Articles | Volume 23, issue 11
https://doi.org/10.5194/acp-23-6591-2023
© Author(s) 2023. 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-23-6591-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Peer-reviewed comment
| 
15 Jun 2023
Peer-reviewed comment |
| 15 Jun 2023
| 15 Jun 2023
Comment on “An approach to sulfate geoengineering with surface emissions of carbonyl sulfide” by Quaglia et al. (2022)
Institute for Energy and Climate Research (IEK-7), Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
Christoph Brühl
Max Planck Institute for Chemistry, Mainz, Germany
Sinikka T. Lennartz
Institute for Chemistry and Biology of the Marine Environment,
University of Oldenburg, Carl-von-Ossietzky-Straße 9–11, 26129
Oldenburg, Germany
Mary E. Whelan
Department of Environmental Sciences, Rutgers University, New
Brunswick, NJ, USA
Aleya Kaushik
Cooperative Institute for Research in Environmental Sciences (CIRES), University of Colorado Boulder, Boulder, CO, USA
NOAA Global Monitoring Laboratory (GML), Boulder, CO, USA
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
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We studied water vapor in a critical region of the atmosphere, the Asian summer monsoon anticyclone, using rare in situ observations. Our study shows that extremely high water vapor values observed in the stratosphere within the Asian monsoon anticyclone still undergo significant freeze-drying and that water vapor concentrations set by the Lagrangian dry point are a better proxy for the stratospheric water vapor budget than rare observations of enhanced water mixing ratios.
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
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Pure trajectory-based transport models driven by meteorology derived from reanalysis products (ERA5) take into account only the resolved, advective part of transport. That means neither mixing processes nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS) includes these processes. We show that isentropic mixing dominates unresolved transport. The second most important transport process is unresolved convection.
Corinna Kloss, Vicheith Tan, J. Brian Leen, Garrett L. Madsen, Aaron Gardner, Xu Du, Thomas Kulessa, Johannes Schillings, Herbert Schneider, Stefanie Schrade, Chenxi Qiu, and Marc von Hobe
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Aerosol–cloud interactions over the Southern Ocean are poorly understood and remain a major source of uncertainty in climate models. This study presents ship-borne measurements, collected during a 6-week voyage into the Southern Ocean in 2018, that are an important supplement to satellite-based measurements. For example, these measurements include data on low-level clouds and aerosol composition in the marine boundary layer, which can be used in climate model evaluation efforts.
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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
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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.
Yunqian Zhu, Hideharu Akiyoshi, Valentina Aquila, Elizabeth Asher, Ewa M. Bednarz, Slimane Bekki, Christoph Brühl, Amy H. Butler, Parker Case, Simon Chabrillat, Gabriel Chiodo, Margot Clyne, Peter R. Colarco, Sandip Dhomse, Lola Falletti, Eric Fleming, Ben Johnson, Andrin Jörimann, Mahesh Kovilakam, Gerbrand Koren, Ales Kuchar, Nicolas Lebas, Qing Liang, Cheng-Cheng Liu, Graham Mann, Michael Manyin, Marion Marchand, Olaf Morgenstern, Paul Newman, Luke D. Oman, Freja F. Østerstrøm, Yifeng Peng, David Plummer, Ilaria Quaglia, William Randel, Samuel Rémy, Takashi Sekiya, Stephen Steenrod, Timofei Sukhodolov, Simone Tilmes, Kostas Tsigaridis, Rei Ueyama, Daniele Visioni, Xinyue Wang, Shingo Watanabe, Yousuke Yamashita, Pengfei Yu, Wandi Yu, Jun Zhang, and Zhihong Zhuo
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SO2 from explosive volcanic eruptions reaching the stratosphere can oxidize and form sulfur aerosols, potentially persisting for several years. We developed a new submodel, Explosive Volcanic ERuptions (EVER), that seamlessly includes stratospheric volcanic SO2 emissions in global numerical simulations based on a novel standard historical model setup, successfully evaluated with satellite observations. Sensitivity studies on the Nabro eruption in 2011 evaluate different emission methods.
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Simulations with a comprehensive chemistry-climate model show that organic aerosol from recent major forest fires strongly enhances heterogeneous ozone depletion by chlorine in the middle and high latitude lower stratosphere, supported by satellite observations. This sunlight-absorbing, self-lofting aerosol perturbs the radiation budget and stratospheric dynamics differently from major volcanic eruptions, which are also included in this study.
