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.     

中国超大城市综合实验:京、沪、穗气溶胶理化和吸湿特性

气溶胶对环境、气象和人体健康都有较大影响,这些影响与气溶胶理化特性(粒子尺度谱、化学组分、混合状态等)密切相关。为了深入研究气溶胶的环境和气候效应,发展了一套气溶胶在线综合观测系统。本文介绍了利用该系统在北京、上海、广州三个超大城市开展的综合观测实验结果。通过对比分析发现,广州气溶胶数浓度最高,其粒子尺度谱分布特征与北京特征相似,均以核模态为主,上海气溶胶数浓度则整体较低。对比三个超大城市的新粒子生成(New Particle Formation,NPF)特征发现,北京NPF的发生频率低于广州,主要由于北京地区大气中大粒径气溶胶更多,较高的碰并汇抑制了NPF的发生和发展。研究发现,观测期间北京和上海站点气溶胶的吸湿性强于广州,人为一次性排放气溶胶吸湿性较弱。气溶胶吸湿性日变化特征与人为活动、气溶胶老化程度密切相关。此外,三个超大城市中气溶胶光吸收系数的日变化特征存在明显差别,北京站点的气溶胶吸收系数呈现白天高、夜间低的特点,而广州站点气溶胶的吸收系数呈现相反的日变化趋势,这可能是由观测站周边的环境差异及大气边界层的变化特征差异造成的。     

Temporal and spatial variations of marine aerosols over the Atlantic Ocean

Aerosol samples, collected daily were analyzed with electron microscopy for particle concentration and size distribution. The chemical compositions of individual particles were determined with X-ray energy spectrometry and specific morphological tests. The results demonstrated clear and significant dependencies of aerosol properties on air trajectories computed from a backtrack model. Air parcels, such as American air pollution and Sahara dust, were identified. Their physical mixing and chemical reactions with marine aerosols as well as aerosol wet deposition are discussed.     

The chemical fractionation of atmospheric aerosol as a result of snow crystal formation and growth

The relationships between the physical and chemical properties of mixed-phase clouds were investigated at Storm Peak Laboratory (3220m MSL) located near the continental divide in northwestern Colorado. Interstitial aerosol particles, cloud droplets and snow crystals were concurrently collected when the laboratory was enveloped by a precipitating cloud. All samples were analyzed for trace elements, soluble anions, electrical conductivity and acidity.The results show average trace constituent concentration ratios of cloud water to snow water range from 0.4 to 26. All but six of the 32 elements and ions measured had ratios greater than one. This result suggests a chemical species dependency of in-cloud aerosol particle scavenging processes. Evidence of a decrease of in-cloud aerosol particle scavenging efficiency by snow due to increases in aerosol concentration is also presented.Differences between the chemical composition of cloud water and snow water are manifested most strongly when snow crystals grow by vapor deposition. In-cloud scavenging efficiencies by snow crystals for most aerosol particle chemical species are dependent on the growth of the snow crystals by accretion of cloud droplets. This chemical fractionation of the atmospheric aerosol by snow crystal formation and growth should be most active where narrow, continental cloud droplet size distributions and low liquid water contents are prevalent, enhancing the probability of snow crystal growth by diffusion.     

近年平流层气溶胶模式研究综述

平流层气溶胶在全球大气的辐射与化学平衡中起着重要作用,对全球气候变化有着重要的影响。数值模拟研究是研究平流层气溶胶浓度、粒径分布及其化学组成的重要手段之一。回顾了平流层气溶胶模式的发展历程,并对现今研究中较有代表性的5种模式进行了比较,着重考察了模拟结果在OCS、SO2分布情况等方面与实测数据的相符程度。结果发现5种模式均可再现平流层气溶胶和它的主要前体气体分布的大部分特征,但同时也都存在各自的局限。最后展望了平流层气溶胶模式未来的发展方向以及需要改进的问题。     

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 physically‐based algorithm for estimating the relationship between aerosol mass and cloud droplet number

