The characterization and distribution of aerosol and gaseous species in the winter monsoon over the western pacific ocean

During the winters of 1981 and 1982, measurements were taken on two Japanese islands of the aerosol and gaseous species which had been carried by northwesterly monsoons over the Pacific Ocean. The aerosols were characterized as sea-salt particles; soil particles, and as particles of sulfate, nitrate, organics and elemental carbon. At Chichi-jima island, which is about 800 km away from the main islands of Japan, it was found that the level of the anthropogenic components of the aerosols was considerably higher than their background level. The mean concentrations of the species on the islands are given in tabular forms. According to a survey made on board a ferry boat, the aerosol and gaseous species were fairly uniformly distributed along the southern coast of the main Japanese islands.     

不同污染条件下气溶胶对短波辐射通量影响的模拟研究

将高光谱分辨率的气溶胶光学参数化方案应用于高精度的辐射传输模式BCC_RAD（974带）中,研究不同污染状况下气溶胶在地表与近地层大气中造成的直接辐射强迫与辐射强迫效率。发现气溶胶在地表产生的直接辐射强迫为负,在近地层大气中产生的直接辐射强迫为正,且随气溶胶浓度的升高变大,说明大气气溶胶的含量越高,单位气溶胶光学厚度产生的直接辐射强迫越大。将短波划分为3个波段:紫外、可见光和近红外,发现在紫外、可见光和近红外波段中,不同污染状况下气溶胶在地表造成的直接辐射强迫范围分别为:-1.36—-13.66、-3.03—-32.41和-2.74—-28.62 W/m2,在近地层大气中产生的直接辐射强迫范围分别为0.44—4.26、0.99—9.80和0.93—8.87 W/m2。通过进一步对比自然和人为气溶胶的影响,发现人为气溶胶在地表和大气层顶产生的负直接辐射强迫以及对整层和近地面大气造成的正直接辐射强迫均大于自然气溶胶的影响,且上述两种排放源的气溶胶对整层大气辐射收支的影响主要集中在800 hPa高度以下的大气中。按照地表直接辐射强迫大小来分析不同种类气溶胶的影响,结果为硫酸盐>有机碳>黑碳>海盐>沙尘;按照近地层大气直接辐射强迫大小排序则为黑碳>有机碳>沙尘>海盐>硫酸盐。最后,通过分析散射型气溶胶与吸收型气溶胶对辐射通量的影响,还探究了大气中散射与吸收过程的异同。      

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.     

Biogenic hydrogen sulphide emissions and non-sea sulfate aerosols over the Indian Sundarban mangrove forest

Temporal variations in atmospheric hydrogen sulphide concentrations and its biosphere-atmosphere exchanges were studied in the World’s largest mangrove ecosystem, Sundarbans, India. The results were used to understand the possible contribution of H₂S fluxes in the formation of atmospheric aerosol of different size classes (e.g. accumulation, nucleation and coarse mode). The mixing ratio of hydrogen sulphide (H₂S) over the Sundarban mangrove atmosphere was found maximum during the post-monsoon season (October to January) with a mean value of 0.59?±?0.02 ppb and the minimum during pre-monsoon (February to May) with a mean value of 0.26?±?0.01 ppb. This forest acted as a perennial source of H₂S and the sediment-air emission flux ranged between 1213?±?276 μg S m^?2 d^?1(December) and 457?±?114 μg S m^?2 d^?1 (August) with an annual mean of 768?±?240 μg S m^?2d^?1. The total annual emissions of H₂S from the Indian Sundarban were estimated to be 1.2?±?0.6 Tg S. The accumulation mode of aerosols was found to be more enriched with non-sea salt sulfate with an average loading of 5.74 μg m^?3 followed by the coarse mode (5.18 μg m^?3) and nucleation mode (1.18 μg m^?3). However, the relative contribution of Non-sea salt sulfate aerosol to total sulfate aerosol was highest in the nucleation mode (83%) followed by the accumulation (73%) and coarse mode (58%). Significant positive relations between H₂S flux and different modes of NSS indicated the likely link between H₂S, a dominant precursor for the non-sea salt sulfate, and non-sea sulfate aerosol particles. An increase in H₂S emissions from the mangrove could result in an increase in enhanced NSS in aerosol and associated cloud albedo, and a decrease in the amount of incoming solar radiation reaching the Sundarban mangrove forest.     

