Articles | Volume 21, issue 4
https://doi.org/10.5194/acp-21-2427-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-2427-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Potential of future stratospheric ozone loss in the midlatitudes under global warming and sulfate geoengineering
Sabine Robrecht
CORRESPONDING AUTHOR
Institute for Energy and Climate research – Stratosphere (IEK-7), Forschungszentrum Jülich, Jülich, Germany
now at: Deutscher Wetterdienst, Offenbach, Germany
Bärbel Vogel
Institute for Energy and Climate research – Stratosphere (IEK-7), Forschungszentrum Jülich, Jülich, Germany
Simone Tilmes
Atmospheric Chemistry Observations and Modeling Lab, National Center for Atmospheric Research, Boulder, CO, USA
Rolf Müller
Institute for Energy and Climate research – Stratosphere (IEK-7), Forschungszentrum Jülich, Jülich, Germany
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Atmos. Chem. Phys., 24, 12557–12574, https://doi.org/10.5194/acp-24-12557-2024, https://doi.org/10.5194/acp-24-12557-2024, 2024
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HCl null cycles in Antarctica are important for maintaining high values of ozone-destroying chlorine in Antarctic spring. These HCl null cycles are not affected by (1) using the most recent recommendations of chemical kinetics (compared to older recommendations), (2) accounting for dehydration in the Antarctic winter vortex, and (3) considering the observed (but unexplained) depletion of HCl in mid-winter in the Antarctic vortex throughout Antarctic winter.
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The potential destruction of stratospheric ozone in the mid-latitudes has been discussed recently. We analysed this ozone loss mechanism and its sensitivities. In a certain temperature range, we found a threshold in water vapour, which has to be exceeded for ozone loss to occur. We show the dependence of this water vapour threshold on temperature, sulfate content and air composition. This study provides a basis to estimate the impact of potential sulphate geoengineering on stratospheric ozone.
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This paper revisits the chemistry leading to strong ozone depletion in the Antarctic. We focus on the heart of the ozone layer in the lowermost stratosphere in the core of the vortex. We argue that chemical cycles (referred to as HCl null cycles) that have hitherto been largely neglected counteract the deactivation of chlorine and are therefore key to ozone depletion in the core of the Antarctic vortex. The key process to full activation of chlorine is the photolysis of formaldehyde.
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Atmos. Chem. Phys., 24, 11759–11774, https://doi.org/10.5194/acp-24-11759-2024, https://doi.org/10.5194/acp-24-11759-2024, 2024
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Atmos. Chem. Phys., 24, 7535–7557, https://doi.org/10.5194/acp-24-7535-2024, https://doi.org/10.5194/acp-24-7535-2024, 2024
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Atmos. Chem. Phys., 24, 4771–4788, https://doi.org/10.5194/acp-24-4771-2024, https://doi.org/10.5194/acp-24-4771-2024, 2024
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Particles were collected during the flight campaign StratoClim 2017 within the Asian tropopause aerosol layer (ATAL). Refractory particles from seven different flights were characterized by scanning and transmission electron microscopy (SEM, TEM). The most abundant refractory particles are silicates and non-volatile organics. The most important sources are combustion processes at the ground and the agitation of soil material. During one flight, small cinnabar particles (HgS) were also detected.
Danny M. Leung, Jasper F. Kok, Longlei Li, David M. Lawrence, Natalie M. Mahowald, Simone Tilmes, and Erik Kluzek
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Danny M. Leung, Jasper F. Kok, Longlei Li, Natalie M. Mahowald, David M. Lawrence, Simone Tilmes, Erik Kluzek, Martina Klose, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 2287–2318, https://doi.org/10.5194/acp-24-2287-2024, https://doi.org/10.5194/acp-24-2287-2024, 2024
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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.
Reinhold Spang, Rolf Müller, and Alexandru Rap
Atmos. Chem. Phys., 24, 1213–1230, https://doi.org/10.5194/acp-24-1213-2024, https://doi.org/10.5194/acp-24-1213-2024, 2024
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Cirrus clouds play an important role in the radiation budget of the Earth. Despite recent progress in their observation, the radiative impact of ultra-thin cirrus clouds (UTC) in the tropopause region and in the lowermost stratosphere remains poorly constrained. Sensitivity model simulations with different ice parameters provide an uncertainty range for the radiative effect of UTCs. There is a need for better observed UTCs to enable the simulation of their potentially large effect on climate.
Abolfazl Rezaei, Khalil Karami, Simone Tilmes, and John C. Moore
Earth Syst. Dynam., 15, 91–108, https://doi.org/10.5194/esd-15-91-2024, https://doi.org/10.5194/esd-15-91-2024, 2024
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Water storage (WS) plays a profound role in the lives of people in the Middle East and North Africa as well as Mediterranean climate "hot spots". WS change by greenhouse gas (GHG) warming is simulated with and without stratospheric aerosol intervention (SAI). WS significantly increases in the Arabian Peninsula and decreases around the Mediterranean under GHG. While SAI partially ameliorates GHG impacts, projected WS increases in dry regions and decreases in wet areas relative to present climate.
Jan Clemens, Bärbel Vogel, Lars Hoffmann, Sabine Griessbach, Nicole Thomas, Suvarna Fadnavis, Rolf Müller, Thomas Peter, and Felix Ploeger
Atmos. Chem. Phys., 24, 763–787, https://doi.org/10.5194/acp-24-763-2024, https://doi.org/10.5194/acp-24-763-2024, 2024
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The source regions of the Asian tropopause aerosol layer (ATAL) are debated. We use balloon-borne measurements of the layer above Nainital (India) in August 2016 and atmospheric transport models to find ATAL source regions. Most air originated from the Tibetan plateau. However, the measured ATAL was stronger when more air originated from the Indo-Gangetic Plain and weaker when more air originated from the Pacific. Hence, the results indicate important anthropogenic contributions to the ATAL.
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.
Rolf Müller, Ulrich Pöschl, Thomas Koop, Thomas Peter, and Ken Carslaw
Atmos. Chem. Phys., 23, 15445–15453, https://doi.org/10.5194/acp-23-15445-2023, https://doi.org/10.5194/acp-23-15445-2023, 2023
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Paul J. Crutzen was a pioneer in atmospheric sciences and a kind-hearted, humorous person with empathy for the private lives of his colleagues and students. He made fundamental scientific contributions to a wide range of scientific topics in all parts of the atmosphere. Paul was among the founders of the journal Atmospheric Chemistry and Physics. His work will continue to be a guide for generations of scientists and environmental policymakers to come.
Simone Tilmes, Michael J. Mills, Yunqian Zhu, Charles G. Bardeen, Francis Vitt, Pengfei Yu, David Fillmore, Xiaohong Liu, Brian Toon, and Terry Deshler
Geosci. Model Dev., 16, 6087–6125, https://doi.org/10.5194/gmd-16-6087-2023, https://doi.org/10.5194/gmd-16-6087-2023, 2023
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We implemented an alternative aerosol scheme in the high- and low-top model versions of the Community Earth System Model Version 2 (CESM2) with a more detailed description of tropospheric and stratospheric aerosol size distributions than the existing aerosol model. This development enables the comparison of different aerosol schemes with different complexity in the same model framework. It identifies improvements compared to a range of observations in both the troposphere and stratosphere.
Wenfu Tang, Louisa K. Emmons, Helen M. Worden, Rajesh Kumar, Cenlin He, Benjamin Gaubert, Zhonghua Zheng, Simone Tilmes, Rebecca R. Buchholz, Sara-Eva Martinez-Alonso, Claire Granier, Antonin Soulie, Kathryn McKain, Bruce C. Daube, Jeff Peischl, Chelsea Thompson, and Pieternel Levelt
Geosci. Model Dev., 16, 6001–6028, https://doi.org/10.5194/gmd-16-6001-2023, https://doi.org/10.5194/gmd-16-6001-2023, 2023
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The new MUSICAv0 model enables the study of atmospheric chemistry across all relevant scales. We develop a MUSICAv0 grid for Africa. We evaluate MUSICAv0 with observations and compare it with a previously used model – WRF-Chem. Overall, the performance of MUSICAv0 is comparable to WRF-Chem. Based on model–satellite discrepancies, we find that future field campaigns in an eastern African region (30°E–45°E, 5°S–5°N) could substantially improve the predictive skill of air quality models.
Yunqian Zhu, Robert W. Portmann, Douglas Kinnison, Owen Brian Toon, Luis Millán, Jun Zhang, Holger Vömel, Simone Tilmes, Charles G. Bardeen, Xinyue Wang, Stephanie Evan, William J. Randel, and Karen H. Rosenlof
Atmos. Chem. Phys., 23, 13355–13367, https://doi.org/10.5194/acp-23-13355-2023, https://doi.org/10.5194/acp-23-13355-2023, 2023
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The 2022 Hunga Tonga eruption injected a large amount of water into the stratosphere. Ozone depletion was observed inside the volcanic plume. Chlorine and water vapor injected by this eruption exceeded the normal range, which made the ozone chemistry during this event occur at a higher temperature than polar ozone depletion. Unlike polar ozone chemistry where chlorine nitrate is more important, hypochlorous acid plays a large role in the in-plume chlorine balance and heterogeneous processes.
Seyed Vahid Mousavi, Khalil Karami, Simone Tilmes, Helene Muri, Lili Xia, and Abolfazl Rezaei
Atmos. Chem. Phys., 23, 10677–10695, https://doi.org/10.5194/acp-23-10677-2023, https://doi.org/10.5194/acp-23-10677-2023, 2023
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Understanding atmospheric dust changes in the Middle East and North Africa (MENA) region under future climate scenarios is essential. By injecting sulfate aerosols into the stratosphere, stratospheric aerosol injection (SAI) geoengineering reflects some of the incoming sunlight back to space. This study shows that the MENA region would experience lower dust concentration under both SAI and RCP8.5 scenarios compared to the current climate (CTL) by the end of the century.
Suvarna Fadnavis, Bernd Heinold, T. P. Sabin, Anne Kubin, Katty Huang, Alexandru Rap, and Rolf Müller
Atmos. Chem. Phys., 23, 10439–10449, https://doi.org/10.5194/acp-23-10439-2023, https://doi.org/10.5194/acp-23-10439-2023, 2023
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The influence of the COVID-19 lockdown on the Himalayas caused increases in snow cover and a decrease in runoff, ultimately leading to an enhanced snow water equivalent. Our findings highlight that, out of the two processes causing a retreat of Himalayan glaciers – (1) slow response to global climate change and (2) fast response to local air pollution – a policy action on the latter is more likely to be within the reach of possible policy action to help billions of people in southern Asia.
Lars Hoffmann, Paul Konopka, Jan Clemens, and Bärbel Vogel
Atmos. Chem. Phys., 23, 7589–7609, https://doi.org/10.5194/acp-23-7589-2023, https://doi.org/10.5194/acp-23-7589-2023, 2023
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Atmospheric convection plays a key role in tracer transport in the troposphere. Global meteorological forecasts and reanalyses typically have a coarse spatiotemporal resolution that does not adequately resolve the dynamics, transport, and mixing of air associated with storm systems or deep convection. We discuss the application of the extreme convection parameterization in a Lagrangian transport model to improve simulations of tracer transport from the boundary layer into the free troposphere.
Duseong S. Jo, Simone Tilmes, Louisa K. Emmons, Siyuan Wang, and Francis Vitt
Geosci. Model Dev., 16, 3893–3906, https://doi.org/10.5194/gmd-16-3893-2023, https://doi.org/10.5194/gmd-16-3893-2023, 2023
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A new simple secondary organic aerosol (SOA) scheme has been developed for the Community Atmosphere Model (CAM) based on the complex SOA scheme in CAM with detailed chemistry (CAM-chem). The CAM with the new SOA scheme shows better agreements with CAM-chem in terms of aerosol concentrations and radiative fluxes, which ensures more consistent results between different compsets in the Community Earth System Model. The new SOA scheme also has technical advantages for future developments.
Abolfazl Rezaei, Khalil Karami, Simone Tilmes, and John C. Moore
Atmos. Chem. Phys., 23, 5835–5850, https://doi.org/10.5194/acp-23-5835-2023, https://doi.org/10.5194/acp-23-5835-2023, 2023
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Teleconnection patterns are important characteristics of the climate system; well-known examples include the El Niño and La Niña events driven from the tropical Pacific. We examined how spatiotemporal patterns that arise in the Pacific and Atlantic oceans behave under stratospheric aerosol geoengineering and greenhouse gas (GHG)-induced warming. In general, geoengineering reverses trends; however, the changes in decadal oscillation for the AMO, NAO, and PDO imposed by GHG are not suppressed.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
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Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Daniele Visioni, Ben Kravitz, Alan Robock, Simone Tilmes, Jim Haywood, Olivier Boucher, Mark Lawrence, Peter Irvine, Ulrike Niemeier, Lili Xia, Gabriel Chiodo, Chris Lennard, Shingo Watanabe, John C. Moore, and Helene Muri
Atmos. Chem. Phys., 23, 5149–5176, https://doi.org/10.5194/acp-23-5149-2023, https://doi.org/10.5194/acp-23-5149-2023, 2023
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Geoengineering indicates methods aiming to reduce the temperature of the planet by means of reflecting back a part of the incoming radiation before it reaches the surface or allowing more of the planetary radiation to escape into space. It aims to produce modelling experiments that are easy to reproduce and compare with different climate models, in order to understand the potential impacts of these techniques. Here we assess its past successes and failures and talk about its future.
Khalil Karami, Rolando Garcia, Christoph Jacobi, Jadwiga H. Richter, and Simone Tilmes
Atmos. Chem. Phys., 23, 3799–3818, https://doi.org/10.5194/acp-23-3799-2023, https://doi.org/10.5194/acp-23-3799-2023, 2023
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Alongside mitigation and adaptation efforts, stratospheric aerosol intervention (SAI) is increasingly considered a third pillar to combat dangerous climate change. We investigate the teleconnection between the quasi-biennial oscillation in the equatorial stratosphere and the Arctic stratospheric polar vortex under a warmer climate and an SAI scenario. We show that the Holton–Tan relationship weakens under both scenarios and discuss the physical mechanisms responsible for such changes.
