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1.
Abstract

We describe a one‐dimensional (1‐D) numerical model developed to simulate the chemistry of minor constituents in the stratosphere. The model incorporates most of the chemical species presently found in the upper atmosphere and has been used to investigate the effect of increasing chlorofluorocarbon (CFC) emissions on ozone (O3).

Our calculations confirm previous results that O3 depletions in the 20–25 km region, the region of the O3 maximum, are very sensitive to the relative abundances of Clx and NOy in the lower stratosphere for high Clx amounts. The individual abundances of lower stratospheric Clx and NOy amounts are very sensitive to upper tropospheric mixing ratios, which, in turn, are determined largely by surface input fluxes and heterogeneous loss processes. Thus the behaviour of column O3 depletions at high Clx levels is greatly affected, albeit indirectly, by tropospheric processes. For high Clx levels the Ox flux from the stratosphere to the troposphere is dramatically reduced, leading to a large reduction in tropospheric O3. Some of the variation between different published 1‐D model results is most likely due to this critical dependence of O3 depletion on NOy‐Clx ratios.

Model simulations of time‐dependent CFC effects on ozone indicate that if CFCs were to remain at constant 1980 emission rates while N2O increased at 0.25% a?1 and CH4 increased at 1% a?1, we could expect a 2.2% decrease in total column O3 (relative to the 1980 atmosphere) by the year 2000. However, if CFC emission rates were to increase by 3% a?1 (current estimates are 5–6% a?1), we would predict a depletion of 2.7% by the year 2000. The calculations for times beyond the year 2000 suggest that the effects on total O3 will begin to accelerate. If methyl chloroform emissions are added at 7% a?1 (current estimates are 7–9% a?1) to the above CFC‐N2O‐CH4 scenario we calculate total O3 depletions by the year 2000 that are 41% larger than those calculated without. This suggests that if the emissions of methyl chloroform continue to increase at their present rate then methyl chloroform could have a significant effect upon total O3.  相似文献   

2.
The set of high-resolution infrared solar observations made with the Atmospheric Trace Molecule Spectroscopy (ATMOS)-Fourier transform spectrometer from onboard Spacelab 3 (30 April-1 May 1985) has been used to evaluate the total budgets of the odd chlorine and fluorine chemical families in the stratosphere. These budgets are based on volume mixing ratio profiles measured for HCl, HF, CH3Cl, ClONO2, CCl4, CCl2F2, CCl3F, CHClF2, CF4, COF2, and SF6 near 30° north latitude. When including realistic concentrations for species not measured by ATMOS, i.e., the source gases CH3CCl3 and C2F3Cl3 below 25 km, and the reservoirs ClO, HOCl and COFCl between 15 and 40 km (five gases actually measured by other techniques), the 30° N zonal 1985 mean total mixing ratio of chlorine, Cl, was found to be equal to (2.58±0.10) ppbv (parts per billion by volume) throughout the stratosphere, with no significant decrease near the stratopause. The results for total fluorine indicate a slight, but steady, decrease of its volume mixing ratio with increasing altitude, around a mean stratospheric value of (1.15±0.12) ppbv. Both uncertainties correspond to one standard deviation. These mean springtime 1985 stratospheric budgets are commensurate with values reported for the tropospheric Cl and F concentrations in the early 1980s, when allowance is made for the growth rates of their source gases at the ground and the time required for tropospheric air to be transported into the stratosphere. The results are discussed with emphasis on conservation of fluorine and chlorine and the partitioning among source, sink, and reservoir gases throughout the stratosphere.  相似文献   

