Novel optical techniques for measurements of light extinction,scattering and absorption by single aerosol particles

Aerosol particles play important roles in a broad range of scientific disciplines, from atmospheric chemistry and physics, to the delivery of fuels for combustion and drugs to the lungs, and extending to industrial processes such as spray drying. Measurements of the light extinction, scattering and absorption by ensembles of aerosol particles can be used to non‐intrusively characterise aerosol particle samples. However, such measurements often lead to ambiguity in interpreting the properties and processes occurring on individual particles. In this review, recent developments in the use of laser based techniques to isolate and manipulate single particles and to characterise them will be highlighted. In particular, the use of cavity ring down spectroscopy, Bessel beams and optical tweezers for investigating light extinction, scattering and absorption, respectively, will be considered. The prospects for using optical techniques to interrogate the fundamental processes occurring in aerosol at the single particle level are discussed.     

气溶胶凝聚粒子散射特性的数值计算

利用Cluster-cluster aggregation (CCA)模型,模拟了由相同数目球形原始微粒凝聚而成的四种随机取向气溶胶凝聚粒子．根据物质的电结构,将气溶胶凝聚粒子离散为一系列偶极子,结合离散偶极子近似方法,在获得每一个偶极子的电偶极矩之后,数值计算了气溶胶凝聚粒子散射强度的角分布,并分析了散射强度随入射光入射角度和气溶胶凝聚粒子尺寸参数变化的规律．结果显示：当散射角较小时,气溶胶凝聚粒子取向和入射光的入射角度对散射强度影响不大,当散射角增大时,散射强度则明显依赖于气溶胶凝聚粒子取向和入射光的入射角度;对于不同尺寸参数的气溶胶凝聚粒子,在同一角度入射情况下,随尺寸参数的增加,气溶胶凝聚粒子的散射主要集中于前向散射．     

Aerosol light absorption and its measurement: A review

Light absorption by aerosols contributes to solar radiative forcing through absorption of solar radiation and heating of the absorbing aerosol layer. Besides the direct radiative effect, the heating can evaporate clouds and change the atmospheric dynamics. Aerosol light absorption in the atmosphere is dominated by black carbon (BC) with additional, significant contributions from the still poorly understood brown carbon and from mineral dust. Sources of these absorbing aerosols include biomass burning and other combustion processes and dust entrainment.For particles much smaller than the wavelength of incident light, absorption is proportional to the particle volume and mass. Absorption can be calculated with Mie theory for spherical particles and with more complicated numerical methods for other particle shapes.The quantitative measurement of aerosol light absorption is still a challenge. Simple, commonly used filter measurements are prone to measurement artifacts due to particle concentration and modification of particle and filter morphology upon particle deposition, optical interaction of deposited particles and filter medium, and poor angular integration of light scattered by deposited particles. In situ methods measure particle absorption with the particles in their natural suspended state and therefore are not prone to effects related to particle deposition and concentration on filters. Photoacoustic and refractive index-based measurements rely on the heating of particles during light absorption, which, for power-modulated light sources, causes an acoustic signal and modulation of the refractive index in the air surrounding the particles that can be quantified with a microphone and an interferometer, respectively. These methods may suffer from some interference due to light-induced particle evaporation. Laser-induced incandescence also monitors particle heating upon absorption, but heats absorbing particles to much higher temperatures to quantify BC mass from the thermal radiation emitted by the heated particles. Extinction-minus-scattering techniques have limited sensitivity for measuring aerosol light absorption unless the very long absorption paths of cavity ring-down techniques are used. Systematic errors can be dominated by truncation errors in the scattering measurement for large particles or by subtraction errors for high single scattering albedo particles. Remote sensing techniques are essential for global monitoring of aerosol light absorption. While local column-integrated measurements of aerosol light absorption with sun and sky radiometers are routinely done, global satellite measurements are so far largely limited to determining a semi-quantitative UV absorption index.     

取向比对椭球气溶胶粒子散射特性的影响

利用T矩阵和离散坐标法研究了取向比对椭球粒子散射特性的影响, 计算了小尺度范围内椭球粒子的散射特征参量, 包括消光效率因子、不对称因子、单次散射反照率、散射相矩阵及双向反射函数(BRDF). 结果表明, 椭球粒子的散射特性与取向比密切相关, 粒子取向比会影响散射参量的振荡频率和振幅, 与球形粒子散射参量的相对差异也呈周期振荡趋势. 研究还发现, 某些特殊粒子尺寸的散射参量与粒子取向比基本无关. 在多次散射条件下, 分析不同取向比粒子群的BRDF随反射角和光学厚度的变化特性. 结果显示: 不同取向比粒子群的BRDF随反射角的变化趋势基本一致, 球形粒子群比非球形粒子群的BRDF曲线波动振幅更大; 球形-非球形粒子的BRDF相对差异随光学厚度和取向比的增大而减小, 随入射角的增大而增大.     