In this study, we present a relationship between total accumulation mode aerosol mass concentrations and cloud droplet number concentrations ( N _d). The fundamental aim with the present method is to arrive at a physically‐based conversion algorithm in which each step in the conversion is based on real physical processes that occur and can be observed in the atmosphere, and in which all of the fields involved can be observed or modeled. In the last conversion (the critical part in the algorithm), we use measurements of the size distributions of cloud droplet residual particles for different pollution conditions. This conversion assumes that the size of the residual particles can be described with a lognormal distribution function and uses the Hatch–Choate relationship to convert between residual volume and number. The relatively sparse data set with which we have developed the present algorithm results in a course classification of the aerosol mass field. Consequently, uncertainties need to be recognized when using the algorithm in its present form in model calculations. The algorithm has been used on data from 15 days and the agreement between calculated and observed N _d values is, with one exception, within a factor of 2 and for many of these cases also much better than a factor of 2. In addition to the results of the algorithm itself, we also present a least‐squares fit to the predicted N _d values. To improve the algorithm in the longer‐term requires more data of scavenging fractions, particle chemical composition and density, and residual particle size distributions as a function of aerosol mass loading and cloud type.     

临安大气污染本底站气溶胶特征分析

本文分析和讨论了1991年8月上旬至11月下旬在浙江临安大气污染本底站（属WMO）所监测的大气气溶胶及气溶胶中元素和离子的浓度、浓度的粒径分布、富集程度、型态特征及其相互关系等物理化学特征，还讨论了天气及某些气象要素对气溶胶浓度分布特征的影响，对气溶胶的来源也作了简单探讨。     

On the influence of the physico-chemical properties of aerosols on the life cycle of radiation fogs

A one-dimensional model of radiation fog with detailed microphysics is presented. Aerosols and cloud droplets are treated in a joint two-dimensional size distribution. Radiative fluxes are calculated as functions of the radiative properties of the time-dependent particle spectra. The droplet growth equation is solved by considering radiative effects. Turbulence is treated by means of a higher order closure model. The interaction between the atmosphere and the earth's surface is explicitly simulated.Three numerical sensitivity studies are performed to investigate the impact of the different physico-chemical properties of urban, rural and maritime aerosols on fog formation. Numerical results elucidate that depending on the aerosol type used, the resulting fog events are completely different. This is particularly true for the times of fog formation and dissipation as well as for the liquid water content and supersaturations within the fogs. In the activated part of the particle spectra, the aerosol mass is very inhomogeneously distributed. The maxima of the curves do not coincide with the maxima of the corresponding liquid water distributions.     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

An AOGCM simulation of the climate response to a volcanic super-eruption

Volcanic ‘super-eruptions’ have been suggested to have significantly influenced the Earth’s climate, perhaps causing glaciations and impacting on the human population. Climatic changes following a hypothetical ‘super-eruption’ are simulated using a coupled atmosphere ocean general circulation model, incorporating scaled volcanic stratospheric aerosols. Assumptions are made about the stratospheric sulphate aerosol loading, size distribution, lifetime, chemical make up and spatial distribution. As this study is concentrating on the physical climatological impacts over long timescales, microphysics and chemical interactive processes are not simulated. Near-surface temperatures fall by as much as 10 K globally for a few months and a considerable deviation from normal temperatures continues for several decades. A warming pattern is evident over northern land masses during the winter due to increased longwave forcing and a positive AO mode. The overturning rate of the North Atlantic thermohaline circulation doubles in intensity. Snow and ice increases in extent to a maximum coverage of 35% of the Earth. Despite these and other impacts longer term climatic changes that could lead to a transition to a glaciation do not occur, for present day boundary conditions and one possible plausible aerosol loading.     

In-Situ Measurements of Cloud-Precipitation Microphysics in the East Asian Monsoon Region Since 1960

