Investigation of Fundamental Processes Governing Secondary Organic Aerosol Formation in Laboratory Chambers

Our understanding of the processes and mechanisms by which secondary organic aerosol (SOA) is formed is derived from laboratory chamber studies. In the atmosphere, SOA formation is primarily driven by progressive photooxidation of SOA precursors, coupled with their gas-particle partitioning. In the chamber environment, SOA-forming vapors undergo multiple chemical and physical processes that involve production and removal via gas-phase reactions; partitioning onto suspended particles vs. particles deposited on the chamber wall; and direct deposition on the chamber wall. The main focus of this dissertation is to characterize the interactions of organic vapors with suspended particles and the chamber wall and explore how these intertwined processes in laboratory chambers govern SOA formation and evolution.

A Functional Group Oxidation Model (FGOM) that represents SOA formation and evolution in terms of the competition between functionalization and fragmentation, the extent of oxygen atom addition, and the change of volatility, is developed. The FGOM contains a set of parameters that are to be determined by fitting of the model to laboratory chamber data. The sensitivity of the model prediction to variation of the adjustable parameters allows one to assess the relative importance of various pathways involved in SOA formation.

A critical aspect of the environmental chamber is the presence of the wall, which can induce deposition of SOA-forming vapors and promote heterogeneous reactions. An experimental protocol and model framework are first developed to constrain the vapor-wall interactions. By optimal fitting the model predictions to the observed wall-induced decay profiles of 25 oxidized organic compounds, the dominant parameter governing the extent of wall deposition of a compound is identified, i.e., wall accommodation coefficient. By correlating this parameter with the molecular properties of a compound via its volatility, the wall-induced deposition rate of an organic compound can be predicted based on its carbon and oxygen numbers in the molecule.

Heterogeneous transformation of δ-hydroxycarbonyl, a major first-generation product from long-chain alkane photochemistry, is observed on the surface of particles and walls. The uniqueness of this reaction scheme is the production of substituted dihydrofuran, which is highly reactive towards ozone, OH, and NO3, thereby opening a reaction pathway that is not usually accessible to alkanes. A spectrum of highly-oxygenated products with carboxylic acid, ester, and ether functional groups is produced from the substituted dihydrofuran chemistry, thereby affecting the average oxidation state of the alkane-derived SOA.

The vapor wall loss correction is applied to several chamber-derived SOA systems generated from both anthropogenic and biogenic sources. Experimental and modeling approaches are employed to constrain the partitioning behavior of SOA-forming vapors onto suspended particles vs. chamber walls. It is demonstrated that deposition of SOA-forming vapors to the chamber wall during photooxidation experiments can lead to substantial and systematic underestimation of SOA. Therefore, it is likely that a lack of proper accounting for vapor wall losses that suppress chamber-derived SOA yields contribute substantially to the underprediction of ambient SOA concentrations in atmospheric models.

Variabilidade espacial e temporal da distribuição do material particulado em suspensão nas proximidades do canal de navegação da baía de Sepetiba (RJ)

