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1.
利用臭氧探空资料,分析了西太平洋地区香港(Hong Kong)、那霸(Naha)和札幌(Sapporo)三个站点2000~2010年期间大气边界层内臭氧(O3)的季节分布和年变化趋势。结果表明,三个站点O3的季节分布存在明显的差异。其中,那霸和香港大气边界层内O3季节平均呈双峰值分布,其峰值分别出现在春季和秋季;而札幌站为单峰分布,峰值出现在春季。造成季节分布差异的主要原因包括人为污染源和自然因素如气象条件。另外,三个站点大气边界层内O3均呈上升趋势。其中札幌、那霸上升最快,分别达0.80 ppb a-1和0.77 ppb a-1。(ppb表示10-9,下同)香港的年际增长较不明显,但秋季增长却非常明显,高达1.21 ppb a-1。结合GOME (Global Ozone Monitoring Experiment) 和SCIAMACHY (Scanning Imaging Absorption Spectro Meter for Atmospheric Chartography)卫星反演的NO2数据发现,过去10年中国京津唐和东北地区的对流层内NO2柱总量增加极为迅速。这些O3前体物通过远距离输送是导致札幌、那霸O3浓度增加的主要原因之一。珠江三角洲人为污染源的增加及偏北气流的影响,是导致香港地区秋季O3增加的主要原因。  相似文献   

2.
Halogens in the atmosphere chemically destroy ozone. In the troposphere, bromine has higher ozone destruction efficiency than chlorine and is the halogen species with the widest geographical spread of natural sources. We investigate the relative strength of various sources of reactive tropospheric bromine and the influence of bromine on tropospheric chemistry using a 6-year simulation with the global chemistry transport model MOZART4. We consider the following sources: short-lived bromocarbons (CHBr3, CH2BrCl, CHBr2Cl, CHBrCl2, and CH2Br2) and CH3Br, bromine from airborne sea salt particles, and frost flowers and sea salt on or in the snowpack in polar regions. The total bromine emissions in our simulations add up to 31.7 Gmol(Br)/yr: 63 % from polar sources, 24.6 % from short-lived bromocarbons and 12.4 % from airborne sea salt particles. We conclude from our analysis that our global bromine emission is likely to be on the lower end of the range, because of too low emissions from airborne sea salt. Bromine chemistry has an effect on the oxidation capacity of the troposphere, not only due to its direct influence on ozone concentrations, but also by reactions with other key chemical species like HO x and NO x . Globally, the impact of bromine chemistry on tropospheric O3 is comparable to the impact of gas-phase sulfur chemistry, since the inclusion of bromine chemistry in MOZART4 leads to a decrease of the O3 burden in the troposphere by 6 Tg, while we get an increase by 5 Tg if gas-phase sulfur chemistry is switched off in the standard model. With decreased ozone burden, the simulated oxidizing capacity of the atmosphere decreases thus affecting species associated with the oxidation capacity of the atmosphere (CH3OOH, H2O2).  相似文献   

3.
Increases in tropospheric ozone (O3) abundance are likely to take place in the near future in the populous and rapidly developing countries in the tropics and subtropics. An accurate evaluation of the future impact of increasing industrial activities in tropical and subtropical areas requires knowledge of the background levels of ozone. New ozone monitoring stations have been installed at several sites by the World Meteorological Organization (WMO) since the mid‐90s. We analyze ozone data collected during two years since April 1996 at Cerro Tololo (30°S, 70°W, 2200 m.a.s.l.) some 50 km east from the city of La Serena. In this paper, we describe some of the atmospheric chemistry and meteorology that characterizes the Tololo site. The data show a seasonal variation with maximum mixing ratios in late winter and spring and minimum mixing ratios in late summer and early fall. These variations are most likely associated with the large‐scale subsidence of the Hadley circulation and the location of the subtropical jet stream (STJ). Also, there is a diurnal variation that is probably partly associated with a mountain wind flow which is strongest in late spring and summer months. No significant mixing with marine boundary layer air perturbed by anthropogenic activities is apparent from the data. We find the Cerro Tololo site to be generally representative for background conditions of free‐tropospheric air in the subtropics of the Southern Hemisphere. This work is done within the framework of a larger effort recently started by several Chilean institutions in cooperation with research centers abroad.  相似文献   

