Articles | Volume 13, issue 3
https://doi.org/10.5194/acp-13-1511-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-1511-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
OCS photolytic isotope effects from first principles: sulfur and carbon isotopes, temperature dependence and implications for the stratosphere
J. A. Schmidt
Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen Ø, Denmark
M. S. Johnson
Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen Ø, Denmark
S. Hattori
Department of Environmental Science and Technology, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, Yokohama, 226-8502, Japan
Department of Environmental Chemistry and Engineering, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, Yokohama, 226-8502, Japan
N. Yoshida
Department of Environmental Science and Technology, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, Yokohama, 226-8502, Japan
Department of Environmental Chemistry and Engineering, Interdisciplinary Graduate School of Science and Engineering, Tokyo Institute of Technology, Yokohama, 226-8502, Japan
S. Nanbu
Faculty of Science and Technology, Sophia University, 7-1 Kioi-Cho, Chiyoda-ku, Tokyo 102-8554, Japan
R. Schinke
Max-Planck-Institut für Dynamik und Selbstorganisation, 37073 Göttingen, Germany
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Sulfate aerosols play an important climatic role and exert adverse effects on the ecological environment and human health. In this study, we present the triple oxygen isotopic composition of sulfate from the Mt. Everest region, southern Tibetan Plateau, and decipher the formation mechanisms of atmospheric sulfate in this pristine environment. The results indicate the important role of the S(IV) + O3 pathway in atmospheric sulfate formation promoted by conditions of high cloud water pH.
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Atmos. Meas. Tech., 13, 2119–2129, https://doi.org/10.5194/amt-13-2119-2020, https://doi.org/10.5194/amt-13-2119-2020, 2020
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We performed an error analysis of SMILES observations for acetonitrile and a validation using the MLS observations by extracting the coincident points between SMILES and MLS data. The major error sources for the SMILES observations were quantitatively estimated. At upper pressure levels the difference between the two datasets increased because of an uncertainty in MLS observations. The results showed that SMILES has an advantage in measuring acetonitrile in the upper stratosphere and mesosphere.
Kazuki Kamezaki, Shohei Hattori, Enno Bahlmann, and Naohiro Yoshida
Atmos. Meas. Tech., 12, 1141–1154, https://doi.org/10.5194/amt-12-1141-2019, https://doi.org/10.5194/amt-12-1141-2019, 2019
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Knowledge related to sulfur isotopic composition of carbonyl sulfide (OCS or COS), the most abundant atmospheric sulfur species, remains scarce. We present a new sampling system for collecting approx. 10 nmol of OCS from ambient air coupled with a purification system. The system presented herein is useful for application of sulfur isotopic compositions for investigation of OCS sources and sinks in the troposphere to elucidate its cycle and its contribution to background stratospheric sulfate.
Mary E. Whelan, Sinikka T. Lennartz, Teresa E. Gimeno, Richard Wehr, Georg Wohlfahrt, Yuting Wang, Linda M. J. Kooijmans, Timothy W. Hilton, Sauveur Belviso, Philippe Peylin, Róisín Commane, Wu Sun, Huilin Chen, Le Kuai, Ivan Mammarella, Kadmiel Maseyk, Max Berkelhammer, King-Fai Li, Dan Yakir, Andrew Zumkehr, Yoko Katayama, Jérôme Ogée, Felix M. Spielmann, Florian Kitz, Bharat Rastogi, Jürgen Kesselmeier, Julia Marshall, Kukka-Maaria Erkkilä, Lisa Wingate, Laura K. Meredith, Wei He, Rüdiger Bunk, Thomas Launois, Timo Vesala, Johan A. Schmidt, Cédric G. Fichot, Ulli Seibt, Scott Saleska, Eric S. Saltzman, Stephen A. Montzka, Joseph A. Berry, and J. Elliott Campbell
Biogeosciences, 15, 3625–3657, https://doi.org/10.5194/bg-15-3625-2018, https://doi.org/10.5194/bg-15-3625-2018, 2018
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Measurements of the trace gas carbonyl sulfide (OCS) are helpful in quantifying photosynthesis at previously unknowable temporal and spatial scales. While CO2 is both consumed and produced within ecosystems, OCS is mostly produced in the oceans or from specific industries, and destroyed in plant leaves in proportion to CO2. This review summarizes the advancements we have made in the understanding of OCS exchange and applications to vital ecosystem water and carbon cycle questions.
