Study on the Chemical Character of Water Soluble Organic Compounds in Fine Atmospheric Aerosol at the Jungfraujoch

In this study the chemical nature of the bulk of water soluble organic compounds in fine atmospheric aerosol collected during summer 1998 at the Jungfraujoch, Switzerland (3580 m asl) is characterised. The mass concentration of water soluble organic substances was similar to those of major inorganic ions, and the water soluble organic matter was found to be composed of two main fractions: (i) highly polyconjugated, acidic compounds with a varying degree of hydrophobicity and (ii) slightly polyconjugated, neutral and very hydrophilic compounds. The contribution of both fractions to the total water soluble organic carbon was about 50%. Separation into individual components was impossible either by HPLC or capillary electrophoresis which indicates the presence of a high number of chemically similar but not identical species. Results obtained by ultrafiltration and HPLC-MS have shown that the molecular weights are of the order of several hundreds. Most of the protonation constants for the acidic compounds determined by capillary electrophoresis were in the range 10⁴–10⁷.     

A Two-Moment Bulk Microphysics Coupled with a Mesoscale Model WRF: Model Description and First Results

The Chinese Academy of Meteorological Sciences (CAMS) two-moment bulk microphysics scheme was adopted in this study to investigate the representation of cloud and precipitation processes under different environmental conditions.The scheme predicts the mixing ratio of water vapor as well as the mixing ratios and number concentrations of cloud droplets,rain,ice,snow,and graupel.A new parameterization approach to simulate heterogeneous droplet activation was developed in this scheme.Furthermore,the improved CAMS scheme was coupled with the Weather Research and Forecasting model (WRF v3.1),which made it possible to simulate the microphysics of clouds and precipitation as well as the cloud-aerosol interactions in selected atmospheric condition.The rain event occurring on 27-28 December 2008 in eastern China was simulated using the CAMS scheme and three sophisticated microphysics schemes in the WRF model.Results showed that the simulated 36-h accumulated precipitations were generally agreed with observation data,and the CAMS scheme performed well in the southern area of the nested domain.The radar reflectivity,the averaged precipitation intensity,and the hydrometeor mixing ratios simulated by the CAMS scheme were generally consistent with those from other microphysics schemes.The hydrometeor number concentrations simulated by the CAMS scheme were also close to the experiential values in stratus clouds.The model results suggest that the CAMS scheme performs reasonably well in describing the microphysics of clouds and precipitation in the mesoscale WRF model.     

华北夏季不同月份降水的年代际变化

利用９５１年到１９９６年华北地区１７个站的月降水资料,分析了华北地区夏季各月降水的年代际变化特征,结果表明：６月降水量较少,且在年代际变化下没有表现出减少趋势;７月降水量较多,年代际变化较大,８０年代是少;８月的降水量在年代际变化上表现出线性减少的趋势并呈准１０年周期的振荡,７月和８月的降水量均在６０年代中期和从７０年代末到８０年代初有两次明显的减少。根据７、８月降水不同的年代际变化特征,我们利用     

Surface Tension Effects of Humic-Like Substances in the Aqueous Extract of Tropospheric Fine Aerosol

Organic aerosol constituents can influence the surface tension of nucleating cloud droplets and thereby modify the critical supersaturation necessary to activate aerosol particles. Model calculations, based on experiments carried out with different surrogates, led to contradictory conclusions on the effect of organic components on activation, indicating that the results depend very much on the surrogate selected. In order to reduce this uncertainty surface tension measurements were performed on real atmospheric aerosol components. Humic-like substances (HULIS) that accounted for 60% of the water-soluble organic carbon present in rural aerosol were isolated from 32 samples covering different seasons. The isolated organic matter present in a concentration of about 1 g L^–1, decreased the surface tension of the aqueous solutions by 25–42% as compared to pure water. This effect was further enhanced when humic-like substances were mixed with ammonium sulphate. In order to support model calculations Szyskowski functions were fitted to the data to formulate the surface tension effect as a function of concentration.Finally, natural humic substances (fulvic and humic acids) were investigated under the same conditions. The experiments revealed that the surface tension decreasing effect of atmospheric humic-like substances differed from that of the studied terrestrial and aquatic humic substances: the latter substances decreased the surface tension of the aqueous solution to a lesser extent (7–23%) than atmospheric HULIS. This deviation can be explained with the different composition (e.g. the ratio of aromatic to aliphatic moieties) of the substances investigated.     

