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1.
李冰  刘小红  洪钟祥 《大气科学》2001,25(2):260-268
利用一个三维的冰雹云模式与化学组分输送模块耦合，得到云输送引起大气光化学组分的再分布，然后用一个包含详细气相化学反应机制的箱模式研究了云输送引起的气相体积分数的变化及其对大气化学系统产生的影响。结果表明，云输送后O3体积分数大于无云个例，但其后两天内两者的变化趋势相差不大；HNO3、NO2、NO3、PAN等的体积分数均明显高于无云个例，分别增长了87％、70％、62％和49％，其中NO2体积分数的增加主要由于云输送造成，而NO3、HNO3、PAN主要是输送对化学扰动的结果。两天内OH和HO2自由基体积分数比无云个例平均增长了13％和11％。  相似文献   

2.
The Model of Multiphase Cloud Chemistry M2C2 has recently been extended to account for nucleation scavenging of aerosol particles in the cloud water chemical composition. This extended version has been applied to multiphase measurements available at the Puy de Dôme station for typical wintertime anthropogenic air masses. The simulated ion concentrations in cloud water are in reasonable agreement with the experimental data. The analysis of the sources of the chemical species in cloud water shows an important contribution from nucleation scavenging of particles which prevails for nitrate, sulphate and ammonium. Moreover, the simulation shows that iron, which comes only from the dissolution of aerosol particles in cloud water, has a significant contribution in the hydroxyl radical production. Finally, the simulated phase partitioning of chemical species in cloud are compared with measurements. Numerical results show an underestimation of interstitial particulate phase fraction with respect to the measurements, which could be due to an overestimation of activated mass by the model. However, the simulated number scavenging efficiency of particles agrees well with the measured value of 40% of total number of aerosol particles activated in cloud droplets. Concerning the origin of chemical species in cloud water, the model reproduces quite well the contribution of gas and aerosol scavenging estimated from measurements. In addition, the simulation provides the contribution of in-cloud chemical reactivity to cloud water concentrations.  相似文献   

3.
During March and April of 1995 a major international field project was conducted at the UMIST field station site on Great Dun Fell in Cumbria, Northern England. The hill cap cloud which frequently envelopes this site was used as a natural flow through reactor to examine the sensitivity of the cloud microphysics to the aerosol entering the cloud and also to investigate the effects of the cloud in changing the aerosol size distribution, chemical composition and associated optical properties. To investigate these processes, detailed measurements of the cloud water chemistry (including the chemistry of sulphur compounds, organic and inorganic oxidised nitrogen and ammonia), cloud microphysics and properties of the aerosol and trace gas concentrations upwind and downwind of the cap cloud were undertaken. It was found that the cloud droplet number was generally strongly correlated to aerosol number concentration, with up to 2000 activated droplets cm−3 being observed in the most polluted conditions. In such conditions it was inferred that hygroscopic organic compounds were important in the activation process. Often, the size distribution of the aerosol was substantially modified by the cloud processing, largely due to the aqueous phase oxidation of S(IV) to sulphate by hydrogen peroxide, but also through the uptake and fixing of gas phase nitric acid as nitrate, increasing the calculated optical scattering of the aerosol substantially (by up to 24%). New particle formation was also observed in the ultrafine aerosol mode (at about 5 nm) downwind of the cap cloud, particularly in conditions of low total aerosol surface area and in the presence of ammonia and HCl gases. This was seen to occur at night as well as during the day via a mechanism which is not yet understood. The implications of these results for parameterising aerosol growth in Global Climate Models are explored.  相似文献   

4.
欧拉型区域硫沉降模式研究   总被引：10，自引：3，他引：10       下载免费PDF全文
建立了一个三维硫沉降欧拉模式，模式中比较全面地考虑了硫沉降过程中的物理、化学机制。包括平流、扩散、干湿沉降和积云的垂直输送作用等物理过程，气相化学、液相化学和气溶胶表面的非均相化学等化学过程。其中非均相化学和积云的垂直输送参数化在国内外同类模式中尚不多见。模式结果与实测及其他模式结果的对比表明，该模式能够较好地模拟出SO2的水平和垂直分布及SO2-4在降水中的浓度。  相似文献   

