Articles | Volume 20, issue 14
https://doi.org/10.5194/acp-20-8405-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-20-8405-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
17 Jul 2020
Research article |
| 17 Jul 2020
| 17 Jul 2020
Strong sensitivity of the isotopic composition of methane to the plausible range of tropospheric chlorine
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
James S. Wang
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
now at: Institute for Advanced Sustainability Studies,
Potsdam, Germany
Michael Manyin
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Science Systems and Applications Inc. (SSAI), Lanham, MD, USA
Bryan Duncan
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Ryan Hossaini
Lancaster Environment Centre, Lancaster University, Lancaster, UK
Christoph A. Keller
Universities Space Research Association, Columbia, MD, USA
NASA Goddard Space Flight Center, Greenbelt, MD, USA
Sylvia E. Michel
Institute of Arctic and Alpine Research, University of Colorado,
Boulder, Boulder, CO, USA
James W. C. White
Institute of Arctic and Alpine Research, University of Colorado,
Boulder, Boulder, CO, USA
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Sarah A. Strode, Junhua Liu, Leslie Lait, Róisín Commane, Bruce Daube, Steven Wofsy, Austin Conaty, Paul Newman, and Michael Prather
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Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
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Jerald R. Ziemke, Sarah A. Strode, Anne R. Douglass, Joanna Joiner, Alexander Vasilkov, Luke D. Oman, Junhua Liu, Susan E. Strahan, Pawan K. Bhartia, and David P. Haffner
Atmos. Meas. Tech., 10, 4067–4078, https://doi.org/10.5194/amt-10-4067-2017, https://doi.org/10.5194/amt-10-4067-2017, 2017
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We combine satellite measurements of ozone and cloud properties from the Aura OMI and MLS instruments for 2004–2016 to measure ozone in the mid–upper levels of deep convective clouds. Our results ascribe upward injection of low boundary layer ozone (varying from low to high amounts) as a major driver of the measured concentrations of ozone in thick clouds. Our OMI/MLS generated ozone product is made available to the public for use in science applications.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
Raquel A. Silva, J. Jason West, Jean-François Lamarque, Drew T. Shindell, William J. Collins, Stig Dalsoren, Greg Faluvegi, Gerd Folberth, Larry W. Horowitz, Tatsuya Nagashima, Vaishali Naik, Steven T. Rumbold, Kengo Sudo, Toshihiko Takemura, Daniel Bergmann, Philip Cameron-Smith, Irene Cionni, Ruth M. Doherty, Veronika Eyring, Beatrice Josse, Ian A. MacKenzie, David Plummer, Mattia Righi, David S. Stevenson, Sarah Strode, Sophie Szopa, and Guang Zengast
Atmos. Chem. Phys., 16, 9847–9862, https://doi.org/10.5194/acp-16-9847-2016, https://doi.org/10.5194/acp-16-9847-2016, 2016
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Using ozone and PM2.5 concentrations from the ACCMIP ensemble of chemistry-climate models for the four Representative Concentration Pathway scenarios (RCPs), together with projections of future population and baseline mortality rates, we quantify the human premature mortality impacts of future ambient air pollution in 2030, 2050 and 2100, relative to 2000 concentrations. We also estimate the global mortality burden of ozone and PM2.5 in 2000 and each future period.
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
S. A. Strode, B. N. Duncan, E. A. Yegorova, J. Kouatchou, J. R. Ziemke, and A. R. Douglass
Atmos. Chem. Phys., 15, 11789–11805, https://doi.org/10.5194/acp-15-11789-2015, https://doi.org/10.5194/acp-15-11789-2015, 2015
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A low bias in carbon monoxide (CO) at northern latitudes is a common feature of chemistry climate models. We find that increasing Northern Hemisphere (NH) CO emissions or reducing NH OH concentrations improves the agreement with CO surface observations, but reducing NH OH leads to a better comparison with MOPITT. Removing model biases in ozone and water vapor increases the simulated methane lifetime, but it does not give the 20% reduction in NH OH suggested by our analysis of the CO bias.
J. L. Schnell, M. J. Prather, B. Josse, V. Naik, L. W. Horowitz, P. Cameron-Smith, D. Bergmann, G. Zeng, D. A. Plummer, K. Sudo, T. Nagashima, D. T. Shindell, G. Faluvegi, and S. A. Strode
Atmos. Chem. Phys., 15, 10581–10596, https://doi.org/10.5194/acp-15-10581-2015, https://doi.org/10.5194/acp-15-10581-2015, 2015
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We test global chemistry--climate models in their ability to simulate present-day surface ozone. Models are tested against observed hourly ozone from 4217 stations in North America and Europe that are averaged over 1°x1° grid cells. Using novel metrics, we find most models match the shape but not the amplitude of regional summertime diurnal and annual cycles and match the pattern but not the magnitude of summer ozone enhancement. Most also match the observed distribution of extreme episode sizes
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
M. Chin, T. Diehl, Q. Tan, J. M. Prospero, R. A. Kahn, L. A. Remer, H. Yu, A. M. Sayer, H. Bian, I. V. Geogdzhayev, B. N. Holben, S. G. Howell, B. J. Huebert, N. C. Hsu, D. Kim, T. L. Kucsera, R. C. Levy, M. I. Mishchenko, X. Pan, P. K. Quinn, G. L. Schuster, D. G. Streets, S. A. Strode, O. Torres, and X.-P. Zhao
Atmos. Chem. Phys., 14, 3657–3690, https://doi.org/10.5194/acp-14-3657-2014, https://doi.org/10.5194/acp-14-3657-2014, 2014
J.-F. Lamarque, F. Dentener, J. McConnell, C.-U. Ro, M. Shaw, R. Vet, D. Bergmann, P. Cameron-Smith, S. Dalsoren, R. Doherty, G. Faluvegi, S. J. Ghan, B. Josse, Y. H. Lee, I. A. MacKenzie, D. Plummer, D. T. Shindell, R. B. Skeie, D. S. Stevenson, S. Strode, G. Zeng, M. Curran, D. Dahl-Jensen, S. Das, D. Fritzsche, and M. Nolan
Atmos. Chem. Phys., 13, 7997–8018, https://doi.org/10.5194/acp-13-7997-2013, https://doi.org/10.5194/acp-13-7997-2013, 2013
V. Naik, A. Voulgarakis, A. M. Fiore, L. W. Horowitz, J.-F. Lamarque, M. Lin, M. J. Prather, P. J. Young, D. Bergmann, P. J. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, T. P. C. van Noije, D. A. Plummer, M. Righi, S. T. Rumbold, R. Skeie, D. T. Shindell, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, https://doi.org/10.5194/acp-13-5277-2013, 2013
K. W. Bowman, D. T. Shindell, H. M. Worden, J.F. Lamarque, P. J. Young, D. S. Stevenson, Z. Qu, M. de la Torre, D. Bergmann, P. J. Cameron-Smith, W. J. Collins, R. Doherty, S. B. Dalsøren, G. Faluvegi, G. Folberth, L. W. Horowitz, B. M. Josse, Y. H. Lee, I. A. MacKenzie, G. Myhre, T. Nagashima, V. Naik, D. A. Plummer, S. T. Rumbold, R. B. Skeie, S. A. Strode, K. Sudo, S. Szopa, A. Voulgarakis, G. Zeng, S. S. Kulawik, A. M. Aghedo, and J. R. Worden
Atmos. Chem. Phys., 13, 4057–4072, https://doi.org/10.5194/acp-13-4057-2013, https://doi.org/10.5194/acp-13-4057-2013, 2013
D. S. Stevenson, P. J. Young, V. Naik, J.-F. Lamarque, D. T. Shindell, A. Voulgarakis, R. B. Skeie, S. B. Dalsoren, G. Myhre, T. K. Berntsen, G. A. Folberth, S. T. Rumbold, W. J. Collins, I. A. MacKenzie, R. M. Doherty, G. Zeng, T. P. C. van Noije, A. Strunk, D. Bergmann, P. Cameron-Smith, D. A. Plummer, S. A. Strode, L. Horowitz, Y. H. Lee, S. Szopa, K. Sudo, T. Nagashima, B. Josse, I. Cionni, M. Righi, V. Eyring, A. Conley, K. W. Bowman, O. Wild, and A. Archibald
Atmos. Chem. Phys., 13, 3063–3085, https://doi.org/10.5194/acp-13-3063-2013, https://doi.org/10.5194/acp-13-3063-2013, 2013
A. Voulgarakis, V. Naik, J.-F. Lamarque, D. T. Shindell, P. J. Young, M. J. Prather, O. Wild, R. D. Field, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, L. W. Horowitz, B. Josse, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, D. S. Stevenson, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2563–2587, https://doi.org/10.5194/acp-13-2563-2013, https://doi.org/10.5194/acp-13-2563-2013, 2013
P. J. Young, A. T. Archibald, K. W. Bowman, J.-F. Lamarque, V. Naik, D. S. Stevenson, S. Tilmes, A. Voulgarakis, O. Wild, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, L. W. Horowitz, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, R. B. Skeie, D. T. Shindell, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, https://doi.org/10.5194/acp-13-2063-2013, 2013
J.-F. Lamarque, D. T. Shindell, B. Josse, P. J. Young, I. Cionni, V. Eyring, D. Bergmann, P. Cameron-Smith, W. J. Collins, R. Doherty, S. Dalsoren, G. Faluvegi, G. Folberth, S. J. Ghan, L. W. Horowitz, Y. H. Lee, I. A. MacKenzie, T. Nagashima, V. Naik, D. Plummer, M. Righi, S. T. Rumbold, M. Schulz, R. B. Skeie, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, A. Voulgarakis, and G. Zeng
Geosci. Model Dev., 6, 179–206, https://doi.org/10.5194/gmd-6-179-2013, https://doi.org/10.5194/gmd-6-179-2013, 2013
Pinchas Nürnberg, Sarah A. Strode, and Ralf Sussmann
Atmos. Chem. Phys., 24, 10001–10012, https://doi.org/10.5194/acp-24-10001-2024, https://doi.org/10.5194/acp-24-10001-2024, 2024
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We created a set of scaling factors describing the diurnal increase in stratospheric nitrogen oxides above Zugspitze, Germany. We used these factors to validate recently published model simulation data. On the one hand, this validation enables the use of the validated data to better understand the stratospheric photochemistry. On the other hand, it can improve satellite validation, which has implications for the understanding of urban smog events and other pollution events in the troposphere.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
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We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Bryan Duncan, Daniel Anderson, Arlene Fiore, Joanna Joiner, Nickolay Krotkov, Can Li, Dylan Millet, Julie Nicely, Luke Oman, Jason St. Clair, Joshua Shutter, Amir Souri, Sarah Strode, Brad Weir, Glenn Wolfe, Helen Worden, and Qindan Zhu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2331, https://doi.org/10.5194/egusphere-2024-2331, 2024
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Trace gases emitted to or formed within the atmosphere may be chemically or physically removed from the atmosphere. One trace gas, the hydroxyl radical (OH), is responsible for initiating the chemical removal of many trace gases, including some climate gases. Despite its importance, scientists have not been able to adequately measure OH. In this opinion piece, we discuss promising new methods to indirectly constrain OH using satellite data of trace gases that control the abundance of OH.