Characterization of Water-Soluble Macromolecular Substances in Cloud Water

In this contribution we present to our knowledge the first investigations of macromolecular, often called humic-like substances (HULIS) in cloud water samples and compare them with water-soluble extracts from atmospheric PM_2.5, soils and waters to study its possible origin. Chemical analysis was done using high performance liquid chromatography (HPLC) coupled with UV and diode array detector, and HPLC coupled with ESI-MS (electrospray ionization mass spectrometer). The data have been treated by principle component analysis (PCA) and cluster analysis to state similarities and/or differences between different types of samples. Our results show that the content of organic and inorganic species is distinctly different in smaller and larger droplets suggesting varying origin. We conclude that smaller droplets are formed more from organic containing condensation nuclei (CCN) and larger droplets more from inorganic containing CCN organic compounds. Putting all experimental findings together we state that HULIS in cloud water—and consequently in particulate CCN precursors—are produced in an atmospheric polymerization process from low molecular weighted organics of different origin. Evidence is found that anthropogenic sources contribute to this pathway. Cloud drops may act as reactor in this HULIS formation process but more likely are gas-phase or gas-to-particle interactions.     

Organic carbon accumulation rates in the Holocene and glacial Arabian Sea: implications for O2-consumption in the deep-sea and atmospheric CO2 variations

Variations in the deep-sea carbon reservoir have been invoked to explain the observed atmospheric carbon dioxide (CO₂) changes during glacial-interglacial cycles. In order to distinguish between the quantity of organic matter remineralized in the deep-sea and that permanently removed into sediments, we compared the bulk- and organic carbon-accumulation rates in Holocene and glacial sediments deposited below the oxygen minimum layer with total- and organic carbon fluxes to the deep Arabian Sea from continuous sediment trap deployments. This comparison shows that the mass of organic carbon remineralized at the sediment water interface is mainly a function of the bulk sediment flux. The oxygen consumed by the organic carbon remineralization is of the order of the observed oxygen deficiency of the modern deep Arabian Sea water. We use the evidence from the northern Indian Ocean to speculate on the possible effect of abiogenic mineral flux on the removal of organic carbon from upper layers of the world ocean to the deep-sea. We assume that if the bulk accumulation rate (not primary productivity) influences the flux of organic carbon (that is fixed from the atmosphere by marine organisms), then mineral matter flux will exert a significant control over atmospheric CO₂ contents. Model calculations incorporating transient changes in global bulk flux, caused by natural or anthropogenic changes, show that significant proportions of the observed changes in atmospheric CO₂ contents can be explained by this mechanism.This paper was presented at Clima Locarno 90, the International Conference on Past and Present Climate Dynamics: Reconstruction of Rates of Change, held in Locarno, Switzerland, September 24 to 28, 1991, organized by the Swiss National Climate Program — ProClim, with support from the Swiss Academy of Sciences. Guest editor for these papers is Dr. K. Kelts Offprint requests to: F Sirocko     

Potential Atmospheric Transport Pathways for Mercury Measured in the Canadian High Arctic

Large-scale transport pathways for atmospheric gaseous mercury emitted from surrounding source regions to reach the Alert sampling site located at the Northwest Territories of Canada between August 1992 and August 1993 were investigated. The 12-month atmospheric mercury data set comprises blank-corrected total gaseous mercury (TGM) concentrations collected on gold-coated sand traps during one-week long sampling intervals. For TGM concentrations above the 12-month mean TGM level, the analysis reveals regions in Eastern Europe (close to East Germany and Poland), areas on Northeastern America in Canada (Northwest Territories), and central Siberia of the former U.S.S.R. Identification of the physical locations of the emission sources was limited by the temporal resolution of weekly averaged data; however, major atmospheric pathways of mercury transport to the Arctic were successfully resolved. The objective of this note is to demonstrate that the potential source contribution function could be applied to resolve the sources and recover transport pathways of atmospheric mercury over a large scale.     