Leonhard Lücken, Michael J. Follows, Jason G. Bragg, and Sinikka T. Lennartz
EGUsphere, https://doi.org/10.5194/egusphere-2025-2227, https://doi.org/10.5194/egusphere-2025-2227, 2025
This preprint is open for discussion and under review for Geoscientific Model Development (GMD).
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The Microbial Community Model (MCoM) is a flexible biogeochemical modeling framework which resolves a rich set of interactions between photosynthetic and heterotrophic microbes, including cross-feeding, metabolite exchange, and nutrient recycling. As such, it allows to assess community-level effects on elemental turnover emerging from microbial interactions. Its scalability allows to represent both simple pairwise interactions and large, diverse communities.
Nic Surawski, Benedikt Steil, Christoph Brühl, Sergey Gromov, Klaus Klingmüller, Anna Martin, Andrea Pozzer, and Jos Lelieveld
EGUsphere, https://doi.org/10.5194/egusphere-2025-1559, https://doi.org/10.5194/egusphere-2025-1559, 2025
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Hydrogen usage will likely increase to achieve net zero emission targets. We undertook calculations with an Earth system model using a high performance computer to explore hydrogen atmospheric dynamics. Simulations with the EMAC model yielded highly accurate results at global scale. Correctly representing hydroxyl radicals in the model is a critical requirement for predicting hydrogen concentrations well. Our hydrogen budget is also in very good agreement with bottom-up literature estimates.
Paul Konopka, Felix Ploeger, Francesco D'Amato, Teresa Campos, Marc von Hobe, Shawn B. Honomichl, Peter Hoor, Laura L. Pan, Michelle L. Santee, Silvia Viciani, Kaley A. Walker, and Michaela I. Hegglin
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We present an improved version of the Chemical Lagrangian Model of the Stratosphere (CLaMS-3.0), which better represents transport from the lower atmosphere to the upper troposphere and lower stratosphere. By refining grid resolution and improving convection representation, the model more accurately simulates carbon monoxide transport. Comparisons with satellite and in situ observations highlight its ability to capture seasonal variations and improve our understanding of atmospheric transport.
Murat Aydin, Melinda R. Nicewonger, Gregory L. Britten, Dominic Winski, Mary Whelan, John D. Patterson, Erich Osterberg, Christopher F. Lee, Tara Harder, Kyle J. Callahan, David Ferris, and Eric S. Saltzman
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We present a new ice core carbonyl sulfide (COS) record from the South Pole, Antarctica, yielding a 52 000-year atmospheric record after correction for production in the ice sheet. The results display a large increase in atmospheric COS concurrent with the last deglaciation. The deglacial COS rise results from an overall strengthening of atmospheric COS sources, implying a large increase in ocean sulfur gas emissions. Atmospheric sulfur gases have negative climate feedbacks.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Paul Konopka, Christian Rolf, Marc von Hobe, Sergey M. Khaykin, Benjamin Clouser, Elisabeth Moyer, Fabrizio Ravegnani, Francesco D'Amato, Silvia Viciani, Nicole Spelten, Armin Afchine, Martina Krämer, Fred Stroh, and Felix Ploeger
Atmos. Chem. Phys., 23, 12935–12947, https://doi.org/10.5194/acp-23-12935-2023, https://doi.org/10.5194/acp-23-12935-2023, 2023
Short summary
Short summary
We studied water vapor in a critical region of the atmosphere, the Asian summer monsoon anticyclone, using rare in situ observations. Our study shows that extremely high water vapor values observed in the stratosphere within the Asian monsoon anticyclone still undergo significant freeze-drying and that water vapor concentrations set by the Lagrangian dry point are a better proxy for the stratospheric water vapor budget than rare observations of enhanced water mixing ratios.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
Short summary
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
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.
Ilaria Quaglia, Claudia Timmreck, Ulrike Niemeier, Daniele Visioni, Giovanni Pitari, Christina Brodowsky, Christoph Brühl, Sandip S. Dhomse, Henning Franke, Anton Laakso, Graham W. Mann, Eugene Rozanov, and Timofei Sukhodolov
Atmos. Chem. Phys., 23, 921–948, https://doi.org/10.5194/acp-23-921-2023, https://doi.org/10.5194/acp-23-921-2023, 2023
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The last very large explosive volcanic eruption we have measurements for is the eruption of Mt. Pinatubo in 1991. It is therefore often used as a benchmark for climate models' ability to reproduce these kinds of events. Here, we compare available measurements with the results from multiple experiments conducted with climate models interactively simulating the aerosol cloud formation.