Yangxin Chen, Duoying Ji, Qian Zhang, John C. Moore, Olivier Boucher, Andy Jones, Thibaut Lurton, Michael J. Mills, Ulrike Niemeier, Roland Séférian, and Simone Tilmes
Earth Syst. Dynam., 14, 55–79, https://doi.org/10.5194/esd-14-55-2023, https://doi.org/10.5194/esd-14-55-2023, 2023
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Solar geoengineering has been proposed as a way of counteracting the warming effects of increasing greenhouse gases by reflecting solar radiation. This work shows that solar geoengineering can slow down the northern-high-latitude permafrost degradation but cannot preserve the permafrost ecosystem as that under a climate of the same warming level without solar geoengineering.
Oliver Appel, Franziska Köllner, Antonis Dragoneas, Andreas Hünig, Sergej Molleker, Hans Schlager, Christoph Mahnke, Ralf Weigel, Max Port, Christiane Schulz, Frank Drewnick, Bärbel Vogel, Fred Stroh, and Stephan Borrmann
Atmos. Chem. Phys., 22, 13607–13630, https://doi.org/10.5194/acp-22-13607-2022, https://doi.org/10.5194/acp-22-13607-2022, 2022
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This paper clarifies the chemical composition of the Asian tropopause aerosol layer (ATAL) by means of airborne in situ aerosol mass spectrometry (AMS). Ammonium nitrate and organics are found to significantly contribute to the particle layer, while sulfate does not show a layered structure. An analysis of the single-particle mass spectra suggests that secondary particle formation and subsequent growth dominate the particle composition, rather than condensation on pre-existing primary particles.
Mari R. Tye, Katherine Dagon, Maria J. Molina, Jadwiga H. Richter, Daniele Visioni, Ben Kravitz, and Simone Tilmes
Earth Syst. Dynam., 13, 1233–1257, https://doi.org/10.5194/esd-13-1233-2022, https://doi.org/10.5194/esd-13-1233-2022, 2022
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We examined the potential effect of stratospheric aerosol injection (SAI) on extreme temperature and precipitation. SAI may cause daytime temperatures to cool but nighttime to warm. Daytime cooling may occur in all seasons across the globe, with the largest decreases in summer. In contrast, nighttime warming may be greatest at high latitudes in winter. SAI may reduce the frequency and intensity of extreme rainfall. The combined changes may exacerbate drying over parts of the global south.
Liubov Poshyvailo-Strube, Rolf Müller, Stephan Fueglistaler, Michaela I. Hegglin, Johannes C. Laube, C. Michael Volk, and Felix Ploeger
Atmos. Chem. Phys., 22, 9895–9914, https://doi.org/10.5194/acp-22-9895-2022, https://doi.org/10.5194/acp-22-9895-2022, 2022
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Brewer–Dobson circulation (BDC) controls the composition of the stratosphere, which in turn affects radiation and climate. As the BDC cannot be measured directly, it is necessary to infer its strength and trends indirectly. In this study, we test in the
model worlddifferent methods for estimating the mean age of air trends based on a combination of stratospheric water vapour and methane data. We also provide simple practical advice of a more reliable estimation of the mean age of air trends.
Suvarna Fadnavis, Prashant Chavan, Akash Joshi, Sunil M. Sonbawne, Asutosh Acharya, Panuganti C. S. Devara, Alexandru Rap, Felix Ploeger, and Rolf Müller
Atmos. Chem. Phys., 22, 7179–7191, https://doi.org/10.5194/acp-22-7179-2022, https://doi.org/10.5194/acp-22-7179-2022, 2022
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We show that large amounts of anthropogenic aerosols are transported from South Asia to the northern Indian Ocean. These aerosols are then lifted into the UTLS by the ascending branch of the Hadley circulation. They are further transported to the Southern Hemisphere and downward via westerly ducts over the tropical Atlantic and Pacific. These aerosols increase tropospheric heating, resulting in an increase in water vapor, which is then transported to the UTLS.
Simone Tilmes, Daniele Visioni, Andy Jones, James Haywood, Roland Séférian, Pierre Nabat, Olivier Boucher, Ewa Monica Bednarz, and Ulrike Niemeier
Atmos. Chem. Phys., 22, 4557–4579, https://doi.org/10.5194/acp-22-4557-2022, https://doi.org/10.5194/acp-22-4557-2022, 2022
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This study assesses the impacts of climate interventions, using stratospheric sulfate aerosol and solar dimming on stratospheric ozone, based on three Earth system models with interactive stratospheric chemistry. The climate interventions have been applied to a high emission (baseline) scenario in order to reach global surface temperatures of a medium emission scenario. We find significant increases and decreases in total column ozone, depending on regions and seasons.
Lars Hoffmann, Paul F. Baumeister, Zhongyin Cai, Jan Clemens, Sabine Griessbach, Gebhard Günther, Yi Heng, Mingzhao Liu, Kaveh Haghighi Mood, Olaf Stein, Nicole Thomas, Bärbel Vogel, Xue Wu, and Ling Zou
Geosci. Model Dev., 15, 2731–2762, https://doi.org/10.5194/gmd-15-2731-2022, https://doi.org/10.5194/gmd-15-2731-2022, 2022
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We describe the new version (2.2) of the Lagrangian transport model MPTRAC, which has been ported for application on GPUs. The model was verified by comparing kinematic trajectories and synthetic tracer simulations for the free troposphere and stratosphere from GPUs and CPUs. Benchmarking showed a speed-up of a factor of 16 of GPU-enabled simulations compared to CPU-only runs, indicating the great potential of applying GPUs for Lagrangian transport simulations on upcoming HPC systems.
Andy Jones, Jim M. Haywood, Adam A. Scaife, Olivier Boucher, Matthew Henry, Ben Kravitz, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Roland Séférian, Simone Tilmes, and Daniele Visioni
Atmos. Chem. Phys., 22, 2999–3016, https://doi.org/10.5194/acp-22-2999-2022, https://doi.org/10.5194/acp-22-2999-2022, 2022
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Simulations by six Earth-system models of geoengineering by introducing sulfuric acid aerosols into the tropical stratosphere are compared. A robust impact on the northern wintertime North Atlantic Oscillation is found, exacerbating precipitation reduction over parts of southern Europe. In contrast, the models show no consistency with regard to impacts on the Quasi-Biennial Oscillation, although results do indicate a risk that the oscillation could become locked into a permanent westerly phase.
Valentin Lauther, Bärbel Vogel, Johannes Wintel, Andrea Rau, Peter Hoor, Vera Bense, Rolf Müller, and C. Michael Volk
Atmos. Chem. Phys., 22, 2049–2077, https://doi.org/10.5194/acp-22-2049-2022, https://doi.org/10.5194/acp-22-2049-2022, 2022
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We show airborne in situ measurements of the very short-lived ozone-depleting substances CH2Cl2 and CHCl3, revealing particularly high concentrations of both species in the lower stratosphere. Back-trajectory calculations and 3D model simulations show that the air masses with high concentrations originated in the Asian boundary layer and were transported via the Asian summer monsoon. We also identify a fast transport pathway into the stratosphere via the North American monsoon and by hurricanes.
Daniele Visioni, Simone Tilmes, Charles Bardeen, Michael Mills, Douglas G. MacMartin, Ben Kravitz, and Jadwiga H. Richter
Atmos. Chem. Phys., 22, 1739–1756, https://doi.org/10.5194/acp-22-1739-2022, https://doi.org/10.5194/acp-22-1739-2022, 2022
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Aerosols are simulated in a simplified way in climate models: in the model analyzed here, they are represented in every grid as described by three simple logarithmic distributions, mixing all different species together. The size can evolve when new particles are formed, particles merge together to create a larger one or particles are deposited to the surface. This approximation normally works fairly well. Here we show however that when large amounts of sulfate are simulated, there are problems.
Dina Khordakova, Christian Rolf, Jens-Uwe Grooß, Rolf Müller, Paul Konopka, Andreas Wieser, Martina Krämer, and Martin Riese
Atmos. Chem. Phys., 22, 1059–1079, https://doi.org/10.5194/acp-22-1059-2022, https://doi.org/10.5194/acp-22-1059-2022, 2022
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Extreme storms transport humidity from the troposphere to the stratosphere. Here it has a strong impact on the climate. With ongoing global warming, we expect more storms and, hence, an enhancement of this effect. A case study was performed in order to measure the impact of the direct injection of water vapor into the lower stratosphere. The measurements displayed a significant transport of water vapor into the lower stratosphere, and this was supported by satellite and reanalysis data.
Nicholas A. Davis, Patrick Callaghan, Isla R. Simpson, and Simone Tilmes
Atmos. Chem. Phys., 22, 197–214, https://doi.org/10.5194/acp-22-197-2022, https://doi.org/10.5194/acp-22-197-2022, 2022
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Specified dynamics schemes attempt to constrain the atmospheric circulation in a climate model to isolate the role of transport in chemical variability, evaluate model physics, and interpret field campaign observations. We show that the specified dynamics scheme in CESM2 erroneously suppresses convection and induces circulation errors that project onto errors in tracers, even using the most optimal settings. Development of a more sophisticated scheme is necessary for future progress.
Anton Laakso, Ulrike Niemeier, Daniele Visioni, Simone Tilmes, and Harri Kokkola
Atmos. Chem. Phys., 22, 93–118, https://doi.org/10.5194/acp-22-93-2022, https://doi.org/10.5194/acp-22-93-2022, 2022
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The use of different spatio-temporal sulfur injection strategies with different magnitudes to create an artificial reflective aerosol layer to cool the climate is studied using sectional and modal aerosol schemes in a climate model. There are significant differences in the results depending on the aerosol microphysical module used. Different spatio-temporal injection strategies have a significant impact on the magnitude and zonal distribution of radiative forcing and atmospheric dynamics.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Prashant Chavan, Suvarna Fadnavis, Tanusri Chakroborty, Christopher E. Sioris, Sabine Griessbach, and Rolf Müller
Atmos. Chem. Phys., 21, 14371–14384, https://doi.org/10.5194/acp-21-14371-2021, https://doi.org/10.5194/acp-21-14371-2021, 2021
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Biomass burning (BB) over Asia is a strong source of carbonaceous aerosols during spring. Here, we show an outflow of Asian BB carbonaceous aerosols into the UTLS. These aerosols enhance atmospheric heating and produce circulation changes that lead to the enhancement of water vapor in the UTLS over the tropics. In the stratosphere, water vapor is further transported to the South Pole by the Brewer–Dobson circulation. Enhancement of water vapor in the UTLS has implications for climate change.
Jayanarayanan Kuttippurath, Wuhu Feng, Rolf Müller, Pankaj Kumar, Sarath Raj, Gopalakrishna Pillai Gopikrishnan, and Raina Roy
Atmos. Chem. Phys., 21, 14019–14037, https://doi.org/10.5194/acp-21-14019-2021, https://doi.org/10.5194/acp-21-14019-2021, 2021
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The Arctic winter/spring 2020 was one of the coldest with a strong and long-lasting vortex, high chlorine activation, severe denitrification, and unprecedented ozone loss. The loss was even equal to the levels of some of the warm Antarctic winters. Total column ozone values below 220 DU for several weeks and ozone loss saturation were observed during the period. These results show an unusual meteorology and warrant dedicated studies on the impact of climate change on ozone loss.
Thierno Doumbia, Claire Granier, Nellie Elguindi, Idir Bouarar, Sabine Darras, Guy Brasseur, Benjamin Gaubert, Yiming Liu, Xiaoqin Shi, Trissevgeni Stavrakou, Simone Tilmes, Forrest Lacey, Adrien Deroubaix, and Tao Wang
Earth Syst. Sci. Data, 13, 4191–4206, https://doi.org/10.5194/essd-13-4191-2021, https://doi.org/10.5194/essd-13-4191-2021, 2021
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Most countries around the world have implemented control measures to combat the spread of the COVID-19 pandemic, resulting in significant changes in economic and personal activities. We developed the CONFORM (COvid-19 adjustmeNt Factors fOR eMissions) dataset to account for changes in emissions during lockdowns. This dataset was created with the intention of being directly applicable to existing global and regional inventories used in chemical transport models.
Ralf Weigel, Christoph Mahnke, Manuel Baumgartner, Antonis Dragoneas, Bärbel Vogel, Felix Ploeger, Silvia Viciani, Francesco D'Amato, Silvia Bucci, Bernard Legras, Beiping Luo, and Stephan Borrmann
Atmos. Chem. Phys., 21, 11689–11722, https://doi.org/10.5194/acp-21-11689-2021, https://doi.org/10.5194/acp-21-11689-2021, 2021
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In July and August 2017, eight StratoClim mission flights of the Geophysica reached up to 20 km in the Asian monsoon anticyclone. New particle formation (NPF) was identified in situ by abundant nucleation-mode aerosols (6–15 nm in diameter) with mixing ratios of up to 50 000 mg−1. NPF occurred most frequently at 12–16 km with fractions of non-volatile residues of down to 15 %. Abundance and productivity of observed NPF indicate its ability to promote the Asian tropopause aerosol layer.
Lukas Krasauskas, Jörn Ungermann, Peter Preusse, Felix Friedl-Vallon, Andreas Zahn, Helmut Ziereis, Christian Rolf, Felix Plöger, Paul Konopka, Bärbel Vogel, and Martin Riese
Atmos. Chem. Phys., 21, 10249–10272, https://doi.org/10.5194/acp-21-10249-2021, https://doi.org/10.5194/acp-21-10249-2021, 2021
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A Rossby wave (RW) breaking event was observed over the North Atlantic during the WISE measurement campaign in October 2017. Infrared limb sounding measurements of trace gases in the lower stratosphere, including high-resolution 3-D tomographic reconstruction, revealed complex spatial structures in stratospheric tracers near the polar jet related to previous RW breaking events. Backward-trajectory analysis and tracer correlations were used to study mixing and stratosphere–troposphere exchange.
Daniele Visioni, Douglas G. MacMartin, Ben Kravitz, Olivier Boucher, Andy Jones, Thibaut Lurton, Michou Martine, Michael J. Mills, Pierre Nabat, Ulrike Niemeier, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 10039–10063, https://doi.org/10.5194/acp-21-10039-2021, https://doi.org/10.5194/acp-21-10039-2021, 2021
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A new set of simulations is used to investigate commonalities, differences and sources of uncertainty when simulating the injection of SO2 in the stratosphere in order to mitigate the effects of climate change (solar geoengineering). The models differ in how they simulate the aerosols and how they spread around the stratosphere, resulting in differences in projected regional impacts. Overall, however, the models agree that aerosols have the potential to mitigate the warming produced by GHGs.