阿尔泰山南坡1821-2014年树轮汞浓度变化及其对气候的响应

研究汞的历史环境水平,对于认识人为汞的再排放和评估汞污染治理的有效性有重要意义。然而全球大气汞的监测站点和监测数据有限,因此需要利用代用资料来表征大气汞的长期变化。树木年轮是记录大气汞变化趋势的潜在优质档案。本研究建立了阿尔泰山南坡青河地区1821-2014年的树轮汞浓度变化序列,分析了气候对树轮汞浓度的影响,并从全球和区域角度探讨了汞浓度变化的原因。结果表明：1821—2014年青河地区平均树轮汞浓度为1.36±0.28 ng·g-1。相关分析显示树轮汞浓度变化与年平均最低气温（r=0.268, p<0.05, n=57）和平均水汽压（r=0.326, p<0.05, n=57）呈显著正相关,与平均2分钟风速呈显著负相关（r=-0.356, p<0.01, n=57）,表明气候可能会影响树木年轮中汞的积累。1820s—1980s树轮汞浓度呈缓慢上升趋势,在此期间出现1850s—1860s中后期和1980s中后期两个峰值。1990s—2000s初期树轮汞浓度相对平稳。自2000s中后期,树轮汞浓度逐渐下降,可能与各国相继实施空气污染控制法规有关。     

Atmospheric driving mechanisms of extreme precipitation events in July of 2017 and 2018 in western Japan

The occurrence of extreme precipitation events is now a serious concern in recent years in Japan. This study explores the atmospheric driving mechanisms of two extreme precipitation events occurred during 5–6 July 2017 and 5–8 July 2018 over western Japan. We identified that the atmospheric transport of large amounts of moisture and wind streams with wind speed of minimum 15 m s⁻¹ from south of Japan towards north on the days before these torrential precipitation events are mainly responsible for the July 2017 and July 2018 floods over western Japan. However, the contributions from the moisture advections (both vertical and horizontal) to the atmospheric water budget plays key roles to intensify the precipitations during the said torrential events. We also find that the prominent moisture flux convergence and well-developed moist conditions mainly maintain these heavy precipitation events over the downpour affected area. Our overall analysis suggests that the atmospheric factors driving to all these two heavy precipitation events are qualitatively robust and vital to explain the mechanism of extreme precipitations.     

A Database for Volatile Organic Compounds

The database for volatile organic compounds (VOC data base) was created with the aim of providing an overview of tropospheric hydrocarbon measurements. The data base contains 202 substances, for which atmospheric and useful kinetic data such as rate coefficients, photolysis frequencies, mixing ratios, emission data and ozone formation potentials are compiled from available literature. The database file can be downloaded without charge from http://www.physchem.uni-wuppertal.de/voc-database. Registered users will be informed about the appearance of updates.     

Analysis of the data of long-term monitoring of atmospheric mercury content and meteorological parameters at Amderma polar station

Mercury is one of the most hazardous heavy metals and the mercury contamination is of serious danger for the Arctic environment. Mercury compounds are rather mobile and can easily migrate both to the water and to the air. Mercury is removed most intensively from the atmosphere during the polar springtime (so-called AMDE effect, i.e., the Atmospheric Mercury Depletion Event). This phenomenon was observed from the beginning of the polar sunrise till the end of the snowmelt, i.e., from April to early June. In 2000–2001, the depletion of atmospheric mercury was discovered in the Antarctic. In 2001, the mercury analyzer was installed at Amderma station located on the Yugor Peninsula, and AMDE cases were registered there during the measurements. The study in the Arctic region demonstrated that the effect of mercury depletion is observed at the rather limited space along the coast of the Arctic seas. The activation of AMDE is associated both with the intensive UV-radiation and with such meteorological parameters as temperature, wind speed and humidity in the surface layer that favors the mercury depletion in the atmosphere. This process is typical for the high latitudes only and is observed during about two-three months from the beginning of the polar sunrise until the end of the snowmelt.     

