共查询到20条相似文献,搜索用时 140 毫秒
1.
本文在参数化云物理模式与化学模式的基础上讨论了积云降水过程中,云内硫酸盐形成的各种反应机制的相对重要性。计算结果表明:在反应的初始降段,(SIV)的H_2O_2液相氧化的氧化速率最大,即对云内硫酸盐形成的贡献为最大。随着反应的进行,其氧化速率很快减小,S(IV)的O_3液相氧化成为硫酸盐形成的最重要的来源。S(IV)的Fe~(3+)、Mn~(2+)催化氧化及SO_2的气相反应的贡献相对来说比较小。计算结果表明:在积云降水过程中,液相反应对云内硫酸盐形成的重要性大于气相反应。 相似文献
2.
硫酸盐和碳黑气溶胶辐射效应的研究 总被引:7,自引:2,他引:7
该文在辐射方案中硫酸盐和碳黑气溶胶辐射效应进行了研究,估算了这两种气溶胶成分的辐射强迫,在气溶胶-辐射方案中考虑了:(1)具有不同尺度的硫酸盐和碳黑气溶胶在太阳辐射波长范围内的光学性质;(2)硫酸盐和碳黑气溶胶浓度的比例变化;(3)硫酸盐和碳黑气溶胶的混合形式,当硫酸盐气溶胶和碳黑气溶胶同时存在时,碳黑气溶胶的加热作用与硫酸盐气溶胶的冷却作用相叠加,会使大气顶的负辐射强迫量减少,减少的负辐射强迫量 相似文献
3.
利用大气气溶胶和云分档模式研究海盐气溶胶和硫酸盐气溶胶在云微物理过程中的作用, 计算结果表明:云中液态水含量随高度的分布并不随海盐、硫酸盐的数目以及云团上升速度的变化而变化; 随着云滴数目的增加, 云滴的有效半径会减小; 硫酸盐对云滴数目影响起主导作用, 海盐在水汽相对充足情况下增加了云滴数目, 在水汽相对不足的情况下减少了云滴数目; 硫酸盐粒子浓度特别强的情况下 (人类活动污染比较严重时), 如果水汽相对不足, 云滴数目会明显小于硫酸盐粒子浓度; 而海盐粒子的存在, 加剧了水汽的供应不足, 从而可以在很大程度上进一步降低云滴数目。也就是说, 在有些情况下, 如果不考虑海盐气溶胶的作用, 硫酸盐气溶胶对云特性的影响会被过高估计。 相似文献
4.
TRACE-P期间硫酸盐、硝酸盐和铵盐气溶胶的模拟研究 总被引:14,自引:7,他引:14
结合最新评估的东亚地区 1°× 1°污染源资料 ,利用由区域大气模式系统 (RAMS)和区域大气质量模式系统 (CMAQ)耦合的空气质量模式系统 ,对东亚地区 2 0 0 1年春季气溶胶的输送及其化学转化过程进行了研究。为了检验模式系统的模拟效果 ,我们将模拟的硫酸盐、硝酸盐和铵盐气溶胶的浓度与TRACE -P观测期间获取的观测值进行了比较。比较结果显示 ,模拟值与观测值具有相当好的一致性 ,模式很好地反映了气溶胶浓度的分布特征和变化规律 ,再现了许多观测到的重要特征。模拟结果表明 ,中国区域硫酸盐气溶胶浓度高值主要是人为排放的二氧化硫造成的 ,10 0°E以东的中国广大地区的硫酸盐气溶胶柱含量超过了 6mg·m- 2 ,最高值达到 2 4mg·m- 2 ,柱含量 >16mg·m- 2 的区域延伸到中国近海的广大海域。东亚地区的人类活动不仅使污染地区气溶胶柱含量显著增加 ,而且使近海无源区的广大海域的污染加重。本模式系统的建立为今后进一步研究区域大气污染物的变化机理提供了有效的手段。 相似文献
5.