A large number of in-situ measurements of cloud-precipitation microphysical properties have been made since 1960, including measurements of particle size distribution, particle concentration, and liquid water content of clouds and rain. These measurements have contributed to considerable progress in understanding microphysical processes in clouds and precipitation and significant improvements in parameterizations of cloud microphysics in numerical models. This work reviews key findings regarding cloud-precipitation microphysics over China. The total number concentrations of various particles vary significantly, with certain characteristic spatial scales. The size distributions of cloud droplets in stratiform clouds can generally be fit with gamma distributions, but the fit parameters cover a wide range. Raindrop size distributions(RSDs)associated with stratiform clouds can be fit with either exponential or gamma distributions, while RSDs associated with convective or mixed stratiform-cumuliform clouds are best fit with gamma distributions.Concentrations of ice nuclei(IN) over China are higher than those observed over other regions, and increase exponentially as temperature decreases. The particle size distributions of ice crystals, snow crystals, and hailstones sampled at a variety of locations can be reliably approximated by using exponential distributions,while aerosol particle size distributions are best described as the sum of a modified gamma distribution and a Junge power-law distribution. These results are helpful for evaluating and improving the fidelity of physical processes and hydrometeor fields simulated by microphysical parameterizations. The comprehensive summary and analysis of previous work presented here also provide useful guidelines for the design of future observational programs.     

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     

基于航测的云底气溶胶活化率与过饱和度估算

2016年11月13日在北京地区上空存在持续稳定的层状云天气背景下,利用飞机开展气溶胶粒径谱、化学组成、云滴谱等参量的垂直观测,研究该个例云底气溶胶的活化能力。结果表明:探测期间北京地区为轻度污染天气,地面气溶胶浓度(0.11~3 μm)达到4600 cm-3。云层高度为800~1200 m,云底气溶胶数浓度相对于近地面大幅度降低,有效粒径显著增大(0.3~0.6 μm)。同时,近地面气溶胶中疏水性的一次有机气溶胶贡献显著,而云底气溶胶中一次有机气溶胶的贡献大幅降低,无机组分和二次有机气溶胶的贡献明显增大,造成吸湿性参数κ由0.25(地面)增大至0.32(云底)。云中气溶胶和云滴的谱分布衔接较好,且两者的数浓度之和与云底气溶胶浓度一致,可分别代表未活化和已活化的粒子。基于云底气溶胶粒径谱和吸湿性参数计算得到不同过饱和比下云凝结核的活化率,通过与云中观测结果对比,反推得到云底过饱和度约为0.048%。     

1960年以来东亚季风区云-降水微物理的直接观测研究

云-降水的直接观测结果是云微物理参数化的重要依据。自1960年以来,处于东亚季风影响下的中国实施了大量对云-降水微物理参数的观测和研究,旨在加深对云-降水微物理过程的认识,从而改进数值模式中云微物理参数化方案和指导人工影响天气作业。云-降水微物理参数包括气溶胶、冰核、云滴、雨滴、冰晶、雪晶、冰雹等粒子浓度和谱分布,以及云滴、雨滴含水量等。中国已有云-降水微物理参数的成果可归纳为:(1)通常云-降水微物理粒子浓度变化较大,但总体变化有一定的范围;(2)采用Γ函数拟合云滴谱更接近实际谱,但不同拟合谱参数差异较大;(3)可用指数函数和Γ函数来拟合层状云降水雨滴谱,Γ函数拟合积云和层积混合云降水雨滴谱精度更高;(4)中国冰核浓度较高,冰核浓度随温度的降低近似成指数变化;(5)冰晶谱、雪晶谱、冰雹谱通常采用指数函数来描述;(6)通常使用荣格(Junge)和Γ函数来分段描述气溶胶粒子谱拟合误差更小。由于云-降水过程及其反馈作用描述不准确是数值模式预报结果不确定性的最大因素,中国正在不断地推进云降水的微物理观测研究,以期进一步加深对东亚季风区云-降水微物理特征的认识,从而为模式中微物理参数化方案的改进提供观测依据和科学指导。基于数值预报模式中云微物理过程参数化发展的需要,总结了中国1960年以来云-降水微物理直接观测的研究成果,可为东亚地区云-降水微物理研究及其模式参数化方案的改进提供观测依据。此外,针对云微物理参化发展的需求,结合过去已有的大量观测提出了几点建议,为今后云-降水物理综合性观测方案的设计提供参考。     