Gerald Wetzel, Felix Friedl-Vallon, Norbert Glatthor, Jens-Uwe Grooß, Thomas Gulde, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Erik Kretschmer, Guido Maucher, Hans Nordmeyer, Hermann Oelhaf, Johannes Orphal, Christof Piesch, Björn-Martin Sinnhuber, Jörn Ungermann, and Bärbel Vogel
Atmos. Chem. Phys., 21, 8213–8232, https://doi.org/10.5194/acp-21-8213-2021, https://doi.org/10.5194/acp-21-8213-2021, 2021
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Measurements of the pollutants C2H6, C2H2, HCOOH, and PAN were performed in the North Atlantic UTLS region with the airborne limb imager GLORIA in 2017. Enhanced amounts of these species were detected in the upper troposphere and even in the lowermost stratosphere (PAN). Main sources of these gases are forest fires in North America and anthropogenic pollution in South Asia. Simulations of EMAC and CAMS are qualitatively able to reproduce the measured data but underestimate the absolute amounts.
Fernando Chouza, Thierry Leblanc, Mark Brewer, Patrick Wang, Sabino Piazzolla, Gabriele Pfister, Rajesh Kumar, Carl Drews, Simone Tilmes, Louisa Emmons, and Matthew Johnson
Atmos. Chem. Phys., 21, 6129–6153, https://doi.org/10.5194/acp-21-6129-2021, https://doi.org/10.5194/acp-21-6129-2021, 2021
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The tropospheric ozone lidar at the JPL Table Mountain Facility (TMF) was used to investigate the impact of Los Angeles (LA) Basin pollution transport and stratospheric intrusions in the planetary boundary layer on the San Gabriel Mountains. The results of this study indicate a dominant role of the LA Basin pollution on days when high ozone levels were observed at TMF (March–October period).
Ben Kravitz, Douglas G. MacMartin, Daniele Visioni, Olivier Boucher, Jason N. S. Cole, Jim Haywood, Andy Jones, Thibaut Lurton, Pierre Nabat, Ulrike Niemeier, Alan Robock, Roland Séférian, and Simone Tilmes
Atmos. Chem. Phys., 21, 4231–4247, https://doi.org/10.5194/acp-21-4231-2021, https://doi.org/10.5194/acp-21-4231-2021, 2021
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This study investigates multi-model response to idealized geoengineering (high CO2 with solar reduction) across two different generations of climate models. We find that, with the exception of a few cases, the results are unchanged between the different generations. This gives us confidence that broad conclusions about the response to idealized geoengineering are robust.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Chaim I. Garfinkel, Ohad Harari, Shlomi Ziskin Ziv, Jian Rao, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Fiona M. O'Connor, Neal Butchart, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, and Sean Davis
Atmos. Chem. Phys., 21, 3725–3740, https://doi.org/10.5194/acp-21-3725-2021, https://doi.org/10.5194/acp-21-3725-2021, 2021
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Water vapor is the dominant greenhouse gas in the atmosphere, and El Niño is the dominant mode of variability in the ocean–atmosphere system. The connection between El Niño and water vapor above ~ 17 km is unclear, with single-model studies reaching a range of conclusions. This study examines this connection in 12 different models. While there are substantial differences among the models, all models appear to capture the fundamental physical processes correctly.
Duseong S. Jo, Alma Hodzic, Louisa K. Emmons, Simone Tilmes, Rebecca H. Schwantes, Michael J. Mills, Pedro Campuzano-Jost, Weiwei Hu, Rahul A. Zaveri, Richard C. Easter, Balwinder Singh, Zheng Lu, Christiane Schulz, Johannes Schneider, John E. Shilling, Armin Wisthaler, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 3395–3425, https://doi.org/10.5194/acp-21-3395-2021, https://doi.org/10.5194/acp-21-3395-2021, 2021
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Secondary organic aerosol (SOA) is a major component of submicron particulate matter, but there are a lot of uncertainties in the future prediction of SOA. We used CESM 2.1 to investigate future IEPOX SOA concentration changes. The explicit chemistry predicted substantial changes in IEPOX SOA depending on the future scenario, but the parameterization predicted weak changes due to simplified chemistry, which shows the importance of correct physicochemical dependencies in future SOA prediction.
Andy Jones, Jim M. Haywood, Anthony C. Jones, Simone Tilmes, Ben Kravitz, and Alan Robock
Atmos. Chem. Phys., 21, 1287–1304, https://doi.org/10.5194/acp-21-1287-2021, https://doi.org/10.5194/acp-21-1287-2021, 2021
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Two different methods of simulating a geoengineering scenario are compared using data from two different Earth system models. One method is very idealised while the other includes details of a plausible mechanism. The results from both models agree that the idealised approach does not capture an impact found when detailed modelling is included, namely that geoengineering induces a positive phase of the North Atlantic Oscillation which leads to warmer, wetter winters in northern Europe.
Marc von Hobe, Felix Ploeger, Paul Konopka, Corinna Kloss, Alexey Ulanowski, Vladimir Yushkov, Fabrizio Ravegnani, C. Michael Volk, Laura L. Pan, Shawn B. Honomichl, Simone Tilmes, Douglas E. Kinnison, Rolando R. Garcia, and Jonathon S. Wright
Atmos. Chem. Phys., 21, 1267–1285, https://doi.org/10.5194/acp-21-1267-2021, https://doi.org/10.5194/acp-21-1267-2021, 2021
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The Asian summer monsoon (ASM) is known to foster transport of polluted tropospheric air into the stratosphere. To test and amend our picture of ASM vertical transport, we analyse distributions of airborne trace gas observations up to 20 km altitude near the main ASM vertical conduit south of the Himalayas. We also show that a new high-resolution version of the global chemistry climate model WACCM is able to reproduce the observations well.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126, https://doi.org/10.5194/acp-21-1105-2021, https://doi.org/10.5194/acp-21-1105-2021, 2021
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We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
Benjamin Gaubert, Louisa K. Emmons, Kevin Raeder, Simone Tilmes, Kazuyuki Miyazaki, Avelino F. Arellano Jr., Nellie Elguindi, Claire Granier, Wenfu Tang, Jérôme Barré, Helen M. Worden, Rebecca R. Buchholz, David P. Edwards, Philipp Franke, Jeffrey L. Anderson, Marielle Saunois, Jason Schroeder, Jung-Hun Woo, Isobel J. Simpson, Donald R. Blake, Simone Meinardi, Paul O. Wennberg, John Crounse, Alex Teng, Michelle Kim, Russell R. Dickerson, Hao He, Xinrong Ren, Sally E. Pusede, and Glenn S. Diskin
Atmos. Chem. Phys., 20, 14617–14647, https://doi.org/10.5194/acp-20-14617-2020, https://doi.org/10.5194/acp-20-14617-2020, 2020
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This study investigates carbon monoxide pollution in East Asia during spring using a numerical model, satellite remote sensing, and aircraft measurements. We found an underestimation of emission sources. Correcting the emission bias can improve air quality forecasting of carbon monoxide and other species including ozone. Results also suggest that controlling VOC and CO emissions, in addition to widespread NOx controls, can improve ozone pollution over East Asia.
Steven T. Turnock, Robert J. Allen, Martin Andrews, Susanne E. Bauer, Makoto Deushi, Louisa Emmons, Peter Good, Larry Horowitz, Jasmin G. John, Martine Michou, Pierre Nabat, Vaishali Naik, David Neubauer, Fiona M. O'Connor, Dirk Olivié, Naga Oshima, Michael Schulz, Alistair Sellar, Sungbo Shim, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, Tongwen Wu, and Jie Zhang
Atmos. Chem. Phys., 20, 14547–14579, https://doi.org/10.5194/acp-20-14547-2020, https://doi.org/10.5194/acp-20-14547-2020, 2020
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A first assessment is made of the historical and future changes in air pollutants from models participating in the 6th Coupled Model Intercomparison Project (CMIP6). Substantial benefits to future air quality can be achieved in future scenarios that implement measures to mitigate climate and involve reductions in air pollutant emissions, particularly methane. However, important differences are shown between models in the future regional projection of air pollutants under the same scenario.
Sreeharsha Hanumanthu, Bärbel Vogel, Rolf Müller, Simone Brunamonti, Suvarna Fadnavis, Dan Li, Peter Ölsner, Manish Naja, Bhupendra Bahadur Singh, Kunchala Ravi Kumar, Sunil Sonbawne, Hannu Jauhiainen, Holger Vömel, Beiping Luo, Teresa Jorge, Frank G. Wienhold, Ruud Dirkson, and Thomas Peter
Atmos. Chem. Phys., 20, 14273–14302, https://doi.org/10.5194/acp-20-14273-2020, https://doi.org/10.5194/acp-20-14273-2020, 2020
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During boreal summer, anthropogenic sources yield the Asian Tropopause Aerosol Layer (ATAL), found in Asia between about 13 and 18 km altitude. Balloon-borne measurements of the ATAL conducted in northern India in 2016 show the strong variability of the ATAL. To explain its observed variability, model simulations are performed to deduce the origin of air masses on the Earth's surface, which is important to develop recommendations for regulations of anthropogenic surface emissions of the ATAL.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Augustin Mortier, Jonas Gliß, Michael Schulz, Wenche Aas, Elisabeth Andrews, Huisheng Bian, Mian Chin, Paul Ginoux, Jenny Hand, Brent Holben, Hua Zhang, Zak Kipling, Alf Kirkevåg, Paolo Laj, Thibault Lurton, Gunnar Myhre, David Neubauer, Dirk Olivié, Knut von Salzen, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 20, 13355–13378, https://doi.org/10.5194/acp-20-13355-2020, https://doi.org/10.5194/acp-20-13355-2020, 2020
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We present a multiparameter analysis of the aerosol trends over the last 2 decades in the different regions of the world. In most of the regions, ground-based observations show a decrease in aerosol content in both the total atmospheric column and at the surface. The use of climate models, assessed against these observations, reveals however an increase in the total aerosol load, which is not seen with the sole use of observation due to partial coverage in space and time.
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.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Wenfu Tang, Benjamin Gaubert, Louisa Emmons, Yonghoon Choi, Joshua P. DiGangi, Glenn S. Diskin, Xiaomei Xu, Cenlin He, Helen Worden, Simone Tilmes, Rebecca Buchholz, Hannah S. Halliday, and Avelino F. Arellano
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-864, https://doi.org/10.5194/acp-2020-864, 2020
Revised manuscript not accepted
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A specific demonstration of the potential use of correlative information from carbon monoxide to refine estimates of regional carbon dioxide emissions from fossil fuel combustion.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
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We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
Yangyang Xu, Lei Lin, Simone Tilmes, Katherine Dagon, Lili Xia, Chenrui Diao, Wei Cheng, Zhili Wang, Isla Simpson, and Lorna Burnell
Earth Syst. Dynam., 11, 673–695, https://doi.org/10.5194/esd-11-673-2020, https://doi.org/10.5194/esd-11-673-2020, 2020
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Two geoengineering schemes to mitigate global warming, (a) capturing atmospheric CO2 and (b) injecting stratospheric sulfur gas, are compared. Based on two sets of large-ensemble model experiments, we show that sulfur injection will effectively mitigate projected terrestrial drying over the Americas, and the mitigation benefit will emerge more quickly than with carbon capture. Innovative means of sulfur injection should continue to be explored as one potential low-cost climate solution.
Ulrike Niemeier, Jadwiga H. Richter, and Simone Tilmes
Atmos. Chem. Phys., 20, 8975–8987, https://doi.org/10.5194/acp-20-8975-2020, https://doi.org/10.5194/acp-20-8975-2020, 2020
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Artificial injections of SO2 into the tropical stratosphere show an impact on the quasi-biennial oscillation (QBO). Different numerical models show only qualitatively but not quantitatively consistent impacts. We show for two models that the response of the QBO is similar when a similar stratospheric heating rate is induced by SO2 injections of different amounts. The reason is very different vertical advection in the two models resulting in different aerosol burden and heating of the aerosols.
Simone Tilmes, Douglas G. MacMartin, Jan T. M. Lenaerts, Leo van Kampenhout, Laura Muntjewerf, Lili Xia, Cheryl S. Harrison, Kristen M. Krumhardt, Michael J. Mills, Ben Kravitz, and Alan Robock
Earth Syst. Dynam., 11, 579–601, https://doi.org/10.5194/esd-11-579-2020, https://doi.org/10.5194/esd-11-579-2020, 2020
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This paper introduces new geoengineering model experiments as part of a larger model intercomparison effort, using reflective particles to block some of the incoming solar radiation to reach surface temperature targets. Outcomes of these applications are contrasted based on a high greenhouse gas emission pathway and a pathway with strong mitigation and negative emissions after 2040. We compare quantities that matter for societal and ecosystem impacts between the different scenarios.
Daniele Visioni, Giovanni Pitari, Vincenzo Rizi, Marco Iarlori, Irene Cionni, Ilaria Quaglia, Hideharu Akiyoshi, Slimane Bekki, Neal Butchart, Martin Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando Garcia, Patrick Joeckel, Douglas Kinnison, Jean-François Lamarque, Marion Marchand, Martine Michou, Olaf Morgenstern, Tatsuya Nagashima, Fiona M. O'Connor, Luke D. Oman, David Plummer, Eugene Rozanov, David Saint-Martin, Robyn Schofield, John Scinocca, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Holger Tost, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-525, https://doi.org/10.5194/acp-2020-525, 2020
Preprint withdrawn
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In this work we analyse the trend in ozone profiles taken at L'Aquila (Italy, 42.4° N) for seventeen years, between 2000 and 2016 and compare them against already available measured ozone trends. We try to understand and explain the observed trends at various heights in light of the simulations from seventeen different model, highlighting the contribution of changes in circulation and chemical ozone loss during this time period.
