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1.
The impact of sulfate aerosol, ClOx and NOx perturbations for two different magnitudes of CH4 sources on lower stratospheric ozone is studied by using a heterogeneous chemical system that consists of 19 species belonging to 5 chemical families （oxygen, hydrogen, nitrogen, chlorine and carbon）. The results show that the present modeled photochemical system can present several different solutions, for instance, periodic states and multi-equilibrium states appearing in turn under certain parameter domains, through chlorine chemistry and nitrogen chemistry together with sulfate aerosol as well as the increasing magnitude of CH4 sources. The existence of catastrophic transitions could produce a dramatic reduction in the ozone concentration with the increase of external sources.  相似文献   

2.
The variability of Antarctic total column ozone in 1980–2018 is considered. The study analyzes trends in Antarctic total column ozone during the study period as well as the physical and chemical processes affecting the seasonal variability of total column ozone. The main attention is paid to the influence of dynamical processes on the stability of the Antarctic polar vortex, to the formation of polar stratospheric clouds, and to the influence of gas-phase and heterogeneous processes on the surface of polar stratospheric clouds and sulfate aerosol. The method of research is the analysis of the results of ground and satellite observations and numerical modeling of physical and chemical processes over the Antarctic using a global chemistry transport model with the dynamical parameters specified from reanalysis data.  相似文献   

3.
A detailed set of reactions treating the gas and aqueous phase chemistry of the most important iodine species in the marine boundary layer (MBL) has been added to a box model which describes Br and Cl chemistry in the MBL. While Br and Cl originate from seasalt, the I compounds are largely derived photochemically from several biogenic alkyl iodides, in particular CH2I2, CH2ClI, C2H5I, C3H7I, or CH3I which are released from the sea. Their photodissociation produces some inorganic iodine gases which can rapidly react in the gas and aqueous phase with other halogen compounds. Scavenging of the iodine species HI, HOI, INO2, and IONO2 by aerosol particles is not a permanent sink as assumed in previous modeling studies. Aqueous-phase chemical reactions can produce the compounds IBr, ICl, and I2, which will be released back into the gas phase due to their low solubility. Our study, although highly theoretical, suggests that almost all particulate iodine is in the chemical form of IO-3. Other aqueous-phase species are only temporary reservoirs and can be re-activated to yield gas phase iodine. Assuming release rates of the organic iodine compounds which yield atmospheric concentrations similar to some measurements, we calculate significant concentrations of reactive halogen gases. The addition of iodine chemistry to our reaction scheme has the effect of accelerating photochemical Br and Cl release from the seasalt. This causes an enhancement in ozone destruction rates in the MBL over that arising from the well established reactions O(1D) + H2O 2OH, HO2 + O3 OH + 2O2, and OH + O3 HO2 + O2. The given reaction scheme accounts for the formation of particulate iodine which is preferably accumulated in the smaller sulfate aerosol particles.  相似文献   

4.
1.IntroductionMethane(CH#)isanimportantgreenhousegasinatmosphere.ThemainremovalprocessofCH4inatmosphereisreactedwithOHwhichisdeterminedbytheabundanceofmethane,carbonmonoxide(CO)andnitrousoxides(NO.)whoseemissionshaveincreasedgreatlybecauseofhumanacti...  相似文献   

5.
A modelling platform for studying photochemical gaseous and aerosol phase processes from localized (e.g., point) sources has been presented. The current approach employs a reactive plume model which extends the regulatory model RPM‐IV by incorporating aerosol processes and heterogeneous chemistry. The physics and chemistry of elemental carbon, organic carbon, sulfate, nitrate, ammonium material of aerosols are treated and attributed to the PM size distribution. A modified version of the carbon bond IV chemical mechanism is included to model the formation of organic aerosol. Aerosol dynamics modeled include mechanisms of nucleation, condensation, dry deposition and gas/particle partitioning of organic matter. The model is first applied to a number of case studies involving emissions from point sources and sulfate particle formation in plumes. Model calculations show that homogeneous nucleation is an efficient process for new particle formation in plumes, in agreement with previous field studies and theoretical predictions. In addition, the model is compared with field data from power plant plumes with satisfactory predictions against gaseous species and total sulphate mass measurements. Finally, the plume model is applied to study secondary organic matter formation due to various emission categories such as vehicles and the oil production sector.  相似文献   

