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1.
Vertical profiles of stratospheric HO2 and NO2 concentrations were determined using matrix isolation and ESR. Up to 10 different samples per flight were collected in situ by a balloon borne cryosampler. Free radicals and trace constituents which are condensable at 68 K are trapped in a polycristalline H2O or D2O matrix. After collection, the samples are stored at a temperature below 83 K until they are analysed in the laboratory by X-band ESR spectroscopy at 4 K. The HO2 and NO2 were identified and calibrated by comparison with standard samples collected in the laboratory under typical stratospheric sampling conditions. From several flights over Southern France (44°N) we obtained two profiles of the stratospheric NO2 mixing ratio. One, from 21 October 1982, agrees well with previous measurements. The other, from 8 October 1981, is lower by one order of magnitude. The few HO2 data obtained around 35 km altitude agree with previous measurements. An isolated measurement at 17 km altitude is one order of magnitude higher than the model predicted HO2 concentration.  相似文献   

2.
利用中尺度大气化学模式WRF/Chem对2013年3月6日华南地区一次平流层入侵事件及其对对流层低层臭氧的影响进行模拟研究。通过加入UBC（Upper Boundary Condition）上边界处理方案,弥补WRF/Chem模式未考虑平流层臭氧化学反应的不足。结合臭氧探空廓线资料、地面O3、CO、NOx、相对湿度、温度和风速等观测资料以及再分析资料对模拟结果进行定量评估,结果表明模式能较为真实地模拟本次平流层入侵过程。模拟分析进一步揭示:（1）副热带高空急流是本次平流层入侵的主要原因。当华南地区处在副热带急流入口区左侧下沉区域时,平流层入侵将富含臭氧的干燥空气输送到对流层中低层。（2）本次平流层入侵对对流层低层臭氧收支有重要影响,导致香港地区近地层臭氧体积混合比浓度明显上升,如塔门站夜间臭氧浓度升高21.3 ppb（1 ppb=1×10-9）。地面气象场和化学物种的分析进一步确认了平流层入侵的贡献。（3）采用动力学对流层顶高度时零维箱式模型和Wei公式计算得到的平流层入侵通量相当,分别为-1.42×10-3 kg m-2 s-1和-1.59×10-3 kg m-2 s-1,这一结果与前人研究相吻合,且与采用热力学对流层顶高度计算所得到的结果具有可比性。  相似文献   

3.
In July 1974 an NO/O3 chemiluminescent instrument was used to obtain measurements of NO in the stratosphere during two balloon flights launched from Churchill (59°N, 95°W). On the first flight, an altitude profile was obtained in which the NO volume mixing ratio was observed to increase from 0.3 to 2.7 ppbv between 19 and 29.5 km. On the second flight, the mixing ratio was observed to increase from 0.25 to 2.7 ppbv between 19 and 29 km and to remain almost constant at about 2.7 ppbv from 29 to 34.5 km. On this flight, the sunset decay of NO was also obtained while the payload was at a constant float altitude of 34.5 km. These decay measurements are compared satisfactorily with the results obtained from a time dependent stratospheric model.  相似文献   

4.
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5.
We outline how ground-based Fourier transform infrared (FTIR) measurements of stratospheric trace species, obtained with high temporal resolution, could be used to detect filaments of polar vortex air at mid-latitudes and therefore test high spatial resolution chemical transport models (CTMs). Vertical column abundances of HCl, ClONO2, HNO3, N2O and HF have been obtained from FTIR solar absorption measurements made throughout the day from Aberdeen, UK (57°N, 2°W) on several days during winter/spring 1993/94 and 1994/95. The short-timescale ( 2 hours) variability observed in the columns is attributed to real atmospheric variations and is often associated with the passage of high latitude air over Aberdeen. This is confirmed by 3D modelling studies which qualitatively reproduce and rationalise the observed changes in the column data on January 19 1994, January 20 1995 and February 26 1995. We describe the viewing geometry of ground-based FTIR measurements and we suggest a measurement strategy which should maximise the information retrieved on horizontal gradients in stratospheric trace species columns from FTIR measurements.  相似文献   