Sakae Toyoda, Naohiro Yoshida, Shinji Morimoto, Shuji Aoki, Takakiyo Nakazawa, Satoshi Sugawara, Shigeyuki Ishidoya, Mitsuo Uematsu, Yoichi Inai, Fumio Hasebe, Chusaku Ikeda, Hideyuki Honda, and Kentaro Ishijima
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By analysis of whole air samples collected by balloon-borne compact cryogenic samplers, we found that apparent isotope effect for stratospheric N2O between 25 and 30 km over the Equator is larger than that observed in other latitudes and that it is almost equal to the effect predicted by laboratory simulation experiments. These results suggest that equatorial middle stratosphere can be treated as an isolated region when we consider the decomposition of N2O by photochemical processes.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
Short summary
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Hannah M. Horowitz, Daniel J. Jacob, Yanxu Zhang, Theodore S. Dibble, Franz Slemr, Helen M. Amos, Johan A. Schmidt, Elizabeth S. Corbitt, Eloïse A. Marais, and Elsie M. Sunderland
Atmos. Chem. Phys., 17, 6353–6371, https://doi.org/10.5194/acp-17-6353-2017, https://doi.org/10.5194/acp-17-6353-2017, 2017
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Mercury is a toxic, global pollutant released to the air from human activities like coal burning. Chemical reactions in air determine how far mercury is transported before it is deposited to the environment, where it may be converted to a form that accumulates in fish. We use a 3-D atmospheric model to evaluate a new set of chemical reactions and its effects on mercury deposition. We find it is consistent with observations and leads to increased deposition to oceans, especially in the tropics.
Sakiko Ishino, Shohei Hattori, Joel Savarino, Bruno Jourdain, Susanne Preunkert, Michel Legrand, Nicolas Caillon, Albane Barbero, Kota Kuribayashi, and Naohiro Yoshida
Atmos. Chem. Phys., 17, 3713–3727, https://doi.org/10.5194/acp-17-3713-2017, https://doi.org/10.5194/acp-17-3713-2017, 2017
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We show the first simultaneous observations of triple oxygen isotopic compositions of atmospheric sulfate, nitrate, and ozone at Dumont d'Urville, coastal Antarctica. The contrasting seasonal trends between oxygen isotopes of ozone and those of sulfate and nitrate indicate that these signatures in sulfate and nitrate are mainly controlled by changes in oxidation chemistry. We also discuss the specific oxidation chemistry induced by the unique phenomena at the site.
Tomás Sherwen, Mat J. Evans, Lucy J. Carpenter, Johan A. Schmidt, and Loretta J. Mickley
Atmos. Chem. Phys., 17, 1557–1569, https://doi.org/10.5194/acp-17-1557-2017, https://doi.org/10.5194/acp-17-1557-2017, 2017
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We model pre-industrial to present day changes using the GEOS-Chem global chemical transport model with halogens (Cl, Br, I). The model better captures pre-industrial O3 observations with halogens included. Halogens buffer the tropospheric forcing of O3 (RFTO3) from pre-industrial to present day, reducing RFTO3 by 0.087 Wm−2. This reduction is greater than that from halogens on stratospheric O3 (−0.05 Wm−2). This suggests that models that do not include halogens will overestimate RFTO3by ~ 25%.
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Qianjie Chen, Lei Geng, Johan A. Schmidt, Zhouqing Xie, Hui Kang, Jordi Dachs, Jihong Cole-Dai, Andrew J. Schauer, Madeline G. Camp, and Becky Alexander
Atmos. Chem. Phys., 16, 11433–11450, https://doi.org/10.5194/acp-16-11433-2016, https://doi.org/10.5194/acp-16-11433-2016, 2016
Short summary
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The formation mechanisms of sulfate in the marine boundary layer are not well understood, which could result in large uncertainties in aerosol radiative forcing. We measure the oxygen isotopic composition (Δ17O) of sulfate collected in the MBL and analyze with a global transport model. Our results suggest that 33–50 % of MBL sulfate is formed via oxidation of S(IV) by hypohalous acids HOBr / HOCl in the aqueous phase, and the daily-mean HOBr/HOCl concentrations are on the order of 0.01–0.1 ppt.
Anders B. Bluhme, Jonas L. Ingemar, Carl Meusinger, and Matthew S. Johnson
Atmos. Meas. Tech., 9, 2669–2673, https://doi.org/10.5194/amt-9-2669-2016, https://doi.org/10.5194/amt-9-2669-2016, 2016
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Hydrogen sulfide (H2S) is a malodorous, very poisonous, and flammable gas. It can be detected as SO2 using fluorescence after conversion using a hot catalyst. This technique is well established and as such also recommended by authorities such as the EPA. Our paper describes how at a relative humidity as low as 5 %, significant amounts of H2S pass the instrument undetected. At ambient levels of relative humidity, up to 1/3 of all H2S passes the instrument unnoticed.
Sakae Toyoda and Naohiro Yoshida
Atmos. Meas. Tech., 9, 2093–2101, https://doi.org/10.5194/amt-9-2093-2016, https://doi.org/10.5194/amt-9-2093-2016, 2016
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Tiny variation in natural abundance ratios of stable isotopes of nitrogen and oxygen in nitrous oxide (N2O) can be used as a fingerprint of this trace gas that causes greenhouse effect and stratospheric ozone depletion. Toward the understanding of the global budget of N2O and its temporal change, we developed an automated sample preparation system that can be used to measure the stable isotope ratios in N2O in various air samples collected into flasks with high precision and less labor.