Paul Konopka, Mengchu Tao, Marc von Hobe, Lars Hoffmann, Corinna Kloss, Fabrizio Ravegnani, C. Michael Volk, Valentin Lauther, Andreas Zahn, Peter Hoor, and Felix Ploeger
Geosci. Model Dev., 15, 7471–7487, https://doi.org/10.5194/gmd-15-7471-2022, https://doi.org/10.5194/gmd-15-7471-2022, 2022
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Pure trajectory-based transport models driven by meteorology derived from reanalysis products (ERA5) take into account only the resolved, advective part of transport. That means neither mixing processes nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS) includes these processes. We show that isentropic mixing dominates unresolved transport. The second most important transport process is unresolved convection.
Camille Abadie, Fabienne Maignan, Marine Remaud, Jérôme Ogée, J. Elliott Campbell, Mary E. Whelan, Florian Kitz, Felix M. Spielmann, Georg Wohlfahrt, Richard Wehr, Wu Sun, Nina Raoult, Ulli Seibt, Didier Hauglustaine, Sinikka T. Lennartz, Sauveur Belviso, David Montagne, and Philippe Peylin
Biogeosciences, 19, 2427–2463, https://doi.org/10.5194/bg-19-2427-2022, https://doi.org/10.5194/bg-19-2427-2022, 2022
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A better constraint of the components of the carbonyl sulfide (COS) global budget is needed to exploit its potential as a proxy of gross primary productivity. In this study, we compare two representations of oxic soil COS fluxes, and we develop an approach to represent anoxic soil COS fluxes in a land surface model. We show the importance of atmospheric COS concentration variations on oxic soil COS fluxes and provide new estimates for oxic and anoxic soil contributions to the COS global budget.
Marine Remaud, Frédéric Chevallier, Fabienne Maignan, Sauveur Belviso, Antoine Berchet, Alexandra Parouffe, Camille Abadie, Cédric Bacour, Sinikka Lennartz, and Philippe Peylin
Atmos. Chem. Phys., 22, 2525–2552, https://doi.org/10.5194/acp-22-2525-2022, https://doi.org/10.5194/acp-22-2525-2022, 2022
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Carbonyl sulfide (COS) has been recognized as a promising indicator of the plant gross primary production (GPP). Here, we assimilate both COS and CO2 measurements into an atmospheric transport model to obtain information on GPP, plant respiration and COS budget. A possible scenario for the period 2008–2019 leads to a global COS biospheric sink of 800 GgS yr−1 and higher oceanic emissions between 400 and 600 GgS yr−1.
Linda M. J. Kooijmans, Ara Cho, Jin Ma, Aleya Kaushik, Katherine D. Haynes, Ian Baker, Ingrid T. Luijkx, Mathijs Groenink, Wouter Peters, John B. Miller, Joseph A. Berry, Jerome Ogée, Laura K. Meredith, Wu Sun, Kukka-Maaria Kohonen, Timo Vesala, Ivan Mammarella, Huilin Chen, Felix M. Spielmann, Georg Wohlfahrt, Max Berkelhammer, Mary E. Whelan, Kadmiel Maseyk, Ulli Seibt, Roisin Commane, Richard Wehr, and Maarten Krol
Biogeosciences, 18, 6547–6565, https://doi.org/10.5194/bg-18-6547-2021, https://doi.org/10.5194/bg-18-6547-2021, 2021
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The gas carbonyl sulfide (COS) can be used to estimate photosynthesis. To adopt this approach on regional and global scales, we need biosphere models that can simulate COS exchange. So far, such models have not been evaluated against observations. We evaluate the COS biosphere exchange of the SiB4 model against COS flux observations. We find that the model is capable of simulating key processes in COS biosphere exchange. Still, we give recommendations for further improvement of the model.
Corinna Kloss, Vicheith Tan, J. Brian Leen, Garrett L. Madsen, Aaron Gardner, Xu Du, Thomas Kulessa, Johannes Schillings, Herbert Schneider, Stefanie Schrade, Chenxi Qiu, and Marc von Hobe
Atmos. Meas. Tech., 14, 5271–5297, https://doi.org/10.5194/amt-14-5271-2021, https://doi.org/10.5194/amt-14-5271-2021, 2021
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We describe the innovative analyzer
AMICAfor airborne trace gas measurements by infrared spectroscopy. Its design makes it robust and allows for sensitive measurements. AMICA has been used on two different aircraft for measuring gases including carbonyl sulfide, carbon monoxide and ozone. With fairly simple adaptions, AMICA can measure many stable trace gases that absorb light in the infrared.
