Evidence for substantial variations of atmospheric hydroxyl radicals in the past two decades

The hydroxyl radical (OH) is the dominant oxidizing chemical in the atmosphere. It destroys most air pollutants and many gases involved in ozone depletion and the greenhouse effect. Global measurements of 1,1,1-trichloroethane (CH3CCl3, methyl chloroform) provide an accurate method for determining the global and hemispheric behavior of OH. Measurements show that CH3CCl3 levels rose steadily from 1978 to reach a maximum in 1992 and then decreased rapidly to levels in 2000 that were lower than the levels when measurements began in 1978. Analysis of these observations shows that global OH levels were growing between 1978 and 1988, but the growth rate was decreasing at a rate of 0.23 +/- 0.18% year(-2), so that OH levels began declining after 1988. Overall, the global average OH trend between 1978 and 2000 was -0.64 +/- 0.60% year(-1). These variations imply important and unexpected gaps in current understanding of the capability of the atmosphere to cleanse itself.     

Atmospheric Trends and Lifetime of CH3CCI3 and Global OH Concentrations

Determination of the atmospheric concentrations and lifetime of trichloroethane (CH(3)CCI(3)) is very important in the context of global change. This halocarbon is involved in depletion of ozone, and the hydroxyl radical (OH) concentrations determined from its lifetime provide estimates of the lifetimes of most other hydrogen-containing gases involved in the ozone layer and climate. Global measurements of trichloroethane indicate rising concentrations before and declining concentrations after late 1991. The lifetime of CH(3)CCI(3) in the total atmosphere is 4.8 +/- 0.3 years, which is substantially lower than previously estimated. The deduced hydroxyl radical concentration, which measures the atmosphere's oxidizing capability, shows little change from 1978 to 1994.     

Arctic ocean ventilation studied with a suite of anthropogenic halocarbon tracers

The chlorofluoromethanes (CFMs: CCl(2)F(2) and CCl(3)F), methyl chloroform (CH(3)CCl(3)), and carbon tetrachloride (CCl(4)) have been measured in deep waters of the Arctic Ocean. Oceanic and atmospheric inventories of these compounds result from known anthropogenic releases; because the CFMs and CCl(4) are also chemically nonreactive, they can be used as transient tracers of ocean circulation. The input history of CCl(4) is longer than that of any other transient tracer identified to date( approximately 70 years). This long input history, together with an e-folding time scale of increase(tau) of approximately 28 years, makes CCl(4) potentially the most useful tracer for calibrating models of the oceanic uptake of the fossil-fuel CO(2) transient(tau approximately 25 years). The bottom water of the Nansen Basin, Arctic Ocean, has detectable CCl(4) but undetectable CFM(s) and CH(3)CCl(3), which suggests either that the bottom water is approximately 50 years old, or that there is a small, nonanthropogenic component of atmospheric CCl(4)(<6 parts per trillion by volume).     

Atmospheric trace gases in antarctica

Trace gases have been measured, by electron-capture gas chromatography and gas chromatography-mass spectrometry techniques, at the South Pole (SP) in Antarctica and in the U.S. Pacific Northwest (PNW) ( approximately 45 degrees N) during January of each year from 1975 to 1980. These measurements show that the concentrations of CCl(3)F, CCl(2)F(2), and CH(3)CCl(3) have increased exponentially at substantial rates. The concentration of CCl(3)F increased at 12 percent per year at the SP and at 8 percent per year in the PNW; CCl(2)F(2) increased at about 9 percent per year at both locations, and CH(3)CCl(3) increased at 17 percent per year at the SP and 11.6 percent per year at the PNW site. There is some evidence that CCl(4) ( approximately 3 percent per year) and N(2)O (0.1 to 0.5 percent per year) may also have increased. Concentrations of nine other trace gases of importance in atmospheric chemistry are also being measured at these two locations. Results of the measurements of CHClF(2)(F-22), C(2)Cl(3)F(3)(F-113), SF(6), C(2)-hydrocarbons, and CH(3)Cl are reported here.     