Alma Hodzic, Pedro Campuzano-Jost, Huisheng Bian, Mian Chin, Peter R. Colarco, Douglas A. Day, Karl D. Froyd, Bernd Heinold, Duseong S. Jo, Joseph M. Katich, John K. Kodros, Benjamin A. Nault, Jeffrey R. Pierce, Eric Ray, Jacob Schacht, Gregory P. Schill, Jason C. Schroder, Joshua P. Schwarz, Donna T. Sueper, Ina Tegen, Simone Tilmes, Kostas Tsigaridis, Pengfei Yu, and Jose L. Jimenez
Atmos. Chem. Phys., 20, 4607–4635, https://doi.org/10.5194/acp-20-4607-2020, https://doi.org/10.5194/acp-20-4607-2020, 2020
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Organic aerosol (OA) is a key source of uncertainty in aerosol climate effects. We present the first pole-to-pole OA characterization during the NASA Atmospheric Tomography aircraft mission. OA has a strong seasonal and zonal variability, with the highest levels in summer and over fire-influenced regions and the lowest ones in the southern high latitudes. We show that global models predict the OA distribution well but not the relative contribution of OA emissions vs. chemical production.
Dan Li, Bärbel Vogel, Rolf Müller, Jianchun Bian, Gebhard Günther, Felix Ploeger, Qian Li, Jinqiang Zhang, Zhixuan Bai, Holger Vömel, and Martin Riese
Atmos. Chem. Phys., 20, 4133–4152, https://doi.org/10.5194/acp-20-4133-2020, https://doi.org/10.5194/acp-20-4133-2020, 2020
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Low ozone and low water vapour signatures in the UTLS were investigated using balloon-borne measurements and trajectory calculations. The results show that deep convection in tropical cyclones over the western Pacific transports boundary air parcels with low ozone into the tropopause region. Subsequently, these air parcels are dehydrated when passing the lowest temperature region (< 190 K) during quasi-horizontal advection.
Sabine Griessbach, Lars Hoffmann, Reinhold Spang, Peggy Achtert, Marc von Hobe, Nina Mateshvili, Rolf Müller, Martin Riese, Christian Rolf, Patric Seifert, and Jean-Paul Vernier
Atmos. Meas. Tech., 13, 1243–1271, https://doi.org/10.5194/amt-13-1243-2020, https://doi.org/10.5194/amt-13-1243-2020, 2020
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In this paper we study the cloud top height derived from MIPAS measurements. Previous studies showed contradictory results with respect to MIPAS, both underestimating and overestimating cloud top height. We used simulations and found that overestimation and/or underestimation depend on cloud extinction. To support our findings we compared MIPAS cloud top heights of volcanic sulfate aerosol with measurements from CALIOP, ground-based lidar, and ground-based twilight measurements.
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.
Xiaolu Yan, Paul Konopka, Felix Ploeger, Aurélien Podglajen, Jonathon S. Wright, Rolf Müller, and Martin Riese
Atmos. Chem. Phys., 19, 15629–15649, https://doi.org/10.5194/acp-19-15629-2019, https://doi.org/10.5194/acp-19-15629-2019, 2019
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The Asian and North American summer monsoons (ASM and NASM) have considerable influence on stratospheric chemistry and physics. More air mass is transported from the monsoon regions to the tropical stratosphere when the tracers are released clearly below the tropopause than when they are released close to the tropopause. Results for different altitudes of air origin reveal two transport pathways (monsoon and tropical) from the upper troposphere over the monsoon regions to the tropical pipe.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
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.
Wenxiu Sun, Peter Hess, Gang Chen, and Simone Tilmes
Atmos. Chem. Phys., 19, 12917–12933, https://doi.org/10.5194/acp-19-12917-2019, https://doi.org/10.5194/acp-19-12917-2019, 2019
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Using both observations and a chemistry climate–model we establish that in most locations changes in the waviness of the 500 hPa flow field, as measured by the local anticyclonic wave activity (AWA), explain a significant fraction of the interannual variability in surface ozone over the United States. In addition, we find that the change in AWA in a future climate (circa 2100) is predicted to cause a change in surface ozone ranging between –6 ppb and 6 ppb.
Suvarna Fadnavis, Rolf Müller, Gayatry Kalita, Matthew Rowlinson, Alexandru Rap, Jui-Lin Frank Li, Blaž Gasparini, and Anton Laakso
Atmos. Chem. Phys., 19, 9989–10008, https://doi.org/10.5194/acp-19-9989-2019, https://doi.org/10.5194/acp-19-9989-2019, 2019
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This paper highlights the impact of Asian anthropogenic emission changes in SO2 on sulfate loading in the Asian upper troposphere–lower stratosphere from a global chemistry–climate model and satellite remote sensing. Estimated seasonal mean direct radiative forcing at the top of the atmosphere induced by the increase in Indian SO2 is −0.2–−1.5 W m2 over India. Chinese SO2 emission reduction leads to a positive radiative forcing of ~0.6–6 W m2 over China. It will likely decrease Indian rainfall.
Ohad Harari, Chaim I. Garfinkel, Shlomi Ziskin Ziv, Olaf Morgenstern, Guang Zeng, Simone Tilmes, Douglas Kinnison, Makoto Deushi, Patrick Jöckel, Andrea Pozzer, Fiona M. O'Connor, and Sean Davis
Atmos. Chem. Phys., 19, 9253–9268, https://doi.org/10.5194/acp-19-9253-2019, https://doi.org/10.5194/acp-19-9253-2019, 2019
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Ozone depletion in the Antarctic has been shown to influence surface conditions, but the effects of ozone depletion in the Arctic on surface climate are unclear. We show that Arctic ozone does influence surface climate in both polar regions and tropical regions, though the proximate cause of these surface impacts is not yet clear.
Bärbel Vogel, Rolf Müller, Gebhard Günther, Reinhold Spang, Sreeharsha Hanumanthu, Dan Li, Martin Riese, and Gabriele P. Stiller
Atmos. Chem. Phys., 19, 6007–6034, https://doi.org/10.5194/acp-19-6007-2019, https://doi.org/10.5194/acp-19-6007-2019, 2019
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We identified the transport pathways of air masses from the region of the Asian monsoon (e.g. pollution and greenhouse gases caused by increasing population and growing industries in Asia) into the lower stratosphere. Even small changes of the chemical composition of the lower stratosphere have an impact on surface climate (e.g. surface temperatures). Therefore, it is important to identify transport pathways to the stratosphere to allow potential environmental risks to be assessed.
Sabine Robrecht, Bärbel Vogel, Jens-Uwe Grooß, Karen Rosenlof, Troy Thornberry, Andrew Rollins, Martina Krämer, Lance Christensen, and Rolf Müller
Atmos. Chem. Phys., 19, 5805–5833, https://doi.org/10.5194/acp-19-5805-2019, https://doi.org/10.5194/acp-19-5805-2019, 2019
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The potential destruction of stratospheric ozone in the mid-latitudes has been discussed recently. We analysed this ozone loss mechanism and its sensitivities. In a certain temperature range, we found a threshold in water vapour, which has to be exceeded for ozone loss to occur. We show the dependence of this water vapour threshold on temperature, sulfate content and air composition. This study provides a basis to estimate the impact of potential sulphate geoengineering on stratospheric ozone.
Huang Yang, Darryn W. Waugh, Clara Orbe, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, Patrick Jöckel, Susan E. Strahan, Kane A. Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 5511–5528, https://doi.org/10.5194/acp-19-5511-2019, https://doi.org/10.5194/acp-19-5511-2019, 2019
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We evaluate the performance of a suite of models in simulating the large-scale transport from the northern midlatitudes to the Arctic using a CO-like idealized tracer. We find a large multi-model spread of the Arctic concentration of this CO-like tracer that is well correlated with the differences in the location of the midlatitude jet as well as the northern Hadley Cell edge. Our results suggest the Hadley Cell is key and zonal-mean transport by surface meridional flow needs better constraint.
Lars Hoffmann, Gebhard Günther, Dan Li, Olaf Stein, Xue Wu, Sabine Griessbach, Yi Heng, Paul Konopka, Rolf Müller, Bärbel Vogel, and Jonathon S. Wright
Atmos. Chem. Phys., 19, 3097–3124, https://doi.org/10.5194/acp-19-3097-2019, https://doi.org/10.5194/acp-19-3097-2019, 2019
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ECMWF's new ERA5 reanalysis provides higher spatiotemporal resolution, yielding an improved representation of meso- and synoptic-scale features of the atmosphere. We assessed the impact of this challenging new data set on Lagrangian trajectory calculations for the free troposphere and stratosphere. Key findings are considerable transport deviations between the ERA5 and ERA-Interim simulations as well as significantly improved conservation of potential temperature in the stratosphere for ERA5.
Ines Tritscher, Jens-Uwe Grooß, Reinhold Spang, Michael C. Pitts, Lamont R. Poole, Rolf Müller, and Martin Riese
Atmos. Chem. Phys., 19, 543–563, https://doi.org/10.5194/acp-19-543-2019, https://doi.org/10.5194/acp-19-543-2019, 2019
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We present Lagrangian simulations of polar stratospheric clouds (PSCs) for the Arctic winter 2009/2010 and the Antarctic winter 2011 using the Chemical Lagrangian Model of the Stratosphere (CLaMS). The paper comprises a detailed model description with ice PSCs and related dehydration being the focus of this study. Comparisons between our simulations and observations from different satellites on season-long and vortex-wide scales as well as for single PSC events show an overall good agreement.
Mohamadou Diallo, Paul Konopka, Michelle L. Santee, Rolf Müller, Mengchu Tao, Kaley A. Walker, Bernard Legras, Martin Riese, Manfred Ern, and Felix Ploeger
Atmos. Chem. Phys., 19, 425–446, https://doi.org/10.5194/acp-19-425-2019, https://doi.org/10.5194/acp-19-425-2019, 2019
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This paper assesses the structural changes in the shallow and transition branches of the BDC induced by El Nino using the Lagrangian model simulations driven by ERAi and JRA-55 combined with MLS observations. We found a clear evidence of a weakening of the transition branch due to an upward shift in the dissipation height of the planetary and gravity waves and a strengthening of the shallow branch due to enhanced GW breaking in the tropics–subtropics and PW breaking at high latitudes.
Dan Li, Bärbel Vogel, Rolf Müller, Jianchun Bian, Gebhard Günther, Qian Li, Jinqiang Zhang, Zhixuan Bai, Holger Vömel, and Martin Riese
Atmos. Chem. Phys., 18, 17979–17994, https://doi.org/10.5194/acp-18-17979-2018, https://doi.org/10.5194/acp-18-17979-2018, 2018
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Balloon-borne measurements performed over Lhasa in August 2013 are investigated using CLaMS trajectory calculations. Here, we focus on high ozone mixing ratios in the free troposphere. Our findings demonstrate that both stratospheric intrusions and convective transport of air pollution play a major role in enhancing middle and upper tropospheric ozone.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
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Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Xinyi Dong, Joshua S. Fu, Qingzhao Zhu, Jian Sun, Jiani Tan, Terry Keating, Takashi Sekiya, Kengo Sudo, Louisa Emmons, Simone Tilmes, Jan Eiof Jonson, Michael Schulz, Huisheng Bian, Mian Chin, Yanko Davila, Daven Henze, Toshihiko Takemura, Anna Maria Katarina Benedictow, and Kan Huang
Atmos. Chem. Phys., 18, 15581–15600, https://doi.org/10.5194/acp-18-15581-2018, https://doi.org/10.5194/acp-18-15581-2018, 2018
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We have applied the HTAP phase II multi-model data to investigate the long-range transport impacts on surface concentration and column density of PM from Europe and Russia, Belarus, and Ukraine to eastern Asia, with a special focus on the long-range transport contribution during haze episodes in China. We found that long-range transport plays a more important role in elevating the background concentration of surface PM during the haze days.
Daniele Visioni, Giovanni Pitari, Glauco di Genova, Simone Tilmes, and Irene Cionni
Atmos. Chem. Phys., 18, 14867–14887, https://doi.org/10.5194/acp-18-14867-2018, https://doi.org/10.5194/acp-18-14867-2018, 2018
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Many side effects of sulfate geoengineering have to be analyzed before the world can even consider deploying this method of solar radiation management. In particular, we show that ice clouds in the upper troposphere are modified by a sulfate injection, producing a change that (by allowing for more planetary radiation to escape to space) would produce a further cooling. This might be important when considering the necessary amount of sulfate that needs to be injected to achieve a certain target.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald Prinn, Simone Tilmes, Louisa Emmons, Jean-François Lamarque, and Philip Cameron-Smith
Geosci. Model Dev., 11, 4155–4174, https://doi.org/10.5194/gmd-11-4155-2018, https://doi.org/10.5194/gmd-11-4155-2018, 2018
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We conduct three simulations of atmospheric chemistry using chemical mechanisms of different levels of complexity and compare their results to observations. We explore situations in which the simplified mechanisms match the output of the most complex mechanism, as well as when they diverge. We investigate how concurrent utilization of chemical mechanisms of different complexities can further our atmospheric-chemistry understanding at various scales and give some strategies for future research.
Mohamadou Diallo, Martin Riese, Thomas Birner, Paul Konopka, Rolf Müller, Michaela I. Hegglin, Michelle L. Santee, Mark Baldwin, Bernard Legras, and Felix Ploeger
Atmos. Chem. Phys., 18, 13055–13073, https://doi.org/10.5194/acp-18-13055-2018, https://doi.org/10.5194/acp-18-13055-2018, 2018
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The unprecedented timing of an El Niño event aligned with the disrupted QBO in 2015–2016 caused a perturbation to the stratospheric circulation, affecting trace gases. This paper resolves the puzzling response of the lower stratospheric water vapor by showing that the QBO disruption reversed the lower stratosphere moistening triggered by the alignment of the El Niño event with a westerly QBO in early boreal winter.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Johannes Flemming, Toshihiko Takemura, Huisheng Bian, Qingzhao Zhu, Cheng-En Yang, and Terry Keating
Atmos. Chem. Phys., 18, 12223–12240, https://doi.org/10.5194/acp-18-12223-2018, https://doi.org/10.5194/acp-18-12223-2018, 2018
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Have contributions of hemispheric air pollution to deposition at global scale been overlooked in the past years? How do we assess the critical load for the acid deposition when we look for the demand of forest and crop? This study highlights the significant impact of hemispheric transport on deposition in coastal regions, open ocean and low-emission regions. Further research is proposed for improving ecosystem and human health in these regions, with regards to the enhanced hemispheric transport.
