[en] Carbon tetrachloride is an ozone-depleting substance, which is controlled by the Montreal Protocol and for which the atmospheric abundance is decreasing. However, the current observed rate of this decrease is known to be slower than expected based on reported CCl4 emissions and its estimated overall atmospheric lifetime. Here we use a three-dimensional (3-D) chemical transport model to investigate the impact on its predicted decay of uncertainties in the rates at which CCl4 is removed from the atmosphere by photolysis, by ocean uptake and by degradation in soils. The largest sink is atmospheric photolysis (76% of total) but a reported 10% uncertainty in its combined photolysis cross-section and quantum yield has only a modest impact on the modelled rate of CCl4 decay. This is partly due to the limiting effect of the rate of transport of CCl4 from the main tropospheric reservoir to the stratosphere where photolytic loss occurs. The model suggests large interannual variability in the magnitude of this stratospheric photolysis sink caused by variations in transport. The impact of uncertainty in the minor soil sink (9% of total) is also relatively small. In contrast, the model shows that uncertainty in ocean loss (15% of total) has the largest impact on modelled CCl4 decay due to its sizeable contribution to CCl4 loss and large uncertainty range (157 to 313 years). With an assumed CCl4 emission rate of 39 Gg/yr, the reference simulation with best estimate of loss processes still underestimates the observed CCl4 (overestimates the decay) over the past two decades but to a smaller extent than previous studies. Changes to the rate of CCl4 loss processes, in line with known uncertainties, could bring the model into agreement with in situ surface and remote-sensing measurements, as could an increase in emissions to around 45 Gg/yr. Further progress in constraining the CCl4 budget is partly limited by systematic biases between observational datasets. For example, surface observations from the NOAA network are larger than from the AGAGE network but have shown a steeper decreasing trend over the past two decades. These differences imply a difference in emissions which is significant relative to uncertainties in the magnitudes of the CCl4 sinks.
Disciplines :
Earth sciences & physical geography
Author, co-author :
Chipperfield, M. P.
Liang, Q.
Rigby, M.
Hossaini, R.
Montzka, S. A.
Dhomse, S.
Feng, W.
Prinn, R. G.
Weiss, R. F.
Harth, C. M.
Salameh, P. K.
Mühle, J.
O'Doherty, S.
Young, D.
Simmonds, P. G.
Krummel, P. B.
Fraser, P. J.
Steele, L. P.
Happell, J. D.
Rhew, R. C.
Butler, J.
Yvon-Lewis, S. A.
Hall, B.
Nance, D.
Moore, F.
Miller, B. R.
Elkins, J. W.
Harrison, J. J.
Boone, C. D.
Atlas, E. L.
Mahieu, Emmanuel ; Université de Liège > Département d'astrophys., géophysique et océanographie (AGO) > Groupe infra-rouge de phys. atmosph. et solaire (GIRPAS)
Allen, N. D. C., Bernath, P. F., Boone, C. D., Chipperfield, M. P., Fu, D., Manney, G. L., Oram, D. E., Toon, G. C., and Weisenstein, D. K.: Global carbon tetrachloride distributions obtained from the Atmospheric Chemistry Experiment (ACE), Atmos. Chem. Phys., 9, 7449-7459, doi:10.5194/acp-9-7449-2009, 2009.
Bernath, P. F.: The Atmospheric Chemistry Experiment (ACE), J. Quant. Spectrosc. Ra., 186, 3-16, doi:10.1016/j.jqsrt.2016.04.006, 2017.
Brown, A. T., Chipperfield, M. P., Boone, C., Wilson, C., Walker, K. A., and Bernath, P. F.: Trends in atmospheric halogen containing gases since 2004, J. Quant. Spectrosc. Ra., 112, 2552-2566, doi:10.1016/j.jqsrt.2011.07.005, 2011.
Burkholder, J. B., Mellouki, W., Fleming, E. L., George, C., Heard, D. E., Jackman, C. H., Kurylo, M. J., Orkin, V. L., Swartz, W. H., and Wallington, T. J.: Evaluation of Atmospheric Loss Processes, Chap. 3 of SPARC Report on the Lifetimes of Stratospheric Ozone-Depleting Substances, Their Replacements, and Related Species, edited by: Ko, M., Newman, P., Reimann, S., and Strahan, S., SPARC Report No. 6, WCRP-15/2013, 2013.
Butler, J. H., Yvon-Lewis, S. A., Lobert, J. M., King, D. B., Montzka, S. A., Bullister, J. L., Koropalov, V., Elkins, J. W., Hall, B. D., Hu, L., and Liu, Y.: A comprehensive estimate for loss of atmospheric carbon tetrachloride (CCl4) to the ocean, Atmos. Chem. Phys., 16, 10899-10910, doi:10.5194/acp-16- 10899-2016, 2016.