5.
The authors quantify the impacts of sulfate and nitrate aerosol formation on surface-layer 03 concentrations over China using the one-way nested-grid capa- bility of the global three-dimensional Goddard Earth Ob- serving System chemical transport model （GEOS-Chem）. Chemical reactions associated with sulfate formation are simulated to generally increase 03 concentrations in China. Over the North China Plain （NCP） and the Si- chuan Basin （SCB）, where simulated sulfate concentra- tions are the largest, ozone concentrations show maximum increases in spring by 1.8 ppbv （3.2%） in the NCP and by 2.6 ppbv （3.7%） in the SCB. On the contrary, nitrate formation is simulated to reduce 03 concentrations by up to 1.0 ppbv in eastern China, with the largest reduc- tions of 1.0 ppbv （1.4%） in summer over the NCE Ac- counting for the formation of both sulfate and nitrate, the surface-layer O3 concentrations over a large fraction of eastern China are simulated to increase in winter, spring, and autumn, dominated by the impact of sulfate forma- tion, but to decrease in summer because of the dominant contribution from nitrate formation.  相似文献   

6.
Model calculations and field measurements have shown that when air masses accumulate emissions of hydrocarbons and nitrogen oxides from sources in continental Europe and then move towards Scandinavia without any synoptic scale break-up of the atmospheric boundary layer (e.g. frontal passages), elevated PAN concentrations in southern Norway or Sweden in the range 1–5 ppb may be caused by long-range transport. The model calculations showed that over sea, the persistence of PAN was comparable to that of ozone in an ageing air mass when the temperatures were fairly low (5–10°C). At higher temperatures the thermal decomposition of PAN made the compound less persistent than ozone. Over land, the situation may be different since the ground removal is typically three times more efficient for ozone than for PAN.According to the model, the concentration of PAN did not change very much when an ageing air mass was exposed to moderate emissions of hydrocarbons, nitrogen oxides, or both. The concentration of PAN decreased less than the concentration of ozone when an ageing air mass was exposed to high emissions of nitrogen oxides.  相似文献   

7.
齐彦斌  冉令坤  洪延超 《气象学报》2009,67(6):1045-1057
大气动力学中"平流输送"是非常重要的宏观动力学过程,云凝结物的平流输送与降水云系的发展演变密切相关,它把宏观动力过程与各种云凝结物粒子的时空演变联系起来,云凝结物的平流输送可以增加或减少局地大气中云凝结物的含量,改变云凝结物的空间分布状况,影响云凝结物的微观物理过程,进而促进或抑制降水云系的发展演变.本文在数值模拟研究中.通过改变云凝结物平流输送的状况来研究宏观动力过程对云微观物理过程的影响,因而利用ARPS模式开展3个分别排除云凝结物水平平流输送、垂直平流输送和三维平流输送的敏感试验,进行关于云凝结物平流输送对降水云系发展演变影响的敏感性数值模拟研究.结果表明,云凝结物的平流输送对水汽比湿的影响很小.云凝结物的三维平流输送有利于增加降水云系中雪和霰的混合比含量,抑制云水、雨水和云冰混合比含量的增长.云凝结物的水平平流输送可以降低降水云系中云水和雨水的混合比含量,增加云冰和雪的混合比含量;云凝结物垂直平流输送的作用是增加降水云系中雨水、雪和霰的混合比含量,减少云与冰混合比含量.云凝结物三维平流输送效应的分析表明,云凝结物的三维平流输送主要通过调整云凝结物的微物理过程源汇项以及降水粒子(雨水、雪和霰)的下落末速项来改变降水云系中云凝结物的垂直结构;另外,雪的三维平流输送对雪本身的分布也有一定影响.  相似文献   

8.
Large-eddy simulations of an evolving cloud field are used to investigate the contribution of microphysical processes to the evolution of the variance of total water and liquid water potential temperature in the boundary layer. While the first hours of such simulations show a transient behaviour and have to be analyzed with caution, the final portion of the simulation provides a quasi-equilibrium situation. This allows investigation of the budgets of the variances of total water and liquid water potential temperature and quantification of the contribution of several source and sink terms. Accretion is found to act as a strong sink for the variances, while the contributions from the processes of evaporation and autoconversion are small. A simple parametrization for the sink term connected to accretion is suggested and tested with a different set of simulations.  相似文献   