Amir H. Souri, Gonzalo González Abad, Glenn M. Wolfe, Tijl Verhoelst, Corinne Vigouroux, Gaia Pinardi, Steven Compernolle, Bavo Langerock, Bryan N. Duncan, and Matthew S. Johnson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1947, https://doi.org/10.5194/egusphere-2024-1947, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We establish a simple yet robust relationship between ozone production rates and several geophysical parameters obtained from several intensive atmospheric composition campaigns. We have shown that satellite remote sensing data can effectively constrain these parameters, enabling us to produce the first global maps of ozone production rates with unprecedented resolution.
Hongyu Liu, Bo Zhang, Richard H. Moore, Luke D. Ziemba, Richard A. Ferrare, Hyundeok Choi, Armin Sorooshian, David Painemal, Hailong Wang, Michael A. Shook, Amy Jo Scarino, Johnathan W. Hair, Ewan C. Crosbie, Marta A. Fenn, Taylor J. Shingler, Chris A. Hostetler, Gao Chen, Mary M. Kleb, Gan Luo, Fangqun Yu, Jason L. Tackett, Mark A. Vaughan, Yongxiang Hu, Glenn S. Diskin, John B. Nowak, Joshua P. DiGangi, Yonghoon Choi, Christoph A. Keller, and Matthew S. Johnson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1127, https://doi.org/10.5194/egusphere-2024-1127, 2024
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We use the GEOS-Chem model to simulate aerosols over the western North Atlantic Ocean (WNAO) during the winter and summer campaigns of ACTIVATE 2020. Model results are evaluated against in situ and remote sensing measurements from two aircraft as well as ground-based and satellite observations. The improved understanding of the aerosol life cycle, composition, transport pathways, and distribution has important implications for characterizing aerosol-cloud-meteorology interactions over the WNAO.
Yasin Elshorbany, Jerald Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca Buchholz, Benjamin Gaubert, Néstor Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
EGUsphere, https://doi.org/10.5194/egusphere-2024-720, https://doi.org/10.5194/egusphere-2024-720, 2024
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We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the Tropospheric Column of Ozone and its precursors, nitrogen dioxide, formaldehyde, and total column of CO as well as ozonesonde data and model simulations.
Lily Gouldsbrough, Ryan Hossaini, Emma Eastoe, Paul J. Young, and Massimo Vieno
Atmos. Chem. Phys., 24, 3163–3196, https://doi.org/10.5194/acp-24-3163-2024, https://doi.org/10.5194/acp-24-3163-2024, 2024
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High-resolution spatial fields of surface ozone are used to understand spikes in ozone concentration and predict their impact on public health. Such fields are routinely output from complex mathematical models for atmospheric conditions. These outputs are on a coarse spatial resolution and the highest concentrations tend to be biased. Using a novel data-driven machine learning methodology, we show how such output can be corrected to produce fields with both lower bias and higher resolution.
Ryan Hossaini, David Sherry, Zihao Wang, Martyn Chipperfield, Wuhu Feng, David Oram, Karina Adcock, Stephen Montzka, Isobel Simpson, Andrea Mazzeo, Amber Leeson, Elliot Atlas, and Charles C.-K. Chou
EGUsphere, https://doi.org/10.5194/egusphere-2024-560, https://doi.org/10.5194/egusphere-2024-560, 2024
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Ethylene dichloride (EDC) is an industrial chemical used to produce polyvinyl chloride (PVC). We analysed EDC production data to estimate global EDC emissions (2002 to 2020). The emissions were included in an atmospheric model and evaluated by comparing simulated EDC to EDC measurements in the troposphere. We show EDC contributes ozone-depleting chlorine to the stratosphere and this has increased with increasing EDC emissions. EDC’s impact on stratospheric ozone is currently small, but non-zero.
Douglas E. J. Worthy, Michele K. Rauh, Lin Huang, Felix R. Vogel, Alina Chivulescu, Kenneth A. Masarie, Ray L. Langenfelds, Paul B. Krummel, Colin E. Allison, Andrew M. Crotwell, Monica Madronich, Gabrielle Pétron, Ingeborg Levin, Samuel Hammer, Sylvia Michel, Michel Ramonet, Martina Schmidt, Armin Jordan, Heiko Moossen, Michael Rothe, Ralph Keeling, and Eric J. Morgan
Atmos. Meas. Tech., 16, 5909–5935, https://doi.org/10.5194/amt-16-5909-2023, https://doi.org/10.5194/amt-16-5909-2023, 2023
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Network compatibility is important for inferring greenhouse gas fluxes at global or regional scales. This study is the first assessment of the measurement agreement among seven individual programs within the World Meteorological Organization community. It compares co-located flask air measurements at the Alert Observatory in Canada over a 17-year period. The results provide stronger confidence in the uncertainty estimation while using those datasets in various data interpretation applications.
Jinsol Kim, John B. Miller, Charles E. Miller, Scott J. Lehman, Sylvia E. Michel, Vineet Yadav, Nick E. Rollins, and William M. Berelson
Atmos. Chem. Phys., 23, 14425–14436, https://doi.org/10.5194/acp-23-14425-2023, https://doi.org/10.5194/acp-23-14425-2023, 2023
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In this study, we present the partitioning of CO2 signals from biogenic, petroleum and natural gas sources by combining CO, 13CO2 and 14CO2 measurements. Using measurements from flask air samples at three sites in the greater Los Angeles region, we find larger and positive contributions of biogenic signals in winter and smaller and negative contributions in summer. The largest contribution of natural gas combustion generally occurs in summer.
Ewa M. Bednarz, Ryan Hossaini, and Martyn P. Chipperfield
Atmos. Chem. Phys., 23, 13701–13711, https://doi.org/10.5194/acp-23-13701-2023, https://doi.org/10.5194/acp-23-13701-2023, 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-VSLSs) on stratospheric ozone using a state-of-the-art chemistry-climate model. We demonstrate that Cl-VSLSs already have a non-negligible impact on stratospheric ozone, including a local reduction of up to ~7 DU in Arctic 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.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
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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 thus aid studies in support of future ozone assessment reports.
Alice Drinkwater, Paul I. Palmer, Liang Feng, Tim Arnold, Xin Lan, Sylvia E. Michel, Robert Parker, and Hartmut Boesch
Atmos. Chem. Phys., 23, 8429–8452, https://doi.org/10.5194/acp-23-8429-2023, https://doi.org/10.5194/acp-23-8429-2023, 2023
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Changes in atmospheric methane over the last few decades are largely unexplained. Previous studies have proposed different hypotheses to explain short-term changes in atmospheric methane. We interpret observed changes in atmospheric methane and stable isotope source signatures (2004–2020). We argue that changes over this period are part of a large-scale shift from high-northern-latitude thermogenic energy emissions to tropical biogenic emissions, particularly from North Africa and South America.
Daniel C. Anderson, Bryan N. Duncan, Julie M. Nicely, Junhua Liu, Sarah A. Strode, and Melanie B. Follette-Cook
Atmos. Chem. Phys., 23, 6319–6338, https://doi.org/10.5194/acp-23-6319-2023, https://doi.org/10.5194/acp-23-6319-2023, 2023
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We describe a methodology that combines machine learning, satellite observations, and 3D chemical model output to infer the abundance of the hydroxyl radical (OH), a chemical that removes many trace gases from the atmosphere. The methodology successfully captures the variability of observed OH, although further observations are needed to evaluate absolute accuracy. Current satellite observations are of sufficient quality to infer OH, but retrieval validation in the remote tropics is needed.
Viral Shah, Daniel J. Jacob, Ruijun Dang, Lok N. Lamsal, Sarah A. Strode, Stephen D. Steenrod, K. Folkert Boersma, Sebastian D. Eastham, Thibaud M. Fritz, Chelsea Thompson, Jeff Peischl, Ilann Bourgeois, Ilana B. Pollack, Benjamin A. Nault, Ronald C. Cohen, Pedro Campuzano-Jost, Jose L. Jimenez, Simone T. Andersen, Lucy J. Carpenter, Tomás Sherwen, and Mat J. Evans
Atmos. Chem. Phys., 23, 1227–1257, https://doi.org/10.5194/acp-23-1227-2023, https://doi.org/10.5194/acp-23-1227-2023, 2023
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NOx in the free troposphere (above 2 km) affects global tropospheric chemistry and the retrieval and interpretation of satellite NO2 measurements. We evaluate free tropospheric NOx in global atmospheric chemistry models and find that recycling NOx from its reservoirs over the oceans is faster than that simulated in the models, resulting in increases in simulated tropospheric ozone and OH. Over the U.S., free tropospheric NO2 contributes the majority of the tropospheric NO2 column in summer.
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.
Sourish Basu, Xin Lan, Edward Dlugokencky, Sylvia Michel, Stefan Schwietzke, John B. Miller, Lori Bruhwiler, Youmi Oh, Pieter P. Tans, Francesco Apadula, Luciana V. Gatti, Armin Jordan, Jaroslaw Necki, Motoki Sasakawa, Shinji Morimoto, Tatiana Di Iorio, Haeyoung Lee, Jgor Arduini, and Giovanni Manca
Atmos. Chem. Phys., 22, 15351–15377, https://doi.org/10.5194/acp-22-15351-2022, https://doi.org/10.5194/acp-22-15351-2022, 2022
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Atmospheric methane (CH4) has been growing steadily since 2007 for reasons that are not well understood. Here we determine sources of methane using a technique informed by atmospheric measurements of CH4 and its isotopologue 13CH4. Measurements of 13CH4 provide for better separation of microbial, fossil, and fire sources of methane than CH4 measurements alone. Compared to previous assessments such as the Global Carbon Project, we find a larger microbial contribution to the post-2007 increase.
Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 15, 8731–8748, https://doi.org/10.5194/gmd-15-8731-2022, https://doi.org/10.5194/gmd-15-8731-2022, 2022
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Atmospheric chemistry models must be able to operate both online as components of Earth system models and offline as standalone models. The widely used GEOS-Chem model operates both online and offline, but the classic offline version is not suitable for massively parallel simulations. We describe a new generation of the offline high-performance GEOS-Chem (GCHP) that enables high-resolution simulations on thousands of cores, including on the cloud, with improved access, performance, and accuracy.
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.
Sarah A. Strode, Ghassan Taha, Luke D. Oman, Robert Damadeo, David Flittner, Mark Schoeberl, Christopher E. Sioris, and Ryan Stauffer
Atmos. Meas. Tech., 15, 6145–6161, https://doi.org/10.5194/amt-15-6145-2022, https://doi.org/10.5194/amt-15-6145-2022, 2022
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We use a global atmospheric chemistry model simulation to generate scaling factors that account for the daily cycle of NO2 and ozone. These factors facilitate comparisons between sunrise and sunset observations from SAGE III/ISS and observations from other instruments. We provide the scaling factors as monthly zonal means for different latitudes and altitudes. We find that applying these factors yields more consistent comparisons between observations from SAGE III/ISS and other instruments.
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.
Daniel C. Anderson, Melanie B. Follette-Cook, Sarah A. Strode, Julie M. Nicely, Junhua Liu, Peter D. Ivatt, and Bryan N. Duncan
Geosci. Model Dev., 15, 6341–6358, https://doi.org/10.5194/gmd-15-6341-2022, https://doi.org/10.5194/gmd-15-6341-2022, 2022
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The hydroxyl radical (OH) is the most important chemical in the atmosphere for removing certain pollutants, including methane, the second-most-important greenhouse gas. We present a methodology to create an easily modifiable parameterization that can calculate OH concentrations in a computationally efficient way. The parameterization, which predicts OH within 5 %, can be integrated into larger climate models to allow for calculation of the interactions between OH, methane, and other chemicals.
Joël Thanwerdas, Marielle Saunois, Antoine Berchet, Isabelle Pison, Bruce H. Vaughn, Sylvia Englund Michel, and Philippe Bousquet
Geosci. Model Dev., 15, 4831–4851, https://doi.org/10.5194/gmd-15-4831-2022, https://doi.org/10.5194/gmd-15-4831-2022, 2022
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Estimating CH4 sources by exploiting observations within an inverse modeling framework is a powerful approach. Here, a new system designed to assimilate δ13C(CH4) observations together with CH4 observations is presented. By optimizing both the emissions and associated source signatures of multiple emission categories, this new system can efficiently differentiate the co-located emission categories and provide estimates of CH4 sources that are consistent with isotopic data.
Eric Saboya, Giulia Zazzeri, Heather Graven, Alistair J. Manning, and Sylvia Englund Michel
Atmos. Chem. Phys., 22, 3595–3613, https://doi.org/10.5194/acp-22-3595-2022, https://doi.org/10.5194/acp-22-3595-2022, 2022
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Continuous measurements of atmospheric methane concentrations and its carbon-13 isotope have been made in central London since early 2018. These measurements were used to evaluate methane emissions reported in global and UK-specific emission inventories for the London area. Compared to atmospheric methane measurements from March 2018 to October 2020, both inventories are under-reporting natural gas leakage for the London area.
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.
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.
Vilma Kangasaho, Aki Tsuruta, Leif Backman, Pyry Mäkinen, Sander Houweling, Arjo Segers, Maarten Krol, Ed Dlugokencky, Sylvia Michel, James White, and Tuula Aalto
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-843, https://doi.org/10.5194/acp-2021-843, 2021
Revised manuscript not accepted
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Understanding the composition of carbon isotopes can help to better understand the changes in methane budgets. This study investigates how methane sources affect the seasonal cycle of the methane carbon-13 isotope during 2000–2012 using an atmospheric transport model. We found that emissions from both anthropogenic and natural sources contribute. The findings raise a need to revise the magnitudes, proportion, and seasonal cycles of anthropogenic sources and northern wetland emissions.
Abigail G. Hughes, Sonja Wahl, Tyler R. Jones, Alexandra Zuhr, Maria Hörhold, James W. C. White, and Hans Christian Steen-Larsen
The Cryosphere, 15, 4949–4974, https://doi.org/10.5194/tc-15-4949-2021, https://doi.org/10.5194/tc-15-4949-2021, 2021
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Water isotope records in Greenland and Antarctic ice cores are a valuable proxy for paleoclimate reconstruction and are traditionally thought to primarily reflect precipitation input. However,
post-depositional processes are hypothesized to contribute to the isotope climate signal. In this study we use laboratory experiments, field experiments, and modeling to show that sublimation and vapor–snow isotope exchange can rapidly influence the isotopic composition of the snowpack.
Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
Geosci. Model Dev., 14, 5977–5997, https://doi.org/10.5194/gmd-14-5977-2021, https://doi.org/10.5194/gmd-14-5977-2021, 2021
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Atmospheric chemistry models like GEOS-Chem are versatile tools widely used in air pollution and climate studies. The simulations used in such studies can be very computationally demanding, and thus it is useful if the model can simulate a specific geographic region at a higher resolution than the rest of the globe. Here, we implement, test, and demonstrate a new variable-resolution capability in GEOS-Chem that is suitable for simulations conducted on supercomputers.
Huisheng Bian, Eunjee Lee, Randal D. Koster, Donifan Barahona, Mian Chin, Peter R. Colarco, Anton Darmenov, Sarith Mahanama, Michael Manyin, Peter Norris, John Shilling, Hongbin Yu, and Fanwei Zeng
Atmos. Chem. Phys., 21, 14177–14197, https://doi.org/10.5194/acp-21-14177-2021, https://doi.org/10.5194/acp-21-14177-2021, 2021
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The study using the NASA Earth system model shows ~2.6 % increase in burning season gross primary production and ~1.5 % increase in annual net primary production across the Amazon Basin during 2010–2016 due to the change in surface downward direct and diffuse photosynthetically active radiation by biomass burning aerosols. Such an aerosol effect is strongly dependent on the presence of clouds. The cloud fraction at which aerosols switch from stimulating to inhibiting plant growth occurs at ~0.8.
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.
Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Emissions are a central component of atmospheric chemistry models. The Harmonized Emissions Component (HEMCO) is a software component for computing emissions from a user-selected ensemble of emission inventories and algorithms. It allows users to select, add, and scale emissions from different sources through a configuration file with no change to the model source code. We demonstrate the implementation of HEMCO in several models, all sharing the same HEMCO core code and database library.
Daniel C. Anderson, Bryan N. Duncan, Arlene M. Fiore, Colleen B. Baublitz, Melanie B. Follette-Cook, Julie M. Nicely, and Glenn M. Wolfe
Atmos. Chem. Phys., 21, 6481–6508, https://doi.org/10.5194/acp-21-6481-2021, https://doi.org/10.5194/acp-21-6481-2021, 2021
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We demonstrate that large-scale climate features are the primary driver of year-to-year variability in simulated values of the hydroxyl radical, the primary atmospheric oxidant, over 1980–2018. The El Niño–Southern Oscillation is the dominant mode of hydroxyl variability, resulting in large-scale global decreases in OH during El Niño events. Other climate modes, such as the Australian monsoon and the North Atlantic Oscillation, have impacts of similar magnitude but on on more localized scales.
Christoph A. Keller, Mathew J. Evans, K. Emma Knowland, Christa A. Hasenkopf, Sruti Modekurty, Robert A. Lucchesi, Tomohiro Oda, Bruno B. Franca, Felipe C. Mandarino, M. Valeria Díaz Suárez, Robert G. Ryan, Luke H. Fakes, and Steven Pawson
Atmos. Chem. Phys., 21, 3555–3592, https://doi.org/10.5194/acp-21-3555-2021, https://doi.org/10.5194/acp-21-3555-2021, 2021
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This study combines surface observations and model simulations to quantify the impact of COVID-19 restrictions on air quality across the world. The presented methodology removes the confounding impacts of meteorology on air pollution. Our results indicate that surface concentrations of nitrogen dioxide, an important air pollutant emitted during the combustion of fossil fuels, declined by up to 60 % following the implementation of COVID-19 containment measures.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 20, 13011–13022, https://doi.org/10.5194/acp-20-13011-2020, https://doi.org/10.5194/acp-20-13011-2020, 2020
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Decadal trends and variations in OH are critical for understanding atmospheric CH4 evolution. We quantify the impacts of OH trends and variations on the CH4 budget by conducting CH4 inversions on a decadal scale with an ensemble of OH fields. We find the negative OH anomalies due to enhanced fires can reduce the optimized CH4 emissions by up to 10 Tg yr−1 during El Niño years and the positive OH trend from 1986 to 2010 results in a ∼ 23 Tg yr−1 additional increase in optimized CH4 emissions.
Abigail G. Hughes, Tyler R. Jones, Bo M. Vinther, Vasileios Gkinis, C. Max Stevens, Valerie Morris, Bruce H. Vaughn, Christian Holme, Bradley R. Markle, and James W. C. White
Clim. Past, 16, 1369–1386, https://doi.org/10.5194/cp-16-1369-2020, https://doi.org/10.5194/cp-16-1369-2020, 2020
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An ice core drilled on the Renland ice cap (RECAP) in east-central Greenland contains a continuous climate record dating through the last glacial period. Here we present the water isotope record for the Holocene, in which high-resolution climate information is retained for the last 8 kyr. We find that the RECAP water isotope record exhibits seasonal and decadal variability which may reflect sea surface conditions and regional climate variability.