中国地区硫酸盐气溶胶的分布特征 总被引:11,自引:2,他引:11
建立了一个三维欧拉型排放/输送/转化/沉降模式,其主要特点是采用独立的气相化学子模式计算各种不同条件下SO2的转化速率,建立转化率的数据库,直接为欧拉模式调用,并对液相化学和湿清除过程进行了参数化处理。这样使模式既考虑了大气化学过程的非线性,又具有较高的计算效率,能够方便地计算年(季)尺度的硫酸盐气溶胶SO2-4的浓度分布。利用中尺度气象模式MM4和欧拉输送模式模拟了中国地区硫酸盐气溶胶的时空分布,其结果可以方便地应用到考虑硫酸盐气溶胶气候效应的气候模式中去。 相似文献
6.
利用卫星资料进一步检验了CAM3.0模式对云的模拟能力,该模式可以较好地再现全球云的分布和季节变化的主要特征。在硫循环过程与辐射和动力过程之间双向耦合的情况下,探讨了硫酸盐气溶胶直接气候效应对水循环过程的影响。模式较好地模拟了硫酸盐气溶胶的浓度和分布变化。硫酸盐气溶胶对水循环因子的影响在不同季节和区域是不同的,其中,北半球夏季的影响最大,这是因为北半球夏季硫酸盐浓度最高。纬向平均的云量、降水和水汽的变化形势大部分相似,存在比较密切的联系。 相似文献
7.
对GOALS4 .0海 陆 气耦合模式的相关部分进行了改进 ,主要改进包括温室气体的扩充和硫酸盐气溶胶“显式”方案的引入 ,并引入 2 0世纪温室气体的实际浓度变化以及硫循环模式模拟的硫酸盐气溶胶的三维全球浓度分布 ,模拟了温室气体和硫酸盐气溶胶造成的辐射强迫的空间分布和时间变化。全球平均的温室气体和硫酸盐气溶胶的辐射强迫分别为 2 .17W /m2 和 - 0 .2 9W /m2 ;温室气体造成的辐射强迫在空间上呈现明显的纬向结构 ,最大值 (大于 2 .5W/m2 )和最小值 (小于 1W /m2 )分别位于副热带和两极地区 ,在北半球主要工业区硫酸盐气溶胶的辐射强迫绝对值接近温室气体的辐射强迫值 (大于 - 2 .0W /m2 )。 相似文献
8.
硫酸盐气溶胶辐射强迫的数值模拟研究 总被引:5,自引:0,他引:5
利用IAP/LASG GOALS 4.0海气耦合模式,\"显式\"考虑了硫酸盐气溶胶的直接作用,并且引入德国马普气象研究所的三维浓度分布资料,模拟计算了硫酸盐气溶胶的辐射强迫.主要结果为:全球气溶胶年平均的辐射强迫为-0.29 W m-2,在IPCC TAR给定的范围内,空间分布上具有明显的地域性,几个大值地区分别为东亚、西欧和北美,它们的中心值均超过-1.5 W m-2,南美、澳大利亚以及非洲南部的辐射强迫介于-0.2~-0.4 W m-2之间,而海洋和偏远的大陆地区,则基本上不受人为硫酸盐气溶胶的影响;计算的东亚地区硫酸盐气溶胶的平均辐射强迫为-0.75 W m-2,约为全球平均的2.5倍,为北半球平均的1.6倍.文中还讨论了全球硫酸盐气溶胶对温室气体辐射强迫的减缓作用. 相似文献
9.
硫酸盐气溶胶(SO42-)和黑碳气溶胶(BC)可以通过散射或吸收太阳辐射改变地气系统能量收支,进而引起局地热力和云过程变化乃至大气环流的调整而影响气候系统。南海夏季风(SCSSM)作为东亚夏季风的子系统之一,与东亚大气环流和降水有着重要的相互影响。前人对SO42-和BC对东亚副热带季风已有详细研究,但对SO42-和BC影响南海夏季风的机制研究较少。本研究利用CESM(The Community Earth System Model)模式CAM5.1模块模拟研究了SO42-和BC对南海—华南经向海陆热力差异、中南半岛对流、西太平洋副热带高压(西太副高)断裂以及南海夏季风爆发的影响,重点探讨了气溶胶影响SCSSM爆发的动力和热力机制。模拟试验结果表明,SO42-和BC均有利于中南半岛对流层整层大气稳定性增强,引发了中南半岛上空的下沉气流异常,动力上抑制了中南半岛对流,分别使... 相似文献
10.