6.
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   

7.
Abstract

The importance of measurements of the vertical distribution of odd nitrogen in studies of ozone chemistry and climate change has long being recognized. In this paper, we use the optimal estimation method developed by Rodgers (1976, 1990) to retrieve NO2 vertical profiles from slant column observations made with a portable ultraviolet (UV)‐visible zenith‐sky spectrometer operated on the ground during the Middle Atmosphere Nitrogen TRend Assessment (MANTRA) balloon campaign carried out at Vanscoy, Saskatchewan, Canada (52°N, 107°W), from 18 to 25 August 1998. Late summer was chosen for the campaign because the stratospheric zonal wind velocity changes sign at that time. Under such conditions the stratospheric winds are at a minimum, leaving the stratosphere in a dynamically quiescent state and closer to photochemical control (Fahey et al., 2001; Fioletov and Shepherd, 2003). The NO2 profile retrieved from the ground‐based observations is compared with the co‐located and simultaneous NO2 profile measured by a balloon‐borne UV‐visible spectrometer during sunrise on 24 August. Good agreement is observed, giving us confidence in the retrieval technique adopted. The retrieved NO2 profiles are also compared with the output of the Model for Evaluating oZONe trends (MEZON) 3D stratospheric chemical transport model. It is observed that, for altitudes below the peak concentration, the model underestimates the NO2 amount, and at the altitude of peak concentration, the model values lie between the values measured from the balloon and those retrieved from the ground‐based measurements. Nevertheless, the model reproduces the general shape of the retrieved profiles, including the altitude of the NO2 maximum, for both sunrise and sunset conditions.  相似文献   

8.
Eleven vertical profiles of stratospheric NO3 have been obtained since 1992 using the AMON and SALOMON balloon-borne UV-visible spectrometers. The measurements are compared to the SLIMCAT 3D model and calculations based on the steady-state hypothesis for NO3. The calculations cannot reproduce some parts of the profiles which exhibit strong concentration fluctuations over few kilometres, as a consequence of the dependence of NO3 on local temperature variations. A statistical use of the data allows us to estimate the influence of the temperature dependence of the absorption cross-section on the data analysis, and the validity of the recommended reaction rates available in the literature. Discrepancies exist between the model based on recommended kinetics and observations at warmer temperatures. Nevertheless, the analysis is biased by local temperature inhomogeneities, and only a low-resolution vertical shape of the NO3 profiles can be retrieved.  相似文献   

9.
Results of a field experiment on studying solar radiation passing in the visible wavelength range are described with the model aerosol media created in the surface atmosphere. High-efficiency thermocondensation generators were used for creating model aerosol media. The index of refraction and an average size of the aerosol particles formed are close to those characteristic of the natural stratospheric aerosol. The composition and technical characteristics of the equipment complex used in the experiments to control aerosol optical and microphysical parameters and meteorological conditions of the experiment are considered. The Gaussian model of impurity dispersion in the boundary layer is used for the analysis and interpretation of measurement results. It is found that with a number concentration of aerosol particles of ～102–103 cm?3 (which corresponds to the aerosol density in the deposited layer of about 1–10 mg/m2 with the layer thickness along the ray path of about 100 m) the solar radiation attenuation with artificial aerosol layers accounts for 1 to 10%. Model estimates are in satisfactory agreement with the measurement results.  相似文献   

10.
Global distributions of carbonyl sulfide and carbon disulfide have been calculated with a three-dimensional global model of the atmospheric general circulation (ECHAM). The model calculates a global sink strength for carbonyl sulfide of 0.3 Tg S yr-1, with vegetation uptake being the largest sink. With this sink strength, the sources have to be close to the lower limit of the present estimate in the literature. The calculated mixing ratios are higher in the Southern Hemisphere than in the Northern Hemisphere. This interhemispheric gradient is the opposite of what is observed demonstrating that the present knowledge of the distribution of sinks and sources is not fully adequate. The model calculations support the idea that the open oceans could act as a net sink of carbonyl sulfide. The calculated stratospheric photolysis of carbonyl sulfide constitutes about 4% of the total sink of carbonyl sulfide. A stratospheric production of sulfate from carbonyl sulfide of 0.013 Tg S yr-1 is obtained, which is 3 to 12 times less than what is needed to maintain the stratospheric sulfate aerosol layer. Although these results are associated with uncertainties, due to the low upper boundary and coarse vertical resolution of the model, they support recent findings of a low stratospheric production of sulfate from carbonyl sulfide. Instead, sulfur dioxide transported from the troposphere is calculated to be the most important precursor for the stratospheric sulfate aerosol layer.  相似文献   