Pakawat Phalitnonkiat, Peter G. M. Hess, Mircea D. Grigoriu, Gennady Samorodnitsky, Wenxiu Sun, Ellie Beaudry, Simone Tilmes, Makato Deushi, Beatrice Josse, David Plummer, and Kengo Sudo
Atmos. Chem. Phys., 18, 11927–11948, https://doi.org/10.5194/acp-18-11927-2018, https://doi.org/10.5194/acp-18-11927-2018, 2018
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The co-occurrence of heat waves and pollution events and the resulting high mortality rates emphasize the importance of the co-occurrence of pollution and temperature extremes. We analyze ozone and temperature extremes and their joint occurrence over the United States during the summer months (JJA) in measurement data and in model simulations of the present and future climates.
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.
Steven T. Turnock, Oliver Wild, Frank J. Dentener, Yanko Davila, Louisa K. Emmons, Johannes Flemming, Gerd A. Folberth, Daven K. Henze, Jan E. Jonson, Terry J. Keating, Sudo Kengo, Meiyun Lin, Marianne Lund, Simone Tilmes, and Fiona M. O'Connor
Atmos. Chem. Phys., 18, 8953–8978, https://doi.org/10.5194/acp-18-8953-2018, https://doi.org/10.5194/acp-18-8953-2018, 2018
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A simple parameterisation was developed in this study to provide a rapid assessment of the impacts and uncertainties associated with future emission control strategies by predicting changes to surface ozone air quality and near-term climate forcing of ozone. Future emissions scenarios based on currently implemented legislation are shown to worsen surface ozone air quality and enhance near-term climate warming, with changes in methane becoming increasingly important in the future.
Jens-Uwe Grooß, Rolf Müller, Reinhold Spang, Ines Tritscher, Tobias Wegner, Martyn P. Chipperfield, Wuhu Feng, Douglas E. Kinnison, and Sasha Madronich
Atmos. Chem. Phys., 18, 8647–8666, https://doi.org/10.5194/acp-18-8647-2018, https://doi.org/10.5194/acp-18-8647-2018, 2018
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We investigate a discrepancy between model simulations and observations of HCl in the dark polar stratosphere. In early winter, the less-well-studied period of the onset of chlorine activation, observations show a much faster depletion of HCl than simulations of three models. This points to some unknown process that is currently not represented in the models. Various hypotheses for potential causes are investigated that partly reduce the discrepancy. The impact on polar ozone depletion is low.
Liubov Poshyvailo, Rolf Müller, Paul Konopka, Gebhard Günther, Martin Riese, Aurélien Podglajen, and Felix Ploeger
Atmos. Chem. Phys., 18, 8505–8527, https://doi.org/10.5194/acp-18-8505-2018, https://doi.org/10.5194/acp-18-8505-2018, 2018
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Water vapour (H2O) in the UTLS is a key player for global radiation, which is critical for predictions of future climate change. We investigate the effects of current uncertainties in tropopause temperature, horizontal transport and small-scale mixing on simulated H2O, using the Chemical Lagrangian Model of the Stratosphere. Our sensitivity studies provide new insights into the leading processes controlling stratospheric H2O, important for assessing and improving climate model projections.
Benjamin Brown-Steiner, Noelle E. Selin, Ronald G. Prinn, Erwan Monier, Simone Tilmes, Louisa Emmons, and Fernando Garcia-Menendez
Atmos. Chem. Phys., 18, 8373–8388, https://doi.org/10.5194/acp-18-8373-2018, https://doi.org/10.5194/acp-18-8373-2018, 2018
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Detecting signals in observations and simulations of atmospheric chemistry is difficult due to the underlying variability in the chemistry, meteorology, and climatology. Here we examine the scale dependence of ozone variability and explore strategies for reducing or averaging this variability and thereby enhancing ozone signal detection capabilities. We find that 10–15 years of temporal averaging, and some level of spatial averaging, reduces the risk of overconfidence in ozone signals.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
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We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
Xiaolu Yan, Paul Konopka, Felix Ploeger, Mengchu Tao, Rolf Müller, Michelle L. Santee, Jianchun Bian, and Martin Riese
Atmos. Chem. Phys., 18, 8079–8096, https://doi.org/10.5194/acp-18-8079-2018, https://doi.org/10.5194/acp-18-8079-2018, 2018
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Many works investigate the impact of ENSO on the troposphere. However, only a few works check the impact of ENSO at higher altitudes.
Here, we analyse the impact of ENSO on the vicinity of the tropopause using reanalysis, satellite, in situ and model data. We find that ENSO shows the strongest signal in winter, but its impact can last until early the next summer. The ENSO anomaly is insignificant in late summer. Our study can help to understand the atmosphere propagation after ENSO.
Xiaokang Wu, Huang Yang, Darryn W. Waugh, Clara Orbe, Simone Tilmes, and Jean-Francois Lamarque
Atmos. Chem. Phys., 18, 7439–7452, https://doi.org/10.5194/acp-18-7439-2018, https://doi.org/10.5194/acp-18-7439-2018, 2018
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The seasonal and interannual variability of transport times from northern mid-latitudes into the southern hemisphere is examined using simulations of
agetracers. The largest variability occurs near the surface close to the tropical convergence zones, but the peak is further south and there is a smaller tropical–extratropical contrast for tracers with more rapid loss. Hence the variability of trace gases in the southern extratropics will vary with their chemical lifetime.
Clara Orbe, Huang Yang, Darryn W. Waugh, Guang Zeng, Olaf Morgenstern, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, David A. Plummer, John F. Scinocca, Beatrice Josse, Virginie Marecal, Patrick Jöckel, Luke D. Oman, Susan E. Strahan, Makoto Deushi, Taichu Y. Tanaka, Kohei Yoshida, Hideharu Akiyoshi, Yousuke Yamashita, Andreas Stenke, Laura Revell, Timofei Sukhodolov, Eugene Rozanov, Giovanni Pitari, Daniele Visioni, Kane A. Stone, Robyn Schofield, and Antara Banerjee
Atmos. Chem. Phys., 18, 7217–7235, https://doi.org/10.5194/acp-18-7217-2018, https://doi.org/10.5194/acp-18-7217-2018, 2018
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In this study we compare a few atmospheric transport properties among several numerical models that are used to study the influence of atmospheric chemistry on climate. We show that there are large differences among models in terms of the timescales that connect the Northern Hemisphere midlatitudes, where greenhouse gases and ozone-depleting substances are emitted, to the Southern Hemisphere. Our results may have important implications for how models represent atmospheric composition.
Jiani Tan, Joshua S. Fu, Frank Dentener, Jian Sun, Louisa Emmons, Simone Tilmes, Kengo Sudo, Johannes Flemming, Jan Eiof Jonson, Sylvie Gravel, Huisheng Bian, Yanko Davila, Daven K. Henze, Marianne T. Lund, Tom Kucsera, Toshihiko Takemura, and Terry Keating
Atmos. Chem. Phys., 18, 6847–6866, https://doi.org/10.5194/acp-18-6847-2018, https://doi.org/10.5194/acp-18-6847-2018, 2018
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We study the distributions of sulfur and nitrogen deposition, which are associated with current environmental issues such as formation of acid rain and ecosystem eutrophication and result in widespread problems such as loss of environmental diversity, harming the crop yield and even food insecurity. According to our study, both the amount and distribution of sulfate and nitrogen deposition have changed significantly in the last decade, particularly in East Asia, South Asia and Southeast Asia.
Reinhold Spang, Lars Hoffmann, Rolf Müller, Jens-Uwe Grooß, Ines Tritscher, Michael Höpfner, Michael Pitts, Andrew Orr, and Martin Riese
Atmos. Chem. Phys., 18, 5089–5113, https://doi.org/10.5194/acp-18-5089-2018, https://doi.org/10.5194/acp-18-5089-2018, 2018
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This paper represents an unprecedented pole-covering day- and nighttime climatology of the polar stratospheric clouds (PSCs) based on satellite measurements, their spatial distribution, and composition of different particle types. The climatology has a high potential for the validation and improvement of PSC schemes in chemical transport and chemistry–climate models, which is important for a better prediction of future polar ozone loss in a changing climate.
Rolf Müller, Jens-Uwe Grooß, Abdul Mannan Zafar, Sabine Robrecht, and Ralph Lehmann
Atmos. Chem. Phys., 18, 2985–2997, https://doi.org/10.5194/acp-18-2985-2018, https://doi.org/10.5194/acp-18-2985-2018, 2018
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This paper revisits the chemistry leading to strong ozone depletion in the Antarctic. We focus on the heart of the ozone layer in the lowermost stratosphere in the core of the vortex. We argue that chemical cycles (referred to as HCl null cycles) that have hitherto been largely neglected counteract the deactivation of chlorine and are therefore key to ozone depletion in the core of the Antarctic vortex. The key process to full activation of chlorine is the photolysis of formaldehyde.
Christian Rolf, Bärbel Vogel, Peter Hoor, Armin Afchine, Gebhard Günther, Martina Krämer, Rolf Müller, Stefan Müller, Nicole Spelten, and Martin Riese
Atmos. Chem. Phys., 18, 2973–2983, https://doi.org/10.5194/acp-18-2973-2018, https://doi.org/10.5194/acp-18-2973-2018, 2018
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The Asian monsoon is a pronounced circulation system linked to rapid vertical transport of surface air from India and east Asia in the summer months. We found, based on aircraft measurements, higher concentration of water vapor in the lowermost stratosphere caused by the Asian monsoon. Enrichment of water vapor concentrations in the lowermost stratosphere impacts the radiation budget and thus climate. Understanding those variations in water vapor is important for climate projections.
Lauren Marshall, Anja Schmidt, Matthew Toohey, Ken S. Carslaw, Graham W. Mann, Michael Sigl, Myriam Khodri, Claudia Timmreck, Davide Zanchettin, William T. Ball, Slimane Bekki, James S. A. Brooke, Sandip Dhomse, Colin Johnson, Jean-Francois Lamarque, Allegra N. LeGrande, Michael J. Mills, Ulrike Niemeier, James O. Pope, Virginie Poulain, Alan Robock, Eugene Rozanov, Andrea Stenke, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, and Fiona Tummon
Atmos. Chem. Phys., 18, 2307–2328, https://doi.org/10.5194/acp-18-2307-2018, https://doi.org/10.5194/acp-18-2307-2018, 2018
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We use four global aerosol models to compare the simulated sulfate deposition from the 1815 Mt. Tambora eruption to ice core records. Inter-model volcanic sulfate deposition differs considerably. Volcanic sulfate deposited on polar ice sheets is used to estimate the atmospheric sulfate burden and subsequently radiative forcing of historic eruptions. Our results suggest that deriving such relationships from model simulations may be associated with greater uncertainties than previously thought.
Lili Xia, Peer J. Nowack, Simone Tilmes, and Alan Robock
Atmos. Chem. Phys., 17, 11913–11928, https://doi.org/10.5194/acp-17-11913-2017, https://doi.org/10.5194/acp-17-11913-2017, 2017
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Ozone is a key air pollutant. We model two geoengineering schemes, stratospheric sulfur injection and solar irradiance reduction, to compare their impacts on atmospheric ozone concentrations. With the nearly identical global mean surface temperature reduction, solar dimming increases global average surface ozone concentration, while sulfate injection decreases it. This difference is due to different stratosphere–troposphere exchange of ozone and tropospheric ozone chemistry in the two scenarios.
Daniele Visioni, Giovanni Pitari, Valentina Aquila, Simone Tilmes, Irene Cionni, Glauco Di Genova, and Eva Mancini
Atmos. Chem. Phys., 17, 11209–11226, https://doi.org/10.5194/acp-17-11209-2017, https://doi.org/10.5194/acp-17-11209-2017, 2017
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Sulfate geoengineering (SG), the sustained injection of SO2 in the lower stratosphere, is being discussed as a way to counterbalance surface warming, mimicking volcanic eruptions. In this paper, we analyse results from two models part of the GeoMIP project in order to understand the effect SG might have on the concentration and lifetime of methane, which acts in the atmosphere as a greenhouse gas. Understanding possible side effects of SG is a crucial step if its viability is to be assessed.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Dan Li, Bärbel Vogel, Jianchun Bian, Rolf Müller, Laura L. Pan, Gebhard Günther, Zhixuan Bai, Qian Li, Jinqiang Zhang, Qiujun Fan, and Holger Vömel
Atmos. Chem. Phys., 17, 4657–4672, https://doi.org/10.5194/acp-17-4657-2017, https://doi.org/10.5194/acp-17-4657-2017, 2017
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High-resolution ozone and water vapour profiles over Lhasa, China, were measured in August 2013. The correlations between ozone and water vapour profiles show a strong variability in the upper troposphere. These relationships were investigated using CLaMS trajectory calculations. The model results demonstrate that three tropical cyclones (Jebi, Utor, and Trami), occurring over the western Pacific, had a strong impact on the vertical structure of ozone and water vapour profiles.
Bin Chen, Bärbel Vogel, Xiangde Xu, and Shuai Yang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2017-216, https://doi.org/10.5194/acp-2017-216, 2017
Revised manuscript has not been submitted
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The Asian summer monsoon anticyclone is associated with a region in which surface emissions have been shown to enter the lower stratosphere in the Northern Hemisphe.We quantitatively characterized the properties of troposphere-to-stratosophere transport in term of the climatological sources and its variability in sub-seasoanal scale. This is the first attempt to examine the spatiotemporal evolution of convection sources at the sub-seasonal scale, particularly from a climatologic perspective.
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.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Chaitri Roy, Suvarna Fadnavis, Rolf Müller, D. C. Ayantika, Felix Ploeger, and Alexandru Rap
Atmos. Chem. Phys., 17, 1297–1311, https://doi.org/10.5194/acp-17-1297-2017, https://doi.org/10.5194/acp-17-1297-2017, 2017
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In the monsoon season, Asian NOx emissions are rapidly transported to the UTLS and can impact ozone in the UTLS. From chemistry–climate model simulations, we show that increasing Asian NOx emissions have enhanced ozone radiative forcing over Southeast Asia, which leads to significant warming over the Tibetan Plateau and increase precipitation over India. However, a further increase in NOx emissions elicited negative precipitation due to reversal of monsoon Hadley circulation.