利用近前向散射图样识别单粒子形状的理论研究

近前向光学散射图样可以用来表征颗粒物的形状.基于球形芽孢杆菌、枯草芽孢杆菌、类鼻疽伯克氏菌的回转长椭球模型, 采用离散偶极子近似方法, 通过模拟3个不同方位探测器接收的散射光强响应信号, 讨论了非球形生物气溶胶颗粒的形状对前向角分辨光强的影响.结合球形指数反演算法, 在一定取向条件下, 前向5°–20° 内角分辨散射光强具有识别长形颗粒物和非长形颗粒物的能力.该研究可以为颗粒物形态测量仪器设计以及快速检测有害生物气溶胶提供依据.     

侧面遮拦式日晕光度计的杂散光理论分析

提出了一种侧面遮拦结构的日晕光度计,在镜筒内通过设置多层挡板结构逐层抑制处于内视场的挡板边缘衍射光,同时采用倾斜布置的上挡板结构抑制处于外视场的入射窗口边缘衍射光和侧壁散射光.建立数学模型对这些杂散光抑制挡板进行了仿真计算,结果表明,优化各挡板的几何参数后,日晕光度计的设计视场可达3.5～10个太阳半径,视场内的杂散光水平均可低于10-8平均太阳亮度.相对于高山天文台的日晕光度计在4～8个太阳半径的视场内总杂散光达到10-2平均太阳亮度,该日晕光度计扩展了可观测视场,并使杂散光抑制提高了一个量级.     

脉冲激光作用下气溶胶导致大气击穿研究

 利用锁模Nd:YAG激光及其倍频激光照射漂浮在大气中的Al₂O₂、ZnO、ZrO₂、18号玻璃粉等气溶胶粒子，在不同光学参数下对光致大气击穿阈值进行了测量。测量结果表明：空气中含较大粒子(d >30 μm)的光致击穿阈值比含较小粒子(d <1μm)的空气击穿阈值低2~3个数量级；含杂空气的击穿阈值随入射激光束直径的增大而下降，随气溶胶粒子直径的增大而减小，且随气溶胶成份的不同而不同；光致击穿阈值随波长的减小而增大。     

沙尘气溶胶粒子群的散射和偏振特性

根据Mie散射理论,以对数正态分布函数描述沙尘气溶胶粒子群的粒径尺度分布,计算了沙尘气溶胶粒子群在0.2～40μm波段间对太阳短波辐射和地球大气长波辐射的单次散射反照率、散射相矩阵函数,揭示了不同相对湿度时,沙尘粒子群对入射辐射的散射和偏振的特征。结果表明,沙尘粒子群的单次散射反照率随着入射波长的增加有较大起伏,不同相对湿度条件下,变化趋势基本一致;在可见光、近红外波段单次散射反照率随湿度增加而变大,湿度95%时非常接近于1;大于10μm的热红外波段单次散射反照率随相对湿度增加而减小,具有较强的吸收辐射能力。散射辐射强度受湿度影响较小,随散射角的增加呈现先减小后增大的趋势,且增大的趋势随着波长的增加而减弱;不同波段上,线偏振和圆偏振随散射角和相对湿度变化存在差异;在前向和后向仅对入射辐射为圆偏振辐射产生圆偏振散射;散射光的偏振特性及其湿度差异主要表现在后向散射区,多以拱形形式体现。拱顶峰值散射角位置存在差异,且峰值散射角随相对湿度的降低向后向漂移。     

非球形生物气溶胶对偏振光的多次散射特性研究

基于回转椭球模型和有限长圆柱模型,采用T矩阵方法研究了非球形生物气溶胶的单次散射特性,计算了鼠疫耶尔森氏杆菌、土拉热杆菌二种生物气溶胶对氦氖激光的单次相矩阵、单次散射反照率以及不对称因子。根据矢量辐射传输理论,研究了激光在生物气溶胶中传输的偏振散射特性,基于累加-倍加法(adding-doubling method)求解矢量辐射传输方程,并计算了非球形生物气溶胶对激光多次散射的斯托克斯参量。计算结果表明,生物气溶胶的尺寸和形状对光的极化更为敏感,因此在利用激光进行生物气溶胶微观特性探测和反演时,利用激光的偏振散射特性为非常有效的方法。     