3.
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   

4.
In this paper, we discuss the results of 2000?C2100 simulations following the emissions associated with the Representative Concentration Pathways (RCPs) with a chemistry-climate model, focusing on the changes in 1) atmospheric composition (troposphere and stratosphere) and 2) associated environmental parameters (such as nitrogen deposition). In particular, we find that tropospheric ozone is projected to decrease (RCP2.6, RCP4.5 and RCP6) or increase (RCP8.5) between 2000 and 2100, with variations in methane a strong contributor to this spread. The associated tropospheric ozone global radiative forcing is shown to be in agreement with the estimate used in the RCPs, except for RCP8.5. Surface ozone in 2100 is projected to change little compared from its 2000 distribution, a much-reduced impact from previous projections based on the A2 high-emission scenario. In addition, globally-averaged stratospheric ozone is projected to recover at or beyond pre-1980 levels. Anthropogenic aerosols are projected to strongly decrease in the 21st century, a reflection of their projected decrease in emissions. Consequently, sulfate deposition is projected to strongly decrease. However, nitrogen deposition is projected to increase over certain regions because of the projected increase in NH3 emissions.  相似文献   

5.
Anomalies found in the isotope ratios of ozone are traceable to the ozone formation process. Metastable electronic states may be responsible for the preferred production of the heavy molecules. While laboratory isotope data and first tropospheric results agree well in the magnitude of isotope enrichments, stratospheric measurements show often higher values. Only through the collection of ozone samples can sufficiently large amounts of gas be obtained to analyze the three isotopes 48O3, 49O3, and 50O3. Collector systems have been developed and successfully operated in the troposphere and in the stratosphere. They will play in the future an important role in atmospheric oxygen isotope studies.  相似文献   

6.
The paper presents a coupled chemical-radiative one-dimensional model which is used to assess the steady-state and time-dependent composition and temperature changes in relation to the release in the atmosphere of chemicals such as CO2, N2O, CH4, NO x and chlorofluorocarbons.The model indicates that a doubling in CO2 leads to an increase in temperature of 12.7 K near the stratopause and to an increase in total ozone of 3.3% with a local enhancement of 17% at 40 km altitude. Additional release of N2O leads to an ozone reduction in the middle stratosphere. The reduction in the ozone column is predicted to be equal to 8.8% when the amount of N2O is doubled. The chemical effect of CH4 on ozone is particularly important in the troposphere. A doubling in the mixing ratio of this gas enhances the O3 concentration by 11% at 5 km. The predicted increase of the ozone column is equal to 1.4%. A constant emission of CFCl3 (230 kT/yr) and CF2Cl2 (300 kT/yr) leads to a steady-state reduction in the ozone column of 1.9% compared to the present-day situation. The effect of some uncertainties in the chemical scheme as well as the impact of a high chlorine perturbation are briefly discussed.Finally the results of a time dependent calculation assuming a realistic scenario for the emission of chemical species are presented and analyzed.  相似文献   

7.
Abstract

A coupled 1‐D radiative‐convective and photochemical diffusion model is used to study the influence of ozone photochemistry on changes in the vertical temperature structure and surface climate resulting from the doubling of atmospheric CO2, N2O, CH4 and increased stratospheric aerosols owing to the El Chichón volcanic eruption. It is found when CO2 alone is doubled, that the total ozone column increases by nearly 6% and the resulting increase in the solar heating contributes a smaller temperature decrease in the stratosphere (up to 4 K near the stratopause level). When the concentration of CO2, N2O and CH4 are simultaneously doubled, the total ozone column amount increases by only 2.5% resulting in a reduced temperature recovery in the stratosphere. Additional results concerning the effect of the interaction of ozone photochemistry with the stratospheric aerosol cloud produced by the El Chichón eruption show that it leads to a reduction in stratospheric ozone, which in turn has the effect of increasing the cooling at the surface and above the cloud centre while causing a slight warming below in the lower stratosphere.  相似文献   

