Aerosol optical properties assessed by an inversion method using the solar principal plane for non-spherical particles

Adequate modeling of light scattering by non-spherical particles is one of the major difficulties in remote sensing of atmospheric aerosols, mainly in desert dust outbreaks. In this paper we test a parameterization of the particle shape in size distribution, single-scattering albedo, phase function and asymmetry parameter retrieval from beam and sky-radiance measurements, based on the model Skyrad.pack, taking into account the principal plane measurements configuration. The method is applied under different Saharan dust outbreaks. We compare the results with those obtained by the almucantar measurements configuration. The results obtained by both methodologies agree and make possible to extend the parameter retrieval to smaller zenith angles than that used in the retrieval from almucantar geometries.     

Transmission of radiation through an aerosol medium

The properties of radiation through an aerosol medium have been achieved. This has been done by employing Mie scattering theory to calculate the radiation transfer scattering parameters in the form of extinction, absorption and scattering efficiencies. The equation of radiative transfer for the heat flux through a plane parallel atmosphere of aerosol has been solved. The aerosol size distributions are found in practical systems. Average efficiencies over size distribution for spherical particles of complex refractive index are calculated. Therefore, the radiative properties of stratospheric aerosols have been done. The obtained results found to be in a good agreement with the previous work.     

Retrieval of aerosol physical and chemical properties from mid-infrared extinction spectra

We report several results that validate the accuracy of a retrieval method for the determination of a number of aerosol particle properties from their mid infrared (600-6000 cm⁻¹) extinction spectra. These properties include the number density, chemical composition, phase, size distribution, and to some extent, shape. The approach is based on information obtained in laboratory studies of micron-sized particles using the aerosol flow tube (AFT) technique. We report here experiments in which our method is used to measure a variety of aerosols including SiO₂ micro-spheres as well as solid NaCl, (NH₄)₂SO₄, ice and liquid water particles. The uncertainties in the retrieved aerosol properties associated with the particle shapes (spheres, spheroids, cylinders, hexagonal and rectangular prisms) as well as the effect of variations in the spectral range were evaluated. To assess the accuracy of the retrieved size distributions and particle shapes, the properties calculated from infrared spectra were compared with corresponding properties determined using alternative methods. We used scanning electron microscopy (SEM) for solid (NH₄)₂SO₄ and NaCl aerosols and direct particle imaging with an optical microscope assembly for liquid water aerosols. On the basis of the validation results, we discuss the boundaries of applicability of the most popular spectral model, single scattering by spherical, homogeneous aerosol particles.     

Extinction coefficients of surface atmospheric aerosol above LHAASO

We investigate the extinction coefficients of the surface atmospheric aerosol