Dipayan Paul, Hubertus A. Scheeren, Henk G. Jansen, Bert A. M. Kers, John B. Miller, Andrew M. Crotwell, Sylvia E. Michel, Luciana V. Gatti, Lucas G. Domingues, Caio S. C. Correia, Raiane A. L. Neves, Harro A. J. Meijer, and Wouter Peters
Atmos. Meas. Tech., 13, 4051–4064, https://doi.org/10.5194/amt-13-4051-2020, https://doi.org/10.5194/amt-13-4051-2020, 2020
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For reliable measurements of CO2 mole fractions and its stable isotope composition in air samples, one needs to carefully dry them during collection. Here we describe evaluation of a portable, consumable-free and power-free Nafion-based drying system that is currently being used for sample collection over the Amazon. Laboratory tests indicate that this Nafion-based system does not influence the mole fraction measurements of CH4, CO, N2O, SF6, and CO2 and the stable isotope composition of CO2.
Haipeng Lin, Xu Feng, Tzung-May Fu, Heng Tian, Yaping Ma, Lijuan Zhang, Daniel J. Jacob, Robert M. Yantosca, Melissa P. Sulprizio, Elizabeth W. Lundgren, Jiawei Zhuang, Qiang Zhang, Xiao Lu, Lin Zhang, Lu Shen, Jianping Guo, Sebastian D. Eastham, and Christoph A. Keller
Geosci. Model Dev., 13, 3241–3265, https://doi.org/10.5194/gmd-13-3241-2020, https://doi.org/10.5194/gmd-13-3241-2020, 2020
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Online coupling of meteorology and chemistry models often presents maintenance issues with hard-wired coding. We present WRF-GC, an one-way online coupling of the WRF meteorological model and GEOS-Chem atmospheric chemistry model for regional atmospheric chemistry and air quality modeling. Our coupling structure allows future versions of either parent model to be immediately integrated into WRF-GC. The WRF-GC model was able to well reproduce regional PM2.5 with greater computational efficiency.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Julie M. Nicely, Bryan N. Duncan, Thomas F. Hanisco, Glenn M. Wolfe, Ross J. Salawitch, Makoto Deushi, Amund S. Haslerud, Patrick Jöckel, Béatrice Josse, Douglas E. Kinnison, Andrew Klekociuk, Michael E. Manyin, Virginie Marécal, Olaf Morgenstern, Lee T. Murray, Gunnar Myhre, Luke D. Oman, Giovanni Pitari, Andrea Pozzer, Ilaria Quaglia, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Kane Stone, Susan Strahan, Simone Tilmes, Holger Tost, Daniel M. Westervelt, and Guang Zeng
Atmos. Chem. Phys., 20, 1341–1361, https://doi.org/10.5194/acp-20-1341-2020, https://doi.org/10.5194/acp-20-1341-2020, 2020
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Differences in methane lifetime among global models are large and poorly understood. We use a neural network method and simulations from the Chemistry Climate Model Initiative to quantify the factors influencing methane lifetime spread among models and variations over time. UV photolysis, tropospheric ozone, and nitrogen oxides drive large model differences, while the same factors plus specific humidity contribute to a decreasing trend in methane lifetime between 1980 and 2015.
Le Kuai, Kevin W. Bowman, Kazuyuki Miyazaki, Makoto Deushi, Laura Revell, Eugene Rozanov, Fabien Paulot, Sarah Strode, Andrew Conley, Jean-François Lamarque, Patrick Jöckel, David A. Plummer, Luke D. Oman, Helen Worden, Susan Kulawik, David Paynter, Andrea Stenke, and Markus Kunze
Atmos. Chem. Phys., 20, 281–301, https://doi.org/10.5194/acp-20-281-2020, https://doi.org/10.5194/acp-20-281-2020, 2020
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The tropospheric ozone increase from pre-industrial to the present day leads to a radiative forcing. The top-of-atmosphere outgoing fluxes at the ozone band are controlled by ozone, water vapor, and temperature. We demonstrate a method to attribute the models’ flux biases to these key players using satellite-constrained instantaneous radiative kernels. The largest spread between models is found in the tropics, mainly driven by ozone and then water vapor.
Fei Liu, Bryan N. Duncan, Nickolay A. Krotkov, Lok N. Lamsal, Steffen Beirle, Debora Griffin, Chris A. McLinden, Daniel L. Goldberg, and Zifeng Lu
Atmos. Chem. Phys., 20, 99–116, https://doi.org/10.5194/acp-20-99-2020, https://doi.org/10.5194/acp-20-99-2020, 2020
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We present a novel method to infer CO2 emissions from individual power plants, based on satellite observations of co-emitted NO2. We find that the CO2 emissions estimated by our satellite-based method during 2005–2017 are in reasonable agreement with the CEMS measurements for US power plants. The broader implication of our methodology is that it has the potential to provide an additional constraint on CO2 emissions from power plants in regions of the world without reliable emissions accounting.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
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The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
Paul I. Palmer, Emily L. Wilson, Geronimo L. Villanueva, Giuliano Liuzzi, Liang Feng, Anthony J. DiGregorio, Jianping Mao, Lesley Ott, and Bryan Duncan
Atmos. Meas. Tech., 12, 2579–2594, https://doi.org/10.5194/amt-12-2579-2019, https://doi.org/10.5194/amt-12-2579-2019, 2019
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We describe the potential impact of a new, low-cost, portable ground instrument (the mini-LHR) that measures methane and carbon dioxide in the atmospheric column. This region is key in quantifying the global carbon budget but has geographical gaps in measurements left by ground-based networks and space-based observations. A deployment of 50 mini-LHRs would add new data products in the Amazon, the Arctic, and southern Asia and significantly improve knowledge of regional and global carbon budgets.
Meghana Velegar, N. Benjamin Erichson, Christoph A. Keller, and J. Nathan Kutz
Geosci. Model Dev., 12, 1525–1539, https://doi.org/10.5194/gmd-12-1525-2019, https://doi.org/10.5194/gmd-12-1525-2019, 2019
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We introduce a new set of algorithmic tools capable of producing scalable, low-rank decompositions of global spatiotemporal atmospheric chemistry data. By exploiting emerging randomized linear algebra algorithms, a suite of decompositions are proposed that efficiently extract the dominant features from global atmospheric chemistry at longitude, latitude, and elevation with improved interpretability. The algorithms provide a strategy for the global monitoring of atmospheric chemistry.
Christoph A. Keller and Mat J. Evans
Geosci. Model Dev., 12, 1209–1225, https://doi.org/10.5194/gmd-12-1209-2019, https://doi.org/10.5194/gmd-12-1209-2019, 2019
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Computer simulations of atmospheric chemistry are a central tool to study the impact of air pollutants on the environment. These models are highly complex and require a lot of computing resources. In this study we show that machine learning can be used to predict air pollution with an accuracy that is comparable to the traditional, computationally expensive method. Such a machine-learning-based model has the potential to be orders of magnitude faster.
Jerry R. Ziemke, Luke D. Oman, Sarah A. Strode, Anne R. Douglass, Mark A. Olsen, Richard D. McPeters, Pawan K. Bhartia, Lucien Froidevaux, Gordon J. Labow, Jacquie C. Witte, Anne M. Thompson, David P. Haffner, Natalya A. Kramarova, Stacey M. Frith, Liang-Kang Huang, Glen R. Jaross, Colin J. Seftor, Mathew T. Deland, and Steven L. Taylor
Atmos. Chem. Phys., 19, 3257–3269, https://doi.org/10.5194/acp-19-3257-2019, https://doi.org/10.5194/acp-19-3257-2019, 2019
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Both a 38-year merged satellite record of tropospheric ozone from TOMS/OMI/MLS/OMPS and a MERRA-2 GMI model simulation show large increases of 6–7 Dobson units from the Near East to India–East Asia and eastward over the Pacific. These increases in tropospheric ozone are attributed to increases in pollution over the region over the last several decades. Secondary 38-year increases of 4–5 Dobson units with both GMI model and satellite measurements occur over central African–tropical Atlantic.
Kai-Lan Chang, Owen R. Cooper, J. Jason West, Marc L. Serre, Martin G. Schultz, Meiyun Lin, Virginie Marécal, Béatrice Josse, Makoto Deushi, Kengo Sudo, Junhua Liu, and Christoph A. Keller
Geosci. Model Dev., 12, 955–978, https://doi.org/10.5194/gmd-12-955-2019, https://doi.org/10.5194/gmd-12-955-2019, 2019
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We developed a new method for combining surface ozone observations from thousands of monitoring sites worldwide with the output from multiple atmospheric chemistry models. The result is a global surface ozone distribution with greater accuracy than any single model can achieve. We focused on an ozone metric relevant to human mortality caused by long-term ozone exposure. Our method can be applied to studies that quantify the impacts of ozone on human health and mortality.
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).
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
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Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Lu Hu, Christoph A. Keller, Michael S. Long, Tomás Sherwen, Benjamin Auer, Arlindo Da Silva, Jon E. Nielsen, Steven Pawson, Matthew A. Thompson, Atanas L. Trayanov, Katherine R. Travis, Stuart K. Grange, Mat J. Evans, and Daniel J. Jacob
Geosci. Model Dev., 11, 4603–4620, https://doi.org/10.5194/gmd-11-4603-2018, https://doi.org/10.5194/gmd-11-4603-2018, 2018
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We present a full-year online global simulation of tropospheric chemistry at 12.5 km resolution. To the best of our knowledge, such a resolution in a state-of-the-science global simulation of tropospheric chemistry is unprecedented. This simulation will serve as the Nature Run for observing system simulation experiments to support the future geostationary satellite constellation for tropospheric chemistry, and can also be used for various air quality applications.
Hinrich Schaefer, Dan Smale, Sylvia E. Nichol, Tony M. Bromley, Gordon W. Brailsford, Ross J. Martin, Rowena Moss, Sylvia Englund Michel, and James W. C. White
Biogeosciences, 15, 6371–6386, https://doi.org/10.5194/bg-15-6371-2018, https://doi.org/10.5194/bg-15-6371-2018, 2018
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To quantify the impact of El Nino–Southern Oscillation (ENSO) climate events on the methane budget, we studied the correlation between CH4 time series and ENSO indices. We find that ENSO explains less than one-third of the variability in CH4 levels and their stable carbon isotopes, which constrain the source processes of emissions. ENSO forcing of the CH4 cycle is too small, episodic, and regional to force atmospheric trends, which are more likely caused by agricultural or industrial emissions.
