Measurement of Ambient,Interstitial, and Residual Aerosol Particles on a Mountaintop Site in Central Sweden using an Aerosol Mass Spectrometer and a CVI

The Aerodyne aerosol mass spectrometer (Q-AMS) was coupled with a counterflow virtual impactor (CVI) for the first time to measure cloud droplet residuals of warm tropospheric clouds on Mt. Åreskutan in central Sweden in July 2003. Operating the CVI in different operational modes generated mass concentration and species-resolved mass distribution data for non-refractory species of the ambient, interstitial, and residual aerosol. The ambient aerosol measurements revealed that the aerosol at the site was mainly influenced by long-range transport and regional photochemical generation of nitrate and organic aerosol components. Four different major air masses were identified for the time interval of the experiment. While two air masses that approached the site from northeastern Europe via Finland showed very similar aerosol composition, the other two air masses from polar regions and the British Islands had a significantly different composition. During cloud events the larger aerosol particles were found to be activated into cloud droplets. On a mass basis the activation cut-off diameter was approximately 150 nm for nitrate and organics dominated particles and 200 nm for sulfate dominated particles. Generally nitrate and organics were found to be activated into cloud droplets with higher efficiency than sulfate. While a significant fraction of the nitrate in ambient particles was organic nitrates or nitrogen-containing organic species, the nitrate found in the cloud droplet residuals was mainly ammonium nitrate. After passage of clouds the ambient aerosol size distribution had shifted to smaller particle sizes due to the predominantly activation of larger aerosol particles without a significant change in the relative composition of the ambient aerosol.     

临安大气气溶胶理化特性季节变化

分别利用碳成分分析仪、离子色谱仪和原子吸收光谱仪等获取浙江省临安地区大气气溶胶在春、夏、秋、冬四季的质量浓度、离子与碳成分特性，并对不同粒径气溶胶成分分布特点作了较详细分析。结果表明:气溶胶质量浓度、可溶性离子浓度以及碳成分浓度具有明显的季节变化趋势。整个尺度范围内，气溶胶质量浓度季节变化特点为春季浓度最高，达到534 μg/m3；冬季次之，质量浓度为117.21 μg/m3；夏季浓度最低，平均为65.7 μg/m3；秋季质量浓度98.6 μg/m3。可溶性离子成分在气溶胶中所占比例具有明显的季节性，其中夏季最高为49.4%，春季最低为11.3%。硫酸根离子SO₄2-和氨根离子NH₄+和硝酸根离子NO₃- 3种离子浓度之和约占离子总量的75%~83%。受温度影响，硝酸根离子NO₃-浓度随季节变化幅度较大，夏季平均浓度为1.7 μg/m3, 冬季平均浓度为11.5 μg/m3，是夏季浓度的6.8倍。碳浓度分布特点显示，气溶胶中元素碳浓度春季最高，夏季最低。有机碳浓度春季最高，冬季最低。气溶胶粒度分布特点也非常明显。四季中粒径小于11 μm（PM₁₁）的气溶胶均占气溶胶总量的90%以上，粒径小于2.1 μm（PM_2.1）的气溶胶占到气溶胶总量的53%以上。可溶性离子在粒径小于2.1 μm气溶胶颗粒中，以硫酸根离子、氨根离子和硝酸根离子为主。碳成分尺度分布特征为颗粒越小，有机碳及元素碳浓度越高。     

Using hourly measurements to explore the role of secondary inorganic aerosol in PM2.5 during haze and fog in Hangzhou,China

This paper explores the role of the secondary inorganic aerosol （SIA） species ammonium,NH4＋,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity （RH）.The contribution of SIA species to PM2.5 mass increased to ～50％ during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11％ during clear to 20％ during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60％-70％ RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.     