11.
The ozone budget inside the middle stratospheric polar vortex(24-36 km) during the 2002-2003 Arctic winter is studied by analyzing Michelson Interferometer for Passive Atmospheric Sounding(MIPAS) satellite data.A comprehensive global chemical transport model(Model for Ozone and Related Chemical Tracers,MOZART-3) is used to analyze the observed variation in polar vortex ozone during the stratospheric sudden warming(SSW) events.Both MIPAS measurement and MOZART-3 calculation show that a pronounced increase(26-28 DU) in the polar vortex ozone due to the SSW events.Due to the weakening of the polar vortex,the exchange of ozone mass across the edge of the polar vortex increases substantially and amounts to about 3.0× 107 kg according to MOZART-3 calculation.The enhanced downward transport offsets about 80% of polar vortex ozone mass increase by horizontal transport.A "passive ozone" experiment shows that only ～55% of the vertical ozone mass flux in February and March can be attributed to the variation in vertical transport.It is also shown that the enhanced downward ozone above ～32 km should be attributed to the springtime photochemical ozone production.Due to the increase of air temperature,the NOx reaction rate increases by 40%-80% during the SSW events.As a result,NOx catalytic cycle causes another 44% decrease in polar vortex ozone compared to the net ozone changes due to dynamical transport.It is also shown that the largest change in polar vortex ozone is due to horizontal advection by planetary waves in January 2003.  相似文献   

12.
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   

13.
A comprehensive model for the prediction of concentration fluctuations in plumes dispersing in the complex and highly disturbed wind flows in an urban environment is formulated. The mean flow and turbulence fields in the urban area are obtained using a Reynolds-averaged Navier-Stokes (RANS) flow model, while the standard k-ϵ turbulence model (k is the turbulence kinetic energy and ϵ is the viscous dissipation rate) is used to close the model. The RANS model provides a specification of the velocity statistics of the highly disturbed wind flow in the urban area, required for the solution of the transport equations for the mean concentration and concentration variance (both of which are formulated in the Eulerian framework). A physically-based formulation for the scalar dissipation time scale t d , required for the closure of the transport equation for , is presented. This formulation relates t d to an inner time scale corresponding to “internal” concentration fluctuation associated with relative dispersion, rather than an outer time scale associated with the entire portion of the fluctuation spectrum. The two lowest-order moments of concentration ( and ) are used to determine the parameters of a pre-chosen functional form for the concentration probability density function (clipped-gamma distribution). Results of detailed comparisons between a water-channel experiment of flow and dispersion in an idealized obstacle array and the model predictions for mean flow, turbulence kinetic energy, mean concentration, concentration variance, and concentration probability density function are presented.  相似文献   

14.
A short review is given of the different methods by which latent heat fluxes (or evaporation) over oceans are determined. In more detail, the applicability of the bulk aerodynamical formula is discussed. This formula is mainly used for climatological studies of heat fluxes and for the application of satellite data. As an example, for climatological studies we selected the work of Isemer and Hasse, who did a re-processing of the so-called Bunker data set to determine heat fluxes over the North Atlantic Ocean. In order to check their results, Isemer and Hasse calculated the annual mean heat budget for each latitudinal delt and derived from it the required ocean heat transport. With the aid of inverse modelling, the derived ocean transport was compared with the observed ocean transport and some of the used coefficients (e.g. bulk coefficients for latent and sensible heat flux) were altered. Though the ocean heat transport is changed by a large amount (at the equator 0.3 PW, original Bunker data; 0 PW, Isemer and Hasse; 0.76 PW, after inverse modelling (all northwards)) the overall patterns of the fields of the energy fluxes remain almost unchanged. The bulk coefficient for latent heat flux for example is altered by 5.6%.The geophysical parameters necessary for the bulk aerodynamic method can be determined from satellite observations: SST, q0, u0. Studies are described which used data from a microwave radiometer on SEASAT and NIMBUS7 to determine latent heat flux. An error calculation shows that the obtained accuracy is between 26 and 35 W m−2. This accuracy is adequate enough to allow reasonable estimates to be made of these fluxes. More satellites are planned for launch with microwave radiometers and scatterometers which will increase the possibility of determining geophysical parameters more accurately for use in the bulk aerodynamic formula. They will provide the database from which large-scale fieldsof latent heat flux (for time scales shorter than a month or even for actual situations) can be derived.  相似文献   

