Atmospheric Chemistry and Physics www.atmos-chem-phys.net 1680-7316 1680-7324 9 22 2009 10.5194/acp-9-8719-2009 http://www.atmos-chem-phys.net/9/8719/2009/ http://www.atmos-chem-phys.net/9/8719/2009/acp-9-8719-2009.html http://www.atmos-chem-phys.net/9/8719/2009/acp-9-8719-2009.pdf 8719 8733 2009-11-16 Explicit calculation of indirect global warming potentials for halons using atmospheric models D. Youn K. O. Patten J.-T. Lin D. J. Wuebbles wuebbles@atmos.uiuc.edu Dept. of Atmospheric Sciences, University of Illinois at Urbana-Champaign, 105 S. Gregory St., Urbana, IL 61801, USA School of Earth & Environmental Sciences, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul 151-747, Republic of Korea School of Engineering and Applied Sciences, Harvard University, 19 Oxford St., Cambridge, MA 02138, USA The concept of Global Warming Potentials (GWPs) has been extensively used in policy consideration as a relative index for comparing the climate impact of an emitted greenhouse gas (GHG), relative to carbon dioxide with equal mass emissions. Ozone depletion due to emission of chlorinated or brominated halocarbons leads to cooling of the climate system in the opposite direction to the direct warming contribution by halocarbons as GHGs. This cooling is a key indirect effect of the halocarbons on climatic radiative forcing, which is accounted for by indirect GWPs. With respect to climate, it is critical to understand net influences considering direct warming and indirect cooling effects especially for Halons due to the greater ozone-depleting efficiency of bromine over chlorine. Until now, the indirect GWPs have been calculated using a parameterized approach based on the concept of Equivalent Effective Stratospheric Chlorine (EESC) and the observed ozone depletion over the last few decades. As a step towards obtaining indirect GWPs through a more robust approach, we use atmospheric models to explicitly calculate the indirect GWPs of Halon-1211 and Halon-1301 for a 100-year time horizon. State-of-the-art global chemistry-transport models (CTMs) were used as the computational tools to derive more realistic ozone depletion changes caused by an added pulse emission of the two major Halons at the surface. The radiative forcings on climate from the ozone changes have been calculated for indirect GWPs using an atmospheric radiative transfer model (RTM). The simulated temporal variations of global average total column Halons after a pulse perturbation follow an exponential decay with an e-folding time which is consistent with the expected chemical lifetimes of the Halons. Our calculated indirect GWPs for the two Halons are much smaller than those from past studies but are within a single standard deviation of WMO (2007) values and the direct GWP values derived agree with the published values. Our model-based assessment of the Halon indirect GWPs thus confirms the significant importance of indirect effects on climate. Briegleb, B. P.: Delta-Eddington Approximation for Solar Radiation in the NCAR Community Climate Model, J. Geophys. Res., 97, 7603–7612, 1992a. Briegleb, B. P.: Longwave Band Model for Thermal Radiation in Climate Studies, J. Geophys. Res., 97, 11 475–11 485, 1992b. 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., 105, 3955–3973, 10.1029/1999JD900932, 2000. Coy, L. and Swinbank, R.: Characteristics of stratospheric winds and temperatures produced by data assimilation, J. Geophys. Res, 102, 25763–25781, 1997. Daniel, J. S., Solomon, S., and Albritton, D. L.: On the Evaluation of Halocarbon Radiative Forcing and Global Warming Potentials, J. Geophys. Res., 100, 1271–1285, 1995. Daniel, J. S, Velders, G. J. M., Douglass, A. R., Forster, P. M. D., Hauglustaine, D. A., Isaksen, I. S. A., Kuijpers, L. J. M., McCulloch, A., and Wallington, T. J.: Halocarbon Scenarios, Ozone Depletion Potentials, and Global Warming Potentials, Chapter 8 in Scientific Assessment of Ozone Depletion: 2006, Global Ozone Research and Monitoring Project – Report No. 50, World Meteorological Organization, Geneva, Switzerland, 572 pp., 2007. DeMore, W. B., Sander, S. P., Golden, D. M., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E., and