gmd-10-3025-2017, 2017
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The TOMCAT chemical transport model has been updated with the chemical degradation of ethene, propene, toluene, butane and monoterpenes. The tropospheric chemical mechanism is documented and the model is evaluated against surface, balloon, aircraft and satellite data. The model is generally able to capture the main spatial and seasonal features of carbon monoxide, ozone, volatile organic compounds and reactive nitrogen. However,
some model biases are found that require further investigation.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Ellen Eckert, Thomas von Clarmann, Alexandra Laeng, Gabriele P. Stiller, Bernd Funke, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Arne Babenhauserheide, Gerald Wetzel, Christopher Boone, Andreas Engel, Jeremy J. Harrison, Patrick E. Sheese, Kaley A. Walker, and Peter F. Bernath
Atmos. Meas. Tech., 10, 2727–2743, https://doi.org/10.5194/amt-10-2727-2017, https://doi.org/10.5194/amt-10-2727-2017, 2017
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We retrieved vertical profiles of CCl4 from MIPAS Envisat IMK/IAA data. A detailed description of all characteristics is included in the paper as well as comparisons with historical measurements and comparisons with collocated measurements of instruments covering the same time span as MIPAS Envisat. A particular focus also lies on the usage of a new CCl4 spectroscopic dataset introduced recently, which leads to more realistic CCl4 volume mixing ratios.
Shantanu H. Jathar, Christopher Heppding, Michael F. Link, Delphine K. Farmer, Ali Akherati, Michael J. Kleeman, Joost A. de Gouw, Patrick R. Veres, and James M. Roberts
Atmos. Chem. Phys., 17, 8959–8970, https://doi.org/10.5194/acp-17-8959-2017, https://doi.org/10.5194/acp-17-8959-2017, 2017
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Our work makes novel emissions measurements of isocyanic acid, a toxic gas, from a modern-day diesel engine and finds that diesel engines emit isocyanic acid but the emissions control devices do not enhance or destroy the isocyanic acid. Air quality model calculations suggest that diesel engines are possibly important sources of isocyanic acid in urban environments although the isocyanic acid levels are ten times lower than levels linked to adverse human health effects.
Wenshou Tian, Yuanpu Li, Fei Xie, Jiankai Zhang, Martyn P. Chipperfield, Wuhu Feng, Yongyun Hu, Sen Zhao, Xin Zhou, Yun Yang, and Xuan Ma
Atmos. Chem. Phys., 17, 6705–6722, https://doi.org/10.5194/acp-17-6705-2017, https://doi.org/10.5194/acp-17-6705-2017, 2017
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Although the principal mechanisms responsible for the formation of the Antarctic ozone hole are well understood, the factors or processes that generate interannual variations in ozone levels in the southern high-latitude stratosphere remain under debate. This study finds that the SST variations across the East Asian marginal seas (5° S–35° N, 100–140° E) could modulate the southern high-latitude stratospheric ozone interannual changes.
Shreeya Verma, Julia Marshall, Mark Parrington, Anna Agustí-Panareda, Sebastien Massart, Martyn P. Chipperfield, Christopher Wilson, and Christoph Gerbig
Atmos. Chem. Phys., 17, 6663–6678, https://doi.org/10.5194/acp-17-6663-2017, https://doi.org/10.5194/acp-17-6663-2017, 2017
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Aircraft profiles are a useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, these are available only up to about 9–13 km altitude and therefore need to be extended synthetically into the stratosphere using other sources. In this study, we analyse three different data sources that are available for extension of CH4 profiles by comparing the error introduced by each into the total column and provide recommendations regarding the best approach.
Hongyu Guo, Jiumeng Liu, Karl D. Froyd, James M. Roberts, Patrick R. Veres, Patrick L. Hayes, Jose L. Jimenez, Athanasios Nenes, and Rodney J. Weber
Atmos. Chem. Phys., 17, 5703–5719, https://doi.org/10.5194/acp-17-5703-2017, https://doi.org/10.5194/acp-17-5703-2017, 2017
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