利用WRF-Chem(Weather Research and Forecasting model coupled with Chemistry)模式研究2006年8月1日—9月1日中国区域硫酸盐和黑碳气溶胶对云特性的影响。模式验证利用了卫星和地面观测的气象要素、化学物质浓度、气溶胶光学特性和云微物理特性。模式性能评估表明该模式能较好地抓住气象要素(温度、降水、相对湿度和风速)的量级和空间分布特征。通过与地面观测和MODIS卫星数据对比发现,尽管模式模拟还存在偏差,但还是能较好模拟出气溶胶物种的地表浓度、气溶胶光学厚度(AOD)、云光学厚度(COD)、云量(CLDF)、云顶云滴有效半径(CER)和云水路径(LWP)。通过两个敏感性试验(分别增加二氧化硫和黑碳排放量至控制试验排放的3倍)与控制试验的对比发现硫酸盐比黑碳更易成为云凝结核,在中国东部云顶云滴数浓度和其它云特性参数对二氧化硫排放增加的响应均从北向南呈递增,这与地面湿度分布有关。云滴有效半径对硫酸盐气溶胶的响应符合气溶胶第一间接效应的定义,即硫酸盐气溶胶增多,云滴数浓度增加,云滴有效半径减少,但是对黑碳气溶胶的响应在各区域不尽相同。还发现黑碳对云量的影响远大于硫酸盐,主要原因是由于黑碳气溶胶直接辐射效应(对太阳光的吸收)导致的云的“燃烧”作用。 相似文献
11.
William R. Stockwell 《Journal of Atmospheric Chemistry》1994,19(3):317-329
The rates and mechanisms of both gas and liquid phase reactions for the oxidation of sulfur dioxide play an important role in the production of atmospheric acids and aerosol particles. Rhodeet al. (1981) concluded that sulfate production rates were highly non-linear functions of sulfur dioxide emission rates. Their modelling study used an HOx termination mechanism for the HO—SO2 reaction in the gas-phase. Stockwell and Calvert (1983) determined that one of the products of the overall reaction of HO with sulfur dioxide was an HO2 radical. The National Research Council (1983) using a version of the Rhodeet al. (1981) model modified to include HO2 production from the HO—SO2 reaction concluded that sulfate production becomes much more linear with respect to reductions in sulfur dioxide emissions. However, the cause of this increased linearity was not explained by the National Research Council report. It is demonstrated that the increased linearity is due to the coupling of gas-phases and aqueous phase chemistry. The gas-phase sulfur dioxide oxidation mechanism has a very significant effect on hydrogen perodide production rates. 相似文献
12.