8.
Oxidation reactions of the proposed CFC substitutes HCFC-123 (CF3CHCl2) and HCFC-141b (CFCl2CH3) have been studied in the laboratory using long-path Fourier transform infrared spectroscopy. The air oxidation of the HCFCs was initiated by the photolysis of Cl2 forming Cl atoms that abstract H atoms from the HCFC. CF3C(O)Cl was the only carbon containing compound observed in the infrared spectrum of the products of the HCFC-123/Cl2 irradiations and its yield was approximately one. The product data are consistent with formation of CF3C(O)Cl by Cl elimination of the intermediate halogenated alkoxy radical CF3CCl2O. The Cl-initiated oxidation of HCFC-141b led to the formation of CO and C(O)FCl. The product data are consistent with a 1 : 1 relationship between C(O)FCl formed and HCFC-141b reacted. Product data were compatible with both decomposition by cleavage of the C–C bond of the radical CFCl2CH2O leading to the prompt generation of C(O)FCl and reaction of the radical with O2 forming the two carbon halogenated aldehyde CFCl2CH(O), which in the presence of Cl was likely oxidized to C(O)FCl. An approximate method was developed in which the ratio was extracted from analysis of the time evolution of HCFC-141b, C(O)FCl, and CO. The data suggest that the contributions are comparable.  相似文献   

9.
Semi-continuous measurements of CFCl3, CF2Cl2, CCl4, CH3CCl3 and N2O were made at Adrigole, Ireland as part of the Atmospheric Lifetime Experiment (ALE). Clean, baseline air from the Atlantic Ocean was measured approximately 70% of the time; pollution events from Europe, for the remainder. The two final years of ALE data from Adrogole give a five-year record from July 1978 to June 1983. This paper extends previous work on the relative enhancements of trace gases during pollution episodes and presents (1) unambiguous identification of elevated levels of N2O concurrent with halocarbon pollution events, (2) detection of trends in emission of CH3CCl3, (3) discovery of seasonal variations in emission of CF2Cl2, CCl4 and CH3CCl3, (4) characterization of typical summer and winter pollution episodes, and (5) identification of weather patterns over Europe that are associated with high concentrations of CFCs at Adrigole. Some of these results assume that CFCl3 represents a uniform, well buffered source from the continent. The latter two results are particularly useful in the testing and calibration of three-dimensional chemical transport models. Observed enhancements are marginally consistent with estimates of halocarbon use by the chemical industry. The source of nitrous oxide correlated with halocarbons is 0.8 Tg(N)/yr from Europe alone and represents approximately 10% of the global stratospheric loss.  相似文献   

10.
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   

11.
The relative variances in stratospheric observations of longlived trace gases CH4, N2O, CF2Cl2, CFCl3 show large differences. These differences are greatly reduced when the local mean standard deviation is normalized to the local vertical gradient. This ratio, called ‘equivalent displacement height’ exhibits a characteristic vertical profile which is very similar for all the longlived trace gases, as well as for O3. With the help of this ratio, it is demonstrated that the variances are essentially due to natural causes, i.e., transport. Using the mixing length hypothesis a theoretical expression for the equivalent displacement height is derived. From it the meridional slope of the mixing surfaces and the mixing length can be calculated as function of the altitude. Additional information is obtained on the variance of that slope. The uncertainty of the measured mean trace gas profiles is defined.  相似文献   

12.
Absorption cross-sections of nine halomethanes (CCl4, CHCl3, CH2Cl2, CH3Cl, CFCl3, CF2Cl2, CF3Cl, CHFCl2, and CHF2Cl), measured between 174 and 250 nm for temperatures ranging from 225 to 295 K, are presented with uncertainties ranging from 2 to 4% and compared with previous determinations made for comparable temperature ranges.The largest temperature effect which takes place near the absorption threshold, decreases the absorption cross-section up to 50% for highly chlorinated methanes, but is negligible for molecules highly stabilized by hydrogen and/or fluorine. Extrapolated values for temperatures of aeronomical interest are presented, as well as parametrical formulas which give absorption cross-section values for given wavelength and temperature ranges.  相似文献   