CAPPS多箱模式中光化学模式的嵌套与城市大气臭氧数值预报

为解决城市边界层中大气O₃浓度的预报问题，选用一种简明有效的光化学反应方案建立光化学模式, 并与大气平流扩散的箱格预报模型进行了嵌套，从而将大气化学过程引入到城市空气污染数值预报系统 (CAPPS) 中。同时，根据实际需要研究了VOC (Volatile Organic Compounds) 浓度及NO_x源排放量等参数缺测时，根据前期监测浓度采用遗传算法反演未知参数的具体方法。利用2001年9月8~17日在北京舞蹈学院监测的O₃、NO_x资料及相应的气象数据，用改进后的CAPPS模式进行了单箱预报试验。预报试验结果表明，嵌套后的模式对O₃浓度的变化具备一定的预报能力。     

Application of Non-Ionic Solid Sorbents (XAD Resins) for the Isolation and Fractionation of Water-Soluble Organic Compounds from Atmospheric Aerosols

A detailed procedure using non-ionic macropourous XAD-8 and XAD-4 resins is presented for the isolation and fractionation of aerosol water-soluble organic compounds (WSOC) from aerosol samples. The procedure entails adsorption of WSOC fraction onto XAD-8 and XAD-4 resins, desalting of the adsorbed organic material with ultra-pure water, elution of the retained organic matter with 40% MeOH solution and freeze-drying. Due to resin’s different properties and to certain hydrophobic/hydrophilic interactions between the resin polymers and the organic matter, two major fractions were obtained; namely the XAD-8 and the XAD-4 eluates. The XAD-8 eluate, which accounts for 55–60% of total aerosol WSOC, is represented by partially acidic compounds with significant hydrophobic moieties. The XAD-4 fraction holds few conjugated systems and a higher content of hydrophilic structures with low molecular size, and accounts for 9% of total WSOC. The isolated WSOC sub-fractions were nearly free from inorganic species, and successful recoveries of organic matter from the resins were accomplished. With this procedure the XAD-8 eluate yields a mixture representative of those WSOC that are highly conjugated compounds in atmospheric aerosols. It also allows a successful characterisation of the organic material by advanced analytical techniques without the interference of inorganic species present in the original sample of atmospheric particles.     

夹卷对郊外大气边界层内臭氧影响的数值模拟研究

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、NO_x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（NO_X）和可挥发性有机物(VOC_S)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。      

Effect of atmospheric humic-like substances on the enhanced dissolution of volatile organic compounds into dew water

Simultaneous sampling of chlorinated hydrocarbons (CHs) and monocyclic aromatic hydrocarbons (MAHs), potentially harmful to humans and/or responsible for the formation of ozone and secondary particles, in dew water and in the ambient air was carried out from August 2004 to July 2005 in Hino City, situated in the western part of Greater Tokyo, Japan. CHs were less contained in dew water than MAHs. Toluene (volume-weighted mean concentration, VWM: 4.77 nM) and m,p-Xylenes (VWM: 5.07 nM) except dichloromethane, which was abnormally high (VWM: 1.14 μM), were abundant among eleven VOCs determined in dew water. Chloroform, carbon tetrachloride, 1,2-dichloroethane, and benzene were not detected in dew water during the study period. Dew water contained higher amounts of VOCs than would have been expected from the ambient gas-phase concentrations and the temperature-corrected Henry's law constants. Following the determination method of humic substances in river water proposed by Hiraide et al. [Hiraide, M., Shima, T., Kawaguchi, H., 1994. Separation and determination of dissolved and particulate humic substances in river water. Mikrochim. Acta 113, 269–276], the VWM of soluble humic and fulvic acid fractions in dew water was found to be 1.00 mg/L and 0.87 mg/L (n = 20), respectively, while the VWM of particulate humic and fulvic acid fractions was found to be 0.61 mg/L and 0.42 mg/L (n = 20), respectively. Surface tension decreased with an increase in dissolved fulvic acid fraction in dew water, indicating that humic-like substances with relatively lower molecular weight, which is soluble in acid solution, could be an effective surface-active species within dew water. The enrichment factors, which were defined as the ratio of the observed VOCs concentration to the estimated, were over 10² for MAHs except for benzene and increased as the increment of total humic-like substances (HULIS) concentration (the sum of humic and fulvic acid fractions in both dissolved and particulate form) normalized by total inorganic ion concentration in dew water. Our results indicate that total HULIS in dew water could enhance the dissolution of atmospheric VOCs into dew droplets.     