L. M. T. Joelsson, J. A. Schmidt, E. J. K. Nilsson, T. Blunier, D. W. T. Griffith, S. Ono, and M. S. Johnson
Atmos. Chem. Phys., 16, 4439–4449, https://doi.org/10.5194/acp-16-4439-2016, https://doi.org/10.5194/acp-16-4439-2016, 2016
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We present experimental kinetic isotope effects (KIE) for the OH oxidation of CH3D and 13CH3D and their temperature dependence. Our determination of the 13CH3D + OH KIE is novel and we find no "clumped" isotope effect within the experimental uncertainty.
Koki Maeda, Sakae Toyoda, Midori Yano, Shohei Hattori, Makoto Fukasawa, Keiichi Nakajima, and Naohiro Yoshida
Biogeosciences, 13, 1341–1349, https://doi.org/10.5194/bg-13-1341-2016, https://doi.org/10.5194/bg-13-1341-2016, 2016
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Nitrogen isotope ratios (δ15N) of NH4+ in dairy manure compost piles were studied. The δ15N–NH4+ values in different pile zones (top, side and core) show that extremely high nitrogen conversion, nitrification–denitrification activity of the microbes and NH3 volatilization occurred in pile top zone, which has very high NH4+ concentrations and significantly high 15N (δ15N: 12.7–29.8 ‰) values.
T. A. Berhanu, J. Savarino, J. Erbland, W. C. Vicars, S. Preunkert, J. F. Martins, and M. S. Johnson
Atmos. Chem. Phys., 15, 11243–11256, https://doi.org/10.5194/acp-15-11243-2015, https://doi.org/10.5194/acp-15-11243-2015, 2015
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In this field study at Dome C, Antarctica, we investigated the effect of solar UV photolysis on the stable isotopes of nitrate in snow via comparison of two identical snow pits while exposing only one to solar UV. From the difference between the average isotopic fractionations calculated for each pit, we determined a purely photolytic nitrogen isotopic fractionation of -55.8‰, in good agreement with what has been recently determined in a laboratory study.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
N. Zhang, K. Yamada, N. Suzuki, and N. Yoshida
Biogeosciences, 11, 5335–5348, https://doi.org/10.5194/bg-11-5335-2014, https://doi.org/10.5194/bg-11-5335-2014, 2014
T. Yamazaki, T. Hozuki, K. Arai, S. Toyoda, K. Koba, T. Fujiwara, and N. Yoshida
Biogeosciences, 11, 2679–2689, https://doi.org/10.5194/bg-11-2679-2014, https://doi.org/10.5194/bg-11-2679-2014, 2014
T. O. Sato, H. Sagawa, N. Yoshida, and Y. Kasai
Atmos. Meas. Tech., 7, 941–958, https://doi.org/10.5194/amt-7-941-2014, https://doi.org/10.5194/amt-7-941-2014, 2014
E. J. K. Nilsson, J. A. Schmidt, and M. S. Johnson
Atmos. Chem. Phys., 14, 551–558, https://doi.org/10.5194/acp-14-551-2014, https://doi.org/10.5194/acp-14-551-2014, 2014
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Physics (physical properties and processes)
Analytical approximation of the definite Chapman integral for arbitrary zenith angles
Moist bias in the Pacific upper troposphere and lower stratosphere (UTLS) in climate models affects regional circulation patterns
Evaluation of vertical transport in ERA5 and ERA-Interim reanalysis using high-altitude aircraft measurements in the Asian summer monsoon 2017
Injection strategy – a driver of atmospheric circulation and ozone response to stratospheric aerosol geoengineering
Quantifying stratospheric ozone trends over 1984–2020: a comparison of ordinary and regularized multivariate regression models
Surface ozone over the Tibetan Plateau controlled by stratospheric intrusion
The role of tropical upwelling in explaining discrepancies between recent modeled and observed lower-stratospheric ozone trends
The roles of the Quasi-Biennial Oscillation and El Niño for entry stratospheric water vapor in observations and coupled chemistry–ocean CCMI and CMIP6 models
Improved estimation of volcanic SO2 injections from satellite retrievals and Lagrangian transport simulations: the 2019 Raikoke eruption
Hemispheric asymmetries in recent changes in the stratospheric circulation
A stratospheric prognostic ozone for seamless Earth system models: performance, impacts and future
The 2019 Raikoke volcanic eruption – Part 1: Dispersion model simulations and satellite retrievals of volcanic sulfur dioxide
The stratospheric Brewer–Dobson circulation inferred from age of air in the ERA5 reanalysis
Simulations of anthropogenic bromoform indicate high emissions at the coast of East Asia
Sensitivity of stratospheric water vapour to variability in tropical tropopause temperatures and large-scale transport
Technical note: Lowermost-stratosphere moist bias in ECMWF IFS model diagnosed from airborne GLORIA observations during winter–spring 2016
The response of stratospheric water vapor to climate change driven by different forcing agents
Influence of convection on stratospheric water vapor in the North American monsoon region
Electricity savings and greenhouse gas emission reductions from global phase-down of hydrofluorocarbons
Impact of convectively lofted ice on the seasonal cycle of water vapor in the tropical tropopause layer
Simulating the atmospheric response to the 11-year solar cycle forcing with the UM-UKCA model: the role of detection method and natural variability
Transport of trace gases via eddy shedding from the Asian summer monsoon anticyclone and associated impacts on ozone heating rates
Detectability of the impacts of ozone-depleting substances and greenhouse gases upon stratospheric ozone accounting for nonlinearities in historical forcings
Multi-decadal records of stratospheric composition and their relationship to stratospheric circulation change