Este estudo teve como objetivo principal caracterizar os padrões de distribuição do material particulado em suspensão ao longo da baía de Sepetiba, associando as variabilidades espaciais e temporais com ciclos de maré. Além disso, o estudo também avalia a utilização de equipamentos acústicos como ferramentas à estimativa das concentrações de material particulado em suspensão. A aquisição de dados foi realizada num total de sete campanhas realizadas entre novembro de 2010 e dezembro de 2011. Sete estações foram posicionadas nas proximidades do canal principal de acesso à baía, ao longo de um transecto que se estende do seu interior até sua desembocadura. As sete campanhas amostrais se distribuem em duas séries longas, de 13 e 25 horas, de aquisição em um ponto fixo, e cinco amostragens ao longo das estações. A aquisição de dados envolve: coleta de amostras de água, utilizadas nas estimativas das concentrações de material particulado; coleta de sedimentos de fundo para caracterização granulométrica das estações amostradas; perfis de parâmetros físico-químicos; dados de correntômetria adquiridos junto ao fundo. O processamento das amostras de água e sedimentos foi realizado no laboratório de Geologia Marinha da Faculdade de Oceanografia da Universidade do Estado do Rio de Janeiro. As concentrações de material particulado em suspensão foram utilizadas na calibração de sensores acústicos e óticos, permitindo uma avaliação espaço-temporal mais detalhada dos padrões de distribuição junto ao fundo e ao longo da coluna dágua. Os dados observados permitiram identificar que as maiores concentrações de material particulado em suspensão ocorrem em condições de maré enchente, e estão associadas à assimetria de maré. A baía pode ser dividida em dois setores: um na porção mais interna, onde se observou maior influência do aporte fluvial, onde as concentrações de material particulado em suspensão respondem à propagação da pluma do canal de São Francisco; e outro que se estende da porção central até sua desembocadura, onde predomina o domínio marinho, com influência de eventos oriundos da plataforma continental. Também pode ser identificada a influência do fenômeno La Niña, que provavelmente foi responsável por: altas salinidades encontradas no interior da baía e ocorrência da Água Central do Atlântico Sul à baixas profundidades. Quanto à utilização de equipamentos acústicos nas estimativas das concentrações de material particulado, os dados se demonstraram ricos em detalhes, que permitiram avaliar o comportamento do material particulado junto ao fundo frente a diferentes condições de maré, turbulência e incidência de oscilações.

Problems associated with the over protection of fishing trawlers against sea water corrosion and fouling

Some presently used anti-fouling materials contain metals and other compounds, which are toxic in the environment. Coating products are not always stable, and there is a resulting pollution hazard. In particular if surfaces are poorly prepared and manufactures' instructions are not closely followed the application of anti-fouling substances becomes pointless and dangerous. In addition the salinity, constant biological activity and suspended particles make seawater a highly corrosive material in its own right.

PCB desorption kinetics under realistic shear and turbulence [progress report]

We hypothesize that the impact of PCB desorption from resuspended sediments depends upon the intensity of the resuspension (which scales to bottom stress in the absence of organisms), the rate at which each congener desorbs (which depends on the size and hydrophobicity of the chemical, the relative amount of 'labile' and 'resistant' forms, and the size distribution of the suspended particles), and the residence time of the particles in the water column (which depends on the time-variable water column turbulence regime and the particle settling velocities). In order to accurately quantify the impact of PCB desorption from Hudson River sediments, we are conducting experiments that realistically mimic bottom shear stress and water column turbulence and rapidly measure PCB congener release. The objectives of this study are to measure the kinetics of PCB congener desorption from Hudson River sediments under realistic bottom shear and water column turbulence conditions and to quantify the impact of shear stress and contaminant aging on PCB desorption kinetics.

Electrorheologic liquid crystals in microsystems: model and measurements

Fluids with a controllable viscosity gained a lot of interest throughout the last years. One of the advantages of these fluids is that they allow to fabricate hydraulic components such as valves with a very simple structure. Although the properties of these fluids are very interesting for microsystems, their applicability is limited at microscale since the particles suspended in these fluids tend to obstruct microchannels. This paper investigates the applicability of electrorheologic Liquid Crystals (LCs) in microsystems. Since LC's do not contain suspended particles, they show intrinsic advantages over classic rheologic active fluids in microapplications. As a matter of fact, LC molecules are usually only a few nanometers long, and therefore, they can probably be used in systems with sub-micrometer channels or other nanoscale applications. This paper presents a novel model describing the electrorheologic behavior of these nanoscale molecules. This model is used to simulate a microvalve controlled by LC's. By comparing measurements and simulations performed on this microvalve it is possible to prove that the model developed in this paper is very accurate. In addition, these simulations and measurements revealed other remarkable properties of LC's, such as high bandwidths and high changes in flow resistance. © 2006 IEEE.

