N2O增加对大气环境影响的模拟及其与甲烷和平流层水汽影响的比较

本文利用美国国家大气环境中心(NCAR)的二维化学、辐射和动力相互作用的模式(SOCRATES),模拟了大气中N₂O增加对O₃和温度的影响,并从化学、辐射和动力过程讨论了影响原因,此外还与大气甲烷和平流层水汽增加对大气环境的影响进行了对比.分析表明:大气中N₂O浓度增加以后,将通过化学过程引起30 km以上O₃损耗,30~40 km损耗较多;30 km以上降温明显,下平流层中低纬度地区以及对流层O₃增加并有微弱升温;30~40 km附近,北半球中高纬地区O₃减少以及降温幅度都大于南半球.对流层升温主要是N₂O和O₃增加所致,而平流层温度变化主要受O₃控制.北半球中高纬地区动力过程对温度变化的反馈较其它地区明显,这种反馈对平流层中高层北半球中高纬地区温度和O₃的变化都有明显影响.大气中甲烷增加引起的O₃损耗在45 km以上,45 km以下O₃增加.平流层水汽增加会引起40 km以上O₃减少,20~40 km大部分地区O₃增加.N₂O增加造成的O₃损耗正好位于臭氧层附近,其排放对未来O₃层恢复至关重要.N₂O增加引起下平流层15~25 km中低纬度地区有弱的升温,这与其它温室气体增加对该地区温度的影响不同,CO₂,CH₄和H₂O等增加后下平流层通常是降温.     

On the vertical distribution of carbon monoxide and methane in the stratosphere

The vertical distribution of the methane concentration in the stratosphere is related to its dissociation by two simultaneous daytime reactions with excited oxygen atoms O(¹D) and with OH radicals and depends on the stratospheric eddy diffusion coefficient.Dissociation of CH₄ in the lower stratosphere leads to the production of CO molecules while in the upper stratosphere thepphotodissociation of CO₂ molecules is an additional process to the CO production.In the upper stratosphere (40±10 km) there is an equilibrium between the formation and destruction processes of carbon monoxide which leads to a minimum of its mixing ratio. There is an increase of the CO mixing ratio in the troposphere and mesosphere compared with that of the stratosphere.The vertical distribution of the CO mixing ratio is closely related to the eddy diffusion coefficient in the whole stratosphere but the absolute values of the hydroxyl radical concentration also determine the values of the CO mixing ratio.     

A discussion of the chemistry of some minor constituents in the stratosphere and troposphere

A discussion is given of atmospheric reactions in the H₂O–CH₄–O₂–O₃–NO _x system. In the lower troposphere such reactions may lead to significant production of ozone. Their role in the odd hydrogen balance, especially of the troposphere and lower stratosphere, is discussed. CH₃OH may be an intermediate in the oxidation cycle of methane, especially in the cold stratosphere. Its photodissociation into H₂ and CH₂O may consequently provide an important source for stratospheric H₂. Catalytic photochemical chains of reactions involving NO _x and HO _x may also lead to tropospheric destruction of ozone. Due to lack of knowledge it is not possible at present to evaluate the importance of the before-mentioned reactions.With the aid of model calculations it is indicated that stratospheric ozone is most sensitive to changes in the adopted lower boundary values of N₂O and that an increase in water vapour concentrations in the lower stratosphere will indeed cause some increase in ozone as predicted.Fluctuations in the flux of solar radiation near 190 nm may cause significant variations in stratospheric ozone concentrations.     

On the theoretical model for vertical ozone density distributions in the mesosphere and upper stratosphere

Diurnal variations in the vertical ozone density distribution have been calculated for the height range 40–150 km by extending our existing computer programs. The steady-state profiles were first calculated for fifteen constituents in the original program and three additional constituents (CH₄, CO and CO₂); the result was used as the initial condition for the time-dependent solution. The profile of the eddy diffusion coefficient used in this study was determined by comparing the model profile with the observations for CH₄, whose density distribution is verysenstive to the eddy diffusion coefficient The effects of hydrogen and nitrogen compounds on the ozone density are discussed somewhat quantitatively; they reduce the ozone density mainly in the mesosphere and stratosphere, respectively. Special attention is given to the large depression of the ozone density at around 70–85 km, which has been obtained in many theoretical models but has neither been explained nor definitely confirmed by observations. Our time-dependent model indicates that the depression develops at night by the effect of hydrogen-oxygen and nitrogen-oxygen reactions and of eddy diffusion transports. The latter effect also produces an increase of the ozone density after midnight at some heights in the depression region.     