9.
春季中国东部气溶胶化学组成及其分布的模拟研究   总被引：2，自引：0，他引：2  
本文利用区域空气质量模式RAQMS（Regional Air Quality Model System）,对2009年春季中国东部气溶胶主要化学成分及其分布进行了模拟研究。与泰山站观测资料的对比结果显示,模式能比较合理地反映气溶胶浓度的逐日变化特征。整体上,模式对无机盐气溶胶的模拟好,分别高估和低估黑碳和有机碳气溶胶浓度,其原因与排放源、二次有机气溶胶化学机制和模式分辨率的不确定性有关。模拟结果显示,春季气溶胶浓度高值主要集中于华北、四川东部、长江中下游等地区。受东南亚生物质燃烧和大气输送的影响,中国的云南和广西等地区有机碳浓度高于中国其他地区。中国西北部沙尘浓度较高,而且向东输送并影响到中国东部和南方部分地区。中国东部的华北、四川东部、长江中下游等地PM2.5（空气动力学直径在2.5微米以下的颗粒物）污染严重,4月平均PM2.5浓度超过了我国日平均PM2.5浓度限值。中国东部泰山站的观测和模拟结果都显示近地面硝酸盐浓度超过硫酸盐,中国北部对流层中硝酸盐的柱含量也大于硫酸盐,而在中国南部则相反,这一方面与春季中国云量 南多北少的分布特征以及云内液相化学反应有关,另一方面也与南北温差对气溶胶形成的影响有关。就整个中国东部而言,虽然硫酸盐的柱含量（46 Gg）仍大于硝酸盐（42 Gg）,但比较接近,反映出我国氮氧化物排放迅速增加的趋势。春季中国地区对流层中PM10（空气动力学直径在10微米以下的颗粒物）及其化学成分柱含量分别为:990.8 Gg（PM10）,52.6 Gg（硫酸盐）,48.2 Gg（硝酸盐）,32.1 Gg（铵盐）,22.9 Gg（黑碳）和74.1 Gg（有机碳）,有机碳（OC）中一次有机碳（POC）和二次有机碳（SOC）分别占60%和40%,中国东部PM10中人为气溶胶和沙尘分别占30%和70%,反映了春季沙尘对我国大气气溶胶的重要贡献。  相似文献   

10.
A chemical module describing the tropospheric photochemistry of ozone precursors in both gaseous and aqueous phases for a remote continental atmosphere has been developed within the framework of a two-dimensional cloud model. Dynamical, microphysical and chemical processes are fully interacting in order to study the influence of clouds on ozone chemistry and to quantify the relative importance of the different processes on the budget and evolution of 12 chemical species. Whereas the concentrations of highly soluble species are strongly affected by evaporation and sedimentation, less soluble species are affected primarily by accretion. The model reproduces previously observed chemical phenomena such as the enrichment of formic acid at the top of the cloud.  相似文献   

11.
During two measuring campaigns in early spring 1994 and 1995 (March/April) and one campaign in summer 1994, measurements of ozone, PAN, sulfur dioxide, nitric acid, and particulate nitrate, sulfate, and ammonium (only 1995) were recorded in the Arctic. Observations were made by aircraft at various sites in the eastern and western Arctic. Ozone concentrations showed a steady increase with altitude both in spring and summer. During five flights in springtime, low ozone events (LOEs) could be observed near the surface and up to altitudes of 2000 m. SO2 background concentrations, ranging from detection limit (0.5 nmol/m3) to 5 nmol/m3, were observed during both spring and summer. Distinct maxima up to 55 nmol/m3 in lower altitudes were only obtained in springtime. Concentrations of the organic nitrate PAN were within a similar range as those of the inorganic nitrate HNO3 during spring campaigns. In contrast, concentrations of particulate nitrate were one half an order of magnitude lower. HNO3 concentrations increased significantly with altitude. Evidently, HNO3 was intruded from the stratosphere into the troposphere. Sulfate concentrations ranged between 5 and 30 nmol/m3; ammonium concentrations were obtained within a range from 10 to 50 nmol/m3.  相似文献   

12.
夹卷对郊外大气边界层内臭氧影响的数值模拟研究   总被引：3，自引：2，他引：3  
夹卷是大气边界层与自由大气进行能量和物质交换的重要途径,对边界层动力结构及边界层内温度、水汽和各种污染物浓度有重要影响。利用化学-地表-大气-土壤(CLASS)模式定量评估了夹卷过程对远郊地区大气边界层内臭氧（O3）浓度的影响并与大气化学反应贡献进行了对比,结合地面O3、NOx及边界层高度、位温和比湿等观测资料和再分析资料对CLASS模拟结果进行了定量评估。结果表明:CLASS模式能较为真实地模拟夹卷和大气光化学反应对远郊地区大气边界层臭氧浓度的影响,且当自由大气层内臭氧浓度达到一定值时,两者对边界层内臭氧峰值影响相当。数值试验结果进一步揭示,夹卷对控制氮氧化物（NOX）和可挥发性有机物(VOCS)排放源控制效果有重要影响,且当夹卷区内O3跳跃值增大到一定时,可完全抵消源排放减排控制的效果。本研究旨在表明,为有效控制近地层臭氧浓度,在制定人为污染源减排措施时必须考虑自由大气层臭氧的夹卷贡献。   相似文献   