Photooxidation of Methacrolein in Fe(Ⅲ)-Oxalate Aqueous System and Its Atmospheric Implication

Iron and oxalic acids are widely distributed in the atmosphere and easily form ferric oxalate complex (Fe(Ⅲ)-Ox). The tropospheric aqueous-phase could provide a medium to enable the photo-Fenton reaction with Fe(Ⅲ)-Ox under solar irradiation. Although the photolysis mechanisms of Fe(Ⅲ)-Ox have been investigated extensively, information about the oxidation of volatile organic compounds (VOC), specifically the potential for Secondary Organic Aerosol (SOA) formation in the Fe(Ⅲ)-Ox system, is lacking. In this study, a ubiquitous VOC methacrolein (MACR) is chosen as a model VOC, and the oxidation of MACR with Fe(Ⅲ)-Ox is investigated under typical atmospheric water conditions. The effects of oxalate concentration, Fe(Ⅲ) concentration, MACR concentration, and pH on the oxidation of MACR are studied in detail. Results show that the oxidation rate of MACR greatly accelerates in the presence of oxalate when compared with only Fe(Ⅲ). The oxidation rate of MACR also accelerates with increasing concentration of oxalate. The effect of Fe(Ⅲ) is found to be more complicated. The oxidation rate of MACR first increases and then decreases with increasing Fe(Ⅲ) concentration. The oxidation rate of MACR increases monotonically with decreasing pH in the common atmospheric water pH range or with decreasing MACR concentration. The production of ferrous and hydrogen peroxide, pH, and aqueous absorbance are monitored throughout the reaction process. The quenching experiments verify that ·OH and (O-·2) are both responsible for the oxidation of MACR. MACR is found to rapidly oxidize into small organic acids with higher boiling points and oligomers with higher molecular weight, which contributes to the yield of SOA. These results suggest that Fe(Ⅲ)-Ox plays an important role in atmospheric oxidation.     

Precipitation Chemistry in the Sahelian Savanna of Niger, Africa

Within the framework of the IDAF (IGAC DEBITS AFRICA) network, we present in this paper data on precipitation and aerosol chemistry in the semiarid savanna of the Sahelian region of Niger. An automatic wet-only precipitation collector was operated at the Banizoumbou station during the entire 1996 rainy season (June to September 1996). Inorganic (Na⁺, NH ₄ ⁺ , K⁺, Mg²⁺, Ca²⁺, Cl^-, NO ₃ ^- , SO ₄ ^2- ) and organic contents of the precipitation (HCOOH, CH₃COOH, C₂H₅COOH) were determined by Ion Chromatography (IC) in 29 rainfall events. Once per week, bulk particle samples were collected on the same site, and soluble water material was determined by IC. We examined the influence of atmospheric gas and particle sources on the precipitation and aerosol chemical contents. We established the influence of marine, terrigenous, and biogenic sources in the Sahelian region. The terrigenous signature is dominant and related to Sahelian soil erosion, with a high calcium content in precipitation (31.2 eq L^-1) and in aerosols (1.8 g m^-3). Two other signatures of atmospheric sources are highlighted by the relatively high nitrogenous (ammonium and nitrate) and organic contents (formate, acetate) in the precipitation. Ammonium (12.9 eq L^-1) and nitrate (12.3 eq L^-1) contents confirm respectively the biogenic source of ammonia released by domestic animal excreta in Niger and the natural emissions from semiarid savannas soils, perturbed by wild or domestic animal grazing. In spite of a high potential acidity given by nitrate, formate and acetate; a weak acidity (H⁺ (2.1 eq L^-1) is calculated from the mean pH of 5.67 measured. A statistical analysis of the aerosol chemical composition clearly indicates that nitrates are strongly correlated at the 1% level with terrigenous ions, i.e., Ca²⁺ and Mg²⁺ (0.95 < r < 1). We observed a similar relationship between all the terrigenous ions and nitrate in the precipitation. In the Sahelian region, alkaline soil dust representative of the terrigenous contribution interact, with gaseous nitrogenous and carbonaceous compounds, leading to the neutralization of acid gases and subsequent weak acidity in precipitation. Finally, taking into account the main chemical characteristics of Banizoumbou precipitations and aerosols, which demonstrate the importance of heterogeneous and multiphase chemical processes, we propose a conceptual model of the atmospheric chemistry in the Sahelian region.     