13.
Abstract

To evaluate future climate change in the middle atmosphere and the chemistry–climate interaction of stratospheric ozone, we performed a long-term simulation from 1960 to 2050 with boundary conditions from the Intergovernmental Panel on Climate Change A1B greenhouse gas scenario and the World Meteorological Organization Ab halogen scenario using the chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC). In addition to this standard simulation we performed five sensitivity simulations from 2000 to 2050 using the rerun files of the simulation mentioned above. For these sensitivity simulations we used the same model setup as in the standard simulation but changed the boundary conditions for carbon dioxide (CO2), methane (CH4), nitrous oxide (N2O), and ozone-depleting substances (ODS). In the first sensitivity simulation we fixed the mixing ratios of CO2, CH4, and N2O in the boundary conditions to the amounts for 2000. In each of the four other sensitivity simulations we fixed the boundary conditions of only one of CO2, CH4, N2O, or ODS to the year 2000.

In our model simulations the future evolution of greenhouse gases leads to significant cooling in the stratosphere and mesosphere. Increasing CO2 mixing ratios make the largest contributions to this radiative cooling, followed by increasing stratospheric CH4, which also forms additional H2O in the upper stratosphere and mesosphere. Increasing N2O mixing ratios makes the smallest contributions to the cooling. The simulated ozone recovery leads to warming of the middle atmosphere.

In the EMAC model the future development of ozone is influenced by several factors. 1) Cooler temperatures lead to an increase in ozone in the upper stratosphere. The strongest contribution to this ozone production is cooling due to increasing CO2 mixing ratios, followed by increasing CH4. 2) Decreasing ODS mixing ratios lead to ozone recovery, but the contribution to the total ozone increase in the upper stratosphere is only slightly higher than the contribution of the cooling by greenhouse gases. In the polar lower stratosphere a decrease in ODS is mainly responsible for ozone recovery. 3) Higher NOx and HOx mixing ratios due to increased N2O and CH4 lead to intensified ozone destruction, primarily in the middle and upper stratosphere, from additional NOx; in the mesosphere the intensified ozone destruction is caused by additional HOx. In comparison to the increase in ozone due to decreasing ODS, ozone destruction caused by increased NOx is of similar importance in some regions, especially in the middle stratosphere. 4) In the stratosphere the enhancement of the Brewer-Dobson circulation leads to a change in ozone transport. In the polar stratosphere increased downwelling leads to additional ozone in the future, especially at high northern latitudes. The dynamical impact on ozone development is higher at some altitudes in the polar stratosphere than the ozone increase due to cooler temperatures. In the tropical lower stratosphere increased residual vertical upward transport leads to a decrease in ozone.  相似文献   

14.
平流层对对流层的作用是准确评估、预测对流层气候变化的一个重要方面。其中平流层成分尤其是臭氧的变化,可以改变平流层乃至对流层的辐射平衡,从而影响平流层、对流层的热动力过程。本文从辐射、动力2个角度介绍了平流层臭氧影响对流层气候变化的若干研究进展。平流层臭氧可以通过长短波辐射的方式对对流层大气造成辐射强迫,利用大气化学气候模式可以定量计算平流层臭氧变化引起的辐射强迫,但是辐射强迫的估算受模式中辐射传输模块本身缺陷的影响存在不确定性。动力方面,平流层臭氧变化产生的辐射效应可以改变温度的垂直和经向梯度,造成波折射指数的变化,进而影响平流层甚至对流层内波的折射与反射,通过上对流层下平流层区域内的波—流相互作用,对对流层气候产生影响。另外,南极臭氧损耗可通过大气环状模影响冬春季中高纬度对流层的天气气候,但是其影响的强度大小以及物理机制仍需进一步的确认。值得注意的是,北极平流层臭氧的变化与北半球中高纬度气候变化之间的关系相比南半球要更加复杂,需要更为深入的研究。  相似文献   

