Methyl Bromide In Preindustrial Air: Measurements From an Antarctic Ice Core

[1] This paper presents the first ice core measurements of methyl bromide (CH3Br). Samples from a shallow Antarctic ice core (Siple Dome, West Antarctica), ranging in mean gas dates from 1671 to 1942, had a mean CH3Br mixing ratio of 5.8 ppt. These results extend the existing historical record derived from air and Antarctic firn air to about 350 years before present. Model simulations illustrate that the ice core results are consistent with estimates of the impact of anthropogenic activity (fumigation, combustion, and biomass burning) on the atmospheric CH3Br burden, given the large current uncertainties in the modern atmospheric CH3Br budget. A preindustrial scenario assuming no fumigation, no combustion, and a 75% reduction in biomass-burning sources yields a Southern Hemisphere mean mixing ratio of 5.8 ppt, in good agreement with the ice core results. There is a significant imbalance between the known CH3Br sources and sinks in the modern atmospheric CH3Br budget. The ice core data do not sufficiently constrain the model to determine how much of the “unknown source” was present in the preindustrial budget. The results do indicate that most of the southern hemispheric component of this “unknown source” is not anthropogenic.

[1]  S. Montzka,et al.  Atmospheric variability of methyl chloride during the last 300 years from an Antarctic ice core and firn air , 2004 .

[2]  S. Montzka,et al.  A decline in tropospheric organic bromine , 2003 .

[3]  C. Reeves Atmospheric budget implications of the temporal and spatial trends in methyl bromide concentration , 2003 .

[4]  R. Weiss,et al.  Controlled substances and other source gases, Chapter 1 of the Scientific Assessment of Ozone Depletion: 2002 , 2003 .

[5]  J. Butler,et al.  Predicting oceanic methyl bromide saturation from SST , 2002 .

[6]  J. Butler,et al.  Effect of oceanic uptake on atmospheric lifetimes of selected trace gases , 2002 .

[7]  Y. Yokouchi,et al.  Recent decline of methyl bromide in the troposphere , 2002 .

[8]  D. Blake,et al.  Photochemically induced production of CH3Br, CH3I, C2H5I, ethene, and propene within surface snow at Summit, Greenland , 2002 .

[9]  E. Saltzman,et al.  Preindustrial atmospheric carbonyl sulfide (OCS) from an Antarctic ice core , 2002 .

[10]  K. Goodwin,et al.  methyl bromide loss rate constants in the north Pacific Ocean , 2001 .

[11]  R. Weiss,et al.  Shrubland fluxes of methyl bromide and methyl chloride , 2001 .

[12]  Earth System Science , 2001, Science.

[13]  E. Saltzman,et al.  Methyl bromide loss rates in surface waters of the North Atlantic Ocean, Caribbean Sea, and eastern Pacific Ocean (8°–45°N) , 2001 .

[14]  W. Sturges,et al.  Methyl bromide, other brominated methanes, and methyl iodide in polar firn air , 2001 .

[15]  R. Cicerone,et al.  Emissions of methyl halides and methane from rice paddies. , 2000, Science.

[16]  S. Montzka,et al.  Implications of methyl bromide supersaturations in the temperate North Atlantic ocean , 2000 .

[17]  R. Weiss,et al.  Reconstructed histories of the annual mean atmospheric mole fractions for the halocarbons CFC‐11 CFC‐12, CFC‐113, and carbon tetrachloride , 2000 .

[18]  E. Holland,et al.  Litter decomposition as a potential natural source of methyl bromide , 2000 .

[19]  Michael B. McElroy,et al.  Three-dimensional climatological distribution of tropospheric OH: Update and evaluation , 2000 .

[20]  R. Weiss,et al.  Natural methyl bromide and methyl chloride emissions from coastal salt marshes , 2000, Nature.

[21]  P. Crill,et al.  Wetlands: A potentially significant source of atmospheric methyl bromide and methyl chloride , 1999 .

[22]  James W. Elkins,et al.  A record of atmospheric halocarbons during the twentieth century from polar firn air , 1999, Nature.

[23]  P. Crill,et al.  An estimate of the uptake of atmospheric methyl bromide by agricultural soils , 1999 .