The single scattering properties of the aerosol particles as aggregated spheres

The light scattering and absorption properties of anthropogenic aerosol particles such as soot aggregates are complicated in the temporal and spatial distribution, which introduce uncertainty of radiative forcing on global climate change. In order to study the single scattering properties of anthorpogenic aerosol particles, the structures of these aerosols such as soot paticles and soot-containing mixtures with the sulfate or organic matter, are simulated using the parallel diffusion limited aggregation algorithm (DLA) based on the transmission electron microscope images (TEM). Then, the single scattering properties of randomly oriented aerosols, such as scattering matrix, single scattering albedo (SSA), and asymmetry parameter (AP), are computed using the superposition T-matrix method. The comparisons of the single scattering properties of these specific types of clusters with different morphological and chemical factors such as fractal parameters, aspect ratio, monomer radius, mixture mode and refractive index, indicate that these different impact factors can respectively generate the significant influences on the single scattering properties of these aerosols. The results show that aspect ratio of circumscribed shape has relatively small effect on single scattering properties, for both differences of SSA and AP are less than 0.1. However, mixture modes of soot clusters with larger sulfate particles have remarkably important effects on the scattering and absorption properties of aggregated spheres, and SSA of those soot-containing mixtures are increased in proportion to the ratio of larger weakly absorbing attachments. Therefore, these complex aerosols come from man made pollution cannot be neglected in the aerosol retrievals. The study of the single scattering properties on these kinds of aggregated spheres is important and helpful in remote sensing observations and atmospheric radiation balance computations.     

气溶胶激光散射信号的特征分析

本文应用Mie散射理论对微球体粒子光散射的性质进行了理论分析与数值计算,得出了散射光分布与微球体尺度参数、复折射率之间的关系。结果表明:不同尺度参数的粒子的散射光强的分布相差极大,随着尺度参数的增加散射光强越来越集中于前向;复折射率的变化对散射光强影响不大。并且在边界层大陆乡村型霾的气溶胶模型下对大气气溶胶的体角散射系数进行了分析与数值计算,得出:气溶胶粒子的散射光强主要分布在前向,并且随着散射角的增加有规律的减小。由此提出了利用气溶胶粒子体散射系数的性质,通过测量散射点前向散射光强和延迟时间来实现激光束的近轴定位的方法。     

Optical properties of single mixed-phase aerosol particles

We examine the light scattering from wet aerosol particles whose core morphology is a random Gaussian sphere coated by different amounts of water. We compare the results with those calculated from a concentric-sphere particle and from a homogeneous-sphere particle whose refractive index is determined from the Bruggeman mixing rule. In nearly all cases the differences between those of the Gaussian-core and the concentric-sphere particles are small. The most significant differences are seen in calculations of the asymmetry parameters and the intensity and polarization phase functions. The results of the homogeneous-sphere particles vary significantly from those of the Gaussian-core particles, typically an order of magnitude greater than for the concentric-sphere particles. It is not uncommon to see differences of 10% in the efficiencies of large, homogeneous-sphere particles; whereas, in the intensity and polarization phase functions, differences of several tens of percent are not uncommon.     

外混合气溶胶粒子光散射的等效性

以两种典型的气溶胶粒子组成的单分散和多分散处理混合气溶胶粒子系统的光散射的各效率因子，各散射截面和散射相函数分析了以等效折射率描述由具有不同折射率的各种粒子组成的混合气溶胶粒子系统的适用性，结果表明，对单分散系统，本不同的混合比下对于许多尺度参数吸收效率因子和散射相函数的等效性很差，对多分散系统，在不同的混合比下等效性较稳定但各散射光学量的余差很大，因而对多分散系外混合气溶胶粒子系统如使用等效折射     

Comparative studies of the reflectance and degree of linear polarization of particulate surfaces and independently scattering particles

We compare measurements of the phase-angle dependencies of the intensity and degree of linear polarization of particles in air and particulate surfaces. The samples were measured at two spectral bands centered near 0.63 and 0.45 μm. The surfaces were measured with the new photometer/polarimeter at the Astronomical Institute of Kharkov National University. The scattering measurements of the particles in air were carried out with the equipment currently located at the University of Amsterdam. We study a suite of samples of natural mineral particles of different sizes all in the micrometer range, i.e. comparable with the wavelengths. The samples are characterized by a variety of particle shapes and albedos. The samples have been studied in several works and in this paper we include new SEM microphotographs of particles and spectra of powders in a wide spectral range, 0.3–50 μm, using the RELAB equipment of Brown University. We made measurements of particulate surfaces in a phase-angle range, 2–60° that is significantly wider than that of our previous studies. We confirm our earlier results that the negative polarization of the surfaces may be a remnant of the negative polarization of the single scattering by the particles that constitute the surfaces. We also find differences in the spectral behavior of the polarization degree of particles in air and particulate surfaces at large phase angles.     