南京地区气溶胶谱分布的湿度相关性分析和等效复折射率预测

通过实验收集大气颗粒物，对南京地区大气气溶胶谱分布进行了描述，对气溶胶分布与相对湿度的相关性进行了探讨。建立了南京地区7—11月气溶胶化学组分的月平均模型，得出气溶胶等效复折射率的预测方法。结果表明：南京地区的大气气溶胶颗粒物，峰值粒径在80~100 nm范围，属于典型的城市型气溶胶。数浓度与相对湿度的相关性与季节和粒径大小有关，在6—9月，相对湿度与细粒子数浓度呈负相关，与粗粒子呈正相关，在10—11月相反，且易受极端天气影响。建立的干气溶胶等效复折射率月平均模型，结合湿度修正模型得到某一日的复折射率，与AERONET站点数据进行了对比，结果较为一致，误差范围在0~0.03。     

成都夏季气溶胶消光特性研究

本文利用成都2017年6~8月的米散射微脉冲激光雷达观测数据,对成都夏季气溶胶消光系数、边界层高度以及气溶胶光学厚度进行了反演,并结合太阳光度计观测资料、地面颗粒物浓度以及大气能见度数据研究了气溶胶消光系数日变化与月变化规律,气溶胶消光系数的垂直分布特征及影响因素。结果表明:气溶胶消光系数的日变化受人类活动以及边界层日变化影响显著,表现出凌晨与傍晚最大,早晨次之,午后最小的特征。消光高值出现在200m以下和300~700m的高度区间,夜间观察到的消光高值可能与颗粒物在夜间近地面浓度较高以及本地夜间降水频发有关。激光雷达反演的消光系数与光度计反演的气溶胶光学厚度在夏季各月的表现一致,夏季各月消光极值均出现在100~150m的近地面层。近地面消光系数与地面颗粒物浓度之间具有较好的正相关,并且粒子粒径更小时相关性更好。气溶胶光学厚度主要来自低层大气的贡献,0.1~0.2μm的细粒子气溶胶占比对于大气消光有主要影响,但气溶胶对大气的消光影响除了与粒子浓度有关,还与粒子的理化性质有关。      

大气气溶胶尺度分布分形特征研究

气溶胶作为大气环境中的重要组成部分,具有复杂的尺度分布结构。为研究其尺度分布特征,采用分形理论首先论述了常用的气溶胶谱分布函数具有分形不变性,然后在分形理论的指导下分别建立了气溶胶粒子和体积分形统计模型,而且以AERONET相关数据验证了分形模型的有效性和实用性,并采用分段分形的方法改进了气溶胶体积分形模型。最后分析研究了分维数的实用意义和分布情况,讨论了气溶胶分维数变化和粒度分布的关系。结果表明：气溶胶粒子数和体积分维数之间存在线性关系,上半年的大气溶胶粒子数分维数的变化幅度明显小于下半年的变化幅度;研究区域大气气溶胶中细粒子分布比较密集,大粒子分布比较分散。分形理论为研究大气气溶胶的尺度分布特征提供了新的方法与手段,具有广阔的研究与应用前景。     

从反射太阳光谱反演大气气溶胶体积谱分布的理论研究

由大气顶射出太阳辐射的形式解出发,结合球形粒子的米散射理论,由反射太阳光谱推导获得了反演整层大气气溶胶粒子体积谱分布的权重函数。在权重函数特征分析的基础上,根据一个简单的线性反演算法,利用大气辐射传输计算模拟的大气顶反射太阳光谱,反演获得了不同气溶胶浓度和复折射率条件下的气溶胶粒子体积谱。结果表明,初步建立了一套自洽的大气气溶胶体积谱分布的反演方法。通过米散射计算获得的反演参数考虑了波长对粒子半径的权重特征,使气溶胶体积谱的反演具有了明确的物理依据;同目前常用的查算表方法相比,简化了反演方案中参数化的复杂程度。     

Processing of Aerosol Particles in Convective Cumulus Clouds: Cases Study in the Mexican East Pacific

In the Mexican Intertropical Convergence Zone, particle size distributions within 500 m of cloud boundaries at altitudes of 1000, 2500, and 4200 m, were compared against size distributions at the same levels but 1500 m away from the clouds. The differences in the distributions near and far from the cloud are related to processes that may change particle properties inside the cloud. Chemical changes in the aerosols are deduced from the particles’ refractive index, as derived from comparisons with the scatter...