Molina, M. J.: Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling, Evaluation Number 12, Jet Propulsion Laboratory (JPL) Publication 97-4, Pasadena, California, 1997. Forster, P., Ramaswamy, V., Artaxo, P., Berntsen, T., Betts, R., Fahey, D. W., Haywood, J., Lean, J., Lowe, D. C., Myhre, G., Nganga, J., Prinn, R., Raga, G., Schulz, M., and Van Dorland, R.: Changes in Atmospheric Constituents and in Radiative Forcing, in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor M., and Miller H. L., Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007. Garcia, R. R., Marsh, D. R., Kinnison, D. E., Boville, B. A., and Sassi, F.: Simulation of secular trends in the middle atmosphere, 1950–2003, J. Geophys. Res., 112, D09301, doi:10.1029/2006JD007485, 2007. Guillas, S., Stein M. L., Wuebbles, D. J., and Xia, J.: Using chemistry-transport modeling in statistical analysis of stratospheric ozone trends from observations, J. Geophys. Res., 109, D22303, 10.1029/2004JD005049, 2004. Hansen, J., Sato, M., and Ruedy, R.: Radiative forcing and climate response, J. Geophys. Res., 102, 6831–6864, 1997. Horowitz, L., Walters, S., Mauzerall, D., Emmons, L., Rasch, P., Granier, C., Tie, X., Lamarque, J.-F., Schultz, M., Tyndall, G., Orlando, J., and Brasseur, G.: A global simulation of tropospheric ozone and related tracers: Description and evaluation of MOZART, version 2. J. Geophys. Res., 108, 4784, doi:10.1029/2002JD002853, 2003. Intergovernmental Panel on Climate Change (IPCC): Climate Change, The IPCC Scientific Assessment, edited by: Houghton, J. T., Jenkins, G. J., Ephraums, J. J., (Chapter 2, Radiative Forcing on Climate, Shine, K. P., Derwent, R. G., Wuebbles, D. J., and Morcrette, J.-J.), Cambridge University Press, New York, 1990. Intergovernmental Panel on Climate Change (IPCC): Climate Change 2001: The Scientific Basis. Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Houghton, J. T., Ding, Y., Griggs, D. J., Noguer, M., van der Linden, P. J., and Xiaosu, D., Cambridge University Press, Cambridge, UK and New York, 881 pp., 2001. Intergovernmental Panel on Climate Change and Technology and Economic Assessment Panel (IPCC/TEAP): IPCC/TEAP Special Report on Safeguarding the Ozone Layer and the Global Climate System: Issues Related to Hydrofluorocarbons and Perfluorocarbons, edited by: Metz, B., Kuijpers, L., Solomon, S., Andersen, S. O., Davidson, O., Pons, J., de Jager, D., Kestin, T., Manning, M., and Meyer, L. A., Cambridge University Press, New York, 478 pp., 2005. Intergovernmental Panel on Climate Change (IPCC): Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K.B., Tignor, M., and Miller, H.L., Cambridge University Press, New York, 996 pp., 2007. Jain, A. K., Briegleb, B. P., Minschwaner, K., and Wuebbles, D. J.: Radiative forcings and global warming potentials of 39 greenhouse gases, J. Geophys. Res., 105, 20 773–20 790, 2000. Joshi, M., Shine, K., Ponater, M., Stuber, N., Sausen, R., and Li, L.: A comparison of climate response to different radiative forcings in three general circulation models: towards an improved metric of climate change, Clim. Dynam., 20, 843–854, 2003. 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., 112, D20302, doi:10.1029/2006JD007879, 2007. Kotamarthi, V. R., Wuebbles, D. J., and Reck, R. A.: Effects of non-methane hydrocarbons on lower stratospheric and upper tropospheric 2-D zonal average model chemical climatology, J. Geophys, Res., 104, 21 537–21 547, 1999. Lacis, A. A., Wuebbles, D. J., and Logan, J. A.: Radiative Forcing of Climate by Changes in the Vertical Distribution of Ozone, J. Geophys. Res., 95, 9971–9981, 1990. Li, Y., Patten, K. O., Youn, D., and Wuebbles, D. J.: Potential impacts of CF₃I on ozone as a replacement for CF₃Br in aircraft applications, Atmos. Chem. Phys., 6, 4559–4568, 2006. Miller, A. J., Nagatani, R. M., Flynn, L. E., Kondragunta, S., Beach, E., Stolarski, R., McPeters, R. D., Bhartia, P. K., De-Land, M. T., Jackman, C. H., Wuebbles, D. J., Patten, K. O., and Cebula, R. P.: A cohesive total ozone data set from the SBUV(/2) satellite system, J. Geophys. Res., 107, 4701, doi:10.1029/2001JD000853, 2002. Naik, V., Jain, A. K., Patten, K. O., and