The use of liquid crystals as electrorheological fluids in microsystems: Model and measurements

Fluids with controllable flow properties have gained considerable interest in the past few years. Some of these fluids such as magnetorheologic fluids are now widely applied to active dampers and valves. Although these fluids show promising properties for microsystems, their applicability is limited to the microscale since particles suspended in these fluids tend to obstruct microchannels. This paper investigates the applicability of electrorheologic liquid crystals (LCs) in microsystems. Since LCs do not contain suspended particles, they show intrinsic advantages over classic rheologic fluids in micro-applications. This paper presents a novel physical model that describes the static and the dynamic behaviour of electrorheologic LCs. The developed model is validated by comparing simulations and measurements performed on a rectangular microchannel. This assessment shows that the model presented in this paper is able to simulate both static and dynamic properties accurately. Therefore, this model is useful for the understanding, simulation and optimization of devices using LCs as electrorheological fluid. In addition, measurements performed in this paper reveal remarkable properties of LCs, such as high bandwidths and high changes in flow resistance. © 2006 IOP Publishing Ltd.

Temporal Coherence of Chlorophyll a during a Spring Phytoplankton Bloom in Xiangxi Bay of Three-Gorges Reservoir, China

Algal bloom phenomenon was defined as "the rapid growth of one or more phytoplankton species which leads to a rapid increase in the biomass of phytoplankton", yet most estimates of temporal coherence are based on yearly or monthly sampling frequencies and little is known of how synchrony varies among phytoplankton or of the causes of temporal coherence during spring algal bloom. In this study, data of chlorophyll a and related environmental parameters were weekly gathered at 15 sampling sites in Xiangxi Bay of Three-Gorges Reservoir (TGR, China) to evaluate patterns of temporal coherence for phytoplankton during spring bloom and test if spatial heterogeneity of nutrient and inorganic suspended particles within a single ecosystem influences synchrony of spring phytoplankton dynamics. There is a clear spatial and temporal variation in chlorophyll a across Xiangxi Bay. The degree of temporal coherence for chlorophyll a between pairs of sites located in Xiangxi Bay ranged from -0.367 to 0.952 with mean and median values of 0.349 and 0.321, respectively. Low levels of temporal coherence were often detected among the three stretches of the bay (Down reach, middle reach and upper reach), while high levels of temporal coherence were often found within the same reach of the bay. The relative difference of DIN between pair sites was the strong predictor of temporal coherence for chlorophyll a in down and middle reach of the bay, while the relative difference in Anorganic Suspended Solids was the important factor regulating temporal coherence in middle and upper reach. Contrary to many studies, these results illustrate that, in a small geographic area (a single reservoir bay of approximately 25 km), spatial heterogeneity influence synchrony of phytoplankton dynamics during spring bloom and local processes may override the effects of regional processes or dispersal.

How polluted is the Yangtze River? Water quality downstream from the Three Gorges Dam

The concentrations of major anions and cations, nitrogen and phosphorus, dissolved and particulate trace elements, and organic pollutants were determined for the middle and lower reaches of the Yangtze River (Changjiang) from below the Three Gorges Dam (TGD) to the mouth at Shanghai in November 2006. The concentration of dissolved inorganic phosphate (DIP) was constant at a low level of 6-8 mu gP/L, but the concentration of nitrate (NO3-) approximately doubled downstream and was closely correlated with K+. This translated to a daily load of well over 1000 It of dissolved inorganic nitrogen (DIN) at Datong. The average concentrations of dissolved Pb (0.078 +/- 0.023 mu g/L), Cd (0.024 +/- 0.009 mu g/L), Cr(0.57 +/- 0.09 mu g/L), Cu (1.9 +/- 0.7 mu g/L), and Ni (0.50 +/- 0.49 mu g/L) were comparable with those in other major world rivers, while As (3.3 +/- 1.3 mu g/L) and Zn (1.5 +/- 0.6 mu g/L) were higher by factors of 5.5 and 2.5, respectively. The trace element contents of suspended particles of As (31 +/- 28 mu g/g), Pb (83 +/- 34 mu g/g), and Ni (52 +/- 16 mu g/g) were close to maximum concentrations recommended for rivers by the European Community (EC). The average concentrations of Cd (2.6 +/- 1.6 mu g/g), Cr (185 +/- 102 mu g/g), Cu (115 +/- 106 mu g/g), and Zn (500 +/- 300 mu g/g) exceeded the EC standards by a factor of two, and Hg (4.4 +/- 4.7 mu g/g) by a factor of 4 to 5. Locally occurring peak concentrations exceed these values up to fourfold, among them the notorious elements As, Hg, and Tl. All dissolved and particulate trace element concentrations were higher than estimates made twenty years ago [Zhang, J., Geochemistry of trace metals from Chinese river/estuary systems: an overview. Estuar Coast Shelf Sci 1995; 41: 631-658.]. The enormous loads of anthropogenic pollutants disposed to the river were diluted by the large water discharge of the Yangtze even during the lowest flow resulting in the relatively low concentration levels of trace elements and organic pollutants observed. We estimated loads of e.g. As, Pb and Ni to the East China Sea to be about 4600 kg As d(-1), 3000 kg Pb d(-1), and 2000 kg Ni d(-1). About 6000 t d(-1) of dissolved organic carbon (DOC) was delivered into the sea at the time of our cruise. We tested for 236 organic pollutants, and only the most infamous were found to be barely above detection limits. We estimated that the load of chlorinated compounds, aromatic hydrocarbons, phenols, and PAHs were between 500 and 3500 kg d(-1). We also detected eight herbicides entering the estuary with loads of 5-350 kg d(-1). The pollutant load, even when at low concentrations, are considerable and pose an increasing threat to the health of the East China Sea ecosystem. (c) 2008 Elsevier B.V. All rights reserved.