Brominated VSLS and their influence on ozone under a changing climate
Contribution of different processes to changes in tropical lower-stratospheric water vapor in chemistry–climate models
Quantifying pollution transport from the Asian monsoon anticyclone into the lower stratosphere
A new time-independent formulation of fractional release
The millennium water vapour drop in chemistry–climate model simulations
Impact of major volcanic eruptions on stratospheric water vapour
Variability of water vapour in the Arctic stratosphere
On the hiatus in the acceleration of tropical upwelling since the beginning of the 21st century
Trends in peroxyacetyl nitrate (PAN) in the upper troposphere and lower stratosphere over southern Asia during the summer monsoon season: regional impacts
Spatial regression analysis on 32 years of total column ozone data
Ozone seasonality above the tropical tropopause: reconciling the Eulerian and Lagrangian perspectives of transport processes
Modeling upper tropospheric and lower stratospheric water vapor anomalies
Evolution of Antarctic ozone in September–December predicted by CCMVal-2 model simulations for the 21st century
Assessment of the interannual variability and influence of the QBO and upwelling on tracer–tracer distributions of N2O and O3 in the tropical lower stratosphere
On the relationship between total ozone and atmospheric dynamics and chemistry at mid-latitudes – Part 2: The effects of the El Niño/Southern Oscillation, volcanic eruptions and contributions of atmospheric dynamics and chemistry to long-term total ozone changes
Relationships between Brewer-Dobson circulation, double tropopauses, ozone and stratospheric water vapour
Simulation of stratospheric water vapor and trends using three reanalyses
Climatological perspectives of air transport from atmospheric boundary layer to tropopause layer over Asian monsoon regions during boreal summer inferred from Lagrangian approach
Solar response in tropical stratospheric ozone: a 3-D chemical transport model study using ERA reanalyses
Geomagnetic activity related NOx enhancements and polar surface air temperature variability in a chemistry climate model: modulation of the NAM index
Forecasts and assimilation experiments of the Antarctic ozone hole 2008
Extreme events in total ozone over Arosa – Part 2: Fingerprints of atmospheric dynamics and chemistry and effects on mean values and long-term changes
Technical Note: Trend estimation from irregularly sampled, correlated data
Modeling the transport of very short-lived substances into the tropical upper troposphere and lower stratosphere
Dongxiao Yue
Atmos. Chem. Phys., 24, 5093–5097, https://doi.org/10.5194/acp-24-5093-2024, https://doi.org/10.5194/acp-24-5093-2024, 2024
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The stunning colors of the sky and clouds result from light scattering in the atmosphere, whose density changes with height. Previously, calculating these colors involves costly, sometimes inaccurate methods. This paper presents a silver bullet: a single elegant formula that simplifies these complex calculations. What is the result? We have faster, more precise predictions of atmospheric colors, from Earth's blue skies and red sunsets to Venus's golden hues.
Felix Ploeger, Thomas Birner, Edward Charlesworth, Paul Konopka, and Rolf Müller
Atmos. Chem. Phys., 24, 2033–2043, https://doi.org/10.5194/acp-24-2033-2024, https://doi.org/10.5194/acp-24-2033-2024, 2024
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We present a novel mechanism of how regional anomalies in water vapour concentrations in the upper troposphere and lower stratosphere impact regional atmospheric circulation systems. These impacts include a displaced upper-level Asian monsoon circulation and strengthened prevailing westerlies in the Pacific region. Current climate models have biases in simulating these regional water vapour anomalies and circulation impacts, but the biases can be avoided by improving the model transport.
Bärbel Vogel, C. Michael Volk, Johannes Wintel, Valentin Lauther, Jan Clemens, Jens-Uwe Grooß, Gebhard Günther, Lars Hoffmann, Johannes C. Laube, Rolf Müller, Felix Ploeger, and Fred Stroh
Atmos. Chem. Phys., 24, 317–343, https://doi.org/10.5194/acp-24-317-2024, https://doi.org/10.5194/acp-24-317-2024, 2024
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Over the Indian subcontinent, polluted air is rapidly uplifted to higher altitudes during the Asian monsoon season. We present an assessment of vertical transport in this region using different wind data provided by the European Centre for Medium-Range Weather Forecasts (ECMWF), as well as high-resolution aircraft measurements. In general, our findings confirm that the newest ECMWF reanalysis product, ERA5, yields a better representation of transport compared to the predecessor, ERA-Interim.
Ewa M. Bednarz, Amy H. Butler, Daniele Visioni, Yan Zhang, Ben Kravitz, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 13665–13684, https://doi.org/10.5194/acp-23-13665-2023, https://doi.org/10.5194/acp-23-13665-2023, 2023
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We use a state-of-the-art Earth system model and a set of stratospheric aerosol injection (SAI) strategies to achieve the same level of global mean surface cooling through different combinations of location and/or timing of the injection. We demonstrate that the choice of SAI strategy can lead to contrasting impacts on stratospheric and tropospheric temperatures, circulation, and chemistry (including stratospheric ozone), thereby leading to different impacts on regional surface climate.