4.
A global two-dimensional (altitude-latitude) chemistry transport model is used to follow the changes in the tropospheric distribution of the two major radiatively active trace gases, methane and ozone, following step changes to the sustained emissions of the short-lived trace gases methane, carbon monoxide and non-methane hydrocarbons. The radiative impacts were dependent on the latitude chosen for the applied change in emissions. Step change global warming potentials (GWPs) were derived for a range of short-lived trace gases to describe their time-integrated radiative forcing impacts for unit emissions relative to that of carbon dioxide. The GWPs show that the tropospheric chemistry of the hydrocarbons can produce significant indirect radiative impacts through changing the tropospheric distributions of hydroxyl radicals, methane and ozone. For aircraft, the indirect radiative forcing impact of the NO x emissions appears to be greater than that from their carbon dioxide emissions. Quantitative results from this two-dimensional model study must, however, be viewed against the known inadequacies of zonally-averaged models and their poor representation of many important tropospheric processes.  相似文献   

5.
A global three-dimensional model of the tropospheric sulfur cycle   总被引：9，自引：0，他引：9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

6.
The impact of natural and anthropogenicnon-methane hydrocarbons (NMHC) on troposphericchemistry is investigated with the global,three-dimensional chemistry-transport model MOGUNTIA.This meteorologically simplified model allows theinclusion of a rather detailed scheme to describeNMHC oxidation chemistry. Comparing model resultscalculated with and without NMHC oxidation chemistryindicates that NMHC oxidation adds 40–60% to surfacecarbon monoxide (CO) levels over the continents andslightly less over the oceans. Free tropospheric COlevels increase by 30–60%. The overall yield of COfrom the NMHC mixture considered is calculated to beabout 0.4 CO per C atom. Organic nitrate formationduring NMHC oxidation, and their transport anddecomposition affect the global distribution of NO x and thereby O3 production. The impact of theshort-lived NMHC extends over the entire tropospheredue to the formation of longer-lived intermediateslike CO, and various carbonyl and carboxyl compounds.NMHC oxidation almost doubles the net photochemicalproduction of O3 in the troposphere and leads to20–80% higher O3 concentration inNO x -rich boundarylayers, with highest increases over and downwind ofthe industrial and biomass burning regions. Anincrease by 20–30% is calculated for the remotemarine atmosphere. At higher altitudes, smaller, butstill significant increases, in O3 concentrationsbetween 10 and 60% are calculated, maximizing in thetropics. NO from lightning also enhances the netchemical production of O3 by about 30%, leading to asimilar increase in the global mean OH radicalconcentration. NMHC oxidation decreases the OH radicalconcentrations in the continental boundary layer withlarge NMHC emissions by up to 20–60%. In the marineboundary layer (MBL) OH levels can increase in someregions by 10–20% depending on season and NO x levels.However, in most of the MBL OH will decrease by10–20% due to the increase in CO levels by NMHCoxidation chemistry. The large decreases especiallyover the continents strongly reduce the markedcontrasts in OHconcentrations between land and oceanwhich are calculated when only the backgroundchemistry is considered. In the middle troposphere, OHconcentrations are reduced by about 15%, although dueto the growth in CO. The overall effect of thesechanges on the tropospheric lifetime of CH4 is a 15%increase from 6.5 to 7.4 years. Biogenic hydrocarbonsdominate the impact of NMHC on global troposphericchemistry. Convection of hydrocarbon oxidationproducts: hydrogen peroxides and carbonyl compounds,especially acetone, is the main source of HO x in theupper troposphere. Convective transport and additionof NO from lightning are important for the O3 budgetin the free troposphere.  相似文献   

