Articles | Volume 17, issue 14
https://doi.org/10.5194/gmd-17-5689-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/gmd-17-5689-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Development and technical paper
| 
30 Jul 2024
Development and technical paper |
| 30 Jul 2024
| 30 Jul 2024
Development of the adjoint of the unified tropospheric–stratospheric chemistry extension (UCX) in GEOS-Chem adjoint v36
Section Aircraft Noise and Climate Effects, Faculty of Aerospace Engineering, Delft University of Technology, Kluyverweg 1, 2629 HS, Delft, the Netherlands
Department of Engineering, University of Cambridge, 1 JJ Thomson Ave, Cambridge, CB3 0DY, United Kingdom
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
Daven K. Henze
Department of Mechanical Engineering, University of Colorado Boulder, 1111 Engineering Drive, Boulder, CO 80309, United States
Sebastian D. Eastham
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
Department of Aeronautics, Imperial College London, South Kensington Campus, London, SW7 2AZ, United Kingdom
Raymond L. Speth
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
Steven R. H. Barrett
Laboratory for Aviation and the Environment, Department of Aeronautics and Astronautics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, MA 02139, United States
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Randall V. Martin, Sebastian D. Eastham, Liam Bindle, Elizabeth W. Lundgren, Thomas L. Clune, Christoph A. Keller, William Downs, Dandan Zhang, Robert A. Lucchesi, Melissa P. Sulprizio, Robert M. Yantosca, Yanshun Li, Lucas Estrada, William M. Putman, Benjamin M. Auer, Atanas L. Trayanov, Steven Pawson, and Daniel J. Jacob
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William Atkinson, Sebastian D. Eastham, Y.-H. Henry Chen, Jennifer Morris, Sergey Paltsev, C. Adam Schlosser, and Noelle E. Selin
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Xueying Yu, Dylan B. Millet, and Daven K. Henze
Geosci. Model Dev., 14, 7775–7793, https://doi.org/10.5194/gmd-14-7775-2021, https://doi.org/10.5194/gmd-14-7775-2021, 2021
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Liam Bindle, Randall V. Martin, Matthew J. Cooper, Elizabeth W. Lundgren, Sebastian D. Eastham, Benjamin M. Auer, Thomas L. Clune, Hongjian Weng, Jintai Lin, Lee T. Murray, Jun Meng, Christoph A. Keller, William M. Putman, Steven Pawson, and Daniel J. Jacob
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Xuan Wang, Daniel J. Jacob, William Downs, Shuting Zhai, Lei Zhu, Viral Shah, Christopher D. Holmes, Tomás Sherwen, Becky Alexander, Mathew J. Evans, Sebastian D. Eastham, J. Andrew Neuman, Patrick R. Veres, Theodore K. Koenig, Rainer Volkamer, L. Gregory Huey, Thomas J. Bannan, Carl J. Percival, Ben H. Lee, and Joel A. Thornton
Atmos. Chem. Phys., 21, 13973–13996, https://doi.org/10.5194/acp-21-13973-2021, https://doi.org/10.5194/acp-21-13973-2021, 2021
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Haipeng Lin, Daniel J. Jacob, Elizabeth W. Lundgren, Melissa P. Sulprizio, Christoph A. Keller, Thibaud M. Fritz, Sebastian D. Eastham, Louisa K. Emmons, Patrick C. Campbell, Barry Baker, Rick D. Saylor, and Raffaele Montuoro
Geosci. Model Dev., 14, 5487–5506, https://doi.org/10.5194/gmd-14-5487-2021, https://doi.org/10.5194/gmd-14-5487-2021, 2021
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Benjamin A. Nault, Duseong S. Jo, Brian C. McDonald, Pedro Campuzano-Jost, Douglas A. Day, Weiwei Hu, Jason C. Schroder, James Allan, Donald R. Blake, Manjula R. Canagaratna, Hugh Coe, Matthew M. Coggon, Peter F. DeCarlo, Glenn S. Diskin, Rachel Dunmore, Frank Flocke, Alan Fried, Jessica B. Gilman, Georgios Gkatzelis, Jacqui F. Hamilton, Thomas F. Hanisco, Patrick L. Hayes, Daven K. Henze, Alma Hodzic, James Hopkins, Min Hu, L. Greggory Huey, B. Thomas Jobson, William C. Kuster, Alastair Lewis, Meng Li, Jin Liao, M. Omar Nawaz, Ilana B. Pollack, Jeffrey Peischl, Bernhard Rappenglück, Claire E. Reeves, Dirk Richter, James M. Roberts, Thomas B. Ryerson, Min Shao, Jacob M. Sommers, James Walega, Carsten Warneke, Petter Weibring, Glenn M. Wolfe, Dominique E. Young, Bin Yuan, Qiang Zhang, Joost A. de Gouw, and Jose L. Jimenez
Atmos. Chem. Phys., 21, 11201–11224, https://doi.org/10.5194/acp-21-11201-2021, https://doi.org/10.5194/acp-21-11201-2021, 2021
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Secondary organic aerosol (SOA) is an important aspect of poor air quality for urban regions around the world, where a large fraction of the population lives. However, there is still large uncertainty in predicting SOA in urban regions. Here, we used data from 11 urban campaigns and show that the variability in SOA production in these regions is predictable and is explained by key emissions. These results are used to estimate the premature mortality associated with SOA in urban regions.