潮州沿海大气气溶胶无机离子浓度分布与气象要素的相关分析

根据2004年广东潮州沿海地区的气溶胶浓度观测资料,分析潮州沿海大气气溶胶无机离子浓度分布特征及气象要素对其的影响。结果表明:离子浓度季节性差异明显,总离子浓度呈现春夏季低、秋冬季高的特征,系由当地不同季节降雨量和风向分布不同造成的;气溶胶无机成分与海水近似,表明海盐是当地气溶胶的重要来源之一,但Cl-与Na+不一致,表明可能存在除海盐颗粒以外的异地气溶胶长距离输送;总离子浓度随采样点高度增加而降低,随采样时海陆风变化而变化;阳离子浓度日际变化不明显,阴离子浓度易受天气条件影响。     

青海瓦里关大气气溶胶元素富集特征及其来源

利用中子活化及PIXE和可见光灰度仪, 对青海瓦里关大气本底基准监测站的大气气溶胶样品进行了测量。通过元素相对浓度、富集因子和主因子分析等数据统计分析, 并结合同期的气团后退轨迹分布资料, 讨论了瓦里关大气气溶胶元素的组成及来源。结果表明, 位于青藏高原偏远地区的瓦里关大气气溶胶以土壤及地壳等自然来源为主, 因子分析的方差百分数给出瓦里关气溶胶中自然源的贡献率平均在70%以上。燃煤、交通及冶炼等人为源也占有一定比例。大气黑碳气溶胶的观测也表明人类活动影响的存在。人为源的影响多与来自东部及河西走廊等经济发达地区的气流有关。     

The aerosol module in the INM RAS climate model

The aerosol module is included into the INM RAS climate model. The module computes the evolution of main aerosols: sea salt, mineral dust, sulfate aerosol, and black and organic carbon. Aerosol surface fluxes, advection, gravitational sedimentation, surface absorption, and scavenging by precipitation are taken into account to compute aerosol concentration variations. Model aerosol distribution is used to compute radiation fluxes. The ten-year run of the climate model is performed. The climatology of model aerosol is considered. The aerosol mass, integral source values, optical thickness, and radiative forcing are presented. The results are compared with the data of other models and observations.     

A study on the precipitation in Izmir,Turkey: chemical composition and source apportionment by receptor models

The chemistry of rainwater was studied in three sites of a metropolitan city of Turkey to determine the spatial variation, sources affecting composition and the extent of their influence. The acidity of rainwater, Ca, Co, Cr, Zn, Ba, V and Ni showed significant spatial variations. The most of measured species were moderately to extremely enriched compared to the local soil, which is likely arisen from the anthropogenic activities. SO₄ ^2?, K and Ca were found to be predominantly non-sea origin. Two receptor models, Positive Matrix Factorization (PMF) and Chemical Mass Balance (CMB), agreed well on the source contribution estimations of Al, K, Zn, V, Pb and Cr. The PMF and CMB resolved very similar source contribution profiles to the elemental concentrations of Ca, Zn, V, Pb, K and Na, which the majority of those resulted from mineral industries, bell casting+steel industries, fossil fuel burning, biomass burning+sea salt and sea salt, respectively. The PMF resolved the source contributions of long-transported emissions, particularly for Ba, Sr and Mn, which could not be estimated by the CMB.     