7.
Growth in subsonic air traffic over the past 20 years has been dramatic, with an annual increase of }6.1% over the decade between 1978 and 1988. Furthermore, aircraft activities in the year 2000 are predicted to be double those of 1990, with a shift towards more high-flying, longhaul subsonics. Aircraft exhaust gases increase the amount of nitrogen oxides (NO x ) in the upper troposphere/lower stratosphere through injection at cruise altitudes. Given that NO x is instrumental in tropospheric ozone production and stratospheric ozone destruction, it is important to determine the influence of subsonic aircraft NO x emissions on levels of atmospheric ozone. This paper describes calculations designed to investigate the impact that subsonic aircraft may already have had on the atmosphere during the 1980s, run in a 2-D chemical-radiative-transport model. The results indicate a significant increase in upper tropospheric ozone over the decade arising from aircraft emissions. However, when comparing model results with observational data, certain discrepancies appear. Lower stratospheric ozone loss over the 1980s does not appear to be greatly altered by the inclusion of aircraft emissions in the model. However, given the trend in greater numbers of long-haul subsonic aircraft, this factor must be considered in any further calculations.  相似文献   

8.
Satellite measurements of tropospheric column O3 and NO2 in eastern and southeastern Asia are analyzed to study the spatial and seasonal characteristics of pollution in these regions. Tropospheric column O3 is derived from differential measurements of total column ozone from Total Ozone Mapping Spectrometer (TOMS), and stratospheric column ozone from the Microwave Limb Sounder (MLS) instrument on the Upper Atmosphere Research Satellite (UARS). The tropospheric column NO2 is measured by Global Ozone Monitoring Experiment (GOME). A global chemical and transport model (Model of Ozone and Related Chemical Tracers, version 2; MOZART-2) is applied to analyze and interpret the satellite measurements. The study, which is based on spring, summer, and fall months of 1997 shows generally good agreement between the model and satellite data with respect to seasonal and spatial characteristics of O3 and NO2 fields. The analysis of the model results show that the industrial emission of NOx (NO + NO2) contributes about 50%–80% to tropospheric column NO2 in eastern Asia and about 20%–50% in southeastern Asia. The contribution of industrial emission of NOx to tropospheric column O3 ranges from 10% to 30% in eastern Asia. Biomass burning and lightning NOx emissions have a small effect on tropospheric O3 in central and eastern Asia, but they have a significant impact in southeastern Asia. The varying effects of NOx on tropospheric column ozone are attributed to differences in relative abundance of volatile organic compounds (VOCs) with respect to total nitrogen in the two regions.  相似文献   

9.
The representation of alkene degradation in version 3 of the Master Chemical Mechanism (MCM v3) has been evaluated, using environmental chamber data on the photo-oxidation of ethene, propene, 1-butene and 1-hexene in the presence of NOx, from up to five chambers at the Statewide Air Pollution Research Center (SAPRC) at the University of California. As part of this evaluation, it was necessary to include a representation of the reactions of the alkenes with O(3P), which are significant under chamber conditions but generally insignificant under atmospheric conditions. The simulations for the ethene and propene systems, in particular, were found to be sensitive to the branching ratios assigned to molecular and free radical forming pathways of the O(3P) reactions, with the extent of radical formation required for proper fitting of the model to the chamber data being substantially lower than the reported consensus. With this constraint, the MCM v3 mechanisms for ethene and propene generally performed well. The sensitivity of the simulations to the parameters applied to a series of other radical sources and sink reactions (radical formation from the alkene ozonolysis reactions and product carbonyl photolysis; radical removal from the reaction of OH with NO2 and β-hydroxynitrate formation) were also considered, and the implications of these results are discussed. Evaluation of the MCM v3 1-butene and 1-hexene degradation mechanisms, using a more limited dataset from only one chamber, was found to be inconclusive. The results of sensitivity studies demonstrate that it is impossible to reconcile the simulated and observed formation of ozone in these systems for ranges of parameter values which can currently be justified on the basis of the literature. As a result of this work, gaps and uncertainties in the kinetic, mechanistic and chamber database are identified and discussed, in relation to both tropospheric chemistry and chemistry important under chamber conditions which may compromise the evaluation procedure, and recommendations are made for future experimental studies. Throughout the study, the performance of the MCM v3 chemistry was also simultaneously compared with that of the corresponding chemistry in the SAPRC-99 mechanism, which was developed and optimized in conjunction with the chamber datasets.  相似文献   