Stefanie Kremser, Mike Harvey, Peter Kuma, Sean Hartery, Alexia Saint-Macary, John McGregor, Alex Schuddeboom, Marc von Hobe, Sinikka T. Lennartz, Alex Geddes, Richard Querel, Adrian McDonald, Maija Peltola, Karine Sellegri, Israel Silber, Cliff S. Law, Connor J. Flynn, Andrew Marriner, Thomas C. J. Hill, Paul J. DeMott, Carson C. Hume, Graeme Plank, Geoffrey Graham, and Simon Parsons
Earth Syst. Sci. Data, 13, 3115–3153, https://doi.org/10.5194/essd-13-3115-2021, https://doi.org/10.5194/essd-13-3115-2021, 2021
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Aerosol–cloud interactions over the Southern Ocean are poorly understood and remain a major source of uncertainty in climate models. This study presents ship-borne measurements, collected during a 6-week voyage into the Southern Ocean in 2018, that are an important supplement to satellite-based measurements. For example, these measurements include data on low-level clouds and aerosol composition in the marine boundary layer, which can be used in climate model evaluation efforts.
Sinikka T. Lennartz, Michael Gauss, Marc von Hobe, and Christa A. Marandino
Earth Syst. Sci. Data, 13, 2095–2110, https://doi.org/10.5194/essd-13-2095-2021, https://doi.org/10.5194/essd-13-2095-2021, 2021
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This study provides a marine emission inventory for the sulphur gases carbonyl sulphide (OCS) and carbon disulphide (CS2), derived from a numerical model of the surface ocean at monthly resolution for the period 2000–2019. Comparison with a database of seaborne observations reveals very good agreement for OCS. Interannual variability in both gases seems to be mainly driven by the amount of chromophoric dissolved organic matter present in surface water.
Fabienne Maignan, Camille Abadie, Marine Remaud, Linda M. J. Kooijmans, Kukka-Maaria Kohonen, Róisín Commane, Richard Wehr, J. Elliott Campbell, Sauveur Belviso, Stephen A. Montzka, Nina Raoult, Ulli Seibt, Yoichi P. Shiga, Nicolas Vuichard, Mary E. Whelan, and Philippe Peylin
Biogeosciences, 18, 2917–2955, https://doi.org/10.5194/bg-18-2917-2021, https://doi.org/10.5194/bg-18-2917-2021, 2021
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The assimilation of carbonyl sulfide (COS) by continental vegetation has been proposed as a proxy for gross primary production (GPP). Using a land surface and a transport model, we compare a mechanistic representation of the plant COS uptake (Berry et al., 2013) to the classical leaf relative uptake (LRU) approach linking GPP and vegetation COS fluxes. We show that at high temporal resolutions a mechanistic approach is mandatory, but at large scales the LRU approach compares similarly.
Keun-Ok Lee, Brice Barret, Eric L. Flochmoën, Pierre Tulet, Silvia Bucci, Marc von Hobe, Corinna Kloss, Bernard Legras, Maud Leriche, Bastien Sauvage, Fabrizio Ravegnani, and Alexey Ulanovsky
Atmos. Chem. Phys., 21, 3255–3274, https://doi.org/10.5194/acp-21-3255-2021, https://doi.org/10.5194/acp-21-3255-2021, 2021
Short summary
Short summary
This paper focuses on the emission sources and pathways of pollution from the boundary layer to the Asian monsoon anticyclone (AMA) during the StratoClim aircraft campaign period. Simulations with the Meso-NH cloud-chemistry model at a horizontal resolution of 15 km are performed over the Asian region to characterize the impact of monsoon deep convection on the composition of AMA and on the formation of the Asian tropopause aerosol layer during the StratoClim campaign.
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
Short summary
Short summary
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.
Cited articles
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Short summary
Carbonyl sulfide plays a role in the climate system as a greenhouse gas and as the major non-volcanic precursor of particles reflecting sunlight. Here, we comment on a proposal to increase the number of particles by emitting extra carbonyl sulfide at the surface. We show that the balance between aerosol cooling and greenhouse gas warming may not be as favorable as suggested and also that much of the carbonyl sulfide emissions will actually be taken up by the biosphere and the oceans.
Carbonyl sulfide plays a role in the climate system as a greenhouse gas and as the major...
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