Differing estrogen activities in the organic phase of air particulate matter collected during sunny and foggy weather in a Chinese city detected by a recombinant yeast bioassay

Total air suspended particles (PM 100) collected from an urban location near a traffic line in Wuhan, China, were examined for estrogen using a recombinant yeast bioassay. Wuhan, located at the central part of China, is the fourth biggest city in China with 7 million populations. Today, Wuhan has developed into the biggest city and the largest traveling center of central China, becoming one of the important bases of industry, education and research. Wuhan is right at the confluent point of Yangzi River, the third longest river in the world, and its largest distributary Hanjiang, with mountains and more than 100 takes in downtown area. Therefore, by its unique landscape, Wuhan has formed clear four seasons with relatively long winter and summer and short spring and autumn. Foggy weather usually happen in early spring. The yeast line used in this assay stably expresses human estrogen receptor-alpha. Weak but clear estrogenic activities were detected in the organic phase of crude extracts of air particle materials (APM) in both sunny and foggy weather by 0.19-0.79 mug E2/gPM(100) which were statistically significantly elevated relative to the blank control responding from 20% to 50% of the maximum E2 response, and the estrogenic activity was much higher in foggy weather than in sunny weather. The estrogenic activities in the sub-fractions from chromatographic separation of APM sampled in foggy days were also determined. The results indicated that the responses of the fractions were obviously higher than the crude extracts. Since there is no other large pollution source nearby, the estrogenic material was most likely from vehicle emissions, house heating sources and oil fumes of house cooking. The GC/MS analysis of the PM100 collected under foggy weather showed that there were many phenol derivatives, oxy-PAHs and resin acids which have been reported as environmental estrogens. These results of the analysis of estrogenic potency in sunny and foggy weather in a subtropical city of China indicate that further studies are required to investigate the actual risks for the associated health and atmospheric system. (C) 2004 Elsevier Ltd. All rights reserved.

Diversity and spatial distribution of sediment ammonia-oxidizing crenarchaeota in response to estuarine and environmental gradients in the Changjiang Estuary and East China Sea

Ammonia-oxidizing archaea (AOA) have recently been found to be potentially important in nitrogen cycling in a variety of environments, such as terrestrial soils, wastewater treatment reactors, marine waters and sediments, and especially in estuaries, where high input of anthropogenic nitrogen is often experienced. The sedimentary AOA diversity, community structure and spatial distribution in the Changjiang Estuary and the adjacent East China Sea were studied. Multivariate statistical analysis indicated that the archaeal amoA genotype communities could be clustered according to sampling transects, and the station located in an estuarine mixing zone harboured a distinct AOA community. The distribution of AOA communities correlated significantly with the gradients of surface-water salinity and sediment sorting coefficient. The spatial distribution of putative soil-related AOA in certain sampling stations indicated a strong impact of the Changjiang freshwater discharge on the marine benthic microbial ecosystem. Besides freshwater, nutrients, organic matter and suspended particles, the Changjiang Diluted Water might also contribute to the transport of terrestrial archaea into the seawater and sediments along its flow path.