10.
Modelling studies were performed with the multiphase mechanism RACM-MIM2ext/CAPRAM 3.0i to investigate the tropospheric multiphase chemistry in deliquesced particles and non-precipitating clouds using the SPACCIM model framework. Simulations using a non-permanent cloud scenario were carried out for two different environmental conditions focusing on the multiphase chemistry of oxidants and other linked chemical subsystems. Model results were analysed by time-resolved reaction flux analyses allowing advanced interpretations. The model shows significant effects of multiphase chemical interactions on the tropospheric budget of gas-phase oxidants and organic compounds. In-cloud gas-phase OH radical concentration reductions of about 90 % and 75 % were modelled for urban and remote conditions, respectively. The reduced in-cloud gas-phase oxidation budget increases the tropospheric residence time of organic trace gases by up to about 30 %. Aqueous-phase oxidations of methylglyoxal and 1,4-butenedial were identified as important OH radical sinks under polluted conditions. The model revealed that the organic C3 and C4 chemistry contributes with about 38 %/48 % and 8 %/9 % considerably to the urban and remote cloud / aqueous particle OH sinks. Furthermore, the simulations clearly implicate the potential role of deliquescent particles to operate as a reactive chemical medium due to an efficient TMI/HOx,y chemical processing including e.g. an effective in-situ formation of OH radicals. Considerable chemical differences between deliquescent particles and cloud droplets, e.g. a circa 2 times more efficient daytime iron processing in the urban deliquescent particles, were identified. The in-cloud oxidation of methylglyoxal and its oxidation products is identified as efficient sink for NO3 radicals in the aqueous phase.  相似文献   

11.
An improvement of long-range air pollution transport and diffusion model which includes planetary boundary layer (PBL) dynamics and chemistry of SO2 and NOx, the processes of dry and wet deposition has been developed and used in the Southeast Europe. The transport and diffusion process are described on the basis of a combination of the Eulerian and Lagrangian approaches. A similarity theory is used for calculation of the PBL characteristics. A known linear chemistry module which includes 5 nitrogen and 2 sulphate species is incorporated. The model results for the region of Southeast Europe are in good agreement with the Meteorological Synthesizing Center West, Oslo information.  相似文献   

12.
Global secondary organic aerosol formation (SOA) is currently assumed to be between 11.2 and 270 Tg/yr. This range of uncertainty is reflected in the gas-phase chemistry. In this study, we focus on the feedback of SOA formation on the concentrations of most important trace gases such as ozone, and compare it to the impact of monoterpene gas-phase chemistry with a newly developed reduced monoterpene mechanism (MMM) for either α- or β-pinene in the global chemistry transport model MATCH-MPIC. With this set-up an uncertainty range of 3.5–4.0% increase in annually averaged tropospheric ozone was found to be caused by the gas-phase chemistry of the investigated monoterpenes. Moreover, a strong feedback has been observed for NOx, HCHO, HNO3 and PAN. These observations are affected remarkably by different SOA formation approaches like partitioning or saturation vapour pressure limitation and by the structure of the monoterpene used, e.g. reducing the impact on tropospheric ozone to 1.2–1.9% by using the partitioning approach versus the simulation with gas-phase chemistry only. Therefore, a consideration of the individual processes associated with SOA formation seems to be necessary to reduce the uncertainty in SOA formation and to understand the impact of VOCs on atmospheric chemistry. An erratum to this article is available at .  相似文献   