非洲地区大气气溶胶光学厚度时空变化及亚速尔高压对沙尘越大西洋传输的影响

研究了非洲地区大气气溶胶光学厚度（AOD）的时空变化及沙尘气溶胶越大西洋海区的传输。结果表明：1）源于撒哈拉沙漠的沙尘及其随赤道东风向西输送使得沙尘气溶胶成为非洲沙漠地区和紧邻的大西洋海区的主要气溶胶组分;AOD高值区和沙尘气溶胶光学厚度高值区在1—7月随赤道辐合带北移同步向北移动,而在8—12月则向南回撤。2）刚果盆地大气气溶胶主要为热带雨林和稀树草原排放的有机碳（OC）和黑碳（BC）气溶胶;其中与生物质燃烧源排放有关的OC、BC高值主要集中在干季（6—9月）的后半段（8—9月）;而生物源OC排放全年连续,其排放峰值出现于雨季开始时;生物质燃烧排放高值期与生物源排放高值期前后相继,形成干季（尤其是后半段）时期的OC、BC光学厚度高值。3）亚马逊河入海口地区主要气溶胶组分为海盐气溶胶,9—11月该区风力输送增强,风向由东南风转变为东风,海盐进入亚马逊河入海口处,形成AOD和海盐气溶胶光学厚度高值区。4）撒哈拉沙漠沙尘气溶胶向大西洋传输的偏北月份为7—9月、偏南月份为1—3月;2000—2016年海区沙尘气溶胶的传输路径存在向南移动的变化趋势,与同期亚速尔高压的增强和沙尘传输路径以北北风分量的增强以及赤道辐合带的移动一致。上述研究结果揭示了利用大气气溶胶时空变化特征反映区域大气环流和气候变化的可能性。     

南京市主城区大气颗粒物来源探讨

在2005-05-03——05-27期间,用Anderson九级采样器在南京市两个采样点采集大气气溶胶样品,同时进行了部分排放源的采集。用X射线—荧光光谱仪(XRF)分析得到气样及源样中PM10的化学成分,分析了南京市大气气溶胶的元素质量谱分布,进行了PM10的富集因子分析,并应用化学质量平衡法(CMB)计算各类源对气溶胶PM10的贡献。结果表明,各类污染源对南京市气溶胶PM10的贡献率分别为:建筑尘(35.45%)、煤烟尘(22.13%)、土壤尘(20.27%)、硫酸盐(5.43%)、汽车尘(4.61%)、海盐(1.91%)、冶炼尘(1.69%)、其它源(8.51%)。文中还结合了南京市TSP和PM2.5的来源解析结果,分析了南京市不同粒径气溶胶颗粒物的污染特征。     

北京地区夏季背景气溶胶的特征

本文通过对观测资料的统计分析和比较研究,初步揭示了北京地区夏季背景气溶胶的一些特征,其中包括元素浓度及其变化、富集因子和气溶胶来源等。     

人为气溶胶对中国东部冬季风影响的模拟研究

采用美国国家大气研究中心(NCAR)的公共大气模式CAM5.1研究了人为气溶胶排放增加对中国东部冬季风的影响,同时通过对比中国东部地区不同人为气溶胶排放源的敏感性试验结果,探讨了人为硫酸盐、黑碳及总人为气溶胶(硫酸盐+黑碳)增加对东亚冬季风的影响。结果表明:冬季硫酸盐气溶胶排放增加的直接和第一间接效应减少了到达地表的短波辐射通量,引起了陆地地表和对流层低层降温,海平面气压升高,增加了海陆间气压梯度,使得东亚冬季风增强。其第二间接效应导致中国南部大尺度降水率减少;黑碳气溶胶排放增加导致到达地表的短波辐射通量减少和大气中短波辐射通量增加,其半直接效应部分抵消了直接效应,故地表温度变化微小且不显著。加热的对流层低层导致中国南部对流活动和对流降水率增加;总人为气溶胶排放增加导致的大气温度变化表现为弱的降温作用,引起中国北部对流和大尺度降水率减少,而南部对流降水率增加。总人为气溶胶和黑碳气溶胶排放增加是导致中国北(南)部的东亚冬季风增强(减弱)的重要因素。     