6.
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   

7.
In recent years there has been increasing concern with the possibility that man's terrestrial economic activities of production, distribution, and consumption contribute pollutants to the environment in sufficient quantities to upset naturally existing chemical equilibria in the atmosphere. Such inadvertent anthropogenic phenomena have become associated with possible changes in climate (temperature, precipitation, and ultraviolet radiation) whose long term consequences may be serious, if not disastrous. Among other societal reactions to this problem, proposals for various environment monitoring systems have been proffered. Such systems, often envisioned as satellite-based, are costly and their benefits often appear largely intangible. In this research we develop a general methodology for identifying and estimating the economic benefits of environment monitoring systems, and we apply the methodology to the cases of stratospheric ozone depletion and aerosol accumulation. The research synthesizes numerous recent efforts in atmospheric chemistry, climatology, engineering, policy analysis, and primarily economic cost benefit analysis. We find that over a broad range of alternative assumptions and parameter choices, the present value of the economic benefits of an ozone/aerosol monitoring system in the range of $0.5 to $2,0 billion. Somewhat surprisingly, the higher values are associated with the smaller deleterious ozone/aerosol atmospheric trends. This work was partially supported by contract NASI-14351 with NASA's Langley Research Center.  相似文献   

8.
1.IntroductionAgreatchangehastakenplaceinglobalatmosphericchemicalcompositionbecauseofhumanactivitiessinceindustrialrevolution.Numericalsimulationisaneffectivetooltostudythechangeoftracegases.Inthelasttwentyyears,two--dimensionalchemical/transportmodelshavebeenextensivelydevelopedtosimulatethedistributionsoftracers(GidelandCrutzen,1983;Hough,1991;LawandPyle1993).Inordertopredictthefuturepossiblechangesofatmosphericspecies,itisnecessarytohaveabetterunderstandingofprocessessuchasemission,trans…  相似文献   

9.
《大气与海洋》2013,51(4):283-299
Abstract

The Middle Atmosphere Nitrogen TRend Assessment (MANTRA) series of high‐altitude balloon flights is being undertaken to investigate changes in the concentrations of northern hemisphere mid‐latitude stratospheric ozone, and of nitrogen and chlorine compounds that play a role in ozone chemistry. Four campaigns have been carried out to date, all from Vanscoy, Saskatchewan, Canada (52°01'N, 107°02'W, 511.0 m). The first MANTRA mission took place in August 1998, with the balloon flight on 24 August 1998 being the first Canadian launch of a large high‐altitude balloon in about fifteen years. The balloon carried a payload of instruments to measure atmospheric composition, and made measurements from a float altitude of 32–38 km for one day. Three of these instruments had been flown on the Stratoprobe flights of the Atmospheric Environment Service (now the Meteorological Service of Canada) in the 1970s and early 1980s, providing a link to historical data predating the onset of mid‐latitude ozone loss.

The primary measurements obtained from the balloon‐borne instruments were vertical profiles of ozone, NO2, HNO3, HCl, CFC‐11, CFC‐12, N2O, CH4, temperature, and aerosol backscatter. Total column measurements of ozone, NO2, SO2, and aerosol optical depth were made by three ground‐based spectrometers deployed during the campaign. Regular ozonesonde and radiosonde launches were also conducted during the two weeks prior to the main launch in order to characterize the local atmospheric conditions (winds, pressure, temperature, humidity) in the vicinity of the primary balloon flight. The data have been compared with the Model for Evaluating oZONe Trends (MEZON) chemical transport model, the University of California at Irvine photochemical box model, and the Canadian Middle Atmosphere Model (CMAM) to test our current understanding of model photochemistry and mid‐latitude species correlations. This paper provides an overview of the MANTRA 1998 mission, and serves as an introduction to the accompanying papers in this issue of Atmosphere‐Ocean that describe specific aspects and results of this campaign.  相似文献   

10.
Understanding the chemical links between ozone (O3) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O3/NOy and O3/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.  相似文献   

11.
地球系统模式是研究全球气候与生态环境变化问题的重要工具，气溶胶与大气化学模式负责为其中的大气环流模式提供与气候效应有关的气态化学物质和气溶胶成分。本文在全球嵌套网格空气质量预报模式系统的基础上发展了一个适用于中国科学院地球系统模式（CAS-ESM）耦合计算的气溶胶与大气化学分量模式（IAP-AACM），采用简化的气相化学机制，不仅考虑了人为气溶胶，同时考虑了海盐、沙尘和二甲基硫等自然气溶胶及其前体物的在线排放。评估结果表明，IAP-AACM氧化剂插值计算可靠，采用简化机制和碳键机制（CBM-Z）模拟的差异较小。和观测的对比表明，得益于CAS-ESM的气溶胶双向反馈作用，简化版能够较好地抓住气溶胶及其前体物的空间分布，为IAP-AGCM提供可靠的气溶胶模拟。另外，简化版能大幅提升计算效率，满足CAS-ESM耦合长期积分的需求。为了在全球气候变化的研究中提供更完善的气溶胶模拟，未来考虑在IAP-AACM中增加氮化学和臭氧平流层化学机制。  相似文献   