Rare earth elements in bottom sediments of major rivers around the Yellow Sea: implications for sediment provenance

Rare earth elements (REEs) of 91 fine-grained bottom sediment samples from five major rivers in Korea (the Han, Keum, and Yeongsan) and China (the Changjiang and Huanghe) were studied to investigate their potential as source indicator for Yellow Sea shelf sediments, this being the first synthetic report on REE trends for bottom sediments of these rivers. The results show distinct differences in REE contents and their upper continental crust (UCC)-normalized patterns: compared to heavy rare earth elements (HREEs), light rare earth elements (LREEs) are highly enriched in Korean river sediments, in contrast to Chinese river sediments that have a characteristic positive Eu anomaly. This phenomenon is observed also in primary source rocks within the river catchments. This suggests that source rock composition is the primary control on the REE signatures of these river sediments, due largely to variations in the levels of chlorite and monazite, which are more abundant in Korean bottom river sediments. Systematic variations in I LREE pound/I HREE pound ratios, and in (La/Yb)-(Gd/Yb)(UCC) but also (La/Lu)-(La/Y)(UCC) and (La/Y)-(Gd/Lu)(UCC) relations have the greatest discriminatory power. These findings are consistent with, but considerably expand on the limited datasets available to date for suspended sediments. Evidently, the REE fingerprints of these river sediments can serve as a useful diagnostic tool for tracing the provenance of sediments in the Yellow Sea, and for reconstructing their dispersal patterns and the circulation system of the modern shelf, as well as the paleoenvironmental record of this and adjoining marginal seas.