Greenhouse-gas versus aerosol forcing and African climate response

There are many indicators that human activity may change climate conditions all around the globe through emissions of greenhouse gases. In addition, aerosol particles are emitted from various natural and anthropogenic sources. One important source of aerosols arises from biomass burning, particularly in low latitudes where shifting cultivation and land degradation lead to enhanced aerosol burden. In this study the counteracting effects of greenhouse gases and aerosols on African climate are compared using climate model experiments with fully interactive aerosols from different sources. The consideration of aerosol emissions induces a remarkable decrease in short-wave solar irradiation near the surface, especially in winter and autumn in tropical West Africa and the Congo Basin where biomass burning is mainly prevailing. This directly leads to a modification of the surface energy budget with reduced sensible heat fluxes. As a consequence, temperature decreases, compensating the strong warming signal due to enhanced trace gas concentrations. While precipitation in tropical Africa is less sensitive to the greenhouse warming, it tends to decrease, if the effect of aerosols from biomass burning is taken into account. This is partly due to the local impact of enhanced aerosol burden and partly to modifications of the large-scale monsoon circulation in the lower troposphere, usually lagging behind the season with maximum aerosol emissions. In the model equilibrium experiments, the greenhouse gas impact on temperature stands out from internal variability at various time scales from daily to decadaland the same holds for precipitation under the additional aerosol forcing. Greenhouse gases and aerosols exhibit an opposite effect on daily temperature extremes, resulting in an compensation of the individual responses under the combined forcing. In terms of precipitation, daily extreme events tend to be reduced under aerosol forcing, particularly over the tropical Atlantic and the Congo basin. These results suggest that the simulation of the multiple aerosol effects from anthropogenic sources represents an important factor in tropical climate change, hence, requiring more attention in climate modelling attempts.     

Size distribution and chemical composition of marine aerosols: a compilation and review

Some 30 years of physical and chemical marine aerosol data are reviewed to derive global‐size distribution parameters and inorganic particle composition on a coarse 15°×15° grid. There are large gaps in geographical and seasonal coverage and chemical and physical aerosol characterisation. About 28% of the grid cells contain physical data while there are compositional data in some 60% of the cells. The size distribution data were parametrized in terms of 2 submicrometer log‐normal distributions. The sparseness of the data did not allow zonal differentiation of the distributions. By segregating the chemical data according to the major aerosol sources, sea salt, dimethylsulfide, crustal material, combustion processes and other anthropogenic sources, much information on mass concentrations and contribution of natural and anthropogenic sources to the marine aerosol can be gleaned from the data base. There are significant meridional differences in the contributions of the different sources to the marine aerosol. Very clearly, we see though that the global marine surface atmosphere is polluted by anthropogenic sulfur. Only in the case of sulfur components did the coverage allow the presentation of very coarse seasonal distributions which reflect the spring blooms in the appropriate parts of the oceans. As an example of the potential value in comparing the marine aerosol data base to chemical transport models, global seasonal meridional MSA distributions were compared to modelled MSA distributions. The general good agreement in mass concentrations is encouraging while some latitudinal discrepancies warrant further investigations covering other aerosol components such as black carbon and metals.     

A Modeling Study of Seasonal Variation of Atmospheric Aerosols over East Asia

In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM₁₀ (particles with aerodynamic diameter ≤10 μm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (～1000 μg m^-3), the Gobi Desert (～400 μg m^-3), and the Huabei Plain (～300 μm^-3) of China. Vertically, high PM₁₀ concentrations ranging from 100 μg m^-3 to 250 μg m^-3 occurred from the surface to an altitude of 6000 m at 30^o--45^oN in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ～42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.     

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。      

Equilibrium climate response of the East Asian summer monsoon to forcing of anthropogenic aerosol species

We used an online aerosol–climate model to study the equilibrium climate response of the East Asian summer monsoon (EASM) to increases in anthropogenic emissions of sulfate, organic carbon, and black carbon aerosols from 1850 to 2000. Our results show that each of these aerosol species has a different effect on the EASM as a result of changes in the local sea–land thermal contrast and atmospheric circulation. The increased emission of sulfate aerosol leads to a decrease in the thermal contrast between the land and ocean, a southward shift of the East Asian subtropical jet, and significant northerly wind anomalies at 850 hPa over eastern China and the ambient oceans, markedly dampening the EASM. An increase in organic carbon aerosol results in pronounced surface cooling and the formation of an anomalous anticyclone over the oceans north of 30°N. These effects cause a slight increase in the sea–land thermal contrast and southerly flow anomalies to the west of the anticyclonic center, strengthening the northern EASM. An increase in organic carbon emission decreases the sea–land thermal contrast over southern China, which weakens the southern EASM. The response of the summer 850-hPa winds and rainfall over the East Asian monsoon region to an increase in black carbon emission is generally consistent with the response to an increase in organic carbon. The increase in black carbon emission leads to a strengthening of the northern EASM north of 35°N and a slight weakening of the southern EASM south of 35°N. The simulated response of the EASM to the increase in black carbon emission is unchanged when the emission of black carbon is scaled up by five times its year 2000 levels, although the intensities of the response is enhanced. The increase in sulfate emission primarily weakens the EASM, whereas the increases in black carbon and organic carbon emissions mitigate weakening of the northern EASM.     