12.
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   

13.
The interactively coupled chemistry-climate model ECHAM4.L39(DLR)/CHEM is employed in sensitivity calculations to investigate feedback mechanisms of dynamic, chemical, and radiative processes. Two multi-year model simulations are carried out, which represent recent atmospheric conditions. It is shown that the model is able to reproduce observed features and trends with respect to dynamics and chemistry of the troposphere and lower stratosphere. In polar regions it is demonstrated that an increased persistence of the winter vortices is mainly due to enhanced greenhouse gas mixing ratios and to reduced ozone concentration in the lower stratosphere. An additional sensitivity simulation is investigated, concerning a possible future development of the chemical composition of the atmosphere and climate. The model results in the Southern Hemisphere indicate that the adopted further increase of greenhouse gas mixing ratios leads to an intensified radiative cooling in the lower stratosphere. Therefore, Antarctic ozone depletion slightly increases due to a larger PSC activity, although stratospheric chlorine is reduced. Interestingly, the behavior in the Northern Hemisphere is different. During winter, an enhanced activity of planetary waves yields a more disturbed stratospheric vortex. This "dynamical heating" compensates the additional radiative cooling due to enhanced greenhouse gas concentrations in the polar region. In connection with reduced stratospheric chlorine loading, the ozone layer clearly recovers.  相似文献   

14.
Abstract

An important objective of middle atmosphere global climate modelling is the development of the capability of predicting the response of the middle atmosphere to natural or anthropogenic perturbations. To achieve this, a comprehensive chemistry package interactively coupled with radiative and dynamical modules is required. This paper presents preliminary results obtained with a photochemistry module which has been incorporated in the Canadian Middle Atmosphere Model (CMAM). The module contains 42 species including necessary oxygen, hydrogen, nitrogen, chlorine, bromine and methane oxidation cycle species. Photochemical balance equations are solved on‐line throughout the middle atmosphere at every dynamical time step. A full diurnal cycle is simulated with photolysis rates provided by a look‐up table. The chemistry solver is a mass conserving, fully implicit, backward difference scheme which currently uses less than 10% of the GCM run time. We present the results obtained from short integrations and compare them with UARS measurements. The model ozone distribution appears in quantitative agreement with observations showing peak values near 10 ppmv and confined to the 35‐km region. The abundance of nitrogen, chlorine, bromine oxides and their respective contributions to the overall ozone budget is realistic. The study illustrates the capability of the model to simulate middle atmosphere photochemistry for the disparate conditions occurring throughout the region.  相似文献   

15.
In this paper the bromine family and radiative effects are considered in an updated box model under the framework of ozone-temperature feedback,in order to further analyze the possible behavior of atmospheric ozone in the lower mid-latitude stratosphere.Results show that this updated photochemical system can present several different solutions,within a certain domain of parameters,with fixed-point and periodic states appearing in turn.The temperature feedback effect introduced in this box model has not changed the topology of the ozone system.This result presents nonlinear characteristics of the ozone system,and possible trends in the stratospheric atmosphere between complex chemistry and radiation processes.  相似文献   

16.
Terry Deshler   《Atmospheric Research》2008,90(2-4):223-ICNAA07
Stratospheric aerosol, noted after large volcanic eruptions since at least the late 1800s, were first measured in the late 1950s, with the modern continuous record beginning in the 1970s. Stratospheric aerosol, both volcanic and non-volcanic are sulfuric acid droplets with radii (concentrations) on the order of 0.1–0.5 µm (0.5–0.005 cm− 3), increasing by factors of 2–4 (10–103) after large volcanic eruptions. The source of the sulfur for the aerosol is either through direct injection from sulfur-rich volcanic eruptions, or from tropical injection of tropospheric air containing OCS, SO2, and sulfate particles. The life cycle of non-volcanic stratospheric aerosol, consisting of photo-dissociation and oxidation of sulfur source gases, nucleation/condensation in the tropics, transport pole-ward and downward in the global planetary wave driven tropical pump, leads to a quasi steady state relative maximum in particle number concentration at around 20 km in the mid latitudes. Stratospheric aerosol have significant impacts on the Earth's radiation balance for several years following volcanic eruptions. Away from large eruptions, the direct radiation impact is small and well characterized; however, these particles also may play a role in the nucleation of near tropopause cirrus, and thus indirectly affect radiation. Stratospheric aerosol play a larger role in the chemical, particularly ozone, balance of the stratosphere. In the mid latitudes they interact with both nitrous oxides and chlorine reservoirs, thus indirectly affecting ozone. In the polar regions they provide condensation sites for polar stratospheric clouds which then provide the surfaces necessary to convert inactive to active chlorine leading to polar ozone loss. Until the mid 1990s the modern record has been dominated by three large sulfur-rich eruptions: Fuego (1974), El Chichón (1982) and Pinatubo (1991), thus definitive conclusions concerning the trend of non-volcanic stratospheric aerosol could only recently be made. Although anthropogenic emissions of SO2 have changed somewhat over the past 30 years, the measurements during volcanically quiescent periods indicate no long term trend in non-volcanic stratospheric aerosol.  相似文献   