Equilibria of the marine multiphase ammonia system

A lack of empirical data has made it difficult to ascertain whether ammonia is in equilibrium between the oceanic, atmospheric gas and atmospheric particle phases in the remote marine environment. Reported here are simultaneous measurements of the saturation concentration of ammonia relative to ammonia concentrations in ocean surface waters; total seawater ammonia; atmospheric gas phase ammonia; and atmospheric particulate-phase ammonium, non-seasalt sulfate, methanesulfonate, and nitrate. Sampling was performed in May of 1987 in the northeast Pacific Ocean environment and in April and May of 1988 in the central Pacific Ocean environment.These measurements were used to determine the degree to which ammonia approached equilibrium between the oceanic and atmospheric gas and aerosol particle phases. The experimental atmospheric gas phase ammonia concentrations were compared with calculated equilibrium concentrations assuming a Henry's law type of partitioning between the gas and condensed phases. Characteristic times of the processes controlling the fate of ammonia in the marine environment also were compared.The measured atmospheric gas phase and oceanic concentrations of ammonia indicate that ammonia is not in a Henry's law equilibrium across the air/sea interface. This disequilibrium is a result of the long air/sea exchange equilibration time relative to the lifetime of ammonia in the atmosphere. Comparison of the calculated equilibrium gas phase ammonia concentrations with the measured gas phase ammonia concentrations shows that attainment of equilibrium between the atmospheric gas and particle phases is a strong function of the chemical composition of the aerosol particles. The data suggest that fully neutralized aerosol particles are not in Henry's law equilibrium with the gas phase while equilibrium is observed for particles with an average ammonium to non-seasalt sulfate molar ratio less than 1.8.     

北京PM1中的化学组成及其控制对策思考

通过分析北京城区2007年夏季和秋季、2008年冬季和春季4个季节PM₁中硫酸盐、硝酸盐、铵盐、有机物和黑碳等气溶胶化学组成,结合对我国及全球主要区域PM₁₀中上述气溶胶组分及矿物气溶胶组成的评估,发现因受干旱区产生的沙尘和城市逸散性粉尘的共同影响,整个亚洲大陆,尤其是我国的矿物气溶胶浓度与欧美国家城市区域气溶胶总和的平均值相当或更高。我国在重视控制PM_2.5等细粒子污染的同时,不应忽视对PM_2.5~PM₁₀之间粗粒子的控制力度;北京城区春、夏、秋、冬的PM₁平均质量浓度分别约为94,74,66 μg·m-3和91 μg·m-3,全年平均约为81 μg·m-3,其中有机物气溶胶约占41%,硫酸盐占16%,硝酸盐占13%,铵盐占8%,黑碳和氯化物分别占11%和3%,细矿物气溶胶约贡献7%。对于PM_2.5污染的控制,关键是消减PM₁中主要气溶胶粒子的排放与转化,其中对有机物的控制更为重要,尽管对于北京而言进一步污染控制的难度已经很大。从科学上来说,即使我国的控制措施能百分之百实现,也很难稳定地达到欧美国家的空气质量水平,因为我国本底矿物气溶胶的浓度较高。应进一步评估各项控制措施的适用性,并制定考虑我国人群健康状况的PM_2.5空气质量标准。     

夏季厄尔尼诺-Modoki和东部型ENSO海表温度异常分布型特征及其与海洋性大陆区域气候异常的联系

2007年,Ashok等揭示了赤道太平洋区域存在一种三极型分布海表温度异常并称之为厄尔尼诺-Modoki,同时定义了相应的海表温度异常指数EMI（记为I_EM）。在此基础上,利用英国哈得来中心逐月海表温度资料、美国NCEP/NCAR月平均再分析数据集、美国国家海洋和大气管理局（NOAA）逐月降水资料（CMAP）,通过在太平洋海表温度异常中扣除厄尔尼诺-Modoki信号后,在Nino1+2区域上定义了东太平洋型海表温度异常指数EPNI（I_EPN）。据此,由I_EPN和I_EM可构成描述热带太平洋海表温度异常变化的一对指数。分析了两个指数相应的海气状态及对海洋性大陆区域气候异常的影响。结果表明,厄尔尼诺-Modoki和东太平洋型海表温度异常及其影响存在显著差异。在北半球夏季,当I_EM处于正位相时,热带太平洋海表温度异常呈现“负-正-负”的结构,海洋性大陆大部分区域海表温度异常为负,此时对流层低层太平洋地区辐合,海洋性大陆地区辐散,对流层高层太平洋地区辐散,海洋性大陆地区辐合。对应于辐合辐散中心,存在着自赤道中太平洋分别向赤道东太平洋和海洋性大陆中东部地区的异常垂直环流圈,同时也存在自海洋性大陆西部向印度洋西部的垂直环流。大气在海洋性大陆区域北部加热,南部冷却;在太平洋地区西部加热而东部冷却;在海洋性大陆区域10°N以南降水偏少,而10°N以北降水偏多。当I_EPN处于正位相时,热带太平洋海表温度异常呈现“西负东正”分布型,海洋性大陆区域海表温度异常呈现“西正东负”分布,对流层低层海洋性大陆地区辐散中心范围偏大、位置偏东、强度偏强,太平洋地区辐合中心范围偏小、位置偏东,热带环流异常在垂直方向上呈斜压结构,海洋性大陆区域北部大气加热而南部冷却,太平洋地区大气均呈加热正异常,海洋性大陆大部分区域降水均偏少,赤道太平洋降水偏多。以上这些结果有利于深刻理解热带太平洋海表温度异常的特征及其对海洋性大陆区域气候的影响。     

Numerical quantification of sources and phase partitioning of chemical species in cloud: application to wintertime anthropogenic air masses at the Puy de Dôme station

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.     