Anthropogenic CO Emissions: Implications for the Atmospheric CO-OH-CH4 Cycle

Present anthropogenic emissions of CO are apparently large enough to perturb the natural CO-OH-CH(4) cycle, which plays a crucial role in the self-cleansing processes in the troposphere. A significant increase in global concentrations of CO, CH(4) CH(3)Cl, and other trace gases may result from a decrease in the OH concentration caused by continued CO emissions. Even if the CO emissions were maintained at the present rate, increases in CO and CH(4) by the year 2025 might be as large as 50 and 25 percent, respectively. The time constants associated with the perturbations of the CO-OH-CH(4) cycle are of the order of a few decades. Perturbation of this cycle may also indirectly affect stratospheric chemistry.     

Atmospheric trace gases: trends and distributions over the last decade

Concentrations of the halocrbons CCl(3)F (F-11), CCl(2)F(2) (F-12), CCl(4), and CH(3)CCl(3), methane (CH(4)), and nitrous oxide (N(2)O) over the decade between 1975 and 1985 are reported, based on measurements taken every January at the South Pole and in the Pacific Northwest. The concentrations of F-11, F-12, and CH(3)CCl(3) in both hemispheres are now more than twice their concentrations 10 years ago. However, the annual rates of increase of F-11, F-12, and CH(3)CC1(3) are now considerably slower than earlier in the decade, reflecting in part the effects of a ban on their nonessential uses. Continued increases in these trace gas concentrations may warm the earth and deplete the stratospheric ozone layer, which may cause widespread climatic changes and affect global habitability.     

植被年际变化对蒸散发影响的模拟研究

利用通用陆面模式(CLM3.0)及其植被动力学模式(DGVM)研究植被覆盖度(FC)和叶面积指数(LAI)的年际变化对全球蒸散发的影响。设计两套实验方案,其植被的FC和LAI的气候态相同,但一套实验中植被的FC和LAI有年际变化,而对照实验中则没有。结果表明:(1)在草、灌木、树占优势的地区植被FC年际变化依次减小;LAI年际变化较大的地区集中在草和灌木覆盖的地区,在落叶林地区,春秋两季植被LAI的年际变化也较大。(2)全球树占优势的大部分地区,植被的年际变化使得年平均蒸散发和地表蒸发增加、冠层蒸发和蒸腾减少;而在灌木和草覆盖区,变化则大致相反。(3)低纬度地区蒸散发季节循环变化比较明显,而北半球中纬度地区,蒸散发变化明显区随着纬度增加而在时间上向后推延。(4)FC和LAI年际变化较大时,蒸散发及地表蒸发降低,而蒸腾增加;这些差异随FC和LAI年际变化的增加而增加。单点分析进一步表明植被年际变化不仅改变蒸散发的多年平均值,同时改变其分量间的相对比例。     

Kinetics of the OH Reaction with Methyl Chloroform and Its Atmospheric Implications

The rate coefficients for the reaction of hydroxyl (OH) radicals with methyl chloroform (CH(3)CCI(3)) were measured between 243 and 379 kelvin with the pulsed photolysis-laserinduced fluorescence method. The measured rate coefficients at 298 and 277 kelvin were approximately 20 and approximately 15%, respectively, lower than earlier values. These results will increase the tropospheric OH concentrations derived from the CH(3)CCI(3) budget analysis by approximately 15%. The predicted atmospheric lifetimes of species whose main loss process is the reaction with OH in the troposphere will be lowered by 15% with consequent changes in their budgets, global warming potentials, and ozone depletion potentials.     

South asian summer monsoon variability in a model with doubled atmospheric carbon dioxide concentration

Doubled atmospheric carbon dioxide concentration in a global coupled ocean-atmosphere climate model produced increased surface temperatures and evaporation and greater mean precipitation in the south Asian summer monsoon region. As a partial consequence, interannual variability of area-averaged monsoon rainfall was enhanced. Consistent with the climate sensitivity results from the model, observations showed a trend of increased interannual variability of Indian monsoon precipitation associated with warmer land and ocean temperatures in the monsoon region.     