Yajuan Li, Sandip S. Dhomse, Martyn P. Chipperfield, Wuhu Feng, Jianchun Bian, Yuan Xia, and Dong Guo
Atmos. Chem. Phys., 23, 13029–13047, https://doi.org/10.5194/acp-23-13029-2023, https://doi.org/10.5194/acp-23-13029-2023, 2023
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For the first time a regularized multivariate regression model is used to estimate stratospheric ozone trends. Regularized regression avoids the over-fitting issue due to correlation among explanatory variables. We demonstrate that there are considerable differences in satellite-based and chemical-model-based ozone trends, highlighting large uncertainties in our understanding about ozone variability. We argue that caution is needed when interpreting results with different methods and datasets.
Xiufeng Yin, Dipesh Rupakheti, Guoshuai Zhang, Jiali Luo, Shichang Kang, Benjamin de Foy, Junhua Yang, Zhenming Ji, Zhiyuan Cong, Maheswar Rupakheti, Ping Li, Yuling Hu, and Qianggong Zhang
Atmos. Chem. Phys., 23, 10137–10143, https://doi.org/10.5194/acp-23-10137-2023, https://doi.org/10.5194/acp-23-10137-2023, 2023
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The monthly mean surface ozone concentrations peaked earlier in the south in April and May and later in the north in June and July over the Tibetan Plateau. The migration of monthly surface ozone peaks was coupled with the synchronous movement of tropopause folds and the westerly jet that created conditions conducive to stratospheric ozone intrusion. Stratospheric ozone intrusion significantly contributed to surface ozone across the Tibetan Plateau.
Sean M. Davis, Nicholas Davis, Robert W. Portmann, Eric Ray, and Karen Rosenlof
Atmos. Chem. Phys., 23, 3347–3361, https://doi.org/10.5194/acp-23-3347-2023, https://doi.org/10.5194/acp-23-3347-2023, 2023
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Ozone in the lower part of the stratosphere has not increased and has perhaps even continued to decline in recent decades. This study demonstrates that the amount of ozone in this region is highly sensitive to the amount of air upwelling into the stratosphere in the tropics and that simulations from a climate model nudged to historical meteorological fields often fail to accurately capture the variations in tropical upwelling that control short-term trends in lower-stratospheric ozone.
Shlomi Ziskin Ziv, Chaim I. Garfinkel, Sean Davis, and Antara Banerjee
Atmos. Chem. Phys., 22, 7523–7538, https://doi.org/10.5194/acp-22-7523-2022, https://doi.org/10.5194/acp-22-7523-2022, 2022
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Stratospheric water vapor is important for Earth's overall greenhouse effect and for ozone chemistry; however the factors governing its variability on interannual timescales are not fully known, and previous modeling studies have indicated that models struggle to capture this interannual variability. We demonstrate that nonlinear interactions are important for determining overall water vapor concentrations and also that models have improved in their ability to capture these connections.
Zhongyin Cai, Sabine Griessbach, and Lars Hoffmann
Atmos. Chem. Phys., 22, 6787–6809, https://doi.org/10.5194/acp-22-6787-2022, https://doi.org/10.5194/acp-22-6787-2022, 2022
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Using AIRS and TROPOMI sulfur dioxide retrievals and the Lagrangian transport model MPTRAC, we present an improved reconstruction of injection parameters of the 2019 Raikoke eruption. Reconstructions agree well between using AIRS nighttime and TROPOMI daytime retrievals, showing the potential of our approach to create a long-term volcanic sulfur dioxide inventory from nearly 20 years of AIRS retrievals.
Felix Ploeger and Hella Garny
Atmos. Chem. Phys., 22, 5559–5576, https://doi.org/10.5194/acp-22-5559-2022, https://doi.org/10.5194/acp-22-5559-2022, 2022
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We investigate hemispheric asymmetries in stratospheric circulation changes in the last 2 decades in model simulations and atmospheric observations. We find that observed trace gas changes can be explained by a structural circulation change related to a deepening circulation in the Northern Hemisphere relative to the Southern Hemisphere. As this asymmetric signal is small compared to internal variability observed circulation trends over the recent past are not in contradiction to climate models.
Beatriz M. Monge-Sanz, Alessio Bozzo, Nicholas Byrne, Martyn P. Chipperfield, Michail Diamantakis, Johannes Flemming, Lesley J. Gray, Robin J. Hogan, Luke Jones, Linus Magnusson, Inna Polichtchouk, Theodore G. Shepherd, Nils Wedi, and Antje Weisheimer
Atmos. Chem. Phys., 22, 4277–4302, https://doi.org/10.5194/acp-22-4277-2022, https://doi.org/10.5194/acp-22-4277-2022, 2022
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The stratosphere is emerging as one of the keys to improve tropospheric weather and climate predictions. This study provides evidence of the role the stratospheric ozone layer plays in improving weather predictions at different timescales. Using a new ozone modelling approach suitable for high-resolution global models that provide operational forecasts from days to seasons, we find significant improvements in stratospheric meteorological fields and stratosphere–troposphere coupling.