Bärbel Vogel, Gebhard Günther, Rolf Müller, Jens-Uwe Grooß, Armin Afchine, Heiko Bozem, Peter Hoor, Martina Krämer, Stefan Müller, Martin Riese, Christian Rolf, Nicole Spelten, Gabriele P. Stiller, Jörn Ungermann, and Andreas Zahn
Atmos. Chem. Phys., 16, 15301–15325, https://doi.org/10.5194/acp-16-15301-2016, https://doi.org/10.5194/acp-16-15301-2016, 2016
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The identification of transport pathways from the Asian monsoon anticyclone into the lower stratosphere is unclear. Global simulations with the CLaMS model demonstrate that source regions in Asia and in the Pacific Ocean have a significant impact on the chemical composition of the lower stratosphere of the Northern Hemisphere by flooding the extratropical lower stratosphere with young moist air masses. Two main horizontal transport pathways from the Asian monsoon anticyclone are identified.
Camilla Weum Stjern, Bjørn Hallvard Samset, Gunnar Myhre, Huisheng Bian, Mian Chin, Yanko Davila, Frank Dentener, Louisa Emmons, Johannes Flemming, Amund Søvde Haslerud, Daven Henze, Jan Eiof Jonson, Tom Kucsera, Marianne Tronstad Lund, Michael Schulz, Kengo Sudo, Toshihiko Takemura, and Simone Tilmes
Atmos. Chem. Phys., 16, 13579–13599, https://doi.org/10.5194/acp-16-13579-2016, https://doi.org/10.5194/acp-16-13579-2016, 2016
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Air pollution can reach distant regions through intercontinental transport. Here we first present results from the Hemispheric Transport of Air Pollution Phase 2 exercise, where many models performed the same set of coordinated emission-reduction experiments. We find that mitigations have considerable extra-regional effects, and show that this is particularly true for black carbon emissions, as long-range transport elevates aerosols to higher levels where their radiative influence is stronger.
Sabine Griessbach, Lars Hoffmann, Reinhold Spang, Marc von Hobe, Rolf Müller, and Martin Riese
Atmos. Meas. Tech., 9, 4399–4423, https://doi.org/10.5194/amt-9-4399-2016, https://doi.org/10.5194/amt-9-4399-2016, 2016
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A new method for detecting aerosol in the UTLS based on infrared limb emission measurements is presented. The method was developed using radiative transfer simulations (including scattering) and Envisat MIPAS measurements. Results are presented for volcanic ash and sulfate aerosol originating from the Grimsvötn (Iceland), Puyehue–Cordon Caulle (Chile), and Nabro (Eritrea) eruptions in 2011 and compared with AIRS volcanic ash and SO2 measurements.
Stefan Müller, Peter Hoor, Heiko Bozem, Ellen Gute, Bärbel Vogel, Andreas Zahn, Harald Bönisch, Timo Keber, Martina Krämer, Christian Rolf, Martin Riese, Hans Schlager, and Andreas Engel
Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, https://doi.org/10.5194/acp-16-10573-2016, 2016
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In situ airborne measurements performed during TACTS/ESMVal 2012 were analysed to investigate the chemical compostion of the upper troposphere and lower stratosphere. N2O, CO and O3 data show an increase in tropospherically affected air masses within the extratropical stratosphere from August to September 2012, which originate from the Asian monsoon region. Thus, the Asian monsoon anticyclone significantly affected the chemical composition of the extratropical stratosphere during summer 2012.
Nicholas A. Davis, Dian J. Seidel, Thomas Birner, Sean M. Davis, and Simone Tilmes
Atmos. Chem. Phys., 16, 10083–10095, https://doi.org/10.5194/acp-16-10083-2016, https://doi.org/10.5194/acp-16-10083-2016, 2016
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In the Hadley cells, air rises at the Equator and sinks over the subtropics, drying the air and creating deserts on land. We investigated simple climate model experiments and found that the Hadley cells expand in response to increasing carbon dioxide. The climate of some models warms more than others, and these models also have greater Hadley cell expansion. This expansion could shift deserts toward more populated areas, with potentially major impacts on water resources and surface climate.
Reinhold Spang, Lars Hoffmann, Michael Höpfner, Sabine Griessbach, Rolf Müller, Michael C. Pitts, Andrew M. W. Orr, and Martin Riese
Atmos. Meas. Tech., 9, 3619–3639, https://doi.org/10.5194/amt-9-3619-2016, https://doi.org/10.5194/amt-9-3619-2016, 2016
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We present a new classification approach for different polar stratospheric cloud types. The so-called Bayesian classifier estimates the most likely probability that one of the three PSC types (ice, NAT, or STS) dominates the characteristics of a measured infrared spectrum. The entire measurement period of the satellite instrument MIPAS from July 2002 to April 2013 is processed using the new classifier.
Jörn Ungermann, Mandfred Ern, Martin Kaufmann, Rolf Müller, Reinhold Spang, Felix Ploeger, Bärbel Vogel, and Martin Riese
Atmos. Chem. Phys., 16, 8389–8403, https://doi.org/10.5194/acp-16-8389-2016, https://doi.org/10.5194/acp-16-8389-2016, 2016
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This paper presents an analysis of temperature and the trace gases PAN and O3 in
the Asian Summer Monsoon (ASM) region. The positive PAN anomaly consisting of
polluted air is confined vertically within the main ASM anticyclone, whereas a
recently shed eddy exhibits enhanced PAN VMRs for 1 to 2 km above the thermal
tropopause. This implies that eddy shedding provides a very rapid horizontal
transport pathway of Asian pollution into the extratropical lowermost
stratosphere.
Martin Ebert, Ralf Weigel, Konrad Kandler, Gebhard Günther, Sergej Molleker, Jens-Uwe Grooß, Bärbel Vogel, Stephan Weinbruch, and Stephan Borrmann
Atmos. Chem. Phys., 16, 8405–8421, https://doi.org/10.5194/acp-16-8405-2016, https://doi.org/10.5194/acp-16-8405-2016, 2016
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Stratospheric aerosol particles were collected within the arctic vortex in late winter. The chemical composition of refractory particles were analyzed by scanning electron microscopy. More than 750 refractory particles with diameters above 500 nm were found consisting of silicates, Fe- and Ca-rich particles and metal mixtures. The detection of refractory particles in the late winter polar stratosphere has strong implications for the formation of polar stratospheric clouds and ozone depletion.
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.
Charlotte Marinke Hoppe, Felix Ploeger, Paul Konopka, and Rolf Müller
Atmos. Chem. Phys., 16, 6223–6239, https://doi.org/10.5194/acp-16-6223-2016, https://doi.org/10.5194/acp-16-6223-2016, 2016
Simone Tilmes, Jean-Francois Lamarque, Louisa K. Emmons, Doug E. Kinnison, Dan Marsh, Rolando R. Garcia, Anne K. Smith, Ryan R. Neely, Andrew Conley, Francis Vitt, Maria Val Martin, Hiroshi Tanimoto, Isobel Simpson, Don R. Blake, and Nicola Blake
Geosci. Model Dev., 9, 1853–1890, https://doi.org/10.5194/gmd-9-1853-2016, https://doi.org/10.5194/gmd-9-1853-2016, 2016
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The state of the art Community Earth System Model, CESM1 CAM4-chem has been used to perform reference and sensitivity simulations as part of the Chemistry Climate Model Initiative (CCMI). Specifics of the model and details regarding the setup of the simulations are described. In additions, the main behavior of the model, including selected chemical species have been evaluated with climatological datasets. This paper is therefore a references for studies that use the provided model results.
L. Xia, A. Robock, S. Tilmes, and R. R. Neely III
Atmos. Chem. Phys., 16, 1479–1489, https://doi.org/10.5194/acp-16-1479-2016, https://doi.org/10.5194/acp-16-1479-2016, 2016
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Climate model simulations show that stratospheric sulfate geoengineering could impact the terrestrial carbon cycle by enhancing the carbon sink. Enhanced downward diffuse radiation, combined with cooling, could stimulate plants to grow more and absorb more carbon dioxide. This beneficial impact of stratospheric sulfate geoengineering would need to be balanced by a large number of potential risks in any future decisions about implementation of geoengineering.
X. Liu, P.-L. Ma, H. Wang, S. Tilmes, B. Singh, R. C. Easter, S. J. Ghan, and P. J. Rasch
Geosci. Model Dev., 9, 505–522, https://doi.org/10.5194/gmd-9-505-2016, https://doi.org/10.5194/gmd-9-505-2016, 2016
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In this study, we describe and evaluate a new four-mode version of the Modal Aerosol Module (MAM4) in the Community Atmosphere Model version 5 (CAM5). Compared to the current three-mode version of MAM in CAM5, MAM4 significantly improves the simulation of seasonal variation of BC concentrations in the polar regions, by increasing the BC concentrations in all seasons and particularly in cold seasons.
J. He, Y. Zhang, S. Tilmes, L. Emmons, J.-F. Lamarque, T. Glotfelty, A. Hodzic, and F. Vitt
Geosci. Model Dev., 8, 3999–4025, https://doi.org/10.5194/gmd-8-3999-2015, https://doi.org/10.5194/gmd-8-3999-2015, 2015
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The global simulations with CB05_GE and MOZART-4x predict similar chemical profiles for major gases compared to aircraft measurements, with better agreement for the NOy profile by CB05_GE. The SOA concentrations of SOA at four sites in CONUS and organic carbon over the IMPROVE sites are better predicted by MOZART-4x. The two simulations result in a global average difference of 0.5W m-2 in simulated shortwave cloud radiative forcing, with up to 13.6W m-2 over subtropical regions.
B. Vogel, G. Günther, R. Müller, J.-U. Grooß, and M. Riese
Atmos. Chem. Phys., 15, 13699–13716, https://doi.org/10.5194/acp-15-13699-2015, https://doi.org/10.5194/acp-15-13699-2015, 2015
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The Asian summer monsoon circulation is an important global circulation system associated with strong upward transport of tropospheric source gases. We show that the contribution of different boundary source regions to the Asian monsoon anticyclone strongly depends on its intra-seasonal variability and that emissions from Asia have a significant impact on the chemical compositions of the lowermost stratosphere of the Northern Hemisphere at the end of the monsoon season in Sep./Oct. 2012.
Y. Zheng, N. Unger, A. Hodzic, L. Emmons, C. Knote, S. Tilmes, J.-F. Lamarque, and P. Yu
Atmos. Chem. Phys., 15, 13487–13506, https://doi.org/10.5194/acp-15-13487-2015, https://doi.org/10.5194/acp-15-13487-2015, 2015
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Nitrogen oxides (NOx) play an important but complex role in secondary organic aerosol (SOA) formation. In this study we update the SOA scheme in a global 3-D chemistry-climate model by implementing a 4-product volatility basis set (VBS) framework with NOx-dependent yields and simplified aging parameterizations. We find that the SOA decrease in response to a 50% reduction in anthropogenic NOx emissions is limited due to the buffering in different chemical pathways.
F. Ploeger, C. Gottschling, S. Griessbach, J.-U. Grooß, G. Guenther, P. Konopka, R. Müller, M. Riese, F. Stroh, M. Tao, J. Ungermann, B. Vogel, and M. von Hobe
Atmos. Chem. Phys., 15, 13145–13159, https://doi.org/10.5194/acp-15-13145-2015, https://doi.org/10.5194/acp-15-13145-2015, 2015
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The Asian summer monsoon provides an important pathway of tropospheric source gases and pollution into the lower stratosphere. This transport is characterized by deep convection and steady upwelling, combined with confinement inside a large-scale anticyclonic circulation in the upper troposphere and lower stratosphere. In this paper, we show that a barrier to horizontal transport in the monsoon can be determined from a local maximum in the gradient of potential vorticity.
B. Kravitz, A. Robock, S. Tilmes, O. Boucher, J. M. English, P. J. Irvine, A. Jones, M. G. Lawrence, M. MacCracken, H. Muri, J. C. Moore, U. Niemeier, S. J. Phipps, J. Sillmann, T. Storelvmo, H. Wang, and S. Watanabe
Geosci. Model Dev., 8, 3379–3392, https://doi.org/10.5194/gmd-8-3379-2015, https://doi.org/10.5194/gmd-8-3379-2015, 2015
M. Gil-Ojeda, M. Navarro-Comas, L. Gómez-Martín, J. A. Adame, A. Saiz-Lopez, C. A. Cuevas, Y. González, O. Puentedura, E. Cuevas, J.-F. Lamarque, D. Kinninson, and S. Tilmes
Atmos. Chem. Phys., 15, 10567–10579, https://doi.org/10.5194/acp-15-10567-2015, https://doi.org/10.5194/acp-15-10567-2015, 2015
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The NO2 seasonal evolution in the free troposphere (FT) has been established for the first time, based on a remote sensing technique (MAXDOAS) and thus avoiding the problems of the local pollution of in situ instruments. A clear seasonality has been found, with background levels of 20-40pptv. Evidence has been found on fast, direct injection of surface air into the free troposphere. This result might have implications on the FT distribution of halogens and other species with marine sources.
M. Tao, P. Konopka, F. Ploeger, J.-U. Grooß, R. Müller, C. M. Volk, K. A. Walker, and M. Riese
Atmos. Chem. Phys., 15, 8695–8715, https://doi.org/10.5194/acp-15-8695-2015, https://doi.org/10.5194/acp-15-8695-2015, 2015
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A remarkable major stratospheric sudden warming during the boreal winter 2008/09 is studied with the Chemical Lagrangian Model of the Stratosphere (CLaMS). We investigate how mixing triggered by this event correlates the wave forcing and how transport and mixing affect the composition of the whole stratosphere in the Northern Hemisphere, by using the tracer-tracer correlation technique.
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.
S. Tilmes, J.-F. Lamarque, L. K. Emmons, D. E. Kinnison, P.-L. Ma, X. Liu, S. Ghan, C. Bardeen, S. Arnold, M. Deeter, F. Vitt, T. Ryerson, J. W. Elkins, F. Moore, J. R. Spackman, and M. Val Martin
Geosci. Model Dev., 8, 1395–1426, https://doi.org/10.5194/gmd-8-1395-2015, https://doi.org/10.5194/gmd-8-1395-2015, 2015
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The Community Atmosphere Model (CAM), version 5, is now coupled to extensive tropospheric and stratospheric chemistry, called CAM5-chem, and is available in addition to CAM4-chem in the Community Earth System Model (CESM) version 1.2. Both configurations are well suited as tools for atmospheric chemistry modeling studies in the troposphere and lower stratosphere.
