Three-dimensional climatological distribution of tropospheric OH: Update and evaluation

被引:652
作者
Spivakovsky, CM
Logan, JA
Montzka, SA
Balkanski, YJ
Foreman-Fowler, M
Jones, DBA
Horowitz, LW
Fusco, AC
Brenninkmeijer, CAM
Prather, MJ
Wofsy, SC
McElroy, MB
机构
[1] Harvard Univ, DEAS, Cambridge, MA 02138 USA
[2] Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA
[3] NOAA, Climate Monitoring & Diagnost Lab, Boulder, CO 80303 USA
[4] Max Planck Inst Chem, D-55128 Mainz, Germany
[5] Univ Calif Irvine, Dept Geosci, Irvine, CA USA
关键词
D O I
10.1029/1999JD901006
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
A global climatological distribution of tropospheric OH is computed using observed distributions of O-3, H2O, NOt (NO2+NO+2N(2)O(5)+NO3+HNO2+HNO4), CO, hydrocarbons, temperature, and cloud optical depth. Global annual mean OH is 1.16 x 10(6) molecules cm(-3) (integrated with respect to mass of air up to 100 hPa within +/-32 degrees latitude and up to 200 hPa outside that region). Mean hemispheric concentrations of OW are nearly equal, While global mean OH increased by 33% compared to that from Spivakovsky et al. [1990], mean loss frequencies of CH3CCl3 and CH4 increased by only 23% because a lower fraction of total OH resides in the lower troposphere in the present distribution. The value for temperature used for determining lifetimes of hydrochlorofluorocarbons (HCFCs) by scaling rate constants [Prather and Spivakovsky, 1990] is revised from 277 It to 272 K. The present distribution of OH is consistent within a few percent with the current budgets of CH3CCl3 and HCFC-22. For CH3CCl3, it results in a lifetime of 4.6 years, including stratospheric and ocean sinks with atmospheric lifetimes of 43 and 80 years, respectively. For HCFC-22, the lifetime is 11.4 years, allowing for the stratospheric sink with an atmospheric lifetime is 11.4 years, allowing for the stratospheric sink with an atmospheric lifetime of 229 years. Corrections suggested by observed levels of CH2Cl2 (annual means) depend strongly on the rate of interhemispheric mixing in the model, An increase in OH in the Northern Hemisphere by 20% combined with a decrease in the southern tropics by 25% is suggested if this rate is at its upper limit consistent with observations of CFCs and Kr-85. For the lower limit, observations of CH2Cl2 imply an increase in OH in the Northern Hemisphere by 35% combined with a decrease in OH in the southern tropics by 60%. However, such large corrections are inconsistent with observations for (CO)-C-14 in the tropics and For the interhemispheric gradient; of CH3CCl3. Industrial sources of CH2Cl2 are sufficient for balancing its budget. The available tests do not establish significant errors in OH except for a possible underestimate in winter in the northern and southern tropics by 15-20% and 10-15%, respectively, and an overestimate in southern extratropics by similar to 25%. Observations of seasonal variations of CH3CCl3, CH2Cl2, (CO)-C-14, and C2H6 offer no evidence for higher levels of OH in the southern than in the northern extratropics. It is expected that in the next few years the latitudinal distribution and annual cycle of CH3CCl3 will be determined primarily by its loss frequency, allowing for additional constraints for OH on scales smaller than global.
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页码:8931 / 8980
页数:50
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