Arlene M. Fiore, Emily V. Fischer, George P. Milly, Shubha Pandey Deolal, Oliver Wild, Daniel A. Jaffe, Johannes Staehelin, Olivia E. Clifton, Dan Bergmann, William Collins, Frank Dentener, Ruth M. Doherty, Bryan N. Duncan, Bernd Fischer, Stefan Gilge, Peter G. Hess, Larry W. Horowitz, Alexandru Lupu, Ian A. MacKenzie, Rokjin Park, Ludwig Ries, Michael G. Sanderson, Martin G. Schultz, Drew T. Shindell, Martin Steinbacher, David S. Stevenson, Sophie Szopa, Christoph Zellweger, and Guang Zeng
Atmos. Chem. Phys., 18, 15345–15361, https://doi.org/10.5194/acp-18-15345-2018, https://doi.org/10.5194/acp-18-15345-2018, 2018
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We demonstrate a proof-of-concept approach for applying northern midlatitude mountaintop peroxy acetyl nitrate (PAN) measurements and a multi-model ensemble during April to constrain the influence of continental-scale anthropogenic precursor emissions on PAN. Our findings imply a role for carefully coordinated multi-model ensembles in helping identify observations for discriminating among widely varying (and poorly constrained) model responses of atmospheric constituents to changes in emissions.
James S. Wang, S. Randolph Kawa, G. James Collatz, Motoki Sasakawa, Luciana V. Gatti, Toshinobu Machida, Yuping Liu, and Michael E. Manyin
Atmos. Chem. Phys., 18, 11097–11124, https://doi.org/10.5194/acp-18-11097-2018, https://doi.org/10.5194/acp-18-11097-2018, 2018
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We used measurements of CO2 in the atmosphere from the GOSAT satellite and from surface sites around the world, together with a transport model and a unique estimation technique, to quantify CO2 sources and removals over a recent period. We find that climate variations can strongly influence uptake by vegetation and release in decay and fires. However, regional gaps in observations and inaccuracies to which current satellite technology is susceptible result in important estimation biases.
Sarah A. Strode, Junhua Liu, Leslie Lait, Róisín Commane, Bruce Daube, Steven Wofsy, Austin Conaty, Paul Newman, and Michael Prather
Atmos. Chem. Phys., 18, 10955–10971, https://doi.org/10.5194/acp-18-10955-2018, https://doi.org/10.5194/acp-18-10955-2018, 2018
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The GEOS-5 atmospheric model provided forecasts for the Atmospheric Tomography Mission (ATom). GEOS-5 shows skill in simulating the carbon monoxide (CO) measured in ATom-1. African fires contribute to high CO over the tropical Atlantic, but non-fire sources are the main contributors elsewhere. ATom aims to provide a chemical climatology, so we consider whether ATom-1 occurred during a typical summer month. Satellite observations suggest ATom-1 occurred in a clean but not exceptional month.
Sebastian D. Eastham, Michael S. Long, Christoph A. Keller, Elizabeth Lundgren, Robert M. Yantosca, Jiawei Zhuang, Chi Li, Colin J. Lee, Matthew Yannetti, Benjamin M. Auer, Thomas L. Clune, Jules Kouatchou, William M. Putman, Matthew A. Thompson, Atanas L. Trayanov, Andrea M. Molod, Randall V. Martin, and Daniel J. Jacob
Geosci. Model Dev., 11, 2941–2953, https://doi.org/10.5194/gmd-11-2941-2018, https://doi.org/10.5194/gmd-11-2941-2018, 2018
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Global atmospheric chemical transport models are crucial tools in atmospheric science, used to address problems ranging from climate change to acid rain. GEOS-Chem High Performance (GCHP) is a new implementation of the widely used GEOS-Chem model, designed for massively parallel architectures. GCHP v11-02c is shown to be highly scalable from 6 to over 500 cores, enabling the routine simulation of global atmospheric chemistry from the surface to the stratopause at resolutions of ~50 km or finer.
Richard Hyde, Ryan Hossaini, and Amber A. Leeson
Geosci. Model Dev., 11, 2033–2048, https://doi.org/10.5194/gmd-11-2033-2018, https://doi.org/10.5194/gmd-11-2033-2018, 2018
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Clustering, the automated grouping of similar data, can provide powerful insight into large/complex data. We demonstrate the benefits of clustering applied to output from climate model inter-comparison initiatives. We focus on modelled tropospheric ozone from the ACCMIP project. Cluster-based subsampling of the model ensemble can (i) remove outlier data on a grid-cell basis, reducing model–observation bias and (ii) provide a useful framework in which to investigate and visualise model diversity.
Michael J. Prather, Clare M. Flynn, Xin Zhu, Stephen D. Steenrod, Sarah A. Strode, Arlene M. Fiore, Gustavo Correa, Lee T. Murray, and Jean-Francois Lamarque
Atmos. Meas. Tech., 11, 2653–2668, https://doi.org/10.5194/amt-11-2653-2018, https://doi.org/10.5194/amt-11-2653-2018, 2018
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A new protocol for merging in situ atmospheric chemistry measurements with 3-D models is developed. This technique can identify the most reactive air parcels in terms of tropospheric production/loss of O3 & CH4. This approach highlights differences in 6 global chemistry models even with composition specified. Thus in situ measurements from, e.g., NASA's ATom mission can be used to develop a chemical climatology of, not only the key species, but also the rates of key reactions in each air parcel.
Pieternel F. Levelt, Joanna Joiner, Johanna Tamminen, J. Pepijn Veefkind, Pawan K. Bhartia, Deborah C. Stein Zweers, Bryan N. Duncan, David G. Streets, Henk Eskes, Ronald van der A, Chris McLinden, Vitali Fioletov, Simon Carn, Jos de Laat, Matthew DeLand, Sergey Marchenko, Richard McPeters, Jerald Ziemke, Dejian Fu, Xiong Liu, Kenneth Pickering, Arnoud Apituley, Gonzalo González Abad, Antti Arola, Folkert Boersma, Christopher Chan Miller, Kelly Chance, Martin de Graaf, Janne Hakkarainen, Seppo Hassinen, Iolanda Ialongo, Quintus Kleipool, Nickolay Krotkov, Can Li, Lok Lamsal, Paul Newman, Caroline Nowlan, Raid Suleiman, Lieuwe Gijsbert Tilstra, Omar Torres, Huiqun Wang, and Krzysztof Wargan
Atmos. Chem. Phys., 18, 5699–5745, https://doi.org/10.5194/acp-18-5699-2018, https://doi.org/10.5194/acp-18-5699-2018, 2018
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The aim of this paper is to highlight the many successes of the Ozone Monitoring Instrument (OMI) spanning more than 13 years. Data from OMI have been used in a wide range of applications. Due to its unprecedented spatial resolution, in combination with daily global coverage, OMI plays a unique role in measuring trace gases important for the ozone layer, air quality, and climate change. OMI data continue to be used for new research and applications.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Olaf Morgenstern, Kane A. Stone, Robyn Schofield, Hideharu Akiyoshi, Yousuke Yamashita, Douglas E. Kinnison, Rolando R. Garcia, Kengo Sudo, David A. Plummer, John Scinocca, Luke D. Oman, Michael E. Manyin, Guang Zeng, Eugene Rozanov, Andrea Stenke, Laura E. Revell, Giovanni Pitari, Eva Mancini, Glauco Di Genova, Daniele Visioni, Sandip S. Dhomse, and Martyn P. Chipperfield
Atmos. Chem. Phys., 18, 1091–1114, https://doi.org/10.5194/acp-18-1091-2018, https://doi.org/10.5194/acp-18-1091-2018, 2018
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We assess how ozone as simulated by a group of chemistry–climate models responds to variations in man-made climate gases and ozone-depleting substances. We find some agreement, particularly in the middle and upper stratosphere, but also considerable disagreement elsewhere. Such disagreement affects the reliability of future ozone projections based on these models, and also constitutes a source of uncertainty in climate projections using prescribed ozone derived from these simulations.
Karen Yu, Christoph A. Keller, Daniel J. Jacob, Andrea M. Molod, Sebastian D. Eastham, and Michael S. Long
Geosci. Model Dev., 11, 305–319, https://doi.org/10.5194/gmd-11-305-2018, https://doi.org/10.5194/gmd-11-305-2018, 2018
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Global simulations of atmospheric chemistry are generally conducted with off-line chemical transport models (CTMs) driven by archived meteorological data from general circulation models (GCMs). The off-line approach has the advantages of simplicity and expediency, but it is unable to reproduce the GCM transport exactly. We investigate the cascade of errors associated with the off-line approach using the GEOS-5 GCM and GEOS-Chem CTM and discuss improvements in the use of archived meteorology.
Ivar R. van der Velde, John B. Miller, Michiel K. van der Molen, Pieter P. Tans, Bruce H. Vaughn, James W. C. White, Kevin Schaefer, and Wouter Peters
Geosci. Model Dev., 11, 283–304, https://doi.org/10.5194/gmd-11-283-2018, https://doi.org/10.5194/gmd-11-283-2018, 2018
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We explored an inverse modeling technique to interpret global atmospheric measurements of CO2 and the ratio of its stable carbon isotopes (δ13C). We detected the possible underestimation of drought stress in biosphere models after applying combined atmospheric CO2 and δ13C constraints. This study highlights the importance of improving the representation of the biosphere in carbon–climate models, in particular in a world where droughts become more extreme and more frequent.
Heather Graven, Colin E. Allison, David M. Etheridge, Samuel Hammer, Ralph F. Keeling, Ingeborg Levin, Harro A. J. Meijer, Mauro Rubino, Pieter P. Tans, Cathy M. Trudinger, Bruce H. Vaughn, and James W. C. White
Geosci. Model Dev., 10, 4405–4417, https://doi.org/10.5194/gmd-10-4405-2017, https://doi.org/10.5194/gmd-10-4405-2017, 2017
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Modelling of carbon isotopes 13C and 14C in land and ocean components of Earth system models provides opportunities for new insights and improved understanding of global carbon cycling, and for model evaluation. We compiled existing historical datasets to define the annual mean carbon isotopic composition of atmospheric CO2 for 1850–2015 that can be used in CMIP6 and other modelling activities.