Ilya Stanevich, Dylan B. A. Jones, Kimberly Strong, Martin Keller, Daven K. Henze, Robert J. Parker, Hartmut Boesch, Debra Wunch, Justus Notholt, Christof Petri, Thorsten Warneke, Ralf Sussmann, Matthias Schneider, Frank Hase, Rigel Kivi, Nicholas M. Deutscher, Voltaire A. Velazco, Kaley A. Walker, and Feng Deng
Atmos. Chem. Phys., 21, 9545–9572, https://doi.org/10.5194/acp-21-9545-2021, https://doi.org/10.5194/acp-21-9545-2021, 2021
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We explore the utility of a weak-constraint (WC) four-dimensional variational (4D-Var) data assimilation scheme for mitigating systematic errors in methane simulation in the GEOS-Chem model. We use data from the Greenhouse Gases Observing Satellite (GOSAT) and show that, compared to the traditional 4D-Var approach, the WC scheme improves the agreement between the model and independent observations. We find that the WC corrections to the model provide insight into the source of the errors.
Na Zhao, Xinyi Dong, Kan Huang, Joshua S. Fu, Marianne Tronstad Lund, Kengo Sudo, Daven Henze, Tom Kucsera, Yun Fat Lam, Mian Chin, and Simone Tilmes
Atmos. Chem. Phys., 21, 8637–8654, https://doi.org/10.5194/acp-21-8637-2021, https://doi.org/10.5194/acp-21-8637-2021, 2021
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Black carbon acts as a strong climate forcer, especially in vulnerable pristine regions such as the Arctic. This work utilizes ensemble modeling results from the task force Hemispheric Transport of Air Pollution Phase 2 to investigate the responses of Arctic black carbon and surface temperature to various source emission reductions. East Asia contributed the most to Arctic black carbon. The response of Arctic temperature to black carbon was substantially more sensitive than the global average.
Zichong Chen, Junjie Liu, Daven K. Henze, Deborah N. Huntzinger, Kelley C. Wells, Stephen Sitch, Pierre Friedlingstein, Emilie Joetzjer, Vladislav Bastrikov, Daniel S. Goll, Vanessa Haverd, Atul K. Jain, Etsushi Kato, Sebastian Lienert, Danica L. Lombardozzi, Patrick C. McGuire, Joe R. Melton, Julia E. M. S. Nabel, Benjamin Poulter, Hanqin Tian, Andrew J. Wiltshire, Sönke Zaehle, and Scot M. Miller
Atmos. Chem. Phys., 21, 6663–6680, https://doi.org/10.5194/acp-21-6663-2021, https://doi.org/10.5194/acp-21-6663-2021, 2021
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NASA's Orbiting Carbon Observatory 2 (OCO-2) satellite observes atmospheric CO2 globally. We use a multiple regression and inverse model to quantify the relationships between OCO-2 and environmental drivers within individual years for 2015–2018 and within seven global biomes. Our results point to limitations of current space-based observations for inferring environmental relationships but also indicate the potential to inform key relationships that are very uncertain in process-based models.
Yilin Chen, Huizhong Shen, Jennifer Kaiser, Yongtao Hu, Shannon L. Capps, Shunliu Zhao, Amir Hakami, Jhih-Shyang Shih, Gertrude K. Pavur, Matthew D. Turner, Daven K. Henze, Jaroslav Resler, Athanasios Nenes, Sergey L. Napelenok, Jesse O. Bash, Kathleen M. Fahey, Gregory R. Carmichael, Tianfeng Chai, Lieven Clarisse, Pierre-François Coheur, Martin Van Damme, and Armistead G. Russell
Atmos. Chem. Phys., 21, 2067–2082, https://doi.org/10.5194/acp-21-2067-2021, https://doi.org/10.5194/acp-21-2067-2021, 2021
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Ammonia (NH3) emissions can exert adverse impacts on air quality and ecosystem well-being. NH3 emission inventories are viewed as highly uncertain. Here we optimize the NH3 emission estimates in the US using an air quality model and NH3 measurements from the IASI satellite instruments. The optimized NH3 emissions are much higher than the National Emissions Inventory estimates in April. The optimized NH3 emissions improved model performance when evaluated against independent observation.