15.
A novel fully-automated airborne gas chromatograph for in situmeasurements of long-lived stratospheric tracers hasbeen developed, combining the high selectivity of a megabore PLOTcapillary column with recently developed sampling and separationtechniques. The Gas cHromatograph for theObservation of Stratospheric Tracers (GHOST)has been successfully operated during three STREAM campaigns(Stratosphere TRoposphere Experiment byAirborne Measurement) onboard a Cessna Citation IIaircraft in two different modes: Either N2O andCF2Cl2(CFC-12) or CFC-12 and CFCl3 (CFC-11) have been measuredsimultaneously, with a time resolution of 2 min for both modes.Under flight conditions the instrument precision (1) forthese species is better than 0.9%, and the accuracy(1) is better than 2.0% of the tropospheric values ofall measured compounds. The detection limits (3) arebelow 28 ppb for N2O, 14 ppt for CFC-12, and 8 ppt forCFC-11, respectively, i.e., well below 10 % of the troposphericvalues of all measured compounds. Post-mission optimization of thechromatographic separation showed a possible enhancement of thetime resolution by up to a factor of 2, associated with acomparable increase in precision and detection limit. As test ofactual performance of GHOST results from an in-flight N2Ointercomparison with a tunable diode laser absorptionspectrometer (TDLAS) are presented. They yield an excellentagreement between both instruments. Furthermore, on the basis ofthe hitherto most extensive set of upper tropospheric and lowerstratospheric data, the relative stratospheric N22O lifetime isre-assessed. When referenced to the WMO reference CFC-11 lifetimeof 45 ± 7 years an N2O lifetime of 91 ± 15 yearsis derived, a value substantially smaller than the WMO referencelifetime of 120 years. Moreover, this value implies astratospheric N2O sink strength of 16.3 ± 2.7 Tg (N)yr–1 which is 30% larger than previous estimates.  相似文献   

16.
A novel cryogenic sampling method combining the matrix isolation technique with FTIR spectroscopy has been developed for atmospheric trace gas analysis. It is applicable to a wide range of molecules with detection limits typically in the 10–50 ppt range. The method is described along with some measurements of N2O, CFCl3, CF2Cl2, OCS, CS2, SO2 and PAN from samples collected at ground level and from an aircraft between 9 and 14 km.  相似文献   

17.
Factors influencing the18O content of stratospheric H2O are reviewed in order to provide a theoretical framework for the interpretation of measurements of this quantity, which are now becoming available. Depletions in18O of 5–10% in stratospheric H2O are expected based on the known correlation between that of D and18O in tropospheric H2O and observed measurements of large (typically 50%) depletions of D in stratospheric H2O. H2O formed in the stratosphere as a result of oxidation of CH4 can be expected to reflect primarily the18O content of stratospheric O2, which is the same as that of tropospheric O2 (slightly enhanced with respect to standard mean ocean water). Thus, a reduction in the18O depletion is expected with increasing altitude, but not a large enhancement in18O in upper stratospheric H2O as found in recent far infrared measurements. The observed large enhancement of18O in stratospheric O3 is not expected to be reflected in stratospheric H2O. Necessary laboratory data for the improved quantification of these effects are reviewed.  相似文献   

18.
The effects of E1Nifio Modoki events on global ozone concentrations are investigated from 1980 to 2010 E1 Nifio Modoki events cause a stronger Brewer-Dobson （BD） circulation which can transports more ozone-poor air from the troposphere to stratosphere, leading to a decrease of ozone inthe lower-middle stratosphere from 90~S to 90~N. These changes in ozone concentrations reduce stratospheric column ozone. The reduction in stratospheric column ozone during E1 Nifio Modoki events is more pronounced over the tropical eastern Pacific than over other tropical areas because transport of ozone-poor air from middle-high latitudes in both hemispheres to low latitudes is the strongest between 60°W and 120°W. Because of the decrease in stratospheric column ozone during E1 Nifio Modoki events more UV radiation reaches the tropical troposphere leading to significant increases in tropospheric column ozone An empirical orthogonal function （EOF） analysis of the time series from 1980 to 2010 of stratospheric and tropospheric ozone monthly anomalies reveals that： E1 Nifio Modoki events are associated with the primary EOF modes of both time series. We also found that E1 Nifio Modoki events can affect global ozone more significantly than canonical E1 Nifio events. These results imply that E1 Nifio Modoki is a key contributor to variations in global ozone from 1980 to 2010.  相似文献   