Jerald R. Ziemke, Sarah A. Strode, Anne R. Douglass, Joanna Joiner, Alexander Vasilkov, Luke D. Oman, Junhua Liu, Susan E. Strahan, Pawan K. Bhartia, and David P. Haffner
Atmos. Meas. Tech., 10, 4067–4078, https://doi.org/10.5194/amt-10-4067-2017, https://doi.org/10.5194/amt-10-4067-2017, 2017
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We combine satellite measurements of ozone and cloud properties from the Aura OMI and MLS instruments for 2004–2016 to measure ozone in the mid–upper levels of deep convective clouds. Our results ascribe upward injection of low boundary layer ozone (varying from low to high amounts) as a major driver of the measured concentrations of ozone in thick clouds. Our OMI/MLS generated ozone product is made available to the public for use in science applications.
Katherine R. Travis, Daniel J. Jacob, Christoph A. Keller, Shi Kuang, Jintai Lin, Michael J. Newchurch, and Anne M. Thompson
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-596, https://doi.org/10.5194/acp-2017-596, 2017
Preprint retracted
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Models severely overestimate surface ozone in the Southeast US during summertime which has implications for the design of air quality regulations. We use a model (GEOS-Chem) to interpret ozone observations from a suite of observations taken during August–September 2013. The model is unbiased relative to observations below 1 km but is biased high at the surface. We attribute this bias to model representation error, an underestimate in low-cloud, and insufficient treatment of vertical mixing.
Michael J. Prather, Xin Zhu, Clare M. Flynn, Sarah A. Strode, Jose M. Rodriguez, Stephen D. Steenrod, Junhua Liu, Jean-Francois Lamarque, Arlene M. Fiore, Larry W. Horowitz, Jingqiu Mao, Lee T. Murray, Drew T. Shindell, and Steven C. Wofsy
Atmos. Chem. Phys., 17, 9081–9102, https://doi.org/10.5194/acp-17-9081-2017, https://doi.org/10.5194/acp-17-9081-2017, 2017
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We present a new approach for comparing atmospheric chemistry models with measurements based on what these models are used to do, i.e., calculate changes in ozone and methane, prime greenhouse gases. This method anticipates a new type of measurements from the NASA Atmospheric Tomography (ATom) mission. In comparing the mixture of species within air parcels, we focus on those responsible for key chemical changes and weight these parcels by their chemical reactivity.
Hyun-Deok Choi, Hongyu Liu, James H. Crawford, David B. Considine, Dale J. Allen, Bryan N. Duncan, Larry W. Horowitz, Jose M. Rodriguez, Susan E. Strahan, Lin Zhang, Xiong Liu, Megan R. Damon, and Stephen D. Steenrod
Atmos. Chem. Phys., 17, 8429–8452, https://doi.org/10.5194/acp-17-8429-2017, https://doi.org/10.5194/acp-17-8429-2017, 2017
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We evaluate global ozone–carbon monoxide (O3–CO) correlations in a chemistry and transport model during July–August with TES-Aura satellite observations and examine the sensitivity of model simulations to input meteorological data and emissions. Results show that O3–CO correlations may be used effectively to constrain the sources of regional tropospheric O3 in global 3-D models, especially for those regions where convective transport of pollution plays an important role.
Jochen Stutz, Bodo Werner, Max Spolaor, Lisa Scalone, James Festa, Catalina Tsai, Ross Cheung, Santo F. Colosimo, Ugo Tricoli, Rasmus Raecke, Ryan Hossaini, Martyn P. Chipperfield, Wuhu Feng, Ru-Shan Gao, Eric J. Hintsa, James W. Elkins, Fred L. Moore, Bruce Daube, Jasna Pittman, Steven Wofsy, and Klaus Pfeilsticker
Atmos. Meas. Tech., 10, 1017–1042, https://doi.org/10.5194/amt-10-1017-2017, https://doi.org/10.5194/amt-10-1017-2017, 2017
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A new limb-scanning Differential Optical Absorption Spectroscopy (DOAS) instrument was developed for NASA’s Global Hawk unmanned aerial system during the Airborne Tropical TRopopause EXperiment to study trace gases in the tropical tropopause layer. A new technique that uses in situ and DOAS O3 observations together with radiative transfer calculations allows the retrieval of mixing ratios from the slant column densities of BrO and NO2 at high accuracies of 0.5 ppt and 15 ppt, respectively.
Tyler R. Jones, James W. C. White, Eric J. Steig, Bruce H. Vaughn, Valerie Morris, Vasileios Gkinis, Bradley R. Markle, and Spruce W. Schoenemann
Atmos. Meas. Tech., 10, 617–632, https://doi.org/10.5194/amt-10-617-2017, https://doi.org/10.5194/amt-10-617-2017, 2017
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New measurement systems have been developed that continuously melt ice core samples, in contrast to other methods that analyze a single sample at a time. These newer systems are capable of reducing analysis time by many years and improving data set resolution. In this study, we introduce improved methodologies that optimize the speed, accuracy, and precision of a water isotope continuous-flow system. The presented system will be used for Antarctic and Greenland ice core projects.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
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We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Bodo Werner, Jochen Stutz, Max Spolaor, Lisa Scalone, Rasmus Raecke, James Festa, Santo Fedele Colosimo, Ross Cheung, Catalina Tsai, Ryan Hossaini, Martyn P. Chipperfield, Giorgio S. Taverna, Wuhu Feng, James W. Elkins, David W. Fahey, Ru-Shan Gao, Erik J. Hintsa, Troy D. Thornberry, Free Lee Moore, Maria A. Navarro, Elliot Atlas, Bruce C. Daube, Jasna Pittman, Steve Wofsy, and Klaus Pfeilsticker
Atmos. Chem. Phys., 17, 1161–1186, https://doi.org/10.5194/acp-17-1161-2017, https://doi.org/10.5194/acp-17-1161-2017, 2017
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The paper reports on inorganic and organic bromine measured in the tropical tropopause layer (TTL) over the eastern Pacific in early 2013. Bryinorg is found to increase from a mean of 2.63 ± 1.04 ppt for θ in the range of 350–360 K to 5.11 ± 1.57 ppt for θ=390 ± 400 K, whereas in the subtropical lower stratosphere, it reaches 7.66 ± 2.95 ppt for θ in the range of 390–400 K. Within the TTL, total bromine is found to range from 20.3 ppt to 22.3 ppt.
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
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Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
Raquel A. Silva, J. Jason West, Jean-François Lamarque, Drew T. Shindell, William J. Collins, Stig Dalsoren, Greg Faluvegi, Gerd Folberth, Larry W. Horowitz, Tatsuya Nagashima, Vaishali Naik, Steven T. Rumbold, Kengo Sudo, Toshihiko Takemura, Daniel Bergmann, Philip Cameron-Smith, Irene Cionni, Ruth M. Doherty, Veronika Eyring, Beatrice Josse, Ian A. MacKenzie, David Plummer, Mattia Righi, David S. Stevenson, Sarah Strode, Sophie Szopa, and Guang Zengast
Atmos. Chem. Phys., 16, 9847–9862, https://doi.org/10.5194/acp-16-9847-2016, https://doi.org/10.5194/acp-16-9847-2016, 2016
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Using ozone and PM2.5 concentrations from the ACCMIP ensemble of chemistry-climate models for the four Representative Concentration Pathway scenarios (RCPs), together with projections of future population and baseline mortality rates, we quantify the human premature mortality impacts of future ambient air pollution in 2030, 2050 and 2100, relative to 2000 concentrations. We also estimate the global mortality burden of ozone and PM2.5 in 2000 and each future period.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Sarah A. Strode, Helen M. Worden, Megan Damon, Anne R. Douglass, Bryan N. Duncan, Louisa K. Emmons, Jean-Francois Lamarque, Michael Manyin, Luke D. Oman, Jose M. Rodriguez, Susan E. Strahan, and Simone Tilmes
Atmos. Chem. Phys., 16, 7285–7294, https://doi.org/10.5194/acp-16-7285-2016, https://doi.org/10.5194/acp-16-7285-2016, 2016
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We use global models to interpret trends in MOPITT observations of CO. Simulations with time-dependent emissions reproduce the observed trends over the eastern USA and Europe, suggesting that the emissions are reasonable for these regions. The simulations produce a positive trend over eastern China, contrary to the observed negative trend. This may indicate that the assumed emission trend over China is too positive. However, large variability in the overhead ozone column also contributes.
Nickolay A. Krotkov, Chris A. McLinden, Can Li, Lok N. Lamsal, Edward A. Celarier, Sergey V. Marchenko, William H. Swartz, Eric J. Bucsela, Joanna Joiner, Bryan N. Duncan, K. Folkert Boersma, J. Pepijn Veefkind, Pieternel F. Levelt, Vitali E. Fioletov, Russell R. Dickerson, Hao He, Zifeng Lu, and David G. Streets
Atmos. Chem. Phys., 16, 4605–4629, https://doi.org/10.5194/acp-16-4605-2016, https://doi.org/10.5194/acp-16-4605-2016, 2016
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We examine changes in SO2 and NO2 over the world's most polluted regions during the first decade of Aura OMI observations. Over the eastern US, both NO2 and SO2 levels decreased by 40 % and 80 %, respectively. OMI confirmed large reductions in SO2 over eastern Europe's largest coal power plants. The North China Plain has the world's most severe SO2 pollution, but a decreasing trend been observed since 2011, with a 50 % reduction in 2012–2014. India's SO2 and NO2 levels are growing at a fast pace.
Yasin F. Elshorbany, Bryan N. Duncan, Sarah A. Strode, James S. Wang, and Jules Kouatchou
Geosci. Model Dev., 9, 799–822, https://doi.org/10.5194/gmd-9-799-2016, https://doi.org/10.5194/gmd-9-799-2016, 2016
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The ECCOH (pronounced "echo") chemistry module interactively simulates the photochemistry of the CH4–CO–OH system within a chemistry climate model, carbon cycle model, or Earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4–CO–OH system. This capability is important for capturing nonlinear feedbacks of the CH4–CO–OH system and understanding the perturbations to methane, CO, and OH and the concomitant climate impacts.