[24]  Yuhang Wang,et al.  Anthropogenic forcing on tropospheric ozone and OH since preindustrial times , 1998 .

[25]  S. Yates,et al.  Production of methyl bromide by terrestrial higher plants , 1998 .

[26]  D. Blake,et al.  Seasonal variation of tropospheric methyl bromide concentrations: Constraints on anthropogenic input , 1998 .

[27]  G. Brasseur,et al.  A global three-dimensional atmosphere-ocean model of methyl bromide distributions , 1998 .

[28]  E. Saltzman,et al.  Removal of methyl bromide in coastal seawater: Chemical and biological rates , 1997 .

[29]  J. Butler,et al.  The potential effect of oceanic biological degradation on the lifetime of atmospheric CH3Br , 1997 .

[30]  E. Saltzman,et al.  Diffusivity of methyl bromide in water , 1997 .

[31]  D. Etheridge,et al.  Modeling air movement and bubble trapping in firn , 1997 .

[32]  E. Saltzman,et al.  The solubility of methyl bromide in pure water, 35%. sodium chloride and seawater , 1997 .

[33]  Ralf Koppmann,et al.  Methyl Halide Emissions from Savanna Fires in Southern Africa , 1996 .

[34]  E. Saltzman,et al.  The oceans: A source or a sink of methyl bromide? , 1996 .

[35]  A. Anbar,et al.  Methyl bromide: ocean sources, ocean sinks, and climate sensitivity. , 1996, Global biogeochemical cycles.

[36]  D. Etheridge,et al.  Natural and anthropogenic changes in atmospheric CO2 over the last 1000 years from air in Antarctic ice and firn , 1996 .

[37]  P. Crill,et al.  Rapid degradation of atmospheric methyl bromide in soils , 1995, Nature.

[38]  F. Rowland,et al.  Methyl halide hydrolysis rates in natural waters , 1995 .

[39]  M. Andreae,et al.  Emission of Methyl Bromide from Biomass Burning , 1994, Science.

[40]  J. Butler The potential role of the ocean in regulating atmospheric CH3Br , 1994 .

[41]  B. Smit,et al.  The Carbon Cycle , 1993, Soil Microbiology.

[42]  M. Khalil,et al.  Atmospheric methyl bromide: Trends and global mass balance , 1993 .

[43]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1992 .

[44]  R. Wanninkhof Relationship between wind speed and gas exchange over the ocean , 1992 .

[45]  I. Levin,et al.  Methane consumption in aerated soils of the temperate zone , 1990 .

[46]  L. Heidt,et al.  Measurements of atmospheric methyl bromide and bromoform , 1988 .

[47]  W. Broecker,et al.  The average vertical mixing coefficient for the oceanic thermocline , 1984 .

[48]  E. Matthews Global Vegetation and Land Use: New High-Resolution Data Bases for Climate Studies , 1983 .

[49]  C. Y. Lee,et al.  Estimation of Diffusion Coefficients for Gases and Vapors , 1955 .

[50]  E. A. Moelwyn-Hughes The Hydrolysis of the Methyl Halides , 1938 .

[51]  D. R. Blakea,et al.  Photochemically induced production of CH 3 Br, CH 3 I, C 2 H 5 I, ethene, and propene within surface snow at Summit, Greenland , 2002 .

[52]  G. Nickless,et al.  Biogenic fluxes of halomethanes from Irish peatland ecosystems , 2001 .

[53]  David John Lary,et al.  Short-Lived Ozone-Related Compounds , 1999 .

[54]  J. Butler,et al.  An improved estimate of the oceanic lifetime of atmospheric CH3Br , 1996 .

[55]  J. A. Kaye,et al.  Report on concentrations, lifetimes, and trends of CFCs, halons, and related species , 1994 .

[56]  W. Paterson The Transformation of Snow to Ice , 1994 .

[57]  L. Shampine,et al.  A 3(2) pair of Runge - Kutta formulas , 1989 .

[58]  Luis G. Vargas,et al.  Dirac distributions and threshold firing in neural networks , 1989 .

[59]  B. Stauffer,et al.  Air Mixing in Firn and the Age of the Air at Pore Close-Off , 1988, Annals of Glaciology.