19.
The paper discusses the potential effects on the ozone layer of gases released by the engines of proposed high altitude supersonic aircraft. The major problem arises from the emissions of nitrogen oxides which have the potential to destroy significant quantities of ozone in the stratosphere. The magnitude of the perturbation is highly dependent on the cruise altitude of the aircraft. Furthermore, the depletion of ozone is substantially reduced when heterogeneous conversion of nitrogen oxides into nitric acid on sulfate aerosol particles is taken into account in the calculation. The sensitivity of the aerosol load on stratospheric ozone is investigated. First, the model indicates that the aerosol load induced by the SO2 released by aircraft is increased by about 10–20% above the background aerosols at mid-high latitude of the Northern Hemisphere at 15 km for the NASA emission scenario A (the NASA emission scenarios are explained in Tables I to III). This increase in aerosol has small effects on stratospheric ozone. Second, when the aerosol load is increased following a volcanic eruption similar to the eruption of El Chichon (Mexico, April 1982), the ozone column in spring increases by as much as 9% in response to the injection of NO x from the aircraft with the NASA emission scenario A. Finally, the modeled suggests that significant ozone depletion could result from the formation of additional polar stratospheric clouds produced by the injection of H2O and HNO3 by the aircraft engines.  相似文献   

20.
An approach to mitigate global warming via sulphur loading in the stratosphere (geoengineering) is studied, employing a large ensemble of numerical experiments with the climate model of intermediate complexity IAP RAS CM. The model is forced by the historical+SRES A1B anthropogenic greenhouse gases+tropospheric sulphates scenario for 1860–2100 with additional sulphur emissions in the stratosphere in the twenty-first century. Different ensemble members are constructed by varying values of the parameters governing mass, horizontal distribution and radiative forcing of the stratospheric sulphates. It is obtained that, given a global loading of the sulphates in the stratosphere, among those studied in this paper latitudinal distributions of geoengineering aerosols, the most efficient one at the global basis is that peaked between 50°N and 70°N and with a somewhat smaller burden in the tropics. Uniform latitudinal distribution of stratospheric sulphates is a little less efficient. Sulphur emissions in the stratosphere required to stop the global temperature at the level corresponding to the mean value for 2000–2010 amount to more than 10 TgS/year in the year 2100. These emissions may be reduced if some warming is allowed to occur in the twenty-first century. For instance, if the global temperature trend S g in every decade of this century is limited not to exceed 0.10 K/decade (0.15 K/decade), geoengineering emissions of 4–14 TgS/year (2–7 TgS/year) would be sufficient. Even if the global warming is stopped, temperature changes in different regions still occur with a magnitude up to 1 K. Their horizontal pattern depends on implied latitudinal distribution of stratospheric sulphates. In addition, for the stabilised global mean surface air temperature, global precipitation decreases by about 10%. If geoengineering emissions are stopped after several decades of implementation, their climatic effect is removed within a few decades. In this period, surface air temperature may grow with a rate of several Kelvins per decade. The results obtained with the IAP RAS CM are further interpreted employing a globally averaged energy–balance climate model. With the latter model, an analytical estimate for sulphate aerosol emissions in the stratosphere required climate mitigation is obtained. It is shown that effective vertical localisation of the imposed radiative forcing is important for geoengineering efficiency.  相似文献   

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