Elemental composition of particulate material sampled from the Arctic haze aerosol

Thirty-six aerosol filter samples collected in tropospheric Arctic haze layers, in the stratosphere, and in the marine boundary layer during the 1983 Arctic Gas and Aerosol Sampling Program were analyzed for trace elements using instrumental neutron activation analysis. Average crustal dust concentrations were 540 ng/m³ and 330 ng/m³ for samples collected in Arctic haze over the North American and Norwegian Arctic, respectively. An average marine salt concentration of 120 ng/m³ was obtained for haze samples collected above the marine boundary layer on both sides of the Arctic.Meteorological and wind trajectory information were used to identify specific haze transport pathways, which brought relatively unmixed aerosol from the central Soviet Union into the AGASP sampling areas. Results from individual filters collected within these transport zones are discussed, with emphasis on certain trace metal ratos which have been proposed by other researchers as discriminators of aerosols from different source regions. Our aircraft-collected data are compared with previously-collected ground-based measurements, and show reasonably good agreement for most tracer elements and ratios. Specifically, we have determined the As/Sb ratio tracer, named by other researchers as the most effective elemental discriminator of aerosol from the central Soviet Union, to be approximately 5–6. This relatively high tracer value is consistent with previous ground-based findings. A significantly lower V/Sb ratio was observed throughout this study, possibly indicating a change in the source signature.     

Aerosol modulation of atmospheric and surface solar heating over the tropical Indian Ocean

The major finding of this study is that aerosols over the tropical Indian Ocean enhance clear sky atmospheric solar heating significantly and decrease the surface solar heating by even a larger amount. The results presented here are based on aerosol chemical, microphysical, and optical and radiometric data collected at the island of Kaashidhoo (4.97°N, 73.47°E) during February and March of 1998, as part of the first field phase of the Indian Ocean experiment (INDOEX). The aerosol optical properties were integrated with a multiple scattering Monte Carlo radiative transfer model which was validated at the surface with broadband flux measurements and at the top of the atmosphere (TOA) with the clouds and earth's radiant energy system (CERES) radiation budget measurements. We consider both externally and internally mixed aerosol models with very little difference between the two models in the estimated forcing. For the February–March period, the aerosols increase the monthly mean clear sky atmospheric solar heating by about 12 W/m²(about 15% of the total atmospheric solar heating) and decrease the sea surface clear sky solar heating by about 16 W/m² with a daily range from 5 to 23 W/m². The net aerosol forcing at the top of the atmosphere is about −4 W/m² with a daily range from −2 to −6 W/m². Although the soot contributes only about 10% to the aerosol optical thickness, it contributes more than 50% to the aerosol induced atmospheric solar heating. The fundamental conclusion of this study is that anthropogenic aerosols over the tropical Indian Ocean are altering the clear sky radiation budget of the atmosphere and surface in a major manner.     

Fine mode aerosol chemistry over a tropical urban atmosphere: characterization of ionic and carbonaceous species

An extensive aerosol sampling program was conducted during January-December 2006 over Kolkata (22o33?? N and 88o20?? E), a mega-city in eastern India in order to understand the sources, distributions and properties of atmospheric fine mode aerosol (PM_2.5). The primary focus of this study is to determine the relative contribution of natural and anthropogenic as well as local and transported components to the total fine mode aerosol loading and their seasonal distributions over the metropolis. The average concentrations of fine mode aerosol was found to be 71.2?±?25.2???gm^-3 varying between 34.5???gm^-3 in monsoon and 112.6???gm^-3 in winter. The formation pathways of major secondary aerosol components like nitrate and sulphate in different seasons are discussed. A long range transport of dust aerosol from arid and semi-arid regions of western India and beyond was observed during pre-monsoon which significantly enriched the total aerosol concentration. Vehicular emissions, biomass burning and transported dust particles were the major sources of PM_2.5 from local and continental regions whereas sea-salt aerosol was the major source of PM_2.5 from marine source regions.