Soil nitrite as a source of atmospheric HONO and OH radicals

Hydroxyl radicals (OH) are a key species in atmospheric photochemistry. In the lower atmosphere, up to ~30% of the primary OH radical production is attributed to the photolysis of nitrous acid (HONO), and field observations suggest a large missing source of HONO. We show that soil nitrite can release HONO and explain the reported strength and diurnal variation of the missing source. Fertilized soils with low pH appear to be particularly strong sources of HONO and OH. Thus, agricultural activities and land-use changes may strongly influence the oxidizing capacity of the atmosphere. Because of the widespread occurrence of nitrite-producing microbes, the release of HONO from soil may also be important in natural environments, including forests and boreal regions.     

Coupling of nitrous oxide and methane by global atmospheric chemistry

Nitrous oxide (N(2)O) and methane (CH(4)) are chemically reactive greenhouse gases with well-documented atmospheric concentration increases that are attributable to anthropogenic activities. We quantified the link between N(2)O and CH(4) emissions through the coupled chemistries of the stratosphere and troposphere. Specifically, we simulated the coupled perturbations of increased N(2)O abundance, leading to stratospheric ozone (O(3)) depletion, altered solar ultraviolet radiation, altered stratosphere-to-troposphere O(3) flux, increased tropospheric hydroxyl radical concentration, and finally lower concentrations of CH(4). The ratio of CH(4) per N(2)O change, -36% by mole fraction, offsets a fraction of the greenhouse effect attributable to N(2)O emissions. These CH(4) decreases are tied to the 108-year chemical mode of N(2)O, which is nine times longer than the residence time of direct CH(4) emissions.     

Tropical tropospheric ozone and biomass burning

New methods for retrieving tropospheric ozone column depth and absorbing aerosol (smoke and dust) from the Earth Probe-Total Ozone Mapping Spectrometer (EP/TOMS) are used to follow pollution and to determine interannual variability and trends. During intense fires over Indonesia (August to November 1997), ozone plumes, decoupled from the smoke below, extended as far as India. This ozone overlay a regional ozone increase triggered by atmospheric responses to the El Ni?o and Indian Ocean Dipole. Tropospheric ozone and smoke aerosol measurements from the Nimbus 7 TOMS instrument show El Ni?o signals but no tropospheric ozone trend in the 1980s. Offsets between smoke and ozone seasonal maxima point to multiple factors determining tropical tropospheric ozone variability.     

Atmospheric residence time of CH3Br estimated from the junge spatial variability relation

The atmospheric residence time for methyl bromide (CH3Br) has been estimated as 0.8 +/- 0.1 years from its empirical spatial variability relative to C2H6, C2Cl4, CHCl3, and CH3Cl. This evaluation of the atmospheric residence time, based on Junge's 1963 general proposal, provides an estimate for CH3Br that is independent of source and sink estimates. Methyl bromide from combined natural and anthropogenic sources furnishes about half of the bromine that enters the stratosphere, where it plays an important role in ozone destruction. This residence time is consistent with the 0.7-year value recently calculated for CH3Br from the combined strength estimates for its known significant sinks.     

Regional changes in carbon dioxide fluxes of land and oceans since 1980

We have applied an inverse model to 20 years of atmospheric carbon dioxide measurements to infer yearly changes in the regional carbon balance of oceans and continents. The model indicates that global terrestrial carbon fluxes were approximately twice as variable as ocean fluxes between 1980 and 1998. Tropical land ecosystems contributed most of the interannual changes in Earth's carbon balance over the 1980s, whereas northern mid- and high-latitude land ecosystems dominated from 1990 to 1995. Strongly enhanced uptake of carbon was found over North America during the 1992-1993 period compared to 1989-1990.     