OH radical concentration in the stratosphere

The consumption of both methane and carbon monoxide in the lower stratosphere is due predominantly to reaction with OH radicals. The possibility of deriving OH concentration from measurements of the decrease of CH₄ and CO mixing ratios above the tropopause is explored. The observations and the basic chemistry are briefly summarized. Simple one-dimensional diffusion models are employed to derive expressions for the decrease of CH₄ and CO mixing ratios with altitude above the tropopause, and the influence of important parameters is discussed. Vertical air velocities resulting from large-scale organized mean motion and from synoptic variations are shown to distort the concentration altitude profiles of methane and carbon monoxide, respectively. Suitable averaging of observational data is required to eliminate the effects due to vertical motion. Then a reliable value for the effective OH number density should be obtainable. At present an estimate of 4×10⁶ molecules/cm³ is derived.     

Evidence for vertical ozone redistribution since 1967

Long-term measurements of the ozone concentration in the vicinity of the city of Berlin have been performed with ground based Dobson spectrophotometers and balloon borne systems. The respective experiments cover the past 24 years. All data have been reevaluated and corrected towards uniform calibration standards, leading to the longest European data set of total column density, altitude-dependent ozone partial pressures and the corresponding temperatures. Smoothing algorithms unravel significant long-term trends.The analysis shows an increase of ozone concentration within the middle stratosphere (below 31 km height) as well as in the troposphere over the past 24 years. On the contrary, ongoing ozone depletion in the lower stratosphere has been found.The large scale vertical redistribution of atmospheric ozone in the troposphere and the lower stratosphere seems to be in agreement with model calculations and trend predictions that have their roots in changes of the chemical composition and the ozone photochemistry due to anthropogenically induced trace gas concentrations.Deutscher Wetterdienst, Meteorologisches Observatorium Potsdam.Deutscher Wetterdienst, Meteorologisches Observatorium Lindenberg.     

Relationships between groundwater in permafrost zone and climate changes

The paper presents the results of statistical analysis and estimation of long-term changes in surface air temperature, the gas composition of the atmosphere, the depth of seasonal thawing, and the temperature and area of permafrost occurrence in the circumpolar zone of the Northern Hemisphere. Preliminary estimates were obtained for the possible influence of the current changes in the thermophysical parameters of permafrost rocks on the albedo of the underlying surface, air moisture content, and the concentrations of carbon dioxide and methane in the atmosphere. The density of anthropogenic and natural methane fluxes from the underlying surface to the atmosphere is evaluated. The possible formation mechanisms of global maximums in carbon dioxide and methane concentration in the atmosphere of circumpolar areas in the context of interaction between methane cycle and the processes of permafrost thawing are described.     

The Global Warming Debate: A Review of the State of Science

A review of the present status of the global warming science is presented in this paper. The term global warming is now popularly used to refer to the recent reported increase in the mean surface temperature of the earth; this increase being attributed to increasing human activity and in particular to the increased concentration of greenhouse gases (carbon dioxide, methane and nitrous oxide) in the atmosphere. Since the mid to late 1980s there has been an intense and often emotional debate on this topic. The various climate change reports (1996, 2001) prepared by the IPCC (Intergovernmental Panel on Climate Change), have provided the scientific framework that ultimately led to the Kyoto protocol on the reduction of greenhouse gas emissions (particularly carbon dioxide) due to the burning of fossil fuels. Numerous peer-reviewed studies reported in recent literature have attempted to verify several of the projections on climate change that have been detailed by the IPCC reports.The global warming debate as presented by the media usually focuses on the increasing mean temperature of the earth, associated extreme weather events and future climate projections of increasing frequency of extreme weather events worldwide. In reality, the climate change issue is considerably more complex than an increase in the earth’s mean temperature and in extreme weather events. Several recent studies have questioned many of the projections of climate change made by the IPCC reports and at present there is an emerging dissenting view of the global warming science which is at odds with the IPCC view of the cause and consequence of global warming. Our review suggests that the dissenting view offered by the skeptics or opponents of global warming appears substantially more credible than the supporting view put forth by the proponents of global warming. Further, the projections of future climate change over the next fifty to one hundred years is based on insufficiently verified climate models and are therefore not considered reliable at this point in time.     