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.
M. Val Martin, C. L. Heald, J.-F. Lamarque, S. Tilmes, L. K. Emmons, and B. A. Schichtel
Atmos. Chem. Phys., 15, 2805–2823, https://doi.org/10.5194/acp-15-2805-2015, https://doi.org/10.5194/acp-15-2805-2015, 2015
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We present for the first time the relative effect of climate, emissions, and land use change on ozone and PM25 over the United States, focusing on the national parks. Air quality in 2050 will likely be dominated by emission patterns, but climate and land use changes alone can lead to a substantial increase in air pollution over most of the US, with important implications for O3 air quality, visibility and ecosystem health degradation in the national parks.
O. Kirner, R. Müller, R. Ruhnke, and H. Fischer
Atmos. Chem. Phys., 15, 2019–2030, https://doi.org/10.5194/acp-15-2019-2015, https://doi.org/10.5194/acp-15-2019-2015, 2015
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We use multi-year simulations of the chemistry--climate model EMAC to investigate
the impact that the various types of PSCs have on Antarctic chlorine activation and ozone loss. Heterogeneous chemistry on liquid particles is responsible for more than 90% of the ozone depletion in Antarctic spring in the model simulations. In high southern latitudes, heterogeneous chemistry on ice particles causes only up to 5 DU of additional ozone depletion and chemistry on NAT particles less than 0.5 DU.
R. Spang, G. Günther, M. Riese, L. Hoffmann, R. Müller, and S. Griessbach
Atmos. Chem. Phys., 15, 927–950, https://doi.org/10.5194/acp-15-927-2015, https://doi.org/10.5194/acp-15-927-2015, 2015
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Here we present observations of the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA) of cirrus cloud and water vapour in August 1997 in the upper troposphere and lower stratosphere (UTLS) region. The observations indicate a considerable flux of moisture from the upper tropical troposphere into the extra-tropical lowermost stratosphere (LMS), resulting in the occurrence of high-altitude optically thin cirrus clouds in the LMS.
S. Tilmes, M. J. Mills, U. Niemeier, H. Schmidt, A. Robock, B. Kravitz, J.-F. Lamarque, G. Pitari, and J. M. English
Geosci. Model Dev., 8, 43–49, https://doi.org/10.5194/gmd-8-43-2015, https://doi.org/10.5194/gmd-8-43-2015, 2015
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A new Geoengineering Model Intercomparison Project (GeoMIP) experiment “G4 specified stratospheric aerosols” (G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmosphere, chemistry, dynamics, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulfur dioxide (SO2) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments.
M. Kaufmann, J. Blank, T. Guggenmoser, J. Ungermann, A. Engel, M. Ern, F. Friedl-Vallon, D. Gerber, J. U. Grooß, G. Guenther, M. Höpfner, A. Kleinert, E. Kretschmer, Th. Latzko, G. Maucher, T. Neubert, H. Nordmeyer, H. Oelhaf, F. Olschewski, J. Orphal, P. Preusse, H. Schlager, H. Schneider, D. Schuettemeyer, F. Stroh, O. Suminska-Ebersoldt, B. Vogel, C. M. Volk, W. Woiwode, and M. Riese
Atmos. Meas. Tech., 8, 81–95, https://doi.org/10.5194/amt-8-81-2015, https://doi.org/10.5194/amt-8-81-2015, 2015
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
R. Pommrich, R. Müller, J.-U. Grooß, P. Konopka, F. Ploeger, B. Vogel, M. Tao, C. M. Hoppe, G. Günther, N. Spelten, L. Hoffmann, H.-C. Pumphrey, S. Viciani, F. D'Amato, C. M. Volk, P. Hoor, H. Schlager, and M. Riese
Geosci. Model Dev., 7, 2895–2916, https://doi.org/10.5194/gmd-7-2895-2014, https://doi.org/10.5194/gmd-7-2895-2014, 2014
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A version of the chemical transport model CLaMS is presented, which features a simplified (numerically inexpensive) chemistry scheme. The model results using this version of CLaMS show a good representation of anomaly fields of CO, CH4, N2O, and CFC-11 in the lower stratosphere. CO measurements of three instruments (COLD, HAGAR, and Falcon-CO) in the lower tropical stratosphere (during the campaign TROCCINOX in 2005) have been compared and show a good agreement within the error bars.
B. Vogel, G. Günther, R. Müller, J.-U. Grooß, P. Hoor, M. Krämer, S. Müller, A. Zahn, and M. Riese
Atmos. Chem. Phys., 14, 12745–12762, https://doi.org/10.5194/acp-14-12745-2014, https://doi.org/10.5194/acp-14-12745-2014, 2014
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Enhanced tropospheric trace gases (e.g. pollutants) were measured in situ in
the lowermost stratosphere over Northern Europe on 26 September 2012
during the TACTS aircraft campaign. We found that the combination of rapid uplift by a typhoon and eastward eddy shedding from the Asian monsoon anticyclone is a novel fast transport pathway
that may carry boundary emissions from Southeast
Asia/western Pacific within approximately 5 weeks to the lowermost
stratosphere in Northern Europe.
L. Hoffmann, C. M. Hoppe, R. Müller, G. S. Dutton, J. C. Gille, S. Griessbach, A. Jones, C. I. Meyer, R. Spang, C. M. Volk, and K. A. Walker
Atmos. Chem. Phys., 14, 12479–12497, https://doi.org/10.5194/acp-14-12479-2014, https://doi.org/10.5194/acp-14-12479-2014, 2014
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Stratospheric lifetimes determine the global warming and ozone depletion potentials of chlorofluorocarbons. We present new estimates of the CFC-11/CFC-12 lifetime ratio from satellite and model data (ACE-FTS, HIRDLS, MIPAS, and EMAC/CLaMS). Our estimates of 0.46+/-0.04 (satellites) and 0.48+/-0.07 (model) are in excellent agreement with the recent SPARC reassessment. Having smaller uncertainties than other studies, our results can help to better constrain future CFC lifetime recommendations.
R. Weigel, C. M. Volk, K. Kandler, E. Hösen, G. Günther, B. Vogel, J.-U. Grooß, S. Khaykin, G. V. Belyaev, and S. Borrmann
Atmos. Chem. Phys., 14, 12319–12342, https://doi.org/10.5194/acp-14-12319-2014, https://doi.org/10.5194/acp-14-12319-2014, 2014
C. M. Hoppe, L. Hoffmann, P. Konopka, J.-U. Grooß, F. Ploeger, G. Günther, P. Jöckel, and R. Müller
Geosci. Model Dev., 7, 2639–2651, https://doi.org/10.5194/gmd-7-2639-2014, https://doi.org/10.5194/gmd-7-2639-2014, 2014
K. Tsigaridis, N. Daskalakis, M. Kanakidou, P. J. Adams, P. Artaxo, R. Bahadur, Y. Balkanski, S. E. Bauer, N. Bellouin, A. Benedetti, T. Bergman, T. K. Berntsen, J. P. Beukes, H. Bian, K. S. Carslaw, M. Chin, G. Curci, T. Diehl, R. C. Easter, S. J. Ghan, S. L. Gong, A. Hodzic, C. R. Hoyle, T. Iversen, S. Jathar, J. L. Jimenez, J. W. Kaiser, A. Kirkevåg, D. Koch, H. Kokkola, Y. H Lee, G. Lin, X. Liu, G. Luo, X. Ma, G. W. Mann, N. Mihalopoulos, J.-J. Morcrette, J.-F. Müller, G. Myhre, S. Myriokefalitakis, N. L. Ng, D. O'Donnell, J. E. Penner, L. Pozzoli, K. J. Pringle, L. M. Russell, M. Schulz, J. Sciare, Ø. Seland, D. T. Shindell, S. Sillman, R. B. Skeie, D. Spracklen, T. Stavrakou, S. D. Steenrod, T. Takemura, P. Tiitta, S. Tilmes, H. Tost, T. van Noije, P. G. van Zyl, K. von Salzen, F. Yu, Z. Wang, Z. Wang, R. A. Zaveri, H. Zhang, K. Zhang, Q. Zhang, and X. Zhang
Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, https://doi.org/10.5194/acp-14-10845-2014, 2014
A. Kunz, N. Spelten, P. Konopka, R. Müller, R. M. Forbes, and H. Wernli
Atmos. Chem. Phys., 14, 10803–10822, https://doi.org/10.5194/acp-14-10803-2014, https://doi.org/10.5194/acp-14-10803-2014, 2014
S. Molleker, S. Borrmann, H. Schlager, B. Luo, W. Frey, M. Klingebiel, R. Weigel, M. Ebert, V. Mitev, R. Matthey, W. Woiwode, H. Oelhaf, A. Dörnbrack, G. Stratmann, J.-U. Grooß, G. Günther, B. Vogel, R. Müller, M. Krämer, J. Meyer, and F. Cairo
Atmos. Chem. Phys., 14, 10785–10801, https://doi.org/10.5194/acp-14-10785-2014, https://doi.org/10.5194/acp-14-10785-2014, 2014
A. Khodayari, S. Tilmes, S. C. Olsen, D. B. Phoenix, D. J. Wuebbles, J.-F. Lamarque, and C.-C. Chen
Atmos. Chem. Phys., 14, 9925–9939, https://doi.org/10.5194/acp-14-9925-2014, https://doi.org/10.5194/acp-14-9925-2014, 2014
K. Sindelarova, C. Granier, I. Bouarar, A. Guenther, S. Tilmes, T. Stavrakou, J.-F. Müller, U. Kuhn, P. Stefani, and W. Knorr
Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, https://doi.org/10.5194/acp-14-9317-2014, 2014
M. Riese, H. Oelhaf, P. Preusse, J. Blank, M. Ern, F. Friedl-Vallon, H. Fischer, T. Guggenmoser, M. Höpfner, P. Hoor, M. Kaufmann, J. Orphal, F. Plöger, R. Spang, O. Suminska-Ebersoldt, J. Ungermann, B. Vogel, and W. Woiwode
Atmos. Meas. Tech., 7, 1915–1928, https://doi.org/10.5194/amt-7-1915-2014, https://doi.org/10.5194/amt-7-1915-2014, 2014
J.-U. Grooß, I. Engel, S. Borrmann, W. Frey, G. Günther, C. R. Hoyle, R. Kivi, B. P. Luo, S. Molleker, T. Peter, M. C. Pitts, H. Schlager, G. Stiller, H. Vömel, K. A. Walker, and R. Müller
Atmos. Chem. Phys., 14, 1055–1073, https://doi.org/10.5194/acp-14-1055-2014, https://doi.org/10.5194/acp-14-1055-2014, 2014
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
K. Minschwaner, L. Hoffmann, A. Brown, M. Riese, R. Müller, and P. F. Bernath
Atmos. Chem. Phys., 13, 4253–4263, https://doi.org/10.5194/acp-13-4253-2013, https://doi.org/10.5194/acp-13-4253-2013, 2013
F. Khosrawi, R. Müller, J. Urban, M. H. Proffitt, G. Stiller, M. Kiefer, S. Lossow, D. Kinnison, F. Olschewski, M. Riese, and D. Murtagh
Atmos. Chem. Phys., 13, 3619–3641, https://doi.org/10.5194/acp-13-3619-2013, https://doi.org/10.5194/acp-13-3619-2013, 2013
A. R. Berg, C. L. Heald, K. E. Huff Hartz, A. G. Hallar, A. J. H. Meddens, J. A. Hicke, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 13, 3149–3161, https://doi.org/10.5194/acp-13-3149-2013, https://doi.org/10.5194/acp-13-3149-2013, 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
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Stratosphere | Science Focus: Chemistry (chemical composition and reactions)
Analysis of the global atmospheric background sulfur budget in a multi-model framework
Stratospheric ozone depletion inside the volcanic plume shortly after the 2022 Hunga Tonga eruption
Effects of denitrification on the distributions of trace gas abundances in the polar regions: a comparison of WACCM with observations
Reconstructing volcanic radiative forcing since 1990, using a comprehensive emission inventory and spatially resolved sulfur injections from satellite data in a chemistry-climate model
Climate response to off-equatorial stratospheric sulfur injections in three Earth system models – Part 1: Experimental protocols and surface changes
Stratospheric ozone response to sulfate aerosol and solar dimming climate interventions based on the G6 Geoengineering Model Intercomparison Project (GeoMIP) simulations
The outflow of Asian biomass burning carbonaceous aerosol into the upper troposphere and lower stratosphere in spring: radiative effects seen in a global model
Mountain-wave-induced polar stratospheric clouds and their representation in the global chemistry model ICON-ART
Co-emission of volcanic sulfur and halogens amplifies volcanic effective radiative forcing
Evaluating the simulated radiative forcings, aerosol properties, and stratospheric warmings from the 1963 Mt Agung, 1982 El Chichón, and 1991 Mt Pinatubo volcanic aerosol clouds
The impact of recent changes in Asian anthropogenic emissions of SO2 on sulfate loading in the upper troposphere and lower stratosphere and the associated radiative changes
Mechanism of ozone loss under enhanced water vapour conditions in the mid-latitude lower stratosphere in summer
Multi-model comparison of the volcanic sulfate deposition from the 1815 eruption of Mt. Tambora
Impacts of Mt Pinatubo volcanic aerosol on the tropical stratosphere in chemistry–climate model simulations using CCMI and CMIP6 stratospheric aerosol data
Potential impact of carbonaceous aerosol on the upper troposphere and lower stratosphere (UTLS) and precipitation during Asian summer monsoon in a global model simulation
Vortex-wide chlorine activation by a mesoscale PSC event in the Arctic winter of 2009/10
Solar geoengineering using solid aerosol in the stratosphere
Lagrangian analysis of microphysical and chemical processes in the Antarctic stratosphere: a case study
Aerosol microphysics simulations of the Mt.~Pinatubo eruption with the UM-UKCA composition-climate model
Modeling of 2008 Kasatochi volcanic sulfate direct radiative forcing: assimilation of OMI SO2 plume height data and comparison with MODIS and CALIOP observations
Microphysical simulations of sulfur burdens from stratospheric sulfur geoengineering
The role of carbonyl sulphide as a source of stratospheric sulphate aerosol and its impact on climate
Christina V. Brodowsky, Timofei Sukhodolov, Gabriel Chiodo, Valentina Aquila, Slimane Bekki, Sandip S. Dhomse, Michael Höpfner, Anton Laakso, Graham W. Mann, Ulrike Niemeier, Giovanni Pitari, Ilaria Quaglia, Eugene Rozanov, Anja Schmidt, Takashi Sekiya, Simone Tilmes, Claudia Timmreck, Sandro Vattioni, Daniele Visioni, Pengfei Yu, Yunqian Zhu, and Thomas Peter
Atmos. Chem. Phys., 24, 5513–5548, https://doi.org/10.5194/acp-24-5513-2024, https://doi.org/10.5194/acp-24-5513-2024, 2024
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The aerosol layer is an essential part of the climate system. We characterize the sulfur budget in a volcanically quiescent (background) setting, with a special focus on the sulfate aerosol layer using, for the first time, a multi-model approach. The aim is to identify weak points in the representation of the atmospheric sulfur budget in an intercomparison of nine state-of-the-art coupled global circulation models.