Carpenter, L. J., Reimann, S., Burkholder, J. B., Clerbaux, C., Hall, B. D., Hossaini, R., Laube, J. C., and Yvon-Lewis, S. A.: Ozone- Depleting Substances (ODSs) and Other Gases of Interest to the Montreal Protocol, Chap. 1 in Scientific Assessment of Ozone Depletion: 2014, Global Ozone Research and Monitoring Project - Report No. 55, World Meteorological Organization, Geneva, Switzerland, 2014.
Chipperfield, M. P.: New version of the TOMCAT/SLIMCAT offline chemical transport model: Intercomparison of stratospheric tracer experiments, Q. J. Roy. Meteor. Soc., 132, 1179-1203, 2006.
Chipperfield, M. P., Liang, Q., Abraham, L., Bekki, S., Braesicke, P., Dhomse, S., Di Genova, G., Fleming, E. L., Hardiman, S., Iachetti, D., Jackman, C. H., Kinnison, D. E., Marchand, M., Pitari, G., Rozanov, E., Stenke, A., and Tummon, F.: Evaluation of Atmospheric Loss Processes, Chap. 5 of SPARC Report on the Lifetimes of Stratospheric Ozone-Depleting Substances, Their Replacements, and Related Species, edited by: Ko, M., Newman, P., Reimann, S., and Strahan, S., SPARC Report No. 6, WCRP-15/2013, 2013.
Chipperfield, M. P., Q. Liang, S. E. Strahan, O. Morgenstern, S. S. Dhomse, N. L. Abraham, A. T. Archibald, S. Bekki, P. Breasicke, G. Di Genova, E. F. Fleming, S. C. Hardiman, D. Iachetti, C. H. Jackman, D. E. Kinnison, M. Marchand, G. Pitari, J. A. Pyle, E. Rozanov, A. Stenke, F. Tummon, Multi-model estimates of atmospheric lifetimes of long-lived Ozone-Depleting- Substances: Present and future, J. Geophys. Res., 119, 2555- 2573, doi:10.1002/2013JD021097, 2014.
Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P., Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P., Bechtold, P., Beljaars, A. C. M., van de Berg, L., Bidlot, J., Bormann, N., Delsol, C., Dragani, R., Fuentes, M., Geer, A. J., Haimberger, L., Healy, S. B., Hersbach, H., Holm, E. V., Isaksen, L., Kallberg, P., Kohler, M., Matricardi, M., McNally, A. P., Monge-Sanz, B. M., Morcrette, J.-J., Park, B.-K., Peubey, C., de Rosnay, P., Tavolato, C., Thepaut, J.-N., and Vitart, F.: The ERA-Interim reanalysis: configuration and performance of the data assimilation system, Q. J. Roy. Meteor. Soc., 137, 553-597, doi:10.1002/qj.828, 2011.
Graziosi, F., Arduini, J., Bonasoni, P., Furlani, F., Giostra, U., Manning, A. J., McCulloch, A., O'Doherty, S., Simmonds, P. G., Reimann, S., Vollmer, M. K., and Maione, M.: Emissions of carbon tetrachloride from Europe, Atmos. Chem. Phys., 16, 12849- 12859, doi:10.5194/acp-16-12849-2016, 2016.
Hall, B. D., Dutton, G. S., Mondeel, D. J., Nance, J. D., Rigby, M., Butler, J. H., Moore, F. L., Hurst, D. F., and Elkins, J. W.: Improving measurements of SF6 for the study of atmospheric transport and emissions, Atmos. Meas. Tech., 4, 2441-2451, doi:10.5194/amt-4-2441-2011, 2011.
Happell, J. D. and Roche, M. P.: Soils: a global sink of atmospheric carbon tetrachloride, Geophys. Res. Lett., 30, 1088, doi:10.1029/2002GL015957, 2003.
Happell, J. D., Mendoza, Y., and Goodwin, K.: A reassessment of the soil sink for atmospheric carbon tetrachloride based on flux chamber measurements, J. Atmos. Chem., 71, 113-123, 2014.
Harrison, J. J., Boone, C. D., and Bernath, P. F.: New and improved infrared absorption cross sections and ACE-FTS retrievals of carbon tetrachloride (CCl4/, J. Quant. Spectrosc. Ra., 186, 139-149, doi:10.1016/j.jqsrt.2016.04.025, 2016.