S. A. Strode, B. N. Duncan, E. A. Yegorova, J. Kouatchou, J. R. Ziemke, and A. R. Douglass
Atmos. Chem. Phys., 15, 11789–11805, https://doi.org/10.5194/acp-15-11789-2015, https://doi.org/10.5194/acp-15-11789-2015, 2015
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A low bias in carbon monoxide (CO) at northern latitudes is a common feature of chemistry climate models. We find that increasing Northern Hemisphere (NH) CO emissions or reducing NH OH concentrations improves the agreement with CO surface observations, but reducing NH OH leads to a better comparison with MOPITT. Removing model biases in ozone and water vapor increases the simulated methane lifetime, but it does not give the 20% reduction in NH OH suggested by our analysis of the CO bias.
S. T. Lennartz, G. Krysztofiak, C. A. Marandino, B.-M. Sinnhuber, S. Tegtmeier, F. Ziska, R. Hossaini, K. Krüger, S. A. Montzka, E. Atlas, D. E. Oram, T. Keber, H. Bönisch, and B. Quack
Atmos. Chem. Phys., 15, 11753–11772, https://doi.org/10.5194/acp-15-11753-2015, https://doi.org/10.5194/acp-15-11753-2015, 2015
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Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
J. L. Schnell, M. J. Prather, B. Josse, V. Naik, L. W. Horowitz, P. Cameron-Smith, D. Bergmann, G. Zeng, D. A. Plummer, K. Sudo, T. Nagashima, D. T. Shindell, G. Faluvegi, and S. A. Strode
Atmos. Chem. Phys., 15, 10581–10596, https://doi.org/10.5194/acp-15-10581-2015, https://doi.org/10.5194/acp-15-10581-2015, 2015
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We test global chemistry--climate models in their ability to simulate present-day surface ozone. Models are tested against observed hourly ozone from 4217 stations in North America and Europe that are averaged over 1°x1° grid cells. Using novel metrics, we find most models match the shape but not the amplitude of regional summertime diurnal and annual cycles and match the pattern but not the magnitude of summer ozone enhancement. Most also match the observed distribution of extreme episode sizes
Z. Lu, D. G. Streets, B. de Foy, L. N. Lamsal, B. N. Duncan, and J. Xing
Atmos. Chem. Phys., 15, 10367–10383, https://doi.org/10.5194/acp-15-10367-2015, https://doi.org/10.5194/acp-15-10367-2015, 2015
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Using an exponentially modified Gaussian method and taking into account the effect of wind on NO2 distributions, we estimate 3-year moving-average emissions of summertime NOx from 35 US urban areas directly from NO2 retrievals of the OMI during 2005−2014. Total OMI-derived NOx emissions over US urban areas decreased by 49%, consistent with reductions of 43, 49, and 44% in the bottom-up NOx emissions, the weak-wind OMI NO2 burdens, and the averaged NO2 concentrations, respectively.
V. Masson-Delmotte, H. C. Steen-Larsen, P. Ortega, D. Swingedouw, T. Popp, B. M. Vinther, H. Oerter, A. E. Sveinbjornsdottir, H. Gudlaugsdottir, J. E. Box, S. Falourd, X. Fettweis, H. Gallée, E. Garnier, V. Gkinis, J. Jouzel, A. Landais, B. Minster, N. Paradis, A. Orsi, C. Risi, M. Werner, and J. W. C. White
The Cryosphere, 9, 1481–1504, https://doi.org/10.5194/tc-9-1481-2015, https://doi.org/10.5194/tc-9-1481-2015, 2015
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The deep NEEM ice core provides the oldest Greenland ice core record, enabling improved understanding of the response of ice core records to local climate. Here, we focus on shallow ice cores providing a stack record of accumulation and water-stable isotopes spanning the past centuries. For the first time, we document the ongoing warming in a Greenland ice core. By combining our data with other Greenland ice cores and model results, we characterise the spatio-temporal patterns of variability.
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
S. R. Arnold, L. K. Emmons, S. A. Monks, K. S. Law, D. A. Ridley, S. Turquety, S. Tilmes, J. L. Thomas, I. Bouarar, J. Flemming, V. Huijnen, J. Mao, B. N. Duncan, S. Steenrod, Y. Yoshida, J. Langner, and Y. Long
Atmos. Chem. Phys., 15, 6047–6068, https://doi.org/10.5194/acp-15-6047-2015, https://doi.org/10.5194/acp-15-6047-2015, 2015
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The extent to which forest fires produce the air pollutant and greenhouse gas ozone (O3) in the atmosphere at high latitudes in not well understood. We have compared how fire emissions produce O3 and its precursors in several models of atmospheric chemistry. We find enhancements in O3 in air dominated by fires in all models, which increase on average as fire emissions age. We also find that in situ O3 production in the Arctic is sensitive to details of organic chemistry and vertical lifting.
A. P. Ballantyne, R. Andres, R. Houghton, B. D. Stocker, R. Wanninkhof, W. Anderegg, L. A. Cooper, M. DeGrandpre, P. P. Tans, J. B. Miller, C. Alden, and J. W. C. White
Biogeosciences, 12, 2565–2584, https://doi.org/10.5194/bg-12-2565-2015, https://doi.org/10.5194/bg-12-2565-2015, 2015
S. A. Monks, S. R. Arnold, L. K. Emmons, K. S. Law, S. Turquety, B. N. Duncan, J. Flemming, V. Huijnen, S. Tilmes, J. Langner, J. Mao, Y. Long, J. L. Thomas, S. D. Steenrod, J. C. Raut, C. Wilson, M. P. Chipperfield, G. S. Diskin, A. Weinheimer, H. Schlager, and G. Ancellet
Atmos. Chem. Phys., 15, 3575–3603, https://doi.org/10.5194/acp-15-3575-2015, https://doi.org/10.5194/acp-15-3575-2015, 2015
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Multi-model simulations of Arctic CO, O3 and OH are evaluated using observations. Models show highly variable concentrations but the relative importance of emission regions and types is robust across the models, demonstrating the importance of biomass burning as a source. Idealised tracer experiments suggest that some of the model spread is due to variations in simulated transport from Europe in winter and from Asia throughout the year.
A. Ghosh, P. K. Patra, K. Ishijima, T. Umezawa, A. Ito, D. M. Etheridge, S. Sugawara, K. Kawamura, J. B. Miller, E. J. Dlugokencky, P. B. Krummel, P. J. Fraser, L. P. Steele, R. L. Langenfelds, C. M. Trudinger, J. W. C. White, B. Vaughn, T. Saeki, S. Aoki, and T. Nakazawa
Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, https://doi.org/10.5194/acp-15-2595-2015, 2015
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Atmospheric CH4 increased from 900ppb to 1800ppb during the period 1900–2010 at a rate unprecedented in any observational records. We use bottom-up emissions and a chemistry-transport model to simulate CH4. The optimized global total CH4 emission, estimated from the model–observation differences, increased at fastest rate during 1940–1990. Using δ13C of CH4 measurements we attribute this emission increase to biomass burning. Total CH4 lifetime is shortened by 4% over the simulation period.
S. Choi, J. Joiner, Y. Choi, B. N. Duncan, A. Vasilkov, N. Krotkov, and E. Bucsela
Atmos. Chem. Phys., 14, 10565–10588, https://doi.org/10.5194/acp-14-10565-2014, https://doi.org/10.5194/acp-14-10565-2014, 2014
L. Kritten, A. Butz, M. P. Chipperfield, M. Dorf, S. Dhomse, R. Hossaini, H. Oelhaf, C. Prados-Roman, G. Wetzel, and K. Pfeilsticker
Atmos. Chem. Phys., 14, 9555–9566, https://doi.org/10.5194/acp-14-9555-2014, https://doi.org/10.5194/acp-14-9555-2014, 2014
H. C. Steen-Larsen, A. E. Sveinbjörnsdottir, A. J. Peters, V. Masson-Delmotte, M. P. Guishard, G. Hsiao, J. Jouzel, D. Noone, J. K. Warren, and J. W. C. White
Atmos. Chem. Phys., 14, 7741–7756, https://doi.org/10.5194/acp-14-7741-2014, https://doi.org/10.5194/acp-14-7741-2014, 2014
T. R. Jones, J. W. C. White, and T. Popp
Clim. Past, 10, 1253–1267, https://doi.org/10.5194/cp-10-1253-2014, https://doi.org/10.5194/cp-10-1253-2014, 2014
M. Chin, T. Diehl, Q. Tan, J. M. Prospero, R. A. Kahn, L. A. Remer, H. Yu, A. M. Sayer, H. Bian, I. V. Geogdzhayev, B. N. Holben, S. G. Howell, B. J. Huebert, N. C. Hsu, D. Kim, T. L. Kucsera, R. C. Levy, M. I. Mishchenko, X. Pan, P. K. Quinn, G. L. Schuster, D. G. Streets, S. A. Strode, O. Torres, and X.-P. Zhao
Atmos. Chem. Phys., 14, 3657–3690, https://doi.org/10.5194/acp-14-3657-2014, https://doi.org/10.5194/acp-14-3657-2014, 2014
D. Helmig, V. Petrenko, P. Martinerie, E. Witrant, T. Röckmann, A. Zuiderweg, R. Holzinger, J. Hueber, C. Thompson, J. W. C. White, W. Sturges, A. Baker, T. Blunier, D. Etheridge, M. Rubino, and P. Tans
Atmos. Chem. Phys., 14, 1463–1483, https://doi.org/10.5194/acp-14-1463-2014, https://doi.org/10.5194/acp-14-1463-2014, 2014
J. X. Warner, R. Yang, Z. Wei, F. Carminati, A. Tangborn, Z. Sun, W. Lahoz, J.-L. Attié, L. El Amraoui, and B. Duncan
Atmos. Chem. Phys., 14, 103–114, https://doi.org/10.5194/acp-14-103-2014, https://doi.org/10.5194/acp-14-103-2014, 2014
S. Tegtmeier, K. Krüger, B. Quack, E. Atlas, D. R. Blake, H. Boenisch, A. Engel, H. Hepach, R. Hossaini, M. A. Navarro, S. Raimund, S. Sala, Q. Shi, and F. Ziska
Atmos. Chem. Phys., 13, 11869–11886, https://doi.org/10.5194/acp-13-11869-2013, https://doi.org/10.5194/acp-13-11869-2013, 2013
J.-F. Lamarque, F. Dentener, J. McConnell, C.-U. Ro, M. Shaw, R. Vet, D. Bergmann, P. Cameron-Smith, S. Dalsoren, R. Doherty, G. Faluvegi, S. J. Ghan, B. Josse, Y. H. Lee, I. A. MacKenzie, D. Plummer, D. T. Shindell, R. B. Skeie, D. S. Stevenson, S. Strode, G. Zeng, M. Curran, D. Dahl-Jensen, S. Das, D. Fritzsche, and M. Nolan