The structure of the natural stratosphere and the impact of chlorofluoromethanes on the ozone layer investigated in a 2-D time dependent model

two-dimensional time dependent model of the stratosphere incorporating the major interactions between radiative-photochemical and dynamical processes is described. The main prognostic equations considered are the thermodynamic equation and the general conservation equation for the minor chemical constituents representing the odd oxygen (O _x =O+('D)+O₃), odd hydrogen (HO _x =HO+HO₂), N₂O, odd nitrogen (NO _x =NO+NO₂+HNO₃), CF₂Cl₂, CFCl₃ and odd chlorine (Cl _x =Cl+ClO+HCl). The zonal wind and mean meridional circulations are determined diagnostically by the integration of the thermal wind equation and the stream function equation in the meridional plane espectively. The large scale eddy processes are parameterized in terms of zonal mean quantities using the generalized diffusion formulation on a sloping surface. The radiative heating and cooling and the hotochemical sources and sinks are incorporated in a form which allows for the major interactions among the minor trace constituents, temperature and mean circulation.Two integrations consisting of natural stratosphere and a stratosphere contaminated by the chlorofluoromethanes through lower boundary fluxes are carried out for 23 model years by changing the declination of the sun every day and using 6-hour time step. The model simulations of temperature, mean circulation, ozone, HO _x , N₂O and NO _x in the meridional plane for the normal stratosphere, show satisfactory agreement with the available observations. Based on the results of second integration it is found that the injection of chlorofluoromethanes in the atmosphere at the estimated current production rates can lead to significant changes in the meridional distribution of ozone, temperature and NO _x in the middle and upper stratosphere. The results also indicate that the percentage total ozone depletion increases from tropics to high latitudes and from summer to winter high latitudes. Also discussed are the results of additional experiments incorporating the reaction of HO₂ with NO and the reactions involving ClNO₃.     

Effect of stratospheric O3 depletion on tropospheric SO2 column in Antarctica

When ozone is depleted in the stratosphere during ozone-hole period, UV-B radiation, which is normally absorbed in this region, penetrates into the troposphere. As a result, the behavior of several species in the troposphere, which interact with UV-B radiation, is likely to change. Sulfur dioxide is predominantly found in the troposphere. To study the behavior of sulfur dioxide during this event, a Brewer spectrophotometer was installed at Maitri (70.7°S, 11.7°E) in Antarctica in July 1999. With this instrument, the vertical column density of SO₂ was measured from September 1999 to December 2003. We have observed an increase in SO₂ column density during an ozone-hole event. The magnitude of increase is different in different years, on average, by a factor of ∼5 (from ∼0.5 to ∼2.5 DU). Simultaneously, the maximum value of UV-B flux at the ground was also measured. We have observed that during the ozone-hole period, the UV-B flux also increased by different amounts during different years, by a factor of ∼3–5. Good correlation has been found between SO₂ column and UV-B flux but no correlation has been found between O₃ column and UV-B flux from the middle of September to the middle of November. Using a simple steady-state chemical reaction scheme, an attempt has been made to examine whether the increase in UV-B flux could increase the SO₂ column during the ozone-hole period.     

Influence of the Precipitating Energetic Particles on Atmospheric Chemistry and Climate

We evaluate the influence of the galactic cosmic rays (GCR), solar proton events (SPE), and energetic electron precipitation (EEP) on chemical composition of the atmosphere, dynamics, and climate using the chemistry-climate model SOCOL. We have carried out two 46-year long runs. The reference run is driven by a widely employed forcing set and, for the experiment run, we have included additional sources of NO _x and HO _x caused by all considered energetic particles. The results show that the effects of the GCR, SPE, and EEP fluxes on the chemical composition are most pronounced in the polar mesosphere and upper stratosphere; however, they are also detectable and statistically significant in the lower atmosphere consisting of an ozone increase up to 3?% in the troposphere and ozone depletion up to 8?% in the middle stratosphere. The thermal effect of the ozone depletion in the stratosphere propagates down, leading to a warming by up to 1?K averaged over 46?years over Europe during the winter season. Our results suggest that the energetic particles are able to affect atmospheric chemical composition, dynamics, and climate.     