细粒沉积物多组分粒度特征及其成因机制研究

By using high-resolution laser grain size instrument Mastersizer 2000, the grain size distribution of windblown depositions (loess and sandy dunes), aqueous sediments (lake, river, riverside and foreshore sand), weathering crust, sloping materials and other fine-grain sediments are systemically measured. The multimodal characteristics of grain size distribution of these sediments are carefully studied. The standard patterns and their grain size characteristics of various sediments are systemically summarized. The discrepancies of multimodal distribution among windblown depositions, aqueous sediments and other sediments are concluded and the physical mechanisms of grain size multimodal distribution of various sediments are also discussed in this paper. The major conclusions are followed: 1. The multimodal characteristic of grain size distribution is a common feature in all sediments and results from properties of transportation medium, dynamic intensity, transportation manner and other factors. 2. The windblown depositions are controlled by aerodynamic forcing, resulting in that the median size of the predominant mode gradually decreases form sandy dunes to loess. Similarly, the aqueous sediments are impacted by dynamic forces of water currents and the median grain size of the predominant mode decreases gradually from river to lake sediments. Because the kinetic viscidity of air is lower than of water, the grain size of modes of windblown depositions is usually finer than that of corresponding modes of aqueous sediments. Typical characteristics of sediments grain size distribution of various sediments have been summarized in the paper: (1) Suspended particles which diameters are less than 75μm are dominant in loess and dust. There are three modes in loess’ grain size distribution: fine, median and coarse (the median size is <1μm、1-10μm、10-75μm, respectively). The coarse mode which percentage is larger than that of others is controlled by source distance and aerodynamic intensity of dust source areas. Some samples also have a saltation mode which median size is about 300-500μm. Our analysis demonstrates that the interaction of wind, atmospheric turbulence, and dust grain gravity along the dust transportation path results in a multimodal grain size distribution for suspended dust. Changes in the median sizes of the coarse and medium modes are related to variation in aerodynamic forcing (lift force related to vertical wind and turbulence) during dust entrainment in the source area and turbulence intensity in the depositional area. (2) There is a predominant coarse saltation mode in grain size distribution of sandy dunes, which median size is about 100-300μm and the content is larger than that of other modes. The grain size distribution curve is near axis symmetric as a standard logarithm normal function. There are some suspended particles in some samples of sandy dunes, which distribution of the fine part is similar to that of loess. Comparing with sandy samples of river sediments, the sorting property of sandy dunes is better than of river samples although both they are the saltation mode. Thus, the sorting property is a criterion to distinguish dune sands and river sands. (3) There are 5~6 modes (median size are <1μm, 1-10μm, 10-70μm, 70-150μm, 150-400μm, >400μm respectively) in grain size distribution of lacustrine sediments. The former 4 modes are suspensive and others are saltated. Lacustrine sediments can be divided into three types: lake shore facies, transitional facies and central lake facies. The grain size distributions of the three facies are distinctly different and, at the same time, the transition among three modes is also clear. In all these modes, the third mode is a criteria to identify the windblown deposition in the watershed. In lake shore sediments, suspended particles are dominant, a saltation mode sometimes occurs and the fourth mode is the most important mode. In the transitional facies, the percentage of the fourth mode decreases and that of the second mode increases from lake shore to central lake. In the central lake facies, the second mode is dominant. A higher content of the second mode indicates its position more close to the central lake. (4) The grain size distribution of river sediments is the most complex. It consist of suspension, saltation and rolling modes. In most situations, the percentage of the saltation mode is larger than that of other modes. The percentage of suspension modes of river sediments is more than of sandy dunes. The grain size distribution of river sediments indicates dynamic strength of river currents. If the fourth mode is dominant, the dynamic forcing of river is weaker, such as in river floodplain. If the five or sixth mode is dominant, the water dynamic forcing of rivers is strong. (5) Sediments can be changed by later forcing in different degree to form some complicated deposition types. In the paper, the grain size distribution of aqueous sediments of windblown deposition, windblown sediments of aqueous deposition, weathering crust and slope materials are discussed and analyzed. 3. The grain size distribution characteristics of different sediments are concluded: (1) Modal difference: Usually there are suspended and saltation modes in the windblown deposition. The third mode is dominant in loess dust and the fifth mode is predominant in sandy dunes. There are suspended, saltation and rolling particles in aqueous sediments. In lacustrine sediments, the second and fourth mode are predominant for central lake facies or lake shore facies, respectively. In river sediments, the fourth, or fifth, or sixth mode is predominant. Suspended modes: the grain size of suspended particles of windblown depositions usually is less than 75μm. The content of suspended particles is lower or none in sandy dunes. However, suspended particles of aqueous sediments may reach 150μm. Difference in grain size of suspended modes represents difference between transitional mediums and the strength of dynamic forcing. Saltation modes: the median size of saltation mode of sandy dunes fluctuates less than that of river sediments. (2) Loess dust and lacustrine sediment: Their suspended particles are clearly different. There is an obvious pit between the second and the third modes in grain size distribution of lacustrine sediments. The phenomenon doesn’t occur in loess dust. In lacustrine sediments, the second mode can be a dominant mode, such as central lake facies, and contents of the second and the third modes change reversely. However, the percentage of the third mode is always the highest in loess dust. (3) Dune Sand and fluvial sand: In these two depositions, the saltation particles are dominant and the median sizes of their saltation modes overlay in distribution range. The fifth mode of dune sand fluctuates is sorted better than that of fluvial sand. (4) Lacustrine and fluvial sediments: In lacustrine sediments, there are 5-6 modes and suspended particles can be predominant. The second mode is dominant in central lake facies and the third mode is dominant in lake shore facies. Saltation or roll modes occurred in central lake facies may indicate strong precipitation events. In fluvial sediments, saltation particles (or rolling particles) usually dominant. 4. A estimation model of lake depth is firstly established by using contents of the second, the third and the fourth modes. 5. The paleoenvironmental history of the eastern part of SongLiao basin is also discussed by analyzing the grain size distribution of Yushu loess-like sediments in Jilin. It was found that there is a tectonic movement before 40ka B.P. in SongLiao basin. After the movement, loess dust deposited in Yushu area as keerqin desert developed. In recent 2000 years, the climate became drier and more deserts activated in the eastern part of Song-Liao basin.

