Radiative forcing of climate change by CFC‐11 and possible CFC replacements

The infrared absorption cross sections of CFC-11 and 16 other halogenated compounds have been measured. These spectra were used in detailed line-by-line calculations to derive radiative forcing values. The radiative forcing values for 14 of these gases have not, to our knowledge, been previously reported in the literature. The accuracy of a computationally inexpensive narrowband scheme, which included the effect of clouds and stratospheric adjustment, was investigated. Global warming potentials are presented where atmospheric lifetimes are available. In light of the substantial disagreement in values for the forcing due to CFC-11 reported in the literature and its use as a standard to which other halogenated gases are often compared, we examined the sensitivity of CFC-11 forcing to a number of assumptions. We find that the uncertainties in the calculated value of the radiative forcing caused by neglect of the temperature and pressure dependence of the IR absorption spectrum are much smaller than those resulting from uncertainties in the absolute absorption cross sections or the vertical profile of CFC-11. Our best estimate is 0.285 W m−2 ppbv−1, which is 30% higher than the value adopted by the Intergovernmental Panel on Climate Change and is believed to be accurate to within about 10%. For the other gases represented here the lack of detailed knowledge of the likely vertical and horizontal distribution probably represents the most significant uncertainty in evaluating their radiative forcing.

[1]  T. Matsuno,et al.  Radiative Effects and Halocarbon Global Warming Potentials of Replacement Compounds for Chlorofluorocarbons , 1995 .

[2]  F. Nicolaisen,et al.  Integrated absorption coefficients of CHClF2 (HCFC-22) and CH3Br in the atmospheric infrared window region , 1994 .

[3]  D. Murcray,et al.  Statistical band model analysis and integrated intensity for the 11.8-microm band of CFCI(3). , 1976, Applied optics.

[4]  W. Malkmus,et al.  Random Lorentz band model with exponential-tailed S-1 line-intensity distribution function , 1967 .

[5]  R. Wayne,et al.  Laboratory studies of some halogenated ethanes and ethers: Measurements of rates of reaction with OH and of infrared absorption cross-sections , 1990 .

[6]  P. Varanasi,et al.  Intensity measurements in freon bands of atmospheric interest , 1977 .

[7]  J. Barnett,et al.  Zonal mean temperature, pressure, zonal wind and geopotential height as functions of latitude , 1990 .

[8]  Michael J. Kurylo,et al.  Rate constants for reactions of the hydroxyl radical with several partially fluorinated ethers , 1992 .

[9]  A. McDaniel,et al.  The temperature dependent, infrared absorption cross-sections for the chlorofluorocarbons: CFC-11, CFC-12, CFC-13, CFC-14, CFC-22, CFC-113, CFC-114, and CFC-115 , 1991 .

[10]  H. Nelson,et al.  Potential chlorofluorocarbon replacements: OH reaction rate constants between 250 and 315 K and infrared absorption spectra , 1993 .

[11]  V. L. Orkin,et al.  Rate constants for reactions of OH radicals with some Br-containing haloalkanes , 1993 .

[12]  D. Fahey,et al.  Quantifying Transport Between the Tropical and Mid-Latitude Lower Stratosphere , 1996, Science.

[13]  R. Wayne,et al.  Tropospheric lifetimes of three compounds for possible replacement of CFC and halons , 1990, Nature.

[14]  R. Boese,et al.  Temperature dependence of intensities of the 8-12 micron bands of CFCl3 , 1980 .

[15]  L. Gray,et al.  The role of ozone‐induced diabatic heating anomalies in the quasi‐biennial oscillation , 1995 .

[16]  R. Garcia,et al.  Ozone depletion and global warming potentials of CF3I , 1994 .

[17]  Robert G. Ellingson,et al.  The intercomparison of radiation codes used in climate models: Long wave results , 1991 .

[18]  A. Ravishankara,et al.  Atmospheric Lifetime of CHF2Br, a Proposed Substitute for Halons , 1991, Science.

[19]  F. X. Kneizys,et al.  Line shape and the water vapor continuum , 1989 .

[20]  P. Varanasi,et al.  A reexamination of the greenhouse effect due to CFC-11 and CFC-12 , 1992 .

[21]  K. Hsu,et al.  Temperature-Dependent Rate Constants and Substituent Effects for the Reactions of Hydroxyl Radicals with Three Partially Fluorinated Ethers , 1995 .

[22]  Prasad Varanasi,et al.  Measurement of the absorption cross-sections of CFC-11 at conditions representing various model atmospheres , 1994 .

[23]  J. Pyle,et al.  Two-dimensional modelling of some CFC replacement compounds , 1996 .

[24]  C. Rodgers,et al.  The computation of infra‐red cooling rate in planetary atmospheres , 1966 .

[25]  Robert L. Sams,et al.  Absolute band strengths of halocarbons F‐11 and F‐12 in the 8‐ to 16‐μm region , 1983 .

[26]  P. Edwards,et al.  GENLN2: A general line-by-line atmospheric transmittance and radiance model. Version 3.0: Description and users guide , 1992 .

[27]  William B. Rossow,et al.  Calculation of surface and top of atmosphere radiative fluxes from physical quantities based on ISCCP data sets: 2. Validation and first results , 1995 .

[28]  A. Ravishankara,et al.  Atmospheric lifetime, its application and its determination: CFC-substitutes as a case study , 1994 .

[29]  M. Molina,et al.  Chemical kinetics and photochemical data for use in stratospheric modeling , 1985 .

[30]  V. M. Devi,et al.  THE HITRAN MOLECULAR DATABASE: EDITIONS OF 1991 AND 1992 , 1992 .

[31]  Michael J. Prather,et al.  Tropospheric OH and the lifetimes of hydrochlorofluorocarbons , 1990 .

[32]  J. Hansen,et al.  Greenhouse effect of chlorofluorocarbons and other trace gases , 1989 .

[33]  J. Hansen,et al.  Radiative forcing and climate response , 1997 .

[34]  Inez Y. Fung,et al.  Global climate changes as forecast by Goddard Institute for Space Studies three‐dimensional model , 1988 .

[35]  C. Clerbaux,et al.  Infrared cross sections and global warming potentials of 10 alternative hydrohalocarbons , 1993 .

[36]  M. Mills,et al.  Atmospheric lifetimes and ozone depletion potentials of methyl bromide (CH3Br) and dibromomethane (CH2Br2) , 1992 .

[37]  K. Shine,et al.  The Effects of Changes in HITRAN and Uncertainties in the Spectroscopy on Infrared Irradiance Calculations , 1998 .

[38]  P. Varanasi,et al.  Infrared intensities of some chlorofluorocarbons capable of perturbing the global climate , 1988 .

[39]  Wei‐Chyung Wang,et al.  Model calculations of the relative effects of CFCs and their replacements on global warming , 1990, Nature.

[40]  T. Wallington,et al.  Radiative forcing of climate by hydrochlorofluorocarbons and hydrofluorocarbons , 1995 .

[41]  K. Shine On the Cause of the Relative Greenhouse Strength of Gases such as the Halocarbons , 1991 .

[42]  RADIATIVE FORCING OF HALOCARBONS : A COMPARISON OF LINE-BY-LINE AND NARROW-BAND MODELS USING CF4 AS AN EXAMPLE , 1996 .