Sensitivity of evapotranspiration and soil moisture in wheat fields to changes in climate and direct effects of carbon dioxide

Abstract

A physically based model of moisture transfer in the soil-canopy-atmosphere system, fitted to measured data in wheat fields, was applied to calculate the sensitivity of evapotranspiration to the combined effect of possible CO₂-induced climate changes and the direct impact of doubling CO₂ content in the atmosphere. The impact of carbon dioxide was taken into account by changing the stomatal resistance and the leaf area index. Several climate change scenarios were used. Simulation studies showed that when the changes of a number of climatic and plant factors are considered, evapotranspiration responses can differ greatly from those that consider only temperature change. The temperature effect of the increase in CO₂ content in the atmosphere can be compensated by changes in the physiological parameters of vegetation. Thus, under certain conditions, one can expect a decrease in evapotranspiration instead of an increase such as is predicted by a number of models which neglect the direct effects of CO₂ on plant behaviour.     

The effects of water vapour and oxides of nitrogen on ozone and temperature structure of the stratosphere

Summary A steady-state mean meridional model of the stratosphere is used to investigate the effects of water vapour and nitrogen oxides on ozone and temperature distributions in the stratosphere. The Chapman classical photochemical scheme for ozone is extended to include the dominant reactions involving hydrogen compounds and nitrogen oxides. The ozone and temperature changes are studied under radiative-photochemical equilibrium conditions and in a model incorporating both transport and radiative-photochemical processes. It is found that both hydrogen and nitrogen reactions contribute to substantial decreases in ozone and temperature under photochemical equilibrium conditions, but the computed distribution do not resemble those observed. The effect of transport processes is to reduce the deviations in the ozone mixing ratio and temperature with the computed distributions having many features in common with the observations. It is found that the ozone and temperature respond more readily to the arbitrary increase of nitrogen oxides than to that of water vapour.     

Stratospheric ozone response to a solar proton event: Hemispheric asymmetries

Ozone depression in the polar stratosphere during the energetic solar proton event on 4 August 1972 was observed by the backscattered ultraviolet (BUV) experiment on the Nimbus 4 satellite. Distinct asymmetries in the columnar ozone content, the amount of ozone depressions and their temporal variations above 4 mb level (38 km) were observed between the two hemispheres. The ozone destroying solar particles precipitate rather symmetrically into the two polar atmospheres due to the geomagnetic dipole field These asymmetries can be therefore ascribed to the differences mainly in dynamics and partly in the solar illumination and the vertical temperature structure between the summer and the winter polar atmospheres. The polar stratosphere is less disturbed and warmer in the summer hemisphere than the winter hemisphere since the propagation of planetary wave from the troposphere is inhibited by the wind system in the upper troposphere, and the air is heated by the prolonged solar insolation. Correspondingly, the temporal variations of stratospheric ozone depletion and its recovery appear to be smooth functions of time in the (northern) summer hemisphere and the undisturbed ozone amount is slighily, less than that of its counterpart. On the other hand, the tempotal variation of the upper stratospheric ozone in the winter polar atmosphere (southern hemisphere) indicates large amplitudes and irregularities due to the disturbances produced by upward propagating waves which prevail in the polar winter atmosphere. These characteristic differences between the two polar atmospheres are also evident in the vertical distributions of temperature and wind observed by balloons and rocker soundings.     

Nonlinear behavior on an ozone photochemical system in the stratosphere

A nonlinear box system describing ozone photochemistry in the stratosphere is presented. Influences of pollutants, such as odd chlorine (Cl_x) and odd nitrogen (NO_x) discharged by human activities, on photochemical states of the system are investigated in detail. The results show that the solutions of the box system constitute a ‘cusp’ catastrophe manifold in the state-parameter space. An increase of about 30% for Cl_x source strength or a decrease of about 30% for NO_x source strength from their current level may lead to catastrophic transition and results in a reduction of ozone concentration about 50 times. Project supported by the National Natural Science Foundation of China and Laboratory for Aeronomy and Global Environmental Observation of IAP.     