H. Berresheim M. O. Andreae G. P. Ayers R. W. Gillett J. T. Merrill V. J. Davis W. L. Chameides 《Journal of Atmospheric Chemistry》1990,10(3):341-370
Vertical distributions of dimethylsulfide (DMS), sulfur dioxide (SO2), aerosol methane-sulfonate (MSA), non-sea-salt sulfate (nss-SO42-), and other aerosol ions were measured in maritime air west of Tasmania (Australia) during December 1986. A few cloudwater and rainwater samples were also collected and analyzed for major anions and cations. DMS concentrations in the mixed layer (ML) were typically between 15–60 ppt (parts per trillion, 10–12; 24 ppt=1 nmol m–3 (20°C, 1013 hPa)) and decreased in the free troposphere (FT) to about <1–2.4 ppt at 3 km. One profile study showed elevated DMS concentrations at cloud level consistent with turbulent transport (cloud pumping) of air below convective cloud cells. In another case, a diel variation of DMS was observed in the ML. Our data suggest that meteorological rather than photochemical processes were responsible for this behavior. Based on model calculations we estimate a DMS lifetime in the ML of 0.9 days and a DMS sea-to-air flux of 2–3 mol m–2 d–1. These estimates pertain to early austral summer conditions and southern mid-ocean latitudes. Typical MSA concentrations were 11 ppt in the ML and 4.7–6.8 ppt in the FT. Sulfur-dioxide values were almost constant in the ML and the lower FT within a range of 4–22 ppt between individual flight days. A strong increase of the SO2 concentration in the middle FT (5.3 km) was observed. We estimate the residence time of SO2 in the ML to be about 1 day. Aqueous-phase oxidation in clouds is probably the major removal process for SO2. The corresponding removal rate is estimated to be a factor of 3 larger than the rate of homogeneous oxidation of SO2 by OH. Model calculations suggest that roughly two-thirds of DMS in the ML are converted to SO2 and one-third to MSA. On the other hand, MSA/nss-SO42- mole ratios were significantly higher compared to values previously reported for other ocean areas suggesting a relatively higher production of MSA from DMS oxidation over the Southern Ocean. Nss-SO42- profiles were mostly parallel to those of MSA, except when air was advected partially from continental areas (Africa, Australia). In contrast to SO2, nss-SO42- values decreased significantly in the middle FT. NH4+/nss-SO42- mole ratios indicate that most non-sea-salt sulfate particles in the ML were neutralized by ammonium. 相似文献
13.
Ambient particulate sulfate measurements have been intermittently performed at a rural site in Israel over a period of more than two years. Concurrent measurements of ambient pollutants (SO2, NO–NOx, and O3), as well as meteorological data, were also carried out. The daily data included four particulate sulfate samples representing four successive 6 h accumulating periods. The measured concentrations of sulfate ions ranged from a low 2 g m-3 observed during the winter season to a high of >50 g m-3 obtained during the summer. Little correlation was obtained between the sulfate concentration and either O3 or SO2, although sulfate and O3 showed a similar diurnal and annual trend. Based on the data distribution and on a photochemical model, it was concluded that a large part of the particulate sulfate observed at the eastern coast of the Mediterranean Sea must be related to long-range transport from distant sources. 相似文献
14.
M. O. Andreae H. Berresheim T. W. Andreae M. A. Kritz T. S. Bates J. T. Merrill 《Journal of Atmospheric Chemistry》1988,6(1-2):149-173
Dimethylsulfide (DMS), sulfur dioxide (SO2), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO42–), sodium (Na+), ammonium (NH4+), and nitrate (NO3–) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO2 concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m–3 (STP). The nonsea-salt sulfate (ns-SO42–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO2 and nss-SO42– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na+ and NO3–, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions. 相似文献
15.
The biogeochemical sulfur cycle in the marine boundary layer over the Northeast Pacific Ocean 总被引:1,自引:0,他引:1
T. S. Bates J. E. Johnson P. K. Quinn P. D. Goldan W. C. Kuster D. C. Covert C. J. Hahn 《Journal of Atmospheric Chemistry》1990,10(1):59-81
The major components of the marine boundary layer biogeochemical sulfur cycle were measured simultaneously onshore and off the coast of Washington State, U.S.A. during May 1987. Seawater dimethylsulfide (DMS) concentrations on the continental shelf were strongly influenced by coastal upwelling. Concentration further offshore were typical of summer values (2.2 nmol/L) at this latitude. Although seawater DMS concentrations were high on the biologically productive continental shelf (2–12 nmol/L), this region had no measurable effect on atmospheric DMS concentrations. Atmospheric DMS concentrations (0.1–12 nmol/m3), however, were extremely dependent upon wind speed and boundary layer height. Although there appeared to be an appreciable input of non-sea-salt sulfate to the marine boundary layer from the free troposphere, the local flux of DMS from the ocean to the atmosphere was sufficient to balance the remainder of the sulfur budget. 相似文献
16.