Johannes de Leeuw, Anja Schmidt, Claire S. Witham, Nicolas Theys, Isabelle A. Taylor, Roy G. Grainger, Richard J. Pope, Jim Haywood, Martin Osborne, and Nina I. Kristiansen
Atmos. Chem. Phys., 21, 10851–10879, https://doi.org/10.5194/acp-21-10851-2021, https://doi.org/10.5194/acp-21-10851-2021, 2021
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Using the NAME dispersion model in combination with high-resolution SO2 satellite data from TROPOMI, we investigate the dispersion of volcanic SO2 from the 2019 Raikoke eruption. NAME accurately simulates the dispersion of SO2 during the first 2–3 weeks after the eruption and illustrates the potential of using high-resolution satellite data to identify potential limitations in dispersion models, which will ultimately help to improve efforts to forecast the dispersion of volcanic clouds.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
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We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
Josefine Maas, Susann Tegtmeier, Yue Jia, Birgit Quack, Jonathan V. Durgadoo, and Arne Biastoch
Atmos. Chem. Phys., 21, 4103–4121, https://doi.org/10.5194/acp-21-4103-2021, https://doi.org/10.5194/acp-21-4103-2021, 2021
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Cooling-water disinfection at coastal power plants is a known source of atmospheric bromoform. A large source of anthropogenic bromoform is the industrial regions in East Asia. In current bottom-up flux estimates, these anthropogenic emissions are missing, underestimating the global air–sea flux of bromoform. With transport simulations, we show that by including anthropogenic bromoform from cooling-water treatment, the bottom-up flux estimates significantly improve in East and Southeast Asia.
Jacob W. Smith, Peter H. Haynes, Amanda C. Maycock, Neal Butchart, and Andrew C. Bushell
Atmos. Chem. Phys., 21, 2469–2489, https://doi.org/10.5194/acp-21-2469-2021, https://doi.org/10.5194/acp-21-2469-2021, 2021
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This paper informs realistic simulation of stratospheric water vapour by clearly attributing each of the two key influences on water vapour entry to the stratosphere. Presenting modified trajectory models, the results of this paper show temperatures dominate on annual and inter-annual variations; however, transport has a significant effect in reducing the annual cycle maximum. Furthermore, sub-seasonal variations in temperature have an important overall influence.
Wolfgang Woiwode, Andreas Dörnbrack, Inna Polichtchouk, Sören Johansson, Ben Harvey, Michael Höpfner, Jörn Ungermann, and Felix Friedl-Vallon
Atmos. Chem. Phys., 20, 15379–15387, https://doi.org/10.5194/acp-20-15379-2020, https://doi.org/10.5194/acp-20-15379-2020, 2020
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The lowermost-stratosphere moist bias in ECMWF analyses and 12 h forecasts is diagnosed for the Arctic winter-spring 2016 period by using two-dimensional GLORIA water vapor observations. The bias is already present in the initial conditions (i.e., the analyses), and sensitivity forecasts on time scales of < 12 h show hardly any sensitivity to modified spatial resolution and output frequency.
Xun Wang and Andrew E. Dessler
Atmos. Chem. Phys., 20, 13267–13282, https://doi.org/10.5194/acp-20-13267-2020, https://doi.org/10.5194/acp-20-13267-2020, 2020
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We investigate the response of stratospheric water vapor (SWV) to different forcing agents, including greenhouse gases and aerosols. For most forcing agents, the SWV response is dominated by a slow response, which is coupled to surface temperature changes and exhibits a similar sensitivity to the surface temperature across all forcing agents. The fast SWV adjustment due to forcing is important when the forcing agent directly heats the cold-point region, e.g., black carbon.
Wandi Yu, Andrew E. Dessler, Mijeong Park, and Eric J. Jensen
Atmos. Chem. Phys., 20, 12153–12161, https://doi.org/10.5194/acp-20-12153-2020, https://doi.org/10.5194/acp-20-12153-2020, 2020
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The stratospheric water vapor mixing ratio over North America (NA) region is up to ~ 1 ppmv higher when deep convection occurs. We find substantial consistency in the interannual variations of NA water vapor anomaly and deep convection and explain both the summer seasonal cycle and interannual variability of the convective moistening efficiency. We show that the NA anticyclone and tropical upper tropospheric temperature determine how much deep convection moistens the lower stratosphere.
Pallav Purohit, Lena Höglund-Isaksson, John Dulac, Nihar Shah, Max Wei, Peter Rafaj, and Wolfgang Schöpp
Atmos. Chem. Phys., 20, 11305–11327, https://doi.org/10.5194/acp-20-11305-2020, https://doi.org/10.5194/acp-20-11305-2020, 2020
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This study shows that if energy efficiency improvements in cooling technologies are addressed simultaneously with a phase-down of hydrofluorocarbons (HFCs), not only will global warming be mitigated through the elimination of HFCs but also by saving about a fifth of future global electricity consumption. This means preventing between 411 and 631 Pg CO2 equivalent of greenhouse gases between today and 2100, thereby offering a significant contribution towards staying well below 2 °C warming.