NaCl Aerosol Particle Hygroscopicity Dependence on Mixing with Organic Compounds

Organic compounds in the atmosphere can influence the activation, growth and lifetimes of haze, fog and cloud droplets by changing the condensation and evaporation rates of liquid water by these aqueous aerosol particles. Depending on the nature and properties of the organic compounds, the change can be to enhance or reduce these rates. In this paper we used a tandem differential mobility analyzer (TDMA) to examine the effect of tetracosane, octanoic acid, and lauric acid on the hygroscopic properties of NaCl aerosol particles at relative humidities (RH) between 30 and 95%. These organic compounds have been identified in ambient aerosol particle samples. A slight lowering of the deliquescence relative humidity (DRH) and suppression of hygroscopic growth for the NaCl-organic compound mixtures were observed when compared to pure NaCl particles. The growth of pure NaCl particles was 2.25 in diameter at 85% RH while the growth of the mixed particles was 1.3 to 1.7 in particle diameter at 85% RH with organic mass fraction of 30–50%. This shows that these organic compounds have to be present in rather large mass fractions to effect the hygroscopic behavior to a similar degree observed for ambient aerosol during field measurements. Despite the mixing of the organic material with NaCl, hysteresis was observed for decreasing RH histories, suggesting the formation of metastable droplets. These laboratory results are strikingly similar to ambient field results. For example, if the total organic mass fraction of the particles is between 0.30 and 0.50, the particle growth at 85% RH is about a factor of 1.4 for the laboratory and field measurements. Such reduction in growth compared to the pure inorganic salt is in contradiction to speculations concerning significant effects by organic compounds on cloud condensation nuclei and thus formation on clouds.     

内蒙古春季降水的气候特征及预测思路

采用1961—2016年春季(3—5月)内蒙古逐月降水资料,应用统计相关分析、REOF,对比分析等方法分析研究了内蒙古地区春季降水类型的气候特征以及海洋和大气环流特征。可以发现,内蒙古春季降水具有明显的地域性特征,分为4个类型:全区偏少型,全区偏多型,中西部偏多、东部偏少型,东部偏多、中西部偏少型。研究结果说明,春季降水的大气环流形势受ENSO事件影响。AO的正、负位相对内蒙古不同地区造成不同影响,正位相时有利于中西部降水偏多,负位相时有利于东部偏多。西伯利亚高压偏强,东亚大槽偏弱、偏西,冬季青藏高原积雪偏多,西太平洋副热带高压偏强、偏西,降水落区处在低压槽后,冷空气较为活跃,配合暖湿水汽输送条件,冷暖气流在内蒙古地区交汇便形成多雨区;反之亦然。研究结果对预报员预测思路具有预测指导意义。     

Chemical character of precipitation and related particles and trace gases in the North and South of China

Rainwater samples were collected at four sites, including Beijing and Mazhuang Town in the north of China, Shenzhen and Mangdang Mountain in the south of China. Character of atmospheric particles and gases were also measured at Mazhuang Town and Mangdang Mountain. Both of Beijing and Shenzhen are urban sites; Mazhuang Town and Mangdang Mountain are rural and remote sites respectively. The atmospheric pollution at rural plain site in the north of China was more serious than that at remote mountain site in the south of China. At Beijing, Mazhuang Town, Shenzhen and Mangdang Mountain the average pH values in rainwater were 6.02, 5.97, 4.72 and 4.81, respectively and the concentrations of total ions in rainwater were 1454, 1125, 187 and 191 μeq/l, respectively. While the acidity of the rain was higher in the south than that in the north, the rainwater in the north of China was more severely polluted than that in the south. The major acidic ion in the rainwater is SO₄^2-, and NH₄⁺ is the most important neutralizing ion in rainwater at the four sites, followed by Ca²⁺. The amounts of organic acid in precipitation were compared with other sites in the world. The ratios of organic acid to total free acid in rainwater at Mangdang Mountain was 13.8% and the influence of organic acid on acidity of rainwater at mountain site in the south of China is more important. The variation of atmospheric particles, gases and components in rainwater and cloud-fog water during special rain and cloud-fog events was discussed. The importance of washout process varied with atmospheric species. The impacts of rainfall, rain duration time and wind speed on wash-out process were estimated by regression analysis.