15.
To investigate an alternative technique of providing background and transboundary transport inputs for ozone (O3) simulations on a regional scale, the EPA’s Community Multi-scale Air Quality (CMAQ) model was integrated with high spectral resolution data from the Tropospheric Emission Spectrometer (TES) aboard the NASA’s Aura satellite. This study presents a comprehensive model evaluation of O3 for the entire year of 2009 over the contiguous United States with a focus on the State of Texas using both ozonesonde and ground measurements. While improving model performance in the upper atmosphere, CMAQ’s initial and boundary conditions (IC/BC) derived from the original TES data do not improve model performance in the troposphere because the satellite data exaggerated concentration of tropospheric O3. With a 10-ppb deduction of O3 concentration from TES, the IC/BC derived from the adjusted TES improves model performance from ground level through the upper atmosphere. The mean bias of daily maximum 8-h average concentration of O3 (MDA8) from the ground monitored in Texas decreased from 7 ppb to 4 ppb. Model results also show small influences of O3 from the upper troposphere on the concentrations at the ground level. With a complete exclusion of stratospheric layers, changes of annual mean MDA8 of O3 concentrations at ground-level were smaller than 1.1 % in Dallas and Houston. In addition, limitations of satellite data are discussed and recommendations are provided regarding the future application of satellite data in regional O3 simulations.  相似文献   

16.
SD-WACCM模式对平流层化学组分的模拟研究   总被引：3，自引：0，他引：3  
利用美国大气研究中心开发的全球气候模式,对2008年平流层的化学组分(HNO3、HCl和O3)进行了模拟研究,并结合了MLS卫星资料进行了对比分析。结果表明,模式可以较好地再现平流层的各化学组分的时空分布状况。并选取了8个区域,将模拟的2008—2009年O3柱浓度与臭氧监测仪资料对比,结果表明,模式可以较好地再现全球O3总量的季节变化情况。  相似文献   

17.
A mean meridional circulation model of the stratosphere, incorporating radiative heating and photochemistry of the oxygen‐hydrogen‐nitrogen atmosphere, is used to simulate the meridional distributions of O3, HOX, N2O,NOX, temperature and the three components of mean motion for the summer and winter seasons under steady‐state conditions. The results are generally in good agreement with the available observations in the normal stratosphere. The model has been applied to assess the effects of water vapour and nitrogen oxide perturbations resulting from aircraft emissions in the stratosphere. It is found that a fleet of 500 Boeing‐type sst's, flying at 20 km and 45°N in the summer hemisphere and inserting NOx at a rate of 1.8 megatons per year, has the effect of reducing the global total ozone by 14.7%. Similar calculations for 342 Concorde/TU‐114's, cruising at 17 km and injecting NOx at a rate of 0.35 megatons per year, show a global‐average total‐ozone reduction of 1.85%. Although water vapour is considered important, because of its ability to convert NO2 into HNO3, the direct effect on global‐average total‐ozone reduction resulting from the 100% increase in the stratospheric water content is less than 1%. The changes in the chemical structure (HO^NO^), temperature, and mean motions associated with the ozone reduction are also investigated in the case of the 1.8‐megaton‐per‐year NOX perturbation. It is shown that the reduced meridional temperature gradient in the middle and upper stratosphere resulting from the NOx perturbation leads to the weakening of the tropical easterly jet in the summer hemisphere and mid‐latitude westerlies in the winter season.

The sensitivity of the model solutions to an alternate choice of input parameters (diffusion coefficients and solar photodissociation data) is tested and the main deficiency of the model is pointed out.  相似文献   

18.
When modelling the turbulent dispersion of a passive tracer using Reynolds-averaged Navier–Stokes (RANS) simulations, two different approaches can be used. The first consists of solving a transport equation for a scalar, where the governing parameters are the mean velocity field and the turbulent diffusion coefficient, given by the ratio of the turbulent viscosity and the turbulent Schmidt number Sc t . The second approach uses a Lagrangian particle tracking algorithm, where the governing parameters are the mean velocity and the fluctuating velocity field, which is determined from the turbulence kinetic energy and the Lagrangian time T L . A comparison between the two approaches and wind-tunnel data for the dispersion in the wake of a rectangular building immersed in a neutral atmospheric boundary layer (ABL) is presented. Particular attention was paid to the influence of turbulence model parameters on the flow and concentration field. In addition, an approach to estimate Sc t and T L based on the calculated flow field is proposed. The results show that applying modified turbulence model constants to enable correct modelling of the ABL improves the prediction for the velocity and concentration fields when the modification is restricted to the region for which it was derived. The difference between simulated and measured concentrations is smaller than 25% or the uncertainty of the data on 76% of the points when solving the transport equation for a scalar with the proposed formulation for Sc t , and on 69% of the points when using the Lagrangian particle tracking with the proposed formulation for T L .  相似文献   

19.
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   

20.
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   

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