Xun Wang, Andrew E. Dessler, Mark R. Schoeberl, Wandi Yu, and Tao Wang
Atmos. Chem. Phys., 19, 14621–14636, https://doi.org/10.5194/acp-19-14621-2019, https://doi.org/10.5194/acp-19-14621-2019, 2019
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We use a trajectory model to diagnose mechanisms that produce the observed and modeled tropical lower stratospheric water vapor seasonal cycle. We confirm that the seasonal cycle of water vapor is primarily determined by the seasonal cycle of tropical tropopause layer (TTL) temperatures. However, between 10° N and 40° N, we find that evaporation of convective ice in the TTL plays a key role contributing to the water vapor seasonal cycle there. The Asian monsoon region is the most important region.
Ewa M. Bednarz, Amanda C. Maycock, Paul J. Telford, Peter Braesicke, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 5209–5233, https://doi.org/10.5194/acp-19-5209-2019, https://doi.org/10.5194/acp-19-5209-2019, 2019
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Following model improvements, the atmospheric response to the 11-year solar cycle forcing simulated in the UM-UKCA chemistry–climate model is discussed for the first time. In contrast to most previous studies in the literature, we compare the results diagnosed using both a composite and a MLR methodology, and we show that apparently different signals can be diagnosed in the troposphere. In addition, we look at the role of internal atmospheric variability for the detection of the solar response.
Suvarna Fadnavis, Chaitri Roy, Rajib Chattopadhyay, Christopher E. Sioris, Alexandru Rap, Rolf Müller, K. Ravi Kumar, and Raghavan Krishnan
Atmos. Chem. Phys., 18, 11493–11506, https://doi.org/10.5194/acp-18-11493-2018, https://doi.org/10.5194/acp-18-11493-2018, 2018
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Rapid industrialization, traffic growth and urbanization resulted in a significant increase in the tropospheric trace gases over Asia. There is global concern about rising levels of these trace gases. The monsoon convection transports these gases to the upper-level-anticyclone. In this study, we show transport of these gases to the extratropics via eddy-shedding from the anticyclone. We also deliberate on changes in ozone heating rates due to the transport of Asian trace gases.
Justin Bandoro, Susan Solomon, Benjamin D. Santer, Douglas E. Kinnison, and Michael J. Mills
Atmos. Chem. Phys., 18, 143–166, https://doi.org/10.5194/acp-18-143-2018, https://doi.org/10.5194/acp-18-143-2018, 2018
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We studied the attribution of stratospheric ozone changes and identified similarities between observations and human fingerprints from both emissions of ozone-depleting substances (ODSs) and greenhouse gases (GHGs). We developed an improvement on the traditional pattern correlation method that accounts for nonlinearities in the climate forcing time evolution. Use of the latter resulted in increased S / N ratios for the ODS fingerprint. The GHG fingerprint was not identifiable.
Anne R. Douglass, Susan E. Strahan, Luke D. Oman, and Richard S. Stolarski
Atmos. Chem. Phys., 17, 12081–12096, https://doi.org/10.5194/acp-17-12081-2017, https://doi.org/10.5194/acp-17-12081-2017, 2017
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Data records from instruments on satellites and on the ground are compared with a simulation for 1980–2016 that is made using winds and temperatures that are derived from measurements. The simulation tracks the observations faithfully after about 2000, but there are systematic errors for earlier years. Scientists must take this into account when trying to detect and quantify changes in the stratospheric circulation that are caused by climate change.
Stefanie Falk, Björn-Martin Sinnhuber, Gisèle Krysztofiak, Patrick Jöckel, Phoebe Graf, and Sinikka T. Lennartz
Atmos. Chem. Phys., 17, 11313–11329, https://doi.org/10.5194/acp-17-11313-2017, https://doi.org/10.5194/acp-17-11313-2017, 2017
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Brominated very short-lived source gases (VSLS) contribute significantly to the tropospheric and stratospheric bromine loading. We find an increase of future ocean–atmosphere flux of brominated VSLS of 8–10 % compared to present day. A decrease in the tropospheric mixing ratios of VSLS and an increase in the lower stratosphere are attributed to changes in atmospheric chemistry and transport. Bromine impact on stratospheric ozone at the end of the 21st century is reduced compared to present day.
Kevin M. Smalley, Andrew E. Dessler, Slimane Bekki, Makoto Deushi, Marion Marchand, Olaf Morgenstern, David A. Plummer, Kiyotaka Shibata, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 17, 8031–8044, https://doi.org/10.5194/acp-17-8031-2017, https://doi.org/10.5194/acp-17-8031-2017, 2017
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This paper explains a new way to evaluate simulated lower-stratospheric water vapor. We use a multivariate linear regression to predict 21st century lower stratospheric water vapor within 12 chemistry climate models using tropospheric warming, the Brewer–Dobson circulation, and the quasi-biennial oscillation as predictors. This methodology produce strong fits to simulated water vapor, and potentially represents a superior method to evaluate model trends in lower-stratospheric water vapor.