贵阳市大气总悬浮颗粒物(TSP)的化学特征及其影响因素研究

气溶胶对气候和人类的健康都有重要影响。因此，研究大气总悬浮颗粒物（TSP）的化学组成和物理特性对更深入地了解气溶胶对气候和人类健康的影响具有重要意义。贵阳是中国受燃煤污染比较严重的城市之一，大气中高含量的SO2是其最明显的特征。尽管最近几年空气质量有所改善，但是该区的大气污染问题还比较严重，空气质量仍然不容乐观。我们于2005年1月1日到2005年12月31日在中科院地球化学研究所内全年采集总悬浮颗粒物（TSP）样品，分析测试了其主要无机离子（F-、Cl-、SO42-、NO3-、NH4+、K+、Na+、Ca2+和Mg2+）的化学性质，并结合当地的气象参数（温度，风速，降雨量和相对湿度）系统地研究了TSP及其水溶性无机离子的季节变化特征。本论文的主要结论有： 1. TSP的浓度变化范围为36.91～313.44µg/m3，年均值106.60µg/m3；各离子摩尔浓度的大小顺序为：SO42-> NH4+> Ca2+ > NO3-> K+ > Na+ > Cl- > Mg2+ > F-；SO42- (23.04±12.16µg/m3)和NH4+(3.05±2.23µg/m3)是最主要的离子，分别占总离子摩尔数的37％和30％。TSP及其组分都有明显的季节变化，TSP、Cl-、SO42-、NO3-、NH4+、K+、Na+、Ca2+和Mg2+浓度的冬/夏比值分别为:1.29、5.23、1.35、2.37、1.73、1.22、1.84、1.23和1.02。 2. 温度对TSP及其水溶性无机组分的影响呈现一定的季节变化模式，冬天随温度的升高TSP及其水溶无机组分的浓度也升高，夏天随温度的升高TSP及其水溶性无机组分的浓度降低。但是从全年来看，温度与TSP及其水溶性无机组分之间有弱的负相关性，即随温度的升高，TSP及其水溶性无机组分的浓度有不同程度的下降。相对湿度与TSP及其水溶性无机组分之间存在明显的负相关关系，即随大气相对湿度的增加，TSP及其水溶性无机组分的浓度下降。在相对湿度与TSP及其水溶性无机组分浓度的日变化图中表现为相对湿度的波谷与TSP及其水溶无机组分的浓度的波峰相对应。风速与TSP及其水溶无机组分的浓度之间呈现弱的负相关性。在贵阳，风速对TSP及其水溶无机组分的影响主要表现为扩散作用和稀释作用，由风速导致的尘土再悬浮作用并不明显。雨量对TSP及其水溶性无机组分的影响主要是湿清除作用，具体表现为无雨天TSP及其水溶性无机组分的浓度较雨天高。影响TSP、Ca2+、Mg2+和F-的主要气象参数是相对湿度(RH)和风速，影响SO42-、NO3-、NH4+和Cl-的主要气象参数是温度。 3. 贵阳大气总悬浮颗粒物（TSP）总体偏酸性，TSP水溶液pH值的年均值为6.27±0.41，与总阴离子与总阳离子的当量比Q的年平均值为0.82一致；TSP中高含量的SO42-是贵阳的TSP显酸性的主要原因。 4. NH4+与SO42-和NO3-的相关系数（R）分别为0.85和0.65，NH4+与SO42-的摩尔比值为0.8，说明贵阳TSP中的NH4+主要以(NH4)2SO4的形式存在。Ca2+和Mg2+有较好的相关性（R=0.72）和相似的变化特征，说明二者可能有共同的来源。 5. 2005年贵阳TSP中SO42-/ Ca2+的平均值为13.64，几乎是干净大陆SO42-/ Ca2+的本底值的20倍，说明贵阳的大气污染主要是人为因素所致。NO3-/SO42-的平均值为0.15，说明固定源对贵阳气溶胶的贡献比移动源（通常指交通工具所排放的尾气）对气溶胶的贡献大；

Extraction of polydispersity information from photon correlation data

Photon correlation spectroscopy (PCS) is a light-scattering technique for particle size diagnosis. It has been used mainly in the investigation of hydrosol particles since it is based on the measurement of the correlation function of the light scattered from the Brownian motion of suspended particles. Recently this technique also proved useful for studying soot particles in flames and similar aerosol systems. In the case of a polydispersed system the problem of recovering the particle size distribution can be reduced to the problem of inverting the Laplace transform. In this paper we review several methods introduced by the authors for the solution of this problem. We present some numerical results and we discuss the resolution limits characterizing the reconstruction of the size distributions. © 1989.