Yunqian Zhu, Robert W. Portmann, Douglas Kinnison, Owen Brian Toon, Luis Millán, Jun Zhang, Holger Vömel, Simone Tilmes, Charles G. Bardeen, Xinyue Wang, Stephanie Evan, William J. Randel, and Karen H. Rosenlof
Atmos. Chem. Phys., 23, 13355–13367, https://doi.org/10.5194/acp-23-13355-2023, https://doi.org/10.5194/acp-23-13355-2023, 2023
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The 2022 Hunga Tonga eruption injected a large amount of water into the stratosphere. Ozone depletion was observed inside the volcanic plume. Chlorine and water vapor injected by this eruption exceeded the normal range, which made the ozone chemistry during this event occur at a higher temperature than polar ozone depletion. Unlike polar ozone chemistry where chlorine nitrate is more important, hypochlorous acid plays a large role in the in-plume chlorine balance and heterogeneous processes.
Michael Weimer, Douglas E. Kinnison, Catherine Wilka, and Susan Solomon
Atmos. Chem. Phys., 23, 6849–6861, https://doi.org/10.5194/acp-23-6849-2023, https://doi.org/10.5194/acp-23-6849-2023, 2023
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We investigate the influence of the number density of nitric acid trihydrate (NAT) particles on associated trace gases in the lower stratosphere using data from a satellite, ozonesondes and simulations by a community chemistry climate model. By comparing probability density functions between observations and the model, we find that the standard NAT number density should be reduced for future simulations with the model.
Jennifer Schallock, Christoph Brühl, Christine Bingen, Michael Höpfner, Landon Rieger, and Jos Lelieveld
Atmos. Chem. Phys., 23, 1169–1207, https://doi.org/10.5194/acp-23-1169-2023, https://doi.org/10.5194/acp-23-1169-2023, 2023
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We characterized the influence of volcanic aerosols for the period 1990–2019 and established a volcanic SO2 emission inventory that includes more than 500 eruptions. From limb-based satellite observations of SO2 and extinction, we derive 3D plumes of SO2 perturbations and injected mass by a novel method. We calculate instantaneous radiative forcing with a comprehensive chemisty climate model. Our results show that smaller eruptions can also contribute to the stratospheric aerosol forcing.
Daniele Visioni, Ewa M. Bednarz, Walker R. Lee, Ben Kravitz, Andy Jones, Jim M. Haywood, and Douglas G. MacMartin
Atmos. Chem. Phys., 23, 663–685, https://doi.org/10.5194/acp-23-663-2023, https://doi.org/10.5194/acp-23-663-2023, 2023
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The paper constitutes Part 1 of a study performing a first systematic inter-model comparison of the atmospheric responses to stratospheric sulfate aerosol injections (SAIs) at various latitudes as simulated by three state-of-the-art Earth system models. We identify similarities and differences in the modeled aerosol burden, investigate the differences in the aerosol approaches between the models, and ultimately show the differences produced in surface climate, temperature and precipitation.
Simone Tilmes, Daniele Visioni, Andy Jones, James Haywood, Roland Séférian, Pierre Nabat, Olivier Boucher, Ewa Monica Bednarz, and Ulrike Niemeier
Atmos. Chem. Phys., 22, 4557–4579, https://doi.org/10.5194/acp-22-4557-2022, https://doi.org/10.5194/acp-22-4557-2022, 2022
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This study assesses the impacts of climate interventions, using stratospheric sulfate aerosol and solar dimming on stratospheric ozone, based on three Earth system models with interactive stratospheric chemistry. The climate interventions have been applied to a high emission (baseline) scenario in order to reach global surface temperatures of a medium emission scenario. We find significant increases and decreases in total column ozone, depending on regions and seasons.
Prashant Chavan, Suvarna Fadnavis, Tanusri Chakroborty, Christopher E. Sioris, Sabine Griessbach, and Rolf Müller
Atmos. Chem. Phys., 21, 14371–14384, https://doi.org/10.5194/acp-21-14371-2021, https://doi.org/10.5194/acp-21-14371-2021, 2021
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Biomass burning (BB) over Asia is a strong source of carbonaceous aerosols during spring. Here, we show an outflow of Asian BB carbonaceous aerosols into the UTLS. These aerosols enhance atmospheric heating and produce circulation changes that lead to the enhancement of water vapor in the UTLS over the tropics. In the stratosphere, water vapor is further transported to the South Pole by the Brewer–Dobson circulation. Enhancement of water vapor in the UTLS has implications for climate change.
Michael Weimer, Jennifer Buchmüller, Lars Hoffmann, Ole Kirner, Beiping Luo, Roland Ruhnke, Michael Steiner, Ines Tritscher, and Peter Braesicke
Atmos. Chem. Phys., 21, 9515–9543, https://doi.org/10.5194/acp-21-9515-2021, https://doi.org/10.5194/acp-21-9515-2021, 2021
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We show that we are able to directly simulate polar stratospheric clouds formed locally in a mountain wave and represent their effect on the ozone chemistry with the global atmospheric chemistry model ICON-ART. Thus, we show the first simulations that close the gap between directly resolved mountain-wave-induced polar stratospheric clouds and their representation at coarse global resolutions.
John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Suvarna Fadnavis, Rolf Müller, Gayatry Kalita, Matthew Rowlinson, Alexandru Rap, Jui-Lin Frank Li, Blaž Gasparini, and Anton Laakso
Atmos. Chem. Phys., 19, 9989–10008, https://doi.org/10.5194/acp-19-9989-2019, https://doi.org/10.5194/acp-19-9989-2019, 2019
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This paper highlights the impact of Asian anthropogenic emission changes in SO2 on sulfate loading in the Asian upper troposphere–lower stratosphere from a global chemistry–climate model and satellite remote sensing. Estimated seasonal mean direct radiative forcing at the top of the atmosphere induced by the increase in Indian SO2 is −0.2–−1.5 W m2 over India. Chinese SO2 emission reduction leads to a positive radiative forcing of ~0.6–6 W m2 over China. It will likely decrease Indian rainfall.
Sabine Robrecht, Bärbel Vogel, Jens-Uwe Grooß, Karen Rosenlof, Troy Thornberry, Andrew Rollins, Martina Krämer, Lance Christensen, and Rolf Müller
Atmos. Chem. Phys., 19, 5805–5833, https://doi.org/10.5194/acp-19-5805-2019, https://doi.org/10.5194/acp-19-5805-2019, 2019
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The potential destruction of stratospheric ozone in the mid-latitudes has been discussed recently. We analysed this ozone loss mechanism and its sensitivities. In a certain temperature range, we found a threshold in water vapour, which has to be exceeded for ozone loss to occur. We show the dependence of this water vapour threshold on temperature, sulfate content and air composition. This study provides a basis to estimate the impact of potential sulphate geoengineering on stratospheric ozone.
Lauren Marshall, Anja Schmidt, Matthew Toohey, Ken S. Carslaw, Graham W. Mann, Michael Sigl, Myriam Khodri, Claudia Timmreck, Davide Zanchettin, William T. Ball, Slimane Bekki, James S. A. Brooke, Sandip Dhomse, Colin Johnson, Jean-Francois Lamarque, Allegra N. LeGrande, Michael J. Mills, Ulrike Niemeier, James O. Pope, Virginie Poulain, Alan Robock, Eugene Rozanov, Andrea Stenke, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, and Fiona Tummon
Atmos. Chem. Phys., 18, 2307–2328, https://doi.org/10.5194/acp-18-2307-2018, https://doi.org/10.5194/acp-18-2307-2018, 2018
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We use four global aerosol models to compare the simulated sulfate deposition from the 1815 Mt. Tambora eruption to ice core records. Inter-model volcanic sulfate deposition differs considerably. Volcanic sulfate deposited on polar ice sheets is used to estimate the atmospheric sulfate burden and subsequently radiative forcing of historic eruptions. Our results suggest that deriving such relationships from model simulations may be associated with greater uncertainties than previously thought.
Laura E. Revell, Andrea Stenke, Beiping Luo, Stefanie Kremser, Eugene Rozanov, Timofei Sukhodolov, and Thomas Peter
Atmos. Chem. Phys., 17, 13139–13150, https://doi.org/10.5194/acp-17-13139-2017, https://doi.org/10.5194/acp-17-13139-2017, 2017
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Compiling stratospheric aerosol data sets after a major volcanic eruption is difficult as the stratosphere becomes too optically opaque for satellite instruments to measure accurately. We performed ensemble chemistry–climate model simulations with two stratospheric aerosol data sets compiled for two international modelling activities and compared the simulated volcanic aerosol-induced effects from the 1991 Mt Pinatubo eruption on tropical stratospheric temperature and ozone with observations.
Suvarna Fadnavis, Gayatry Kalita, K. Ravi Kumar, Blaž Gasparini, and Jui-Lin Frank Li
Atmos. Chem. Phys., 17, 11637–11654, https://doi.org/10.5194/acp-17-11637-2017, https://doi.org/10.5194/acp-17-11637-2017, 2017
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In this study, the model simulations show that monsoon convection over the Bay of Bengal, the South China Sea and southern flanks of the Himalayas transports Asian carbonaceous aerosol into the UTLS. Carbonaceous aerosol induces enhancement in heating rate, vertical velocity and water vapor transport in the UTLS. Doubling of carbonaceous aerosols creates an anomalous warming over the TP. It generates monsoon Hadley circulation and thus increases precipitation over India and northeast China.
Tobias Wegner, Michael C. Pitts, Lamont R. Poole, Ines Tritscher, Jens-Uwe Grooß, and Hideaki Nakajima
Atmos. Chem. Phys., 16, 4569–4577, https://doi.org/10.5194/acp-16-4569-2016, https://doi.org/10.5194/acp-16-4569-2016, 2016
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Satellite observations are used to constrain areas with large backscatter values areas inside the polar vortex. Surface area is derived from these observations and used in heterogeneous modeling. Satellite gas species observations show a decrease in HCl downwind of areas with large surface area density indicating heterogeneous processing inside these areas. This decrease can only be simulated if a realistic surface area is assumed demonstrating the importance of polar stratospheric cloud.
D. K. Weisenstein, D. W. Keith, and J. A. Dykema
Atmos. Chem. Phys., 15, 11835–11859, https://doi.org/10.5194/acp-15-11835-2015, https://doi.org/10.5194/acp-15-11835-2015, 2015
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We investigate stratospheric aerosol geoengineering with solid particle injection by modeling the fractal structure of alumina aerosols and their interaction with background sulfate. We analyze the efficacy (W m^-2 of radiative forcing per megaton of injection) and risks (ozone loss, s) for both alumina and diamond particles as a function of injected monomer radius, finding 240nm alumina and 160nm diamond optimal. We discuss the limitations of our 2-D model study and associated uncertainties.
L. Di Liberto, R. Lehmann, I. Tritscher, F. Fierli, J. L. Mercer, M. Snels, G. Di Donfrancesco, T. Deshler, B. P. Luo, J-U. Grooß, E. Arnone, B. M. Dinelli, and F. Cairo
Atmos. Chem. Phys., 15, 6651–6665, https://doi.org/10.5194/acp-15-6651-2015, https://doi.org/10.5194/acp-15-6651-2015, 2015
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We investigated chemical and microphysical processes in the late winter Antarctic stratosphere, for the first time (to our knowledge) coupling a detailed microphysical box model to a chemistry model.
Model results have been compared with in situ and remote sensing measurements of particles along trajectories.
Our goal is to contribute to the most recent discussion of the relative role of PSC and liquid (background) aerosol in the ozone depletion.
S. S. Dhomse, K. M. Emmerson, G. W. Mann, N. Bellouin, K. S. Carslaw, M. P. Chipperfield, R. Hommel, N. L. Abraham, P. Telford, P. Braesicke, M. Dalvi, C. E. Johnson, F. O'Connor, O. Morgenstern, J. A. Pyle, T. Deshler, J. M. Zawodny, and L. W. Thomason
Atmos. Chem. Phys., 14, 11221–11246, https://doi.org/10.5194/acp-14-11221-2014, https://doi.org/10.5194/acp-14-11221-2014, 2014
J. Wang, S. Park, J. Zeng, C. Ge, K. Yang, S. Carn, N. Krotkov, and A. H. Omar
Atmos. Chem. Phys., 13, 1895–1912, https://doi.org/10.5194/acp-13-1895-2013, https://doi.org/10.5194/acp-13-1895-2013, 2013
J. M. English, O. B. Toon, and M. J. Mills
Atmos. Chem. Phys., 12, 4775–4793, https://doi.org/10.5194/acp-12-4775-2012, https://doi.org/10.5194/acp-12-4775-2012, 2012
C. Brühl, J. Lelieveld, P. J. Crutzen, and H. Tost
Atmos. Chem. Phys., 12, 1239–1253, https://doi.org/10.5194/acp-12-1239-2012, https://doi.org/10.5194/acp-12-1239-2012, 2012
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Short summary
Column ozone protects life on Earth from radiation damage. Stratospheric chlorine compounds cause immense ozone loss in polar winter. Whether similar loss processes can occur in the lower stratosphere above North America today or in future is a matter of debate. We show that these ozone loss processes are very unlikely today or in future independently of whether sulfate geoengineering is applied and that less than 0.1 % of column ozone would be destroyed by this process in any future scenario.
Column ozone protects life on Earth from radiation damage. Stratospheric chlorine compounds...
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