Felix Ploeger, Paul Konopka, Kaley Walker, and Martin Riese
Atmos. Chem. Phys., 17, 7055–7066, https://doi.org/10.5194/acp-17-7055-2017, https://doi.org/10.5194/acp-17-7055-2017, 2017
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Pollution transport from the surface to the stratosphere within the Asian summer monsoon circulation may cause harmful effects on stratospheric chemistry and climate. We investigate air mass transport from the monsoon anticyclone into the stratosphere, combining model simulations with satellite trace gas measurements. We show evidence for two transport pathways from the monsoon: (i) into the tropical stratosphere and (ii) into the Northern Hemisphere extratropical lower stratosphere.
Jennifer Ostermöller, Harald Bönisch, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 17, 3785–3797, https://doi.org/10.5194/acp-17-3785-2017, https://doi.org/10.5194/acp-17-3785-2017, 2017
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We analysed the temporal evolution of fractional release factors (FRFs) from EMAC model simulations for several halocarbons and nitrous oxide. The current formulation of FRFs yields values that depend on the tropospheric trend of the species. This is a problematic issue for the application of FRF in the calculation of steady-state quantities (e.g. ODP). Including a loss term in the calculation, we develop a new formulation of FRF and find that the time dependence can almost be compensated.
Sabine Brinkop, Martin Dameris, Patrick Jöckel, Hella Garny, Stefan Lossow, and Gabriele Stiller
Atmos. Chem. Phys., 16, 8125–8140, https://doi.org/10.5194/acp-16-8125-2016, https://doi.org/10.5194/acp-16-8125-2016, 2016
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This study investigates the water vapour decline in the stratosphere beginning in the year 2000 and other similarly strong stratospheric water vapour reductions. The driving forces are tropical sea surface temperature (SST) changes due to coincidence with a preceding ENSO event and supported by the west to east change of the QBO.
There are indications that both SSTs and the specific dynamical state of the atmosphere contribute to the long period of low water vapour values from 2001 to 2006.
Michael Löffler, Sabine Brinkop, and Patrick Jöckel
Atmos. Chem. Phys., 16, 6547–6562, https://doi.org/10.5194/acp-16-6547-2016, https://doi.org/10.5194/acp-16-6547-2016, 2016
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After the two major volcanic eruptions of El Chichón in Mexico in 1982 and Mount Pinatubo on the Philippines in 1991, stratospheric water vapour is significantly increased. This results from increased stratospheric heating rates due to volcanic aerosol and the subsequent changes in stratospheric and tropopause temperatures in the tropics. The tropical vertical advection and the South Asian summer monsoon are identified as important sources for the additional water vapour in the stratosphere.
Laura Thölix, Leif Backman, Rigel Kivi, and Alexey Yu. Karpechko
Atmos. Chem. Phys., 16, 4307–4321, https://doi.org/10.5194/acp-16-4307-2016, https://doi.org/10.5194/acp-16-4307-2016, 2016
J. Aschmann, J. P. Burrows, C. Gebhardt, A. Rozanov, R. Hommel, M. Weber, and A. M. Thompson
Atmos. Chem. Phys., 14, 12803–12814, https://doi.org/10.5194/acp-14-12803-2014, https://doi.org/10.5194/acp-14-12803-2014, 2014
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This study compares observations and simulation results of ozone in the lower tropical stratosphere. It shows that ozone in this region decreased from 1985 up to about 2002, which is consistent with an increase in tropical upwelling predicted by climate models. However, the decrease effectively stops after 2002, indicating that significant changes in tropical upwelling have occurred. The most important factor appears to be that the vertical ascent in the tropics is no longer accelerating.
S. Fadnavis, M. G. Schultz, K. Semeniuk, A. S. Mahajan, L. Pozzoli, S. Sonbawne, S. D. Ghude, M. Kiefer, and E. Eckert
Atmos. Chem. Phys., 14, 12725–12743, https://doi.org/10.5194/acp-14-12725-2014, https://doi.org/10.5194/acp-14-12725-2014, 2014
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The Asian summer monsoon transports pollutants from local emission sources to the upper troposphere and lower stratosphere (UTLS). The increasing trend of these pollutants may have climatic impact. This study addresses the impact of convectively lifted Indian and Chinese emissions on the ULTS. Sensitivity experiments with emission changes in particular regions show that Chinese emissions have a greater impact on the concentrations of NOY species than Indian emissions.
J. S. Knibbe, R. J. van der A, and A. T. J. de Laat
Atmos. Chem. Phys., 14, 8461–8482, https://doi.org/10.5194/acp-14-8461-2014, https://doi.org/10.5194/acp-14-8461-2014, 2014
M. Abalos, F. Ploeger, P. Konopka, W. J. Randel, and E. Serrano
Atmos. Chem. Phys., 13, 10787–10794, https://doi.org/10.5194/acp-13-10787-2013, https://doi.org/10.5194/acp-13-10787-2013, 2013
M. R. Schoeberl, A. E. Dessler, and T. Wang
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