Wuebbles, D. J.: Consistent sets of atmospheric lifetimes and radiative forcings on climate for CFC replacements: HCFCs and HFCs, J. Geophys. Res., 105, 6903–6914, 2000. Newman, P. A., Daniel, J. S., Waugh, D. W., and Nash, E. R.: A new formulation of equivalent effective stratospheric chlorine (EESC), Atmos. Chem. Phys., 7, 4537–4552, 2007. Newman, P. A., Nash, E. R., Kawa, S. R., Montzka, S. A., and Schauffler, S. M.; When will the Antarctic ozone hole recover?, Geophys. Res. Lett., 33, L12814, doi:10.1029/2005GL025232, 2006. Pan, L. L., Wei, J. C., Kinnison, D. E., Garcia, R.R., Wuebbles, D. J., and Brasseur, G. P.: A set of diagnostics for evaluating chemistry-climate models in the extratropical tropopause region, J. Geophys. Res., 112, D09316, doi:10.1029/2006JD007792, 2007. Pfister, G. G., Emmons, L. K., Hess, P. G., Lamarque, J.-F., Orlando, J. J., Walters, S., Guenther, A., Palmer, P. I., and Lawrence, P. J.: Contribution of isoprene to chemical budgets: A model tracer study with the NCAR CTM MOZART-4, J. Geophys. Res., 113, D05308, doi:10.1029/2007JD008948, 2008. Ramaswamy, V., Schwarzkopf, M. D., and Shine, K. P.: Radiative forcing of climate from halocarbon induced global stratospheric ozone loss, Nature, 355, 810–812, 1992. Rothman, L. S., Jacquemart, D., Barbe, A., Chris Benner, D., Birk, M., Brown, L. R., Carleer, M. R., Chackerian Jr., C., Chance, K., Coudert, L. H., Dana, V., Devi, V. M., Flaud, J.-M., Gamache, R. R., Goldman, A., Hartmann, J.-M., Jucks, K. W., Maki, A. G., Mandin, J.-Y., Massie, S. T., Orphal, J., Perrin, A., Rinsland, C. P., Smith, M. A. H., Tennyson, J., Tolchenov, R. N., Toth, R. A., Vander Auwera, J., Varanasi, P., and Wagner, G.: The HITRAN 2004 molecular spectroscopic database, J. Quant. Spectrosc. Ra., 96, 139-204, ISSN 0022-4073, doi:10.1016/j.jqsrt.2004.10.008, 2005. Sander, S. P., Friedl, R. R., Golden, D. M., Kurylo, M. J., Huie, R. E., Orkin, V. L., Moortgat, G. K., Ravishankara, A. R., Kolb, C. E., Molina, M. J., and Finlayson-Pitts, B. J.: Chemical kinetics and photochemical data for use in atmospheric studies, NASA/JPL Publication 02-25. Pasadena, California, 334 pp., 2003. Sassi, F., Garcia, R. R., Boville, B. A., and Liu, H.: On temperature inversions and the mesospheric surf zone, J. Geophys. Res., 107, 4380, doi:10.1029/2001JD001525, 2002. Stamnes, K., Tsay, S.-C., Wiscombe, W., and Jayaweera, K.: Numerically stable algorithm for discrete-ordinate-method radiative transfer in multiple scattering and emitting layered media, Appl. Optimizat., 27, 2502–2509, 1988. Velders, G. J. M., Anderson S. O., Daniel J. S., Fahey D. W., and McFarland, M.: The importance of the Montreal Protocol in protecting climate, P. Natl. Acad. Sci. USA, 104, 4814–4819, 2007. World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 1994, Global Ozone, Research and Monitoring Project – Report 37, Geneva, Switzerland, 1995. World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 1998, Global Ozone, Research and Monitoring Project – Report 44, Geneva, Switzerland, 1999. World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 2002, Global Ozone, Research and Monitoring Project – Report 47, Geneva, Switzerland, 2003. World Meteorological Organization (WMO): Scientific Assessment of Ozone Depletion: 2006, Global Ozone, Research and Monitoring Project – Report 50, Geneva, Switzerland, 2007. Wuebbles, D. J.: Weighing functions for ozone depletion and greenhouse gas effects on climate, Annu. Rev. Energ. Env., 20, 45–70, 1995. Wuebbles, D. J., Patten, K. O., Johnson, M. T., and Kotamarthi, R.: The new methodology for Ozone Depletion Potentials of short-lived compounds: n-propyl bromide as an example, J. Geophys. Res., 106, 14 551–14 571, 2001. Wuebbles, D. J. and Patten, K. O.: Three-Dimensional Modeling of HCFC-123 in the Atmosphere: Assessing Its Potential Environmental Impacts and Rationale for Continued Use, Environ. Sci. Technol., 43, 3208–3213, 2009. Youn, D., Choi, W., Lee, H., and Wuebbles, D. J.: Interhemispheric differences in changes of long-lived tracers in the middle stratosphere over the last decade, Geophys. Res. Lett., 33, L03807, doi:10.1029/2005GL024274, 2006.