北京春季沙尘和霾期间气溶胶的对比模拟研究

利用气象模式WRF驱动区域空气质量模式RAQMS,模拟研究了2014年北京地区春季颗粒物及气溶胶化学组分的时空变化,对比分析了沙尘期（3月17日、29日）和霾期（3月25～27日）的天气形势、气象要素和气溶胶化学组分特征,比较了沙尘和人为气溶胶表面非均相化学反应对大气化学成分的影响及相对贡献。结果显示,模式对于气象要素、PM2.5、PM10及其化学组分具有较好的模拟能力,考虑了气溶胶表面非均相化学反应后明显提高了模式对PM2.5及气溶胶化学组分模拟的准确性。沙尘期间,沙尘对PM10质量浓度贡献占主导地位（50.7%）,对PM2.5的贡献与有机气溶胶（OM）和人为排放的一次颗粒物（PPM）相当;霾期间,硝酸盐NO₃?（25.6%）和OM（23.6%）对PM2.5的贡献最大,在PM10中NO₃?、PPM和OM的贡献相当。沙尘期,粗粒子明显增加,在PM10中所占比例与细粒子相当,为45.5%;霾期,细粒子占主导地位,占PM10质量浓度的85.6%。非均相化学反应使沙尘期间硫酸盐（SO₄2–）和NO₃–浓度分别增加16.9%和83.8%,使霾期间的SO₄2?和NO₃–浓度分别增加14.5%和45.0%。2014年3月,非均相化学反应使北京月均SO₂、NO₂、O₃、SO₄2?、NH₄+和NO₃?的浓度分别变化了?2.5%、?5.7%、?3.4%、11.7%、18.6%和58.5%,本文结果表明非均相化学反应对二次无机气溶胶的生成有重要贡献。     

关于硝酸盐气溶胶光学特征和辐射强迫的研究进展

在过去的20多年里,中外对硫酸盐气溶胶做了大量的研究,对它在大气中的排放、含量、光学特征和辐射强迫有了深入的认识;由于硝酸盐气溶胶在大气中平均含量比硫酸盐低很多,因此过去人们对硝酸盐的研究没有给予重视。然而,近年来的研究表明,硝酸盐气溶胶的散射性质在某些波段甚至强于硫酸盐;同时,由于未来对人为硫酸盐前体物的减排,硫酸盐气溶胶排放会大幅度减少,而硝酸盐气溶胶的排放却增长迅速,其在人为气溶胶中所占的比重越来越高,将会导致其在未来造成的辐射强迫有可能超过硫酸盐,使得其在地区范围内和季节尺度上成为重要的辐射强迫和气候影响因子。中国是硝酸盐气溶胶排放量较大的地区,硝酸盐对未来中国气候和气候变化的影响显得越来越重要。因此,就近年来有关硝酸盐气溶胶的排放和在大气中的浓度变化、光学厚度分布特征及其辐射强迫的研究进展做了回顾和介绍,并对其未来的研究做了展望。     

Impacts of aerosol chemical composition on microphysics and precipitation in deep convection