17.
Near-total depletions of ozone have been observed in the Arctic spring since the mid 1980s. The autocatalytic reaction cycles involving reactive halogens are now recognized to be of main importance for ozone depletion events in the polar boundary layer. We present sensitivity studies using the model MISTRA in the box-model mode on the influence of chemical species on these ozone depletion processes. In order to test the sensitivity of the chemistry under polar conditions, we compared base runs undergoing fluxes of either Br2, BrCl, or Cl2 to induce ozone depletions, with similar runs including a modification of the chemical conditions. The role of HCHO, H2O2, DMS, Cl2, C2H6, HONO, NO2, and RONO2 was investigated. Cases with elevated mixing ratios of HCHO, H2O2, DMS, Cl2, and HONO induced a shift in bromine speciation from Br / BrO to HOBr/HBr, while high mixing ratios of C2H6 induced a shift from HOBr/HBr to Br/BrO. The shifts from Br/BrO to HOBr/HBr accelerated the aerosol debromination, but also increased the total amount of deposited bromine at the surface (mainly via increased deposition of HOBr). For all NOy species studied (HONO, NO2, RONO2) the chemistry is characterized by an increased bromine deposition on snow reducing the amount of reactive bromine in the air. Ozone is less depleted under conditions of high mixing ratios of NOx. The production of HNO3 led to the acid displacement of HCl, and the release of chlorine out of salt aerosol (Cl2 or BrCl) increased.  相似文献   

18.
The objective of this study is to present differences in the variability of observed and ozone-mixing ratios simulated by a three-dimensional atmospheric chemical model using two chemical mechanisms. In this study the Comprehensive Air Quality Model with Extensions is used to make ozone simulations with the Carbon Bond mechanism, versions 4 and 5. The Paso del Norte region is used as a test-bed for these simulations. The shared variance between the simulations and measurements is typical for air quality models ranging from 0.51 to 0.86 for both mechanisms. The smallest mean normalized gross error is about 31 % with CB4 but the normalized bias is over 30 % as well. Boundary conditions, emissions and other factors affect the levels of ozone of the simulated mixing ratios and therefore error and bias but these factors have a much less affect on the simulated ozone variability. The differences in the ozone variability of the measurements and the simulations are very large and different for the two chemical mechanisms. There are many more instances of low ozone mixing ratios in the measurements than in the simulated ozone. One possible explanation is that these differences are due to problems associated with comparing point measurements with grid averages. A more disturbing possibility is that the bias could be due to the procedures used in the development and testing of air quality modeling systems. Air quality mechanisms are evaluated against environmental chamber data where the chemistry occurs at high concentrations and this may lead to a systematic positive bias in ozone simulations.  相似文献   

19.
利用MLS卫星资料和ERA-Interim再分析资料,比较了青藏高原和北美夏季臭氧谷的垂直结构和形成机制。结果如下:青藏高原夏季臭氧谷在垂直方向上存在两个低值中心,一个中心位于对流层顶附近,强度约为-15 DU,形成原因主要为水平幅散,另一个中心位于上平流层,强度约为-1 DU,形成原因可能为光化学反应参与的氯自由基的催化损耗。北美夏季臭氧谷仅存在一个低值中心,位于对流层顶附近,该中心强度约为-5 DU,其形成的主要原因是水平辐散。  相似文献   

20.
1992年大气甲烷增长速率异常 下降的模拟研究   总被引：4，自引：0，他引：4  
张仁健  王明星 《大气科学》2000,24(3):355-362
应用初步建立的全球二维大气化学模式,模拟了甲烷、一氧化碳和OH自由基自工业革命以来的长期变化,对1992年大气中甲烷增长速率突然下降这一异常现象的可能原因如平流层O3下降,皮纳图博火山引起对流层温度下降、甲烷排放源减少等逐一进行了定量研究。研究还发现一氧化碳排放源的减少是另一重要影响因子,并进行了验证。结果表明,1992年甲烷增长速率急剧下降的主要原因来自甲烷和一氧化碳排放源的减少。  相似文献   

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