13.
为了进一步认识闪电活动与对流层氮氧化物的关系及更准确地估算中国地区闪电产生的氮氧化物(LNOx)总量,选取人口稀疏,工业生产水平较低的青藏高原地区作为研究区域,基于LIS(Lightning Imaging Sensor)和GOME-2(The Global Ozone Monitoring Experiment-2)卫星探测仪资料,分析了青藏高原中部区域2009年1月至2012年2月闪电与对流层NO2垂直浓度(VCD)月均值资料的时空分布特性和相关性。在此基础上,结合Beirle et al.(2004)的LNOx估算方法,估算了中国内陆地区的LNOx产量。结果表明:青藏高原地区对流层NO2与闪电与在年际趋势、空间分布及季节变化上保持很好的一致性,闪电密度与NO2VCD的线性拟合相关系数为0.84,这表明青藏高原地区NOx受人为源影响小,是研究LNOx的理想区域。基于拟合结果,估算得到中国内陆地区LNOx的年均产量为0.15(0.03~0.38)Tg(N)a-1。这一结论进一步缩小了以往研究中中国地区LNOx产量估算的不确定范围,有助于更清楚地认识闪电在中国气候变化中的重要作用。  相似文献   

14.
By means of a three-dimensional meteorological model (MM5) and a chemical model,the distributions of tropospheric ozone and its precursors over China have been simulated in summer and winter time,16-18 August 1994 and 7-9 January 1995.The distribution of ozone over the Tibetan Plateau in summer time is deeply discussed.The simulated results indicate that thedistributions of surface ozone and NOx are in good agreement with observed results,and human activities and photochemical reactions are the main factors controlling the surface ozone and NOx concentrations.In addition,higher ozone concentrations are coincided with the air convergence,and the lower concentrations are related to the air divergence.In summer,over the Tibetan Plateau the strong flow convergence results in higher ozone concentrations in the lower troposphere:and the strong flow divergence results in lower ozone concentrations in the upper troposphere.In winter time ozone concentrations show large-scale characteristics controlled by westerly flow,and in the jet area they are lower than those outside the jet.  相似文献   

15.
Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH4 and NO x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO x emissions during this period while the contribution of CH4 to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.  相似文献   

16.
A chemical module describing the tropospheric photochemistry of ozone precursors in both gaseous and aqueous phases for a remote continental atmosphere has been developed within the framework of a two-dimensional cloud model. Dynamical, microphysical and chemical processes are fully interacting in order to study the influence of clouds on ozone chemistry and to quantify the relative importance of the different processes on the budget and evolution of 12 chemical species. Whereas the concentrations of highly soluble species are strongly affected by evaporation and sedimentation, less soluble species are affected primarily by accretion. The model reproduces previously observed chemical phenomena such as the enrichment of formic acid at the top of the cloud.  相似文献   

17.
Performance of national centers for environmental prediction based global forecast system (GFS) T574/L64 and GFS T382/L64 over Indian region has been evaluated for the summer monsoon season of 2011. The real-time model outputs are generated daily at India Meteorological Department, New Delhi for the forecasts up to 7 days. Verification of rainfall forecasts has been carried out against observed rainfall analysis. Performance of the model is also examined in terms of lower tropospheric wind circulation, vertical structure of specific humidity and precipitable water content. Case study of a monsoon depression is also illustrated. Results obtained show that, in general, both the GFS T382 and T574 forecasts are skillful to capture climatologically heavy rainfall regions. However, the accuracy in prediction of location and magnitude of rainfall fluctuates considerably. The verification results, at the spatial scale of 50 km resolution, in a regional spatial scale and country as a whole, in terms of continuous skill score, time series and categorical statistics, have demonstrated superiority of GFS T574 against T382 over Indian region. Both the model shows bias of lower tropospheric drying and upper tropospheric moistening. A bias of anti-cyclonic circulation in the lower tropospheric level lay over the central India, where rainfall as well as precipitable water content shows negative bias. Considerable differences between GFS T574 and T382 are noticed in the structure of model bias in terms of lower tropospheric wind circulation, vertical structure of specific humidity and precipitable water contents. The magnitude of error for these parameters increases with forecast lead time in both GFS T574 and T382. The results documented are expected to be useful to the forecasters, monsoon researchers and modeling community.  相似文献   