Aerosols affect precipitation by modifying cloud properties such as cloud droplet number concentration (CDNC). Aerosol effects on CDNC depend on aerosol properties such as number concentration, size spectrum, and chemical composition. This study focuses on the effects of aerosol chemical composition on CDNC and, thereby, precipitation in a mesoscale cloud ensemble (MCE) driven by deep convective clouds. The MCE was observed during the 1997 department of energy's Atmospheric Radiation Measurement (ARM) summer experiment. Double-moment microphysics with explicit nucleation parameterization, able to take into account those three properties of aerosols, is used to investigate the effects of aerosol chemical composition on CDNC and precipitation. The effects of aerosol chemical compositions are investigated for both soluble and insoluble substances in aerosol particles. The effects of soluble substances are examined by varying mass fractions of two representative soluble components of aerosols in the continental air mass: sulfate and organics. The increase in organics with decreasing sulfate lowers critical supersaturation (S_c) and leads to higher CDNC. Higher CDNC results in smaller autoconversion of cloud liquid to rain. This provides more abundant cloud liquid as a source of evaporative cooling, leading to more intense downdrafts, low-level convergence, and updrafts. The resultant stronger updrafts produce more condensation and thus precipitation, as compared to the case of 100% sulfate aerosols. The conventional assumption of sulfate aerosol as a surrogate for the whole aerosol mass can be inapplicable for the case with the strong sources of organics. The less precipitation is simulated when an insoluble substance replaces organics as compared to when it replaces sulfate. When the effects of organics on the surface tension of droplet and solution term in the Köhler curve are deactivated by the insoluble substance, S_c is raised more than when the effects of sulfate on the solution term are deactivated by the insoluble substance. This leads to lower CDNC and, thus, larger autoconversion of cloud liquid to rain, providing less abundant cloud liquid as a source of evaporative cooling. The resultant less evaporative cooling produces less intense downdrafts, weaker low-level convergence, updrafts, condensation and, thereby, less precipitation in the case where organics is replaced by the insoluble substance than in the case where sulfate is replaced by the insoluble substance. The variation of precipitation caused by the change in the mass fraction between the soluble and insoluble substances is larger than that caused by the change in the mass fraction between the soluble substances.     

Assessment of Individual Direct Radiative Effects of Major Aerosol Species in East Asia

To assess individual direct radiative effects of diverse aerosol species on a regional scale,the air quality modeling system RAMS-CMAQ(Regional Atmospheric Modeling System and Community Multiscale Air Quality) coupled with an aerosol optical properties/radiative transfer module was used to simulate the temporal and spatial distributions of their optical and radiative properties over East Asia throughout 2005.Annual and seasonal averaged aerosol direct radiative forcing(ADRF) of all important aerosols and individual components,such as sulfate,nitrate,ammonium,black carbon(BC),organic carbon(OC),and dust at top-of-atmosphere(TOA) in clear sky are analyzed.Analysis of the model results shows that the annual average ADRF of all important aerosols was in the range of 0 to-18 W m?2,with the maximum values mainly distributed over the Sichuan Basin.The direct radiative effects of sulfate,nitrate,and ammonium make up most of the total ADRF in East Asia,being concentrated mainly over North and Southeast China.The model domain is also divided into seven regions based on different administrative regions or countries to investigate detailed information about regional ADRF variations over East Asia.The model results show that the ADRFs of sulfate,ammonium,BC,and OC were stronger in summer and weaker in winter over most regions of East Asia,except over Southeast Asia.The seasonal variation in the ADRF of nitrate exhibited the opposite trend.A strong ADRF of dust mainly appeared in spring over Northwest China and Mongolia.     

A study of marine aerosols over the Pacific Ocean

Aerosol samples were collected on a Pacific cruise from 47°N to 55°S. Particle morphology, concentrations, and size distributions were analyzed with an electron microscope; elemental compositions of individual particles were determined with an X-ray energy spectrometer; and chemical compositions of bulk samples were measured with an ion chromatograph. Temporal and spatial variations of aerosol physico-chemical characteristics were studied in relation to ocean currents and atmospheric parameters. The results show that number and mass concentrations of primary particles depend mainly on surface wind speeds. However the ratios between the major ions, e.g., Na⁺, Cl^-, and Mg⁺⁺, are similar to the ratios in seawater regardless of location or meteorological conditions. The concentrations of secondary aerosols, e.g., non-seasalt sulfate, nitrate, and ammonium particles, show maxima at upwelling regions, such as along the California coast, at the Equator, and near the Chatham Rise where ascending motion brings nutrient-riched deep water into the surface layer. The number concentrations of small sulfate particles and large nitrate-coated particles showed diurnal variations with maxima in the early afternoon and minima at night, indicating that the particles are the products of photo-chemical reactions. Their precursor gases, e.g., CH₃SCH₃, NO, and NH₃ are known to be released from seawater in upwelling regions where biological activities thrive.     