Hu, L., Montzka, S. A., Miller, B. R., Andrews, A. E., Miller, J. B., Lehman, S. J., Sweeney, C., Miller, S., Thoning, K., Siso, C., Atlas, E., Blake, D., de Gouw, J. A., Gilman, J. B., Dutton, G., Elkins, J. W., Hall, B. D., Chen, H., Fischer, M. L., Mountain, M., Nehrkorn, T., Biraud, S. C., Moore, F., and Tans, P. P.: Continued emissions of carbon tetrachloride from the U.S. nearly two decades after its phase-out for dispersive uses, P. Natl. Acad. Sci., 113, 2880-2885, doi:10.1073/pnas.1522284113, 2016.
Krysell, M., Fogelqvist, E., and Tanhua, T.: Apparent removal of the transient tracer carbon tetrachloride from anoxic seawater, Geophys. Res. Lett., 21, 2511-2514, doi:10.1029/94GL02336, 1994.
Liang, Q., Newman, P. A., Daniel, J. S., Reimann, S., Hall, B. D., Dutton, G., and Kuijpers, L. J. M.: Constraining the carbon tetrachloride (CCl4/ budget using its global trend and inter-hemispheric gradient, Geophys. Res. Lett., 41, 5307-5315, doi:10.1002/2014GL060754, 2014.
Monge-Sanz, B., Chipperfield, M. P., Simmons, A., and Uppala, S.: Mean age of air and transport in a CTM: Comparison of different ECMWF analyses, Geophys. Res. Lett., 34, L04801, doi:10.1029/2006GL028515, 2007.
O'Doherty, S., Simmonds, P. G., Cunnold, D. M.,Wang, H. J., Sturrock, G. A., Fraser, P. J., Ryall, D., Derwent, R. G., Weiss, R. F., Salameh, P., Miller, B. R., and Prinn, R. G.: In situ chloroform measurements at Advanced Global Atmospheric Gases Experiment atmospheric research stations from 1994 to 1998, J. Geophys. Res., 106, 20429-20444, doi:10.1029/2000JD900792, 2001.
Prinn, R., Weiss, R., Fraser, P., Simmonds, P., Cunnold, D., Alyea, F., O'Doherty, S., Salameh, P., Miller, B., and Huang, J.: A history of chemically and radiatively important gases in air deduced from ALE/GAGE/AGAGE, J. Geophys. Res., 105, 17751- 17792, 2000.
Prinn, R. G., Weiss, R. F., Fraser, P. J., Simmonds, P. G., Cunnold, D. M., O'Doherty, S., Salameh, P. K., Porter, L.W., Krummel, P. B., Wang, R. H. J., Miller, B. R., Harth, C., Greally, B. R., Van Woy, F. A., Steele, L. P., Muhle, J., Sturrock, G. A., Alyea, F. N., Huang, J., and Hartley, D. E.: The ALE/GAGE AGAGE Network, Carbon Dioxide Information Analysis Center (CDIAC), Oak Ridge National Laboratory (ORNL), US Department of Energy (DOE), 2016.
Rhew, R. C. and Happell, J. D.: The atmospheric partial lifetime of carbon tetrachloride with respect to the global soil sink, Geophys. Res. Lett., 43, 2889-2895, doi:10.1002/2016GL067839, 2016.
Rigby, M., Prinn, R. G., O'Doherty, S., Miller, B. R., Ivy, D., Muhle, J., Harth, C. M., Salameh, P. K., Arnold, T., Weiss, R. F., Krummel, P. B., Steele, L. P., Fraser, P. J., Young, D., and Simmonds, P. G.: Recent and future trends in synthetic greenhouse gas radiative forcing, Geophys. Res. Lett., 41, 2623-2630, doi:10.1002/2013GL059099, 2014.
Rinsland, C. P., Mahieu, E., Demoulin, P., Zander, R., Servais, C., and Hartmann, J.-M.: Decrease of the carbon tetrachloride (CCl4/ loading above Jungfraujoch, based on high resolution infrared solar spectra recorded between 1999 and 2011, J. Quant. Spectrosc. Ra., 113, 1322-1329, doi:10.1016/j.jqsrt.2012.02.016, 2012.
Sander, S. P., Friedl, R. R., Abbatt, J. P. D., Barker, J. R., Burkholder, J. B., Golden, D. M., Kolb, C. E., Kurylo, M. J., Moortgat, G. K., Wine, P. H., Huie, R. E., and Orkin, V. L.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies Evaluation Number 17, JPL Publication, 10-6, Jet Propulsion Laboratory, Pasadena, USA, 2011.