18.
The NO3 radical initiated oxidation of cyclopentene, cyclohexene and 1-methyl-cyclohexene has been studied. The products formed in an N2O5-NO2-N2-O2-cycloalkene-static reactor system, at 0.1 MPa and 296 K, were investigated using long path FTIR. The principal products were aldehydes formed via a ring opening process. The reactions also resulted in significant yields of three types of ring retaining nitrooxy-substituted compounds. The average yields of alkyl nitrates from, e.g., reactions with cycloalkene were 25.1% 2-oxo-cyclohexyl nitrate, 22.8% 2-hydroxy-cyclohexyl nitrate and 4.0% 1,2-cyclohexyl dinitrate. The mechanisms involved resembles those proposed for acyclic alkenes. In absence of NO, -oxo and -hydroxy-cycloalkyl nitrates are formed via self reactions of -nitrooxy substituted cycloalkyl peroxy radicals. Estimated branching ratios for the reactants leading to ring retaining products in the presence and in the absence of NO are given and the possible relevance of these reactions for cycloalkenes under tropospheric conditions is discussed.  相似文献   

19.
We use a global atmospheric chemistry transport model to study the possible influence of aqueous phase reactions of peroxynitric acid (HNO4) on the concentrations and budgets of NOx, SOx, O3 and H2O2. Laboratory studies have shown that the aqueous reaction of HNO4aq withHSO– 3aq, and the uni-molecular decomposition of the NO4 – anion to form NO2 – (nitrite) occur on a time scale of about a second. Despite a substantial contribution of the reaction of HSO– 3aq with HNO4aq to the overall in-cloud conversion of SO2 to SO4 2–, a simultaneous decrease of other oxidants (most notably H2O2) more than compensated the increase in SO4 2– production. The strongest influence of heterogeneous HNO4 chemistry was found in the boundary layer, where calculated monthly average ozone concentrations were reduced between 2% to 10% andchanges of H2O2 between –20% to +10%compared to a simulation which ignores this reaction. Furthermore, SO2 was increased by 10% to 20% and SO4 2–depleted by up to 10%. Since the resolution of our global model does not enable a detailed comparison with measurements in polluted regions, it is not possible to verify whether considering heterogeneous HNO4 reactions results in a substantial improvement of atmospheric chemistry transport models. However, the conversion of HNO4 in the aqueous phase seems to be efficient enough to warrant further laboratory investigations and more detailed model studies on this topic.  相似文献   

20.
A one-dimensional coupled climate and chemistry model has been developed to estimate past and possible future changes in atmospheric temperatures and chemical composition due to human activities. The model takes into account heat flux into the oceans and uses a new tropospheric temperature lapse rate formulation. As found in other studies, we estimate that the combined greenhouse effect of CH4, O3, CF2Cl2, CFCl3 and N2O in the future will be about as large as that of CO2. Our model calculates an increase in average global surface temperatures by about 0.6°C since the start of the industrial era and predicts for A.D. 2050 a twice as large additional rise. Substantial depletions of ozone in the upper stratosphere by between 25% and 55% are calculated, depending on scenario. Accompanying temperature changes are between 15°C and 25°C. Bromine compounds are found to be important, if no rigid international regulations on CFC emissions are effective. Our model may, however, concivably underestimate possible effects of CFCl3, CF2Cl2, C2F3Cl3 and other CFC and organic bromine emissions on lower stratospheric ozone, because it can not simulate the rapid breakdown of ozone which is now being observed worldwide. An uncertainty study regarding the photochemistry of stratospheric ozone, especially in the region below about 25 km, is included. We propose a reaction, involving excited molecular oxygen formation from ozone photolysis, as a possible solution to the problem of ozone concentrations calculated to be too low above 45 km. We also estimate that tropospheric ozone concentrations have grown strongly in the northern hemisphere since pre-industrial times and that further large increases may take place, especially if global emissions of NOx from fossil fuel and biomass burning were to continue to increase. Growing NOx emissions from aircraft may play an important role in ozone concentrations in the upper troposphere and low stratosphere.  相似文献   

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