Inés Sanz-Morère, Sebastian D. Eastham, Florian Allroggen, Raymond L. Speth, and Steven R. H. Barrett
Atmos. Chem. Phys., 21, 1649–1681, https://doi.org/10.5194/acp-21-1649-2021, https://doi.org/10.5194/acp-21-1649-2021, 2021
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Contrails cause ~50 % of aviation climate impacts, but this is highly uncertain. This is partly due to the effect of overlap between contrails and other cloud layers. We developed a model to quantify this effect, finding that overlap with natural clouds increased contrails' radiative forcing in 2015. This suggests that cloud avoidance may help in reducing aviation's climate impacts. We also find that contrail–contrail overlap reduces impacts by ~3 %, increasing non-linearly with optical depth.
Xueying Yu, Dylan B. Millet, Kelley C. Wells, Daven K. Henze, Hansen Cao, Timothy J. Griffis, Eric A. Kort, Genevieve Plant, Malte J. Deventer, Randall K. Kolka, D. Tyler Roman, Kenneth J. Davis, Ankur R. Desai, Bianca C. Baier, Kathryn McKain, Alan C. Czarnetzki, and A. Anthony Bloom
Atmos. Chem. Phys., 21, 951–971, https://doi.org/10.5194/acp-21-951-2021, https://doi.org/10.5194/acp-21-951-2021, 2021
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Methane concentrations have doubled since 1750. The US Upper Midwest is a key region contributing to such trends, but sources are poorly understood. We collected and analyzed aircraft data to resolve spatial and timing biases in wetland and livestock emission estimates and uncover errors in inventory treatment of manure management. We highlight the importance of intensive agriculture for the regional and US methane budgets and the potential for methane mitigation through improved management.
Zhen Qu, Daven K. Henze, Owen R. Cooper, and Jessica L. Neu
Atmos. Chem. Phys., 20, 13109–13130, https://doi.org/10.5194/acp-20-13109-2020, https://doi.org/10.5194/acp-20-13109-2020, 2020
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We use satellite observations and chemical transport modeling to quantify sources of NOx, a major air pollutant, over the past decade. We find improved simulations of the magnitude, seasonality, and trends of NO2 and ozone concentrations using these derived emissions. Changes in ozone pollution driven by human and natural sources are identified in different regions. This work shows the benefits of remote-sensing data and inverse modeling for more accurate ozone simulations.
Yiqi Zheng, Joel A. Thornton, Nga Lee Ng, Hansen Cao, Daven K. Henze, Erin E. McDuffie, Weiwei Hu, Jose L. Jimenez, Eloise A. Marais, Eric Edgerton, and Jingqiu Mao
Atmos. Chem. Phys., 20, 13091–13107, https://doi.org/10.5194/acp-20-13091-2020, https://doi.org/10.5194/acp-20-13091-2020, 2020
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This study aims to address a challenge in biosphere–atmosphere interactions: to what extent can biogenic organic aerosol (OA) be modified through human activities? From three surface network observations, we show OA is weakly dependent on sulfate and aerosol acidity in the summer southeast US, on both long-term trends and monthly variability. The results are in strong contrast to a global model, GEOS-Chem, suggesting the need to revisit the representation of aqueous-phase secondary OA formation.
Cited articles
Ball, W. T., Alsing, J., Mortlock, D. J., Staehelin, J., Haigh, J. D., Peter, T., Tummon, F., Stübi, R., Stenke, A., Anderson, J., Bourassa, A., Davis, S. M., Degenstein, D., Frith, S., Froidevaux, L., Roth, C., Sofieva, V., Wang, R., Wild, J., Yu, P., Ziemke, J. R., and Rozanov, E. V.: Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery, Atmos. Chem. Phys., 18, 1379–1394, https://doi.org/10.5194/acp-18-1379-2018, 2018.
Bey, I., Jacob, D. J., Yantosca, R. M., Logan, J. A., Field, B. D., Fiore, A. M., Li, Q., Liu, H. Y., Mickley, L. J., and Schultz, M. G.: Global modeling of tropospheric chemistry with assimilated meteorology: Model description and evaluation, J. Geophys. Res., 106, 23073–23095, https://doi.org/10.1029/2001JD000807, 2001.
Bian, H. and Prather, M. J.: Fast-J2: Accurate Simulation of Stratospheric Photolysis in Global Chemical Models, J. Atmos. Chem., 41, 281–296, https://doi.org/10.1023/A:1014980619462, 2002.
Brasseur, G. P., Cox, R. A., Hauglustaine, D., Isaksen, I., Lelieveld, J., Lister, D. H., Sausen, R., Schumann, U., Wahner, A., and Wiesen, P.: European scientific assessment of the atmospheric effects of aircraft emissions, Atmos. Environ., 32, 2329–2418, https://doi.org/10.1016/S1352-2310(97)00486-X, 1998.
Butchart, N.: The Brewer-Dobson circulation, Rev. Geophys., 52, 157–184, https://doi.org/10.1002/2013RG000448, 2014.
Capps, S. L., Henze, D. K., Hakami, A., Russell, A. G., and Nenes, A.: ANISORROPIA: the adjoint of the aerosol thermodynamic model ISORROPIA, Atmos. Chem. Phys., 12, 527–543, https://doi.org/10.5194/acp-12-527-2012, 2012.