利用APD对大气气溶胶空气动力学直径测量分析

详细介绍了气溶胶大气粒子经过两个激光束后通过雪崩二极管（APD）探测其形成的双峰信号,从而得到气溶胶粒子飞行时间的方法,利用标准粒子对飞行时间进行校准后,实现了对大气气溶胶粒子直径的实时监测.通过不同粒径多组的实验数据进行分析组成专家模式,代入系统进行空气测量或标准粒子测量,得到的实验值与理论值一致.     

MAX-DOAS仪器观测O4吸收对气溶胶参量的敏感性研究

研究了基于地基差分吸收光谱技术观测的O4吸收反演气溶胶光学参量的敏感性.利用大气辐射传输模型McArtim分析了不同波长、不同气溶胶光学参量(光学厚度、边界层高度、单次散射反照率、非对称因子)对O4吸收(大气质量因子)的影响.结果表明,大气质量因子对中心波长变化不敏感,气溶胶光学厚度和边界层高度对O4吸收具有重要影响,气溶胶光学厚度从0.1增加到1时,3°仰角测量的大气质量因子减少了28%,边界层高度从0.1 km增加到1 km,3°仰角测量的大气质量因子增加了9.2%.平纬圈观测模式下O4吸收对单次散射反照率和非对称因子具有较好的灵敏度,提供了一种基于地基MAX-DOAS观测O4吸收反演气溶胶光学参量的新方法.     

Scattered Light Photometer for On-Line monitoring of size distribution parameters and particle number concentration

A scattered light photometer which monitors the particle number concentration of aerosols is described. The photometer measures the scattered light from illuminated submicron particle clouds with known material properties at certain scattering angles. Intensity ratios in combination with the degree of polarization are used to determine the mean particle diameter and the geometric standard deviation of an assumed log-normal particle size distribution. The determination of the particle size distribution is based on an algorithm which compares the measured and calculated (Mie theory) relative intensity quantities described. Furthermore, the particle number concentration is monitored from a single absolute intensity measurement at one scattering angle. In order to obtain quantitative results a spherical particle shape is required.     

LIDAR investigation of properties of atmospheric aerosol

In the paper application of lidars for investigation of aerosol particle size distribution and for observation of aerosol consisting of solid state particles is presented. For size distribution the multiwavelength lidar and original method of data analysis was applied. For registration of dust transported to Central Europe from Sahara and Middle East deserts analysis of depolarization of the backscattered signals was used. In order to solve the lidar equation measurements of total atmospheric optical depth by means of Microtops sun photometer was done. Mean size and the aspect ratio of dust particles were determined by comparing of lidar observations with data from T-matrix calculations.     

Effect of electric field on light scattering by aqueous colloids of diamond and graphite

We present the results of our experimental investigation of light scattering by polydisperse colloids of diamond and graphite. The scattering is studied at a random orientation of particles and in an external radiofrequency electric field, which orients particles along the strength. The average dimensions of particles in both colloids are close to each other and comparable with the wavelength of the incident light. The shape of particles and the optical and electrooptical properties of diamond and graphite colloids are significantly different. We analyze the polarization components of scattered light energy when the light incident on the colloids is linearly polarized. We show that the quadrupole light scattering by isotropic diamond particles has the main effect on angular dependences of depolarization of scattered light. For light scattering by anisotropic graphite particles, the depolarization of scattered light is mainly determined by a particular feature of the dipole scattering of particles. It is shown that, in both colloids, the orientational order of particles considerably reduces the depolarization of light scattered by particles. We show that relative changes in the intensity and depolarization of scattered light, which depend on the scattering angle and polarization direction of light, as well as on the parameters of particles, can be used as a measure of electrooptical effects observed in colloids.     

内混合强吸收气溶胶粒子光散射的等效性

 以黑碳和水两种成分组成的内混合单分散气溶胶粒子为例,根据其各消光效率因子、吸收效率因子和散射相函数,分析了用等效折射率来描述含有不同成分的内混合气溶胶系统的适用性。结果表明：在瑞利散射区和几何光学区内,内核（碳粒）体积比为0.01,0.1,0.5,0.9时,消光效率在大多数尺度参数下等效性都很好,但在米散射区内相对较差;当体积比大于0.3时,其吸收效率、消光效率等效性较好;除瑞利散射区外,散射相函数在各体积比下的等效性都很差。当考虑内混合气溶胶粒子系统的散射和吸收特性时,一般不难找到等效折射率,但在光散射技术中,应用相函数反演等效折射率的可靠性还有待商榷。