13.
Apparent moisture sink and water vapor transport flux are calculated by using NCAR/NCEP reanalyzed daily data for water vapor and wind fields at various levels from 1980 to 1989. With the aid of EOF analysis method, temporal and spatial characteristics of moisture budgets over Asian and Australian monsoon regions are studied. The results show that there is apparent seasonal transition of moisture sink and water vapor transport between Asian monsoon region and Australian monsoon region. In winter, the Asian monsoon region is a moisture source, in which three cross-equatorial water vapor transport channels in the "continent bridge". at 80°E and 40°E ～ 50°E transport water vapor to the Australian monsoon region and southern Indian Ocean which are moisture sinks. In summer, Australian monsoon region and southern Indian Ocean are moisture sources and by the three cross-equatorial transport channels water vapor is transport to the Asian monsoon region which is a moisture sink. In spring and autumn, ITCZ is the main moisture sink and there is no apparent water vapor transport between Asian monsoon region and Australian monsoon region.  相似文献   

14.
深对流云输送对于对流层O3、NOx在分析的作用   总被引：4，自引：0，他引：4  
利用一个冰雹云模式与云化学输送模块耦合而成的三维对流云化学／输送模式, 研究对流云对重要的大气污染物臭氧 （Ｏ３）、氮氧化物 （ＮＯｘ, 包括ＮＯ 和ＮＯ２） 的输送作用。模式较好地体现了一个单体积云的发展过程及其特征。云化学／输送模式的结果表明, 云内强烈的垂直输送能在３０ ｍ ｉｎ 左右, 把低层低体积分数的Ｏ３和高体积分数的ＮＯ２快速、有效地输送到对流层的上部, 造成化学物种的再分布。而在云顶附近, 由于对流穿透了对流层的顶部,造成了上层高体积分数Ｏ３的向下侵入,说明云的对流活动除了能把边界层内的污染物向上输送, 其夹卷作用还可以造成平流层和对流层化学物质的交换。  相似文献   

15.
This study simulates optical depth of marine warm clouds for year 2001 based on interactively predicted aerosol concentrations with a global chemical transport model (CTM) driven by the ERA-40 re-analysis meteorological data. The simulated aerosol and cloud droplet number concentrations (CDNC) largely reproduce the variations between polluted and pristine marine environment as revealed by surface and aircraft measurements. By constraining cloud liquid water path (CLWP) with satellite microwave measurements, the simulated global and southern hemispheric aerosol optical depth (AOD) and cloud optical depth (COD) are well within 10% of the observed values. As a result of larger anthropogenic aerosol loadings over the northern oceans, the simulated CDNC and COD are, respectively, by 51 and 18% higher than those over the southern oceans, while the column-averaged droplet effective radius is 13% smaller. These simulated interhemispheric differences, while qualitatively consistent with satellite observations, are larger than the observations. Inclusion of drizzle effect improved the disparities but not entirely. The constrained CTM generally captures the seasonality in AOD and CLWP observations, and demonstrates that annual cycle of COD is dominated by CLWP. During winter monsoon the simulated and observed COD correlate more strongly with changes in AOD over the N. Indian Ocean.  相似文献   

16.
A convective cloud transport model, without chemical processes, is developed by joining a set of concentration conservative equations into a two-dimensional, slab-symmetric and fully elastic numerical cloud model, and a numerical experiment is completed to simulate the vertical transport of ground-borne, inert gaseous pollutant by deepthunderstorm. The simulation shows that deep convective storm can very effectively transport high concentrated pollutant gas from PBL upward to the upper troposphere in 30 to 40 minutes, where the pollutant spreads laterally outward with strong anvil outflow, forming an extensive high concentration area. Meanwhile, relatively low concentration areas are formed in PBL both below and beside the cloud, mainly caused by dynamic pumping effect and sub-cloud downdraft flow. About 80% of the pollutant gas transported to the upper troposphere is from the layer below 1.5 km AGL (above ground level).  相似文献   