Chipperfield, M. P., Cariolle, D., and Simon, P.: A 3D transport model study of chlorine activation during EASOE, Geophys. Res. Lett., 21, 1467–1470, https://doi.org/10.1029/93GL01679, 1994.
Clappier, A., Belis, C. A., Pernigotti, D., and Thunis, P.: Source apportionment and sensitivity analysis: two methodologies with two different purposes, Geosci. Model Dev., 10, 4245–4256, https://doi.org/10.5194/gmd-10-4245-2017, 2017.
Considine, D. B., Douglass, A. R., Connell, P. S., Kinnison, D. E., and Rotman, D. A.: A polar stratospheric cloud parameterization for the global modeling initiative three-dimensional model and its response to stratospheric aircraft, J. Geophys. Res.-Atmos., 105, 3955–3973, https://doi.org/10.1029/1999JD900932, 2000.
Crutzen, P. J.: The influence of nitrogen oxides on the atmospheric ozone content, Q. J. Roy. Meteor. Soc., 96, 320–325, https://doi.org/10.1002/qj.49709640815, 1970.
Cunnold, D. M., Alyea, F. N., and Prinn, R. G.: Relative effects on atmospheric ozone of latitude and altitude of supersonic flight, 15, 337–345, https://doi.org/10.2514/3.7327, 1977.
Daescu, D. N., Sandu, A., and Carmichael, G. R.: Direct and adjoint sensitivity analysis of chemical kinetic systems with KPP: II – Numerical validation and applications, Atmos. Environ., 37, 5097–5114, https://doi.org/10.1016/j.atmosenv.2003.08.020, 2003.
Damian, V., Sandu, A., Damian, M., Potra, F., and Carmichael, G. R.: The kinetic preprocessor KPP-a software environment for solving chemical kinetics, Comput. Chem. Eng., 26, 1567–1579, https://doi.org/10.1016/S0098-1354(02)00128-X, 2002.
Daniel, J. S., Solomon, S., Portmann, R. W., and Garcia, R. R.: Stratospheric ozone destruction: The importance of bromine relative to chlorine, J. Geophys. Res.-Atmos., 104, 23871–23880, https://doi.org/10.1029/1999JD900381, 1999.
Dedoussi, I. C., Eastham, S. D., Monier, E., and Barrett, S. R. H.: Premature mortality related to United States cross-state air pollution, Nature, 578, 261–265, https://doi.org/10.1038/s41586-020-1983-8, 2020.
Dedoussi, I. C., Henze, D. K., Eastham, S. D., Speth, R. L., and Barrett, S. R. H.: GEOS-Chem UCX adjoint model code (v35f), Zenodo [code], https://doi.org/10.5281/zenodo.4300535, 2024.
Eastham, S. D. and Barrett, S. R. H.: Aviation-attributable ozone as a driver for changes in mortality related to air quality and skin cancer, Atmos. Environ., 144, 17–23, https://doi.org/10.1016/j.atmosenv.2016.08.040, 2016.
Eastham, S. D., Weisenstein, D. K., and Barrett, S. R. H.: Development and evaluation of the unified tropospheric-stratospheric chemistry extension (UCX) for the global chemistry-transport model GEOS-Chem, Atmos. Environ., 89, 52–63, https://doi.org/10.1016/j.atmosenv.2014.02.001, 2014.
Eastham, S. D., Keith, D. W., and Barrett, S. R. H.: Mortality tradeoff between air quality and skin cancer from changes in stratospheric ozone, Environ. Res. Lett., 13, 034035, https://doi.org/10.1088/1748-9326/aaad2e, 2018.
Eastham, S. D., Fritz, T., Sanz-Morère, I., Prashanth, P., Allroggen, F., Prinn, R. G., Speth, R. L., and Barrett, S. R. H.: Impacts of a near-future supersonic aircraft fleet on atmospheric composition and climate, Environ. Sci. Atmos., 2, 388–403, https://doi.org/10.1039/D1EA00081K, 2022.
Emmons, L. K., Hess, P. G., Lamarque, J.-F., and Pfister, G. G.: Tagged ozone mechanism for MOZART-4, CAM-chem and other chemical transport models, Geosci. Model Dev., 5, 1531–1542, https://doi.org/10.5194/gmd-5-1531-2012, 2012.
Farman, J. C., Gardiner, B. G., and Shanklin, J. D.: Large losses of total ozone in Antarctica reveal seasonal
Fritz, T. M., Dedoussi, I. C., Eastham, S. D., Speth, R. L., Henze, D. K., and Barrett, S. R. H.: Identifying the ozone-neutral aircraft cruise altitude, Atmos. Environ., 276, 119057, https://doi.org/10.1016/j.atmosenv.2022.119057, 2022.
Giering, R. and Kaminski, T.: Recipes for adjoint code construction, ACM T. Math. Software, 24, 437–474, https://doi.org/10.1145/293686.293695, 1998.