A Net Sink for Atmospheric CH3Br in the East Pacific Ocean

Surface waters along a cruise track in the East Pacific Ocean were undersaturated in methyl bromide (CH(3)Br) in most areas except for coastal and upwelling regions, with saturation anomalies ranging from + 100 percent in coastal waters to -50 percent in open ocean areas, representing a regionally weighted mean of -16 (-13 to -20) percent. The partial lifetime of atmospheric CH(3)Br with respect to calculated oceanic degradation along this cruise track is 3.0 (2.9 to 3.6) years. The global, mean dry mole fraction of CH3Br in the atmosphere was 9.8 +/- 0.6 parts per trillion, with an interhemispheric ratio of 1.31 +/- 0.08. These data indicate that approximately 8 percent (0.2 parts per trillion) of the observed interhemispheric difference in atmospheric CH3Br could be attributed to an uneven global distribution of oceanic sources and sinks.     

Air pollution and climate-forcing impacts of a global hydrogen economy

If today's surface traffic fleet were powered entirely by hydrogen fuel cell technology, anthropogenic emissions of the ozone precursors nitrogen oxide (NOx) and carbon monoxide could be reduced by up to 50%, leading to significant improvements in air quality throughout the Northern Hemisphere. Model simulations of such a scenario predict a decrease in global OH and an increased lifetime of methane, caused primarily by the reduction of the NOx emissions. The sign of the change in climate forcing caused by carbon dioxide and methane depends on the technology used to generate the molecular hydrogen. A possible rise in atmospheric hydrogen concentrations is unlikely to cause significant perturbations of the climate system.     

Modern global climate change

Modern climate change is dominated by human influences, which are now large enough to exceed the bounds of natural variability. The main source of global climate change is human-induced changes in atmospheric composition. These perturbations primarily result from emissions associated with energy use, but on local and regional scales, urbanization and land use changes are also important. Although there has been progress in monitoring and understanding climate change, there remain many scientific, technical, and institutional impediments to precisely planning for, adapting to, and mitigating the effects of climate change. There is still considerable uncertainty about the rates of change that can be expected, but it is clear that these changes will be increasingly manifested in important and tangible ways, such as changes in extremes of temperature and precipitation, decreases in seasonal and perennial snow and ice extent, and sea level rise. Anthropogenic climate change is now likely to continue for many centuries. We are venturing into the unknown with climate, and its associated impacts could be quite disruptive.     

Atmospheric trends in methylchloroform and the global average for the hydroxyl radical

Frequent atmospheric measurements of the anthropogenic compound methylchloroform that were made between 1978 and 1985 indicate that this species is continuing to increase significantly around the world. Reaction with the major atmospheric oxidant, the hydroxyl radical (OH), is the principal sink for this species. The observed mean trends for methylchloroform are 4.8, 5.4, 6.4, and 6.9 percent per year at Aldrigole (Ireland) and Cape Meares (Oregon), Ragged Point (Barbados), Point Matatula (American Samoa), and Cape Grim (Tasmania), respectively, from July 1978 to June 1985. These measured trends, combined with knowledge of industrial emissions, were used in an optimal estimation inversion scheme to deduce a globally averaged methylchloroform atmospheric lifetime of 6.3 (+ 1.2, -0.9) years (1sigma uncertainty) and a globally averaged tropospheric hydroxyl radical concentration of (7.7 +/- 1.4) x 10(5) radicals per cubic centimeter (1sigma uncertainty). These 7 years of gas chromatographic measurements, which comprise about 60,000 individual calibrated real-time air analyses, provide the most accurate estimates yet of the trends and lifetime of methylchloroform and of the global average for tropospheric hydroxyl radical levels. Accurate determination of hydroxyl radical levels is crucial to understanding global atmospheric chemical cycles and trends in the levels of trace gases such as methane.     

我国夏季降水类型初探（英文）

[Objective] Study on the spatial distribution of summer precipitation patterns and interannual and interdecadal variability.[Method] The summer precipitation patterns were obtained from standard field of summer precipitation data for 160 observation stations in China during 1951-2000 by the utilization of empirical orthogonal function(EOF),and characteristics of interannual and interdecadal variability were analyzed.[Result] The summer precipitation mainly distributes in eastern part of China;The 1st,2nd and 3rd EOF modes of spatial distribution are especially remarkable as well consistent with the results of previous reports about three rainfall patterns from analysis on the percentages of precipitation anomaly of summer.[Conclusion] There exists interannual and interdecadal variability for summer precipitation in China.