Low ozone event at Madrid in November 1996

A sudden transient increase of the solar ultraviolet (UV) radiation was detected with a ground-based photometer in Madrid (Spain, 41°N, 3°W) on 25 November 1996 (Cordoba et al., 2000. UV-B irradiance at Madrid during 1996, 1997 and 1998. J. Geophys. Res. 105 (D4) (2000) 4903–4906). The data obtained by the TOMS satellite instrument revealed that this event was related to a reduction of the total ozone column values. This low ozone episode has been analysed. The ozone decrease was accompanied by a reduction of air temperature in the lower stratosphere. The anti-correlation between total ozone and air parcel height along the three-dimensional isentropic back-trajectories suggests that the adiabatic uplift of air contributed significantly to both the ozone and the temperature decreases observed. The uplift could be caused by the propagation into the lower stratosphere of the high-pressure cell located over the mid-Atlantic region.     

平流层O3、O动力系统的平衡性质及南极平流层O3季节变化规律的研究

本文首次利用常微分方程定性理论对平流层O₃、O动力系统的平衡性质进行了讨论.结果表明,如果在平流层O₃的主要分布高度内,大气扩散作用小于光化学作用,那么平流层的O₃层处于稳定状态;反之,平流层的O₃层将遭到破坏.利用这一机制,我们可以解释南极平流层O₃的季度变化规律和每年9-10月份出现的南极O₃洞.     

Statistical characteristics of the vertical ozone distribution in mid-latitudes

Summary The correlation matrix for the vertical ozone distribution and the temperature-ozone cross-correlation matrix, which was calculated from ozone soundings made over Berlin between 1967 and 1970, the statistical structure of the vertical ozone profile (correlation coefficients, average profiles, average standard deviation, relative variability) was derived for the three ozone seasons. The partial ozone pressure does not at all heights follow a normal distribution (e. g. at tropopause level). Generally, the correlation between tropospheric and stratospheric ozone is rather poor. In some layers the highest correlation coefficients, i.e. –0.3 and +0.4, occur in autumn (October to December) and in winter and spring (January to April). The correlation between the ozone amounts of various stratospheric layers is distinct in autumn, less distinct in summer (May to September) and entirely missing from January to April. Conspicuous cross-correlations between temperature and ozone have been found for all three seasons. a) With a negative correlation between tropospheric temperature and middle tropospheric to middle stratospheric ozone (maximum up to –0.8); b) with a rather strong positive correlation between the ozone amount and the temperature in the lower stratosphere (maximum up to +0.84); c) with a positive correlation between the ozone amount of the middle stratosphere and the temperature of the middle stratosphere (maximum up to +0.8). The highest correlation coefficients occur in autumn.     

The present-day and future impact of NOx emissions from subsonic aircraft on the atmosphere in relation to the impact of NOx surface sources

The effect of present-day and future NO_x emissions from aircraft on the NO_x and ozone concentrations in the atmosphere and the corresponding radiative forcing were studied using a three-dimensional chemistry transport model (CTM) and a radiative model. The effects of the aircraft emissions were compared with the effects of the three most important anthropogenic NO_x surface sources: road traffic, electricity generation and industrial combustion. From the model results, NO_x emissions from aircraft are seen to cause an increase in the NO_x and ozone concentrations in the upper troposphere and lower stratosphere, and a positive radiative forcing. For the reference year 1990, the aircraft emissions result in an increase in the NO_x concentration at 250 hPa of about 20 ppt in January and 50 ppt in July over the eastern USA, the North Atlantic Flight Corridor and Western Europe, corresponding to a relative increase of about 50%. The maximum increase in the ozone concentrations due to the aircraft emissions is about 3-4 ppb in July over the northern mid-latitudes, corresponding to a relative increase of about 3-4%. The aircraft-induced ozone changes cause a global average radiative forcing of 0.025 W/m² in July. According to the ANCAT projection for the year 2015, the aircraft NO_x emissions in that year will be 90% higher than in the year 1990. As a consequence of this, the calculated NO_x perturbation by aircraft emissions increases by about 90% between 1990 and 2015, and the ozone perturbation by about 50-70%. The global average radiative forcing due to the aircraft-induced ozone changes increases by about 50% between 1990 and 2015. In the year 2015, the effects of the aircraft emissions on the ozone burden and radiative forcing are clearly larger than the individual effects of the NO_x surface sources. Taking chemical conversion in the aircraft plume into account in the CTM explicitly, by means of modified aircraft NO_x emissions, a significant reduction of the aircraft-induced NO_x and ozone perturbations is realised. The NO_x perturbation decreases by about 40% and the ozone perturbation by about 30% in July over Western Europe, the eastern USA and the North Atlantic Flight Corridor.