Giles, M. B. and Pierce, N. A.: An introduction to the adjoint approach to design, Flow, Turbulence and Combustion, 65, 393–415, https://doi.org/10.1023/A:1011430410075, 2000.
Greenslade, J. W., Alexander, S. P., Schofield, R., Fisher, J. A., and Klekociuk, A. K.: Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere, Atmos. Chem. Phys., 17, 10269–10290, https://doi.org/10.5194/acp-17-10269-2017, 2017.
Gu, Y., Henze, D. K., Nawaz, M. O., Cao, H., and Wagner, U. J.: Sources of PM2.5-Associated Health Risks in Europe and Corresponding Emission-Induced Changes During 2005–2015, GeoHealth, 7, e2022GH000767, https://doi.org/10.1029/2022GH000767, 2023.
Hakami, A., Henze, D. K., Seinfeld, J. H., Singh, K., Sandu, A., Kim, S., Byun, D., and Li, Q.: The adjoint of CMAQ, Environmental Science and Technology, 41, 7807–7817, https://doi.org/10.1021/es070944p, 2007.
Hascoet, L. and Pascual, V.: The Tapenade Automatic Differentiation Tool: Principles, Model, and Specification, ACM Trans. Math. Softw., 39, 20, https://doi.org/10.1145/2450153.2450158, 2013.
Henze, D. K., Hakami, A., and Seinfeld, J. H.: Development of the adjoint of GEOS-Chem, Atmos. Chem. Phys., 7, 2413–2433, https://doi.org/10.5194/acp-7-2413-2007, 2007.
Henze, D. K., Seinfeld, J. H., and Shindell, D. T.: Inverse modeling and mapping US air quality influences of inorganic PM2.5 precursor emissions using the adjoint of GEOS-Chem, Atmos. Chem. Phys., 9, 5877–5903, https://doi.org/10.5194/acp-9-5877-2009, 2009.
Hossaini, R., Chipperfield, M. P., Montzka, S. A., Rap, A., Dhomse, S., and Feng, W.: Efficiency of short-lived halogens at influencing climate through depletion of stratospheric ozone, Nat. Geosci., 8, 186–190, https://doi.org/10.1038/ngeo2363, 2015.
Hossaini, R., Chipperfield, M. P., Montzka, S. A., Leeson, A. A., Dhomse, S. S., and Pyle, J. A.: The increasing threat to stratospheric ozone from dichloromethane, Nat. Commun., 8, 15962, https://doi.org/10.1038/ncomms15962, 2017.
Huijnen, V., Williams, J., van Weele, M., van Noije, T., Krol, M., Dentener, F., Segers, A., Houweling, S., Peters, W., de Laat, J., Boersma, F., Bergamaschi, P., van Velthoven, P., Le Sager, P., Eskes, H., Alkemade, F., Scheele, R., Nédélec, P., and Pätz, H.-W.: The global chemistry transport model TM5: description and evaluation of the tropospheric chemistry version 3.0, Geosci. Model Dev., 3, 445–473, https://doi.org/10.5194/gmd-3-445-2010, 2010.
Jaeglé, L., Webster, C. R., May, R. D., Scott, D. C., Stimpfle, R. M., Kohn, D. W., Wennberg, P. O., Hanisco, T. F., Cohen, R. C., Proffitt, M. H., Kelly, K. K., Elkins, J., Baumgardner, D., Dye, J. E., Wilson, J. C., Pueschel, R. F., Chan, K. R., Salawitch, R. J., Tuck, A. F., Hovde, S. J., and Yung, Y. L.: Evolution and stoichiometry of heterogeneous processing in the Antarctic stratosphere, J. Geophys. Res.-Atmos., 102, 13235–13253, https://doi.org/10.1029/97JD00935, 1997.
Johnston, H.: Reduction of stratospheric ozone by nitrogen oxide catalysts from supersonic transport exhaust, Science, 173, 517–522, https://doi.org/10.1126/science.173.3996.517, 1971.
Kinnison, D. E., Brasseur, G. P., Walters, S., Garcia, R. R., Marsh, D. R., Sassi, F., Harvey, V. L., Randall, C. E., Emmons, L., Lamarque, J. F., Hess, P., Orlando, J. J., Tie, X. X., Randel, W., Pan, L. L., Gettelman, A., Granier, C., Diehl, T., Niemeier, U., and Simmons, A. J.: Sensitivity of chemical tracers to meteorological parameters in the MOZART-3 chemical transport model, J. Geophys. Res.-Atmos., 112, D20302, https://doi.org/10.1029/2006JD007879, 2007.
Köhler, M. O., Rädel, G., Dessens, O., Shine, K. P., Rogers, H. L., Wild, O., and Pyle, J. A.: Impact of perturbations to nitrogen oxide emissions from global aviation, J. Geophys. Res.-Atmos., 113, D11305, https://doi.org/10.1029/2007JD009140, 2008.