17.
A new detailed multiphase halogen mechanism, the CAPRAM Halogen Module 2.0 (HM2), has been developed and coupled to the multiphase chemistry mechanism RACM-MIM2ext/CAPRAM 3.0n. The overall mechanism comprises 1,705 reactions including 595 reactions of the HM2. Halogen chemistry box model studies have been, for the first time, performed with a non-permanent cloud scenario for pristine open ocean regions in mid-latitudes. Moreover, detailed time-resolved reaction flux analysis has been used to investigate the multiphase halogen reaction cycles in more detail. Clouds significantly change the multiphase halogen chemical system and new reaction cycles are proposed for in-cloud conditions. While most gas phase concentrations are decreased for chlorine and iodine species, they are increased for bromine. Flux analyses determined the relative contributions of the methylene dihalides CH2IX (X = Cl, Br, I) as the main I atom source with a contribution of about 80 % to the total iodocarbon sources. Furthermore, HOI was confirmed to be important for chlorine activation. It is shown that 25 % of the ozone loss can be attributed to halogens. VOC oxidation by halogens is important as halogens account for about 20 % of the methane oxidation and up to 80 % of the oxidation of other VOCs. In other cases, enhanced VOC and VOC oxidation product concentration levels were found. For example, 15 % of the methyl peroxyl radicals are formed after the reaction of chlorine atoms with methane or methyl hydroperoxide. In the aqueous phase, changes in the oxidation of organics do only occur for highly oxidised organics without a C-H bond. For example, over 80 % of oxalic acid are oxidised by electron transfer with Cl2 ? in deliquescent particles during non-cloud periods.  相似文献   

18.
2020年6月,我国江淮区域出现大范围持续性强降水过程,并引发了洪涝灾害。利用ERA5再分析资料对江淮区域的水汽收支平衡进行分析,并利用HYSPLIT后向轨迹模式分析了其水汽源地。结果表明:(1)ERA5再分析资料能较好地描述本次过程中江淮区域的水汽收支特征,其中水汽辐合项为主要贡献项,对水汽汇有较好的指示作用,同时,降水和水汽汇之间保持了较好的一致性变化。(2)南海是江淮区域6月持续性降水最主要的水汽源地,约50%的水汽来自南海。(3)6月江淮区域降水分布与水汽的输送密切相关,而水汽输送主要取决于西太平洋副热带高压的位置及其与北侧冷涡活动的共同作用。  相似文献   

19.
During February 1997, one of the 2 observational periods of CIME ( c loud i ce m ountain e xperiment), a joint field experiment funded by the European Commission, took place on the summit of the Puy de Dōme in the centre of France. During this experiment the droplet spectra were measured with an FSSP and the aerosol particles in the drops and in the interstitial particle phase were measured with a counterflow virtual impactor and a round jet impactor inside a windtunnel. Very low aerosol particle and drop concentrations were observed and particles as small as 25 nm in diameter were found to activate. Two datasets obtained on 15 February and 17 February were used to study the activation of the small Aitken‐mode particles and the spectral form of the droplet spectrum and the scavenging fraction. Numerous sensitivity studies were performed investigating the rôle of the number density and chemical composition of the aerosol particles. The rôle of mixing inside the orographic cloud was studied by using a new technique. It considers the fact that the air arriving on the summit of the Puy de Dôme is a mixture of air of different origins. Thus, it weighs the results of a spectral scavenging model (DESCAM or EXMIX) calculated along a number of individual trajectories. The weighing function is derived from tracer and trajectory studies with a 3‐dimensional mesoscale model. The model was able to reproduce the activation of aerosol particles as small as 25 nm. It was caused by the low aerosol particle number concentrations. In general, we can conclude that the variability found in the sensitivity tests of the dynamical and chemical factors allows to reproduce the shape of the observed results. As too many free parameters exit at the moment we cannot quantify the contribution of each factor studied to the observed scavenging fraction, however, it seems that dynamics dominates.  相似文献   

20.
The role of perturbations of reactive trace gas concentration distributions in turbulent flows in the planetary boundary layer (PBL) is discussed. The paper focuses on disturbances with larger spatial scales. Sequential nesting of a chemical transport model is applied to assess the effect of neglecting subgrid chemical perturbations on the formation and loss of ozone, NO x , peroxyacetyl nitrate (PAN) and HNO3 calculated with a highly complex chemical mechanism. The results point to characteristic differences regarding the process of mixing of chemically reactive species in the PBL and lower troposphere.  相似文献   

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