Simmonds, P. G., Cunnold, D. M.,Weiss, R. F., Prinn, R. G., Fraser, P. J., McCulloch, A., Alyea, F. N., and O'Doherty, S.: Global trends and emission estimates of carbon tetrachloride (CCl4/ from in-situ background observations from July 1978 to June 1996, J. Geophys., Res., 103, 16017-16028, 1998.
SPARC: Lifetimes of stratospheric ozone-depleting substances, their replacements and related species, SPARC Report no. 6, WCRP-15/32013, 2013.
SPARC: Report on the mystery of carbon tetrachloride, SPARC Report no. 7, WCRP-13/2016, 2016.
SPARC CCMVal (Stratospheric Processes And their Role in Climate): Report on the Evaluation of Chemistry-Climate Models, edited by: Eyring, V., Shepherd, T. G., and Waugh, D. W., SPARC Report No. 5, WCRP-132, WMO/TD-No. 1526, 2010.
Sukhodolov, T., Rozanov, E., Ball, W. T., Bais, A., Tourpali, K., Shapiro, A. I., Telford, P., Smyshlyaev, S., Fomin, B., Sander, R., Bossay, S., Bekki, S., Marchand, M., Chipperfield, M. P., Dhomse, S., Haigh, J. D., Peter, T., and Schmutz, W.: Evaluation of the simulated photolysis rates and their response to solar irradiance variability, J. Geophys. Res., 121, 6066-6084, 2016.
Velders, G. J. M. and Daniel, J. S.: Uncertainty analysis of projections of ozone-depleting substances: mixing ratios, EESC, ODPs, and GWPs, Atmos. Chem. Phys., 14, 2757-2776, doi:10.5194/acp-14-2757-2014, 2014.
Vollmer, M. K., Zhou, L. X., Greally, B. R., Henne, S., Yao, B., Reimann, S., Stordal, F., Cunnold, D. M., Zhang, X. C., Maione, M., Zhang, F., Huang, J., and Simmonds, P. G.: Emissions of ozone-depleting halocarbons from China, Geophys. Res. Lett., 36, L15823, doi:10.1029/2009GL038659, 2009.
WMO: Scientific Assessment of Ozone Depletion: 2014, Global Ozone Research and Monitoring Project - Report No. 55, 416 pp., Geneva, Switzerland, 2014.
Wofsy, S. C.: HIAPER Pole-to-Pole Observations (HIPPO): finegrained, global-scale measurements of climatically important atmospheric gases and aerosols, Philos. T. R. Soc. A, 369, 2073- 2086, doi:10.1098/rsta.2010.0313, 2011.
Wofsy, S. C., Daube, B. C., Jimenez, R., Kort, E., Pittman, J. V., Park, S., Commane, R., Xiang, B., Santoni, G., Jacob, D., Fisher, J., Pickett-Heaps, C., Wang, H., Wecht, K., Wang, Q.-Q., Stephens, B. B., Shertz, S., Watt, A. S., Romashkin, P., Campos, T., Haggerty, J., Cooper,W. A., Rogers, D., Beaton, S., Hendershot, R., Elkins, J. W., Fahey, D. W., Gao, R. S., Moore, F., Montzka, S. A., Schwarz, J. P., Perring, A. E., Hurst, D., Miller, B. R., Sweeney, C., Oltmans, S., Nance, D., Hintsa, E., Dutton, G., Watts, L. A., Spackman, J. R., Rosenlof, K. H., Ray, E. A., Hall, B., Zondlo, M. A., Diao, M., Keeling, R., Bent, J., Atlas, E. L., Lueb, R., and Mahoney, M. J.: HIPPO aircraftdata, HIPPO Combined Discrete Flask and GC Sample GHG, Halo-, Hydrocarbon Data (R-20121129), Carbon Dioxide Infor-mation Analysis Center, Oak Ridge National Laboratory, OakRidge, Tennessee, USA, doi:10.3334/CDIAC/hippo-012, 2012.
Xiao, X., Prinn, R. G., Fraser, P. J., Weiss, R. F., Simmonds, P. G., O'Doherty, S., Miller, B. R., Salameh, P. K., Harth, C. M., Krummel, P. B., Golombek, A., Porter, L. W., Butler, J. H., Elkins, J. W., Dutton, G. S., Hall, B. D., Steele, L. P., Wang, R. H. J., and Cunnold, D. M.: Atmospheric three-dimensional inverse modeling of regional industrial emissions and global oceanic uptake of carbon tetrachloride, Atmos. Chem. Phys., 10, 10421-10434, doi:10.5194/acp-10-10421-2010, 2010.