京津冀周边秸秆燃烧对PM2.5无机组分影响

华北平原是我国主要农作物产区,田间秸秆焚烧现象普遍存在,选取秋收季节（2014年10月）分析了秸秆燃烧的排放特征,利用区域化学传输模型WRF-Chem模拟研究了燃烧排放对气态前体物及其氧化产物的影响,以及最终导致的PM_2.5中硫酸盐、硝酸盐和铵盐的变化。研究表明:2014年秋收季节,河南和山东等省份的秸秆燃烧排放会在东南风的输送作用下影响京津冀地区;秸秆燃烧排放大量挥发性有机物（VOCs）,导致火点源及周边地区大气中主要氧化剂浓度上升,提升了区域大气氧化能力;当携带大量VOCs的秸秆燃烧烟羽与以化石燃料排放为主的城市气团相混合时,大气氧化性增强会加速城市地区人为源排放的NO_x和SO₂等气态前体物的氧化过程,提高硫酸盐和硝酸盐的形成速率、促进二次无机气溶胶的生成。     

Observed changes in aerosol physical and optical properties before and after precipitation events

Precipitation scavenging of aerosol particles is an important removal process in the atmosphere that can change aerosol physical and optical properties. This paper analyzes the changes in aerosol physical and optical properties before and after four rain events using in situ observations of mass concentration, number concentration, particle size distribution, scattering and absorption coefficients of aerosols in June and July 2013 at the Xianghe comprehensive atmospheric observation station in China. The results show the effect of rain scavenging is related to the rain intensity and duration, the wind speed and direction. During the rain events, the temporal variation of aerosol number concentration was consistent with the variation in mass concentration, but their size-resolved scavenging ratios were different. After the rain events, the increase in aerosol mass concentration began with an increase in particles with diameter 0.8 μm [measured using an aerodynamic particle sizer(APS)], and fine particles with diameter 0.1 μm [measured using a scanning mobility particle sizer(SMPS)]. Rainfall was most efficient at removing particles with diameter ～0.6 μm and greater than 3.5 μm. The changes in peak values of the particle number distribution(measured using the SMPS) before and after the rain events reflect the strong scavenging effect on particles within the 100–120 nm size range. The variation patterns of aerosol scattering and absorption coefficients before and after the rain events were similar, but their scavenging ratios differed, which may have been related to the aerosol particle size distribution and chemical composition.     

Size Distributions of Aerosol Sulfates and Nitrates in Beijing during the 2008 Olympic Games: Impacts of Pollution Control Measures and Regional Transport

For the 2008 Olympic Games, drastic control measures were implemented on industrial and urban emissions of sulfur dioxide (SO₂), nitrogen oxides (NO_x) and other pollutants to address the issues of poor air quality in Beijing. To investigate the effects of SO₂ and NO_x reductions on the particulate sulfate and nitrate concentrations as well as their size distributions, size-segregated aerosol samples were collected using micro-orifice uniform deposit impactors (MOUDIs) at urban and downwind rural sites in Beijing before and after full-scale controls. During the sampling period, the mass concentrations of fine particles (PM_1.8) at the urban and rural sites were 94.0 and 85.9 μg m^-3, respectively. More than 90% of the sulfates and ～60% of nitrates formed as fine particles. Benefiting from the advantageous meteorological conditions and the source controls, sulfates were observed in rather low concentrations and primarily in condensation mode during the Olympics. The effects of the control measures were separately analyzed for the northerly and the southerly air-mass-dominated days to account for any bias. After the control measures were implemented, PM, sulfates, and nitrates were significantly reduced when the northerly air masses prevailed, with a higher percentage of reduction in larger particles. The droplet mode particles, which dominated the sulfates and nitrates before the controls were implemented, were remarkably reduced in mass concentration after the control measures were implemented. Nevertheless, when the polluted southerly air masses prevailed, the local source control measures in Beijing did not effectively reduce the ambient sulfate concentration due to the enormous regional contribution from the North China Plain.     

泽当、景洪大气气溶胶粒子的物理、化学特性

利用 1 997～ 1 999年在西藏泽当、云南景洪观测地飞得到的大气气溶胶资料 ,分析了气溶胶粒子的物理化学特性 ,包括质量浓度、数浓度、光学吸收系数和化学组成 ,初步讨论了有关的影响因子 ,并同国内外其它地区的观测结果进行了比较。结果表明 ,大气气溶胶粒子在以上两地以及与其它地区之间存在明显的差异     

Size dependent partitioning of organic material: evidence for the formation of organic coatings on aqueous aerosols