Based on data collected during the first U.S.Department of Energy(DOE) Atmospheric Radiation Measurement(ARM) field campaigns at Shouxian,eastern China in 2008,the effects of clouds and aerosols on the surface radiation budget during the period October-December 2008 were studied.The results revealed that the largest longwave(LW),shortwave(SW),and net Aerosol Radiative Effects(AREs) are 12.7,-37.6,and-24.9 W m-2,indicating that aerosols have LW warming impact,a strong SW cooling effect,and a net cooling effect on the surface radiation budget at Shouxian during the study period 15 October-15 December 2008.The SW cloud radiative forcing(CRF) is-135.1 W m-2,much cooler than ARE(about 3.6 times),however,the LW CRF is 43.6 W m-2,much warmer than ARE,and resulting in a net CRF of-91.5 W m-2,about 3.7 times of net ARE.These results suggest that the clouds have much stronger LW warming effect and SW cooling effect on the surface radiation budget than AREs.The net surface radiation budget is dominated by SW cooling effect for both ARE and CRF.Furthermore,the precipitatable clouds(PCs) have the largest SW cooling effect and LW warming effect,while optically thin high clouds have the smallest cooling effect and LW warming on the surface radiation budget.Comparing the two selected caseds,CloudSat cloud radar reflectivity agrees very well with the AMF(ARM Mobile Facility) WACR(W-band ARM Cloud Radar) measurements,particularly for cirrus cloud case.These result will provide a ground truth to validate the model simulations in the future. 相似文献
17.
Warren J. de Bruyn Mike Harvey Jill M. Cainey Eric S. Saltzman 《Journal of Atmospheric Chemistry》2002,41(2):189-209
Atmospheric dimethyl sulfide (DMS) and sulfur dioxide (SO2) concentrations were measured at Baring Head, New Zealandduring February and March 2000. Anti-correlated DMS and SO2 diurnalcycles, consistent with the photochemical production of SO2 from DMS, were observed in clean southerly air off the ocean. The data is used to infer a yield of SO2 from DMS oxidation. The estimated yields are highly dependent on assumptions about the DMS oxidation rate. Fitting the measured data in a photochemical box model using model-generated OH levels and the Hynes et al. (1986) DMS + OH rate constant suggests that theSO2 yield is 50–100%, similar to current estimates for the tropical Pacific.However, the observed amplitude of the DMS diurnal cycle suggests that the oxidation rate is higher than that used by the model, and therefore, that theSO2 yield is lower in the range of 20–40%. 相似文献
18.
High-volume aerosol filters, exposed in maritime air masses at Cape Grim since late 1976, were analysed for excess sulfate (not of seasalt origin) and methanesulfonate. The mean concentrations (standard errors) of 2.80(0.59) and 0.176(0.027) nmole/m3 respectively are about half those reported in a recent study of aerosol samples from various locations in the Atlantic and Pacific oceans.Methanesulfonate concentration varied seasonally by at least an order of magnitude with a summer maximum and winter minimum. No comparable cycle was found for excess sulfate. 相似文献
19.
利用2020年7月30日山西省人工增雨防雷技术中心在山西省忻州地区开展的大陆性浓积云飞机探测资料,分析了积云微物理参量、云滴谱离散度随时间和高度的变化以及云滴谱离散度的影响因子。结果表明,该大陆性浓积云云滴谱离散度随高度的增加先递增后递减,但变化范围较小。云滴谱离散度随数浓度、含水量增大而逐渐收敛,呈弱正相关关系;离散度与体积平均半径的相关性随体积平均半径的增大由正转负,与垂直速度呈现正相关关系。云中碰并过程对云滴谱离散度及其影响因子影响较大,建议未来云滴谱离散度的参数化增加对碰并过程的考虑。 相似文献
20.
Measurements are presented of sulfate and nitrate production in clouds on the East and West coasts of the United States. Sulfate production measured on the mid-Atlantic Coast was significantly greater than on the Pacific Northwest Coast. Nitrate production was significant on the mid-Atlantic Coast but, on average, insignificant on the Pacific Northwest Coast. Measurements of sulfate and nitrate scavenging coefficients by clouds are also presented. 相似文献