Atmos. Chem. Phys., 13, 7997–8018, https://doi.org/10.5194/acp-13-7997-2013, https://doi.org/10.5194/acp-13-7997-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
V. Naik, A. Voulgarakis, A. M. Fiore, L. W. Horowitz, J.-F. Lamarque, M. Lin, M. J. Prather, P. J. Young, D. Bergmann, P. J. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. Doherty, V. Eyring, G. Faluvegi, G. A. Folberth, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, T. P. C. van Noije, D. A. Plummer, M. Righi, S. T. Rumbold, R. Skeie, D. T. Shindell, D. S. Stevenson, S. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, https://doi.org/10.5194/acp-13-5277-2013, 2013
K. W. Bowman, D. T. Shindell, H. M. Worden, J.F. Lamarque, P. J. Young, D. S. Stevenson, Z. Qu, M. de la Torre, D. Bergmann, P. J. Cameron-Smith, W. J. Collins, R. Doherty, S. B. Dalsøren, G. Faluvegi, G. Folberth, L. W. Horowitz, B. M. Josse, Y. H. Lee, I. A. MacKenzie, G. Myhre, T. Nagashima, V. Naik, D. A. Plummer, S. T. Rumbold, R. B. Skeie, S. A. Strode, K. Sudo, S. Szopa, A. Voulgarakis, G. Zeng, S. S. Kulawik, A. M. Aghedo, and J. R. Worden
Atmos. Chem. Phys., 13, 4057–4072, https://doi.org/10.5194/acp-13-4057-2013, https://doi.org/10.5194/acp-13-4057-2013, 2013
D. S. Stevenson, P. J. Young, V. Naik, J.-F. Lamarque, D. T. Shindell, A. Voulgarakis, R. B. Skeie, S. B. Dalsoren, G. Myhre, T. K. Berntsen, G. A. Folberth, S. T. Rumbold, W. J. Collins, I. A. MacKenzie, R. M. Doherty, G. Zeng, T. P. C. van Noije, A. Strunk, D. Bergmann, P. Cameron-Smith, D. A. Plummer, S. A. Strode, L. Horowitz, Y. H. Lee, S. Szopa, K. Sudo, T. Nagashima, B. Josse, I. Cionni, M. Righi, V. Eyring, A. Conley, K. W. Bowman, O. Wild, and A. Archibald
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Related subject area
Subject: Isotopes | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Using ship-borne observations of methane isotopic ratio in the Arctic Ocean to understand methane sources in the Arctic
Global inorganic nitrate production mechanisms: comparison of a global model with nitrate isotope observations
Rethinking Craig and Gordon's approach to modeling isotopic compositions of marine boundary layer vapor
Photochemical box modelling of volcanic SO2 oxidation: isotopic constraints
Uncertainties of fluxes and 13C ∕ 12C ratios of atmospheric reactive-gas emissions
Using δ13C-CH4 and δD-CH4 to constrain Arctic methane emissions
Air–snow transfer of nitrate on the East Antarctic Plateau – Part 2: An isotopic model for the interpretation of deep ice-core records
Interannual variability of isotopic composition in water vapor over western Africa and its relationship to ENSO
Continental-scale enrichment of atmospheric 14CO2 from the nuclear power industry: potential impact on the estimation of fossil fuel-derived CO2
Global modelling of H2 mixing ratios and isotopic compositions with the TM5 model
Simulation of the diurnal variations of the oxygen isotope anomaly (Δ17O) of reactive atmospheric species
The impact of anthropogenic emissions on atmospheric sulfate production pathways, oxidants, and ice core Δ17O(SO42–)
Quantifying atmospheric nitrate formation pathways based on a global model of the oxygen isotopic composition (Δ17O) of atmospheric nitrate
Antoine Berchet, Isabelle Pison, Patrick M. Crill, Brett Thornton, Philippe Bousquet, Thibaud Thonat, Thomas Hocking, Joël Thanwerdas, Jean-Daniel Paris, and Marielle Saunois
Atmos. Chem. Phys., 20, 3987–3998, https://doi.org/10.5194/acp-20-3987-2020, https://doi.org/10.5194/acp-20-3987-2020, 2020
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Methane isotopes in the atmosphere can help us differentiate between emission processes. A large variety of natural and anthropogenic emission types are active in the Arctic and are unsatisfactorily understood and documented up to now. A ship-based campaign was carried out in summer 2014, providing a unique dataset of isotopic measurements in the Arctic Ocean. Using a chemistry-transport model, we link these measurements to circumpolar emissions and retrieve information about their signature.
Becky Alexander, Tomás Sherwen, Christopher D. Holmes, Jenny A. Fisher, Qianjie Chen, Mat J. Evans, and Prasad Kasibhatla
Atmos. Chem. Phys., 20, 3859–3877, https://doi.org/10.5194/acp-20-3859-2020, https://doi.org/10.5194/acp-20-3859-2020, 2020
Short summary
Short summary
Nitrogen oxides are important for the formation of tropospheric oxidants and are removed from the atmosphere mainly through the formation of nitrate. We compare observations of the oxygen isotopes of nitrate with a global model to test our understanding of the chemistry nitrate formation. We use the model to quantify nitrate formation pathways in the atmosphere and identify key uncertainties and their relevance for the oxidation capacity of the atmosphere.
Xiahong Feng, Eric S. Posmentier, Leslie J. Sonder, and Naixin Fan
Atmos. Chem. Phys., 19, 4005–4024, https://doi.org/10.5194/acp-19-4005-2019, https://doi.org/10.5194/acp-19-4005-2019, 2019
Short summary
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We present a 1-D model to simulate H2O isotopologues of vapor and their vertical fluxes in the first kilometer above the sea surface. The model includes two processes not in earlier Craig–Gordon isotope evaporation models: height-dependent diffusion/mixing and ascending/converging air. Calculated isotopic ratios compare well with data from seven cruises. The model explains how sea surface meteorology can affect atmospheric vapor, precipitation isotope ratios, and paleoisotope records.
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.
Sergey Gromov, Carl A. M. Brenninkmeijer, and Patrick Jöckel
Atmos. Chem. Phys., 17, 8525–8552, https://doi.org/10.5194/acp-17-8525-2017, https://doi.org/10.5194/acp-17-8525-2017, 2017
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We revisit the proxies/uncertainties for the 13C/12C ratios of emissions of reactive C into the atmosphere. Our main findings are (i) a factor of 2 less uncertain estimate of tropospheric CO surface sources δ13C, (ii) a confirmed disagreement between the bottom-up and top-down 13CO-inclusive emission estimates, and (iii) a novel estimate of the δ13C signatures of a range of NMHCs/VOCs to be used in modelling studies. Results are based on the EMAC model emission set-up evaluated for 2000.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
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Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
J. Erbland, J. Savarino, S. Morin, J. L. France, M. M. Frey, and M. D. King
Atmos. Chem. Phys., 15, 12079–12113, https://doi.org/10.5194/acp-15-12079-2015, https://doi.org/10.5194/acp-15-12079-2015, 2015
Short summary
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In this paper, we describe the development of a numerical model which aims at representing nitrate recycling at the air-snow interface on the East Antarctic Plateau. Stable isotopes are used as diagnostic and evaluation tools by comparing the model's results to recent field measurements of nitrate and key atmospheric species at Dome C, Antarctica. From sensitivity tests conducted with the model, we propose a framework for the interpretation of the nitrate isotope record in deep ice cores.
A. Okazaki, Y. Satoh, G. Tremoy, F. Vimeux, R. Scheepmaker, and K. Yoshimura
Atmos. Chem. Phys., 15, 3193–3204, https://doi.org/10.5194/acp-15-3193-2015, https://doi.org/10.5194/acp-15-3193-2015, 2015
H. D. Graven and N. Gruber
Atmos. Chem. Phys., 11, 12339–12349, https://doi.org/10.5194/acp-11-12339-2011, https://doi.org/10.5194/acp-11-12339-2011, 2011
G. Pieterse, M. C. Krol, A. M. Batenburg, L. P. Steele, P. B. Krummel, R. L. Langenfelds, and T. Röckmann
Atmos. Chem. Phys., 11, 7001–7026, https://doi.org/10.5194/acp-11-7001-2011, https://doi.org/10.5194/acp-11-7001-2011, 2011
S. Morin, R. Sander, and J. Savarino
Atmos. Chem. Phys., 11, 3653–3671, https://doi.org/10.5194/acp-11-3653-2011, https://doi.org/10.5194/acp-11-3653-2011, 2011
E. D. Sofen, B. Alexander, and S. A. Kunasek
Atmos. Chem. Phys., 11, 3565–3578, https://doi.org/10.5194/acp-11-3565-2011, https://doi.org/10.5194/acp-11-3565-2011, 2011
B. Alexander, M. G. Hastings, D. J. Allman, J. Dachs, J. A. Thornton, and S. A. Kunasek
Atmos. Chem. Phys., 9, 5043–5056, https://doi.org/10.5194/acp-9-5043-2009, https://doi.org/10.5194/acp-9-5043-2009, 2009
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Short summary
The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss of CH4 by reaction with OH and chlorine (Cl) also affects this ratio. Tropospheric Cl provides a small and uncertain sink for CH4 but has a large effect on its isotopic ratio. We use the GEOS model with several different Cl fields to test the sensitivity of methane's isotopic composition to tropospheric Cl. Cl affects the global mean, hemispheric gradient, and seasonal cycle of the isotopic ratio.
The 13C : 12C isotopic ratio in methane (CH4) provides information about CH4 sources, but loss...
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