Kopacz, M., Jacob, D. J., Fisher, J. A., Logan, J. A., Zhang, L., Megretskaia, I. A., Yantosca, R. M., Singh, K., Henze, D. K., Burrows, J. P., Buchwitz, M., Khlystova, I., McMillan, W. W., Gille, J. C., Edwards, D. P., Eldering, A., Thouret, V., and Nedelec, P.: Global estimates of CO sources with high resolution by adjoint inversion of multiple satellite datasets (MOPITT, AIRS, SCIAMACHY, TES), Atmos. Chem. Phys., 10, 855–876, https://doi.org/10.5194/acp-10-855-2010, 2010.
Kuttippurath, J. and Nair, P. J.: The signs of Antarctic ozone hole recovery, Scientific Reports, 7, 585, https://doi.org/10.1038/s41598-017-00722-7, 2017.
Lickley, M., Solomon, S., Fletcher, S., Velders, G. J. M., Daniel, J., Rigby, M., Montzka, S. A., Kuijpers, L. J. M., and Stone, K.: Quantifying contributions of chlorofluorocarbon banks to emissions and impacts on the ozone layer and climate, Nat. Commun., 11, 1380, https://doi.org/10.1038/s41467-020-15162-7, 2020.
Maruhashi, J., Grewe, V., Frömming, C., Jöckel, P., and Dedoussi, I. C.: Transport patterns of global aviation NOx and their short-term O3 radiative forcing – a machine learning approach, Atmos. Chem. Phys., 22, 14253–14282, https://doi.org/10.5194/acp-22-14253-2022, 2022.
McElroy, M. B., Salawitch, R. J., Wofsy, S. C., and Logan, J. A.: Reductions of Antarctic ozone due to synergistic interactions of chlorine and bromine, Nature, 321, 759–762, https://doi.org/10.1038/321759a0, 1986.
Molina, M. J. and Rowland, F. S.: Stratospheric sink for chlorofluoromethanes: chlorine atom-catalysed destruction of ozone, Nature, 249, 810–812, https://doi.org/10.1038/249810a0, 1974.
Montzka, S. A., Dutton, G. S., Yu, P., Ray, E., Portmann, R. W., Daniel, J. S., Kuijpers, L., Hall, B. D., Mondeel, D., Siso, C., Nance, J. D., Rigby, M., Manning, A. J., Hu, L., Moore, F., Miller, B. R., and Elkins, J. W.: An unexpected and persistent increase in global emissions of ozone-depleting CFC-11, Nature, 557, 413–417, https://doi.org/10.1038/s41586-018-0106-2, 2018.
Murray, L. T., Jacob, D. J., Logan, J. A., Hudman, R. C., and Koshak, W. J.: Optimized regional and interannual variability of lightning in a global chemical transport model constrained by LIS/OTD satellite data, J. Geophys. Res.-Atmos., 117, D20307, https://doi.org/10.1029/2012JD017934, 2012.
NASA Ozone Watch: NASA Ozone Watch: Images, data, and information for atmospheric ozone, https://ozonewatch.gsfc.nasa.gov/meteorology/ozone_2009_MERRA_NH.html, last access: 25 March 2018.
Nawaz, M. O., Henze, D. K., Anenberg, S. C., Braun, C., Miller, J., and Pronk, E.: A Source Apportionment and Emission Scenario Assessment of PM2.5- and O3-Related Health Impacts in G20 Countries, GeoHealth, 7, e2022GH000713, https://doi.org/10.1029/2022GH000713, 2023.
Qu, Z., Henze, D. K., Cooper, O. R., and Neu, J. L.: Impacts of global NOx inversions on NO2 and ozone simulations, Atmos. Chem. Phys., 20, 13109–13130, https://doi.org/10.5194/acp-20-13109-2020, 2020.
Quadros, F., Snellen, M., and Dedoussi, I. C.: Regional sensitivities of air quality and human health impacts to aviation emissions, Environ. Res. Lett., 15, 105013, https://doi.org/10.1088/1748-9326/abb2c5, 2020.
Rigby, M., Park, S., Saito, T., Western, L. M., Redington, A. L., Fang, X., Henne, S., Manning, A. J., Prinn, R. G., Dutton, G. S., Fraser, P. J., Ganesan, A. L., Hall, B. D., Harth, C. M., Kim, J., Kim, K.-R., Krummel, P. B., Lee, T., Li, S., Liang, Q., Lunt, M. F., Montzka, S. A., Mühle, J., O'Doherty, S., Park, M.-K., Reimann, S., Salameh, P. K., Simmonds, P., Tunnicliffe, R. L., Weiss, R. F., Yokouchi, Y., and Young, D.: Increase in CFC-11 emissions from eastern China based on atmospheric observations, Nature, 569, 546–550, https://doi.org/10.1038/s41586-019-1193-4, 2019.
Ross, M., Toohey, D., Peinemann, M., and Ross, P.: Limits on the space launch market related to stratospheric ozone depletion, Astropolitics, 7, 50–82, https://doi.org/10.1080/14777620902768867, 2009.
Rotman, D. A., Tannahill, J. R., Kinnison, D. E., Connell, P. S., Bergmann, D., Proctor, D., Rodriguez, J. M., Lin, S. J., Rood, R. B., Prather, M. J., Rasch, P. J., Considine, D. B., Ramaroson, R., and Kawa, S. R.: Global Modeling Initiative assessment model: Model description, integration, and testing of the transport shell, J. Geophys. Res.-Atmos., 106, 1669–1691, https://doi.org/10.1029/2000JD900463, 2001.
Ryan, R. G., Marais, E. A., Balhatchet, C. J., and Eastham, S. D.: Impact of Rocket Launch and Space Debris Air Pollutant Emissions on Stratospheric Ozone and Global Climate, Earth's Future, 10, e2021EF002612, https://doi.org/10.1029/2021EF002612, 2022.
Sander, S. P., Friedl, R. R., DeMore, W. B., Ravishankara, A. R., Golden, D. M., Kolb, C. E., Kurylo, M. J., Hampson, R. F., Huie, R. E., Molina, M. J., and Moortgat, G. K.: Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling; Supplement to Evaluation 12: Update of Key Reactions, https://jpldataeval.jpl.nasa.gov/pdf/JPL_00-03.pdf (last access: 22 July 2024), 2000.
Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Moortgat, G. K., Wine, P. H., Ravishankara, a R., Kolb, C. E., Molina, M. J., Diego, S., Jolla, L., Huie, R. E., and Orkin, V. L.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies, Evaluation No. 17, JPL Publication 10-6, Pasadena, https://jpldataeval.jpl.nasa.gov/pdf/JPL 10-6 Final 15June2011.pdf (last access: 22 July 2024), 2011.
Sandu, A., Daescu, D. N., and Carmichael, G. R.: Direct and adjoint sensitivity analysis of chemical kinetic systems with KPP: Part I – Theory and software tools, Atmos. Environ., 37, 5083–5096, https://doi.org/10.1016/j.atmosenv.2003.08.019, 2003.
Sandu, A., Daescu, D. N., Carmichael, G. R., and Chai, T.: Adjoint sensitivity analysis of regional air quality models, J. Comput. Phys., 204, 222–252, https://doi.org/10.1016/j.jcp.2004.10.011, 2005.
Sausen, R., Deckert, R., Jöckel, P., Aquila, V., Brinkop, S., Burkhardt, U., Cionni, I., Dall'Amico, M., Dameris, M., Dietmüller, S., Eyring, V., Gottschaldt, K., Grewe, V., Hendricks, J., Ponater, M., and Righi, M.: Global Chemistry-Climate Modelling with EMAC BT – High Performance Computing in Science and Engineering, Garching/Munich 2009, 663–674, https://doi.org/10.1007/978-3-642-13872-0, 2010.
Schäfer, A., Heywood, J. B., Jacoby, H. D., and Waitz, I. A.: Transportation in a Climate-Constrained World, The MIT Press, ISBN 9780262512343, 2009.
Sherwen, T., Schmidt, J. A., Evans, M. J., Carpenter, L. J., Großmann, K., Eastham, S. D., Jacob, D. J., Dix, B., Koenig, T. K., Sinreich, R., Ortega, I., Volkamer, R., Saiz-Lopez, A., Prados-Roman, C., Mahajan, A. S., and Ordóñez, C.: Global impacts of tropospheric halogens (Cl, Br, I) on oxidants and composition in GEOS-Chem, Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, 2016.
Singh, K., Eller, P., Sandu, A., Bowman, K., Jones, D., and Lee, M.: Improving GEOS-Chem Model Tropospheric Ozone through Assimilation of Pseudo Tropospheric Emission Spectrometer Profile Retrievals, in: Computational Science – ICCS 2009, ICCS 2009, Lecture Notes in Computer Science, vol. 5545, edited by: Allen, G., Nabrzyski, J., Seidel, E., van Albada, G. D., Dongarra, J., and Sloot, P. M. A., Springer, Berlin, Heidelberg, https://doi.org/10.1007/978-3-642-01973-9_34, 2009.
Slaper, H., Velders, G. J. M., Daniel, J. S., de Gruijl, F. R., and van der Leun, J. C.: Estimates of ozone depletion and skin cancer incidence to examine the Vienna Convention achievements, Nature, 384, 256, https://doi.org/10.1038/384256a0, 1996.
Solomon, S.: Stratospheric ozone depletion: A review of concepts and history, Rev. Geophys., 37, 275–316, https://doi.org/10.1029/1999RG900008, 1999.
Solomon, S., Garcia, R. R., Rowland, F. S., and Wuebbles, D. J.: On the depletion of Antarctic ozone, Nature, 321, 755–758, https://doi.org/10.1038/321755a0, 1986.
Solomon, S., Kinnison, D., Bandoro, J., and Garcia, R.: Simulation of polar ozone depletion: An update, J. Geophys. Res.-Atmos., 120, 7958–7974, https://doi.org/10.1002/2015JD023365, 2015.
Solomon, S., Ivy, D. J., Kinnison, D., Mills, M. J., Neely, R. R., and Schmidt, A.: Emergence of healing in the Antarctic ozone layer, Science, 353, 269–274, https://doi.org/10.1126/science.aae0061, 2016.
Søvde, O. A., Prather, M. J., Isaksen, I. S. A., Berntsen, T. K., Stordal, F., Zhu, X., Holmes, C. D., and Hsu, J.: The chemical transport model Oslo CTM3, Geosci. Model Dev., 5, 1441–1469, https://doi.org/10.5194/gmd-5-1441-2012, 2012.
Tang, Z., Jiang, Z., Chen, J., Yang, P., and Shen, Y.: The capabilities of the adjoint of GEOS-Chem model to support HEMCO emission inventories and MERRA-2 meteorological data, Geosci. Model Dev., 16, 6377–6392, https://doi.org/10.5194/gmd-16-6377-2023, 2023.
Toon, G. C., Farmer, C. B., Lowes, L. L., Schaper, P. W., Blavier, J.-F., and Norton, R. H.: Infrared aircraft measurements of stratospheric composition over Antarctica during September 1987, J. Geophys. Res.-Atmos., 94, 16571–16596, https://doi.org/10.1029/JD094iD14p16571, 1989.
Wang, J., Xu, X., Henze, D. K., Zeng, J., Ji, Q., Tsay, S.-C., and Huang, J.: Top-down estimate of dust emissions through integration of MODIS and MISR aerosol retrievals with the GEOS-Chem adjoint model, Geophys. Res. Lett., 39, L08802, https://doi.org/10.1029/2012GL051136, 2012.
Wang, X., Jacob, D. J., Eastham, S. D., Sulprizio, M. P., Zhu, L., Chen, Q., Alexander, B., Sherwen, T., Evans, M. J., Lee, B. H., Haskins, J. D., Lopez-Hilfiker, F. D., Thornton, J. A., Huey, G. L., and Liao, H.: The role of chlorine in global tropospheric chemistry, Atmos. Chem. Phys., 19, 3981–4003, https://doi.org/10.5194/acp-19-3981-2019, 2019.
Weatherhead, E. C. and Andersen, S. B.: The search for signs of recovery of the ozone layer, Nature, 441, 39–45, https://doi.org/10.1038/nature04746, 2006.
Weber, M., Coldewey-Egbers, M., Fioletov, V. E., Frith, S. M., Wild, J. D., Burrows, J. P., Long, C. S., and Loyola, D.: Total ozone trends from 1979 to 2016 derived from five merged observational datasets – the emergence into ozone recovery, Atmos. Chem. Phys., 18, 2097–2117, https://doi.org/10.5194/acp-18-2097-2018, 2018.
Weisenstein, D. K., Yue, G. K., Ko, M. K. W., Sze, N.-D., Rodriguez, J. M., and Scott, C. J.: A two-dimensional model of sulfur species and aerosols, J. Geophys. Res.-Atmos., 102, 13019–13035, https://doi.org/10.1029/97JD00901, 1997.
WMO/UNEP: World Meteorological Organization/United Nations Environment Programme Scientific Assessment of Ozone Depletion: 2014, https://csl.noaa.gov/assessments/ozone/2014/report/2014OzoneAssessment.pdf (last access: 22 July 2024), 2014.
Zhao, S., Russell, M. G., Hakami, A., Capps, S. L., Turner, M. D., Henze, D. K., Percell, P. B., Resler, J., Shen, H., Russell, A. G., Nenes, A., Pappin, A. J., Napelenok, S. L., Bash, J. O., Fahey, K. M., Carmichael, G. R., Stanier, C. O., and Chai, T.: A multiphase CMAQ version 5.0 adjoint, Geosci. Model Dev., 13, 2925–2944, https://doi.org/10.5194/gmd-13-2925-2020, 2020.
Zhu, L., Jacob, D. J., Eastham, S. D., Sulprizio, M. P., Wang, X., Sherwen, T., Evans, M. J., Chen, Q., Alexander, B., Koenig, T. K., Volkamer, R., Huey, L. G., Le Breton, M., Bannan, T. J., and Percival, C. J.: Effect of sea salt aerosol on tropospheric bromine chemistry, Atmos. Chem. Phys., 19, 6497–6507, https://doi.org/10.5194/acp-19-6497-2019, 2019.
Short summary
Atmospheric model gradients provide a meaningful tool for better understanding the underlying atmospheric processes. Adjoint modeling enables computationally efficient gradient calculations. We present the adjoint of the GEOS-Chem unified chemistry extension (UCX). With this development, the GEOS-Chem adjoint model can capture stratospheric ozone and other processes jointly with tropospheric processes. We apply it to characterize the Antarctic ozone depletion potential of active halogen species.
Atmospheric model gradients provide a meaningful tool for better understanding the underlying...