Organic aerosol formation resulting from the ozonolysis of α-pinene, myrcene and sabinene was investigated in a large aerosol chamber in the presence of aqueous seed aerosols. The chemical composition of the particles was monitored by an aerosol mass spectrometer (Aerodyne Research Inc.) as a function of time and the particle size. Smaller particles were found to contain more organics relative to sulfate than the larger ones. In contrast, the water to sulfate mass ratio was not dependent on the particle size. These experimental findings indicate the formation of organic layers on the particles. With the aid of an aerosol dynamic model we demonstrate that the observations are consistent with the formation of multilayered organic films having thicknesses of approximately 10 nm. The results also suggest that the films were formed through condensation of low-volatile oxidation products that did not take up water considerably. Even though dissolution of oxidation products into the particle aqueous phase cannot be conclusively ruled out, the most plausible interpretation of the results is that the monoterpene ozonolysis lead to the formation of organic coatings on aqueous aerosols. Such films are likely to form in regions with monoterpene emissions.     

Development of RAMS-CMAQ to Simulate Aerosol Optical Depth and Aerosol Direct Radiative Forcing and Its Application to East Asia

The air quality modeling system RAMS （Regional Atmospheric Modeling System）-CMAQ （Models-3 Community Multi-scale Air Quality） is developed to simulate the aerosol optical depth （AOD） and aerosol direct forcing （DF）. The aerosol-specific extinction, single scattering albedo, and asymmetry factor are parameterized based on Mie theory taking into account the aerosol size distribution, composition, refractive index, and water uptake of solution particles. A two-stream solar radiative model considers all gaseous molecular absorption, Rayleigh scattering, and aerosols and clouds. RAMSCMAQ is applied to simulate all major aerosol concentrations （e.g., sulfate, nitrate, ammonium, organic carbon, black carbon, fine soil, and sea salt） and AOD and DF over East Asia in 2005. To evaluate its performance, the simulated AOD values were compared with ground-based in situ measurements. The comparison shows that RAMSCMAQ performed well in most of the model domain and generally captured the observed variations. High AOD values （0.2-1.0） mainly appear in the Sichuan Basin as well as in central and southeastern China. The geographic distribution of DF generally follows the AOD distribution patterns, and the DF at the top-of-the-atmosphere is less than -25 and -20 W m^-2 in clear-sky and all-sky over the Sichuan Basin. Both AOD and DF exhibit seasonal variations with lower values in July and higher ones in January. The DF could obviously be impacted by high cloud fractions.     

Assessment of the first indirect radiative effect of ammonium-sulfate-nitrate aerosols in East Asia

A physically based cloud nucleation parameterization was introduced into an optical properties/radiative transfer module incorporated with the off-line air quality modeling system Regional Atmospheric Modeling System (RAMS)-Models-3 Community Multi Scale Air Quality (CMAQ) to investigate the distribution features of the first indirect radiative effects of sulfate, nitrate, and ammonium-sulfate-nitrate (ASN) over East Asia for the years of 2005, 2010, and 2013. The relationship between aerosol particles and cloud droplet number concentration could be properly described by this parameterization because the simulated cloud fraction and cloud liquid water path were generally reliable compared with Moderate Resolution Imaging Spectroradiometer (MODIS) retrieved data. Simulation results showed that the strong effect of indirect forcing was mainly concentrated in Southeast China, the East China Sea, the Yellow Sea, and the Sea of Japan. The highest indirect radiative forcing of ASN reached ?3.47 W m^?2 over Southeast China and was obviously larger than the global mean of the indirect forcing of all anthropogenic aerosols. In addition, sulfate provided about half of the contribution to the ASN indirect forcing effect. However, the effect caused by nitrate was weak because the mass burden of nitrate was very low during summer, whereas the cloud fraction was the highest. The analysis indicated that even though the interannual variation of indirect forcing magnitude generally followed the trend of aerosol mass burden from 2005 to 2013, the cloud fraction was an important factor that determined the distribution pattern of indirect forcing. The heaviest aerosol loading in North China did not cause a strong radiative effect because of the low cloud fraction over this region.     

不同吸湿性的气溶胶对云和降水影响研究进展

气溶胶、云、降水相互关系是现今大气科学的前沿领域。本文总体概括了气溶胶作为云凝结核和冰核,对云宏微观物理特性及降水的影响原理研究的主要成果。并根据气溶胶自身化学性质的吸湿性,从吸湿性气溶胶和非吸湿性气溶胶两方面,重点探讨了模拟研究中,硫酸盐、海盐、沙尘、黑碳气溶胶对于云和降水的影响,以及各类气溶胶与其它类型气溶胶相比,作用于云降水的不同方式。提出之前研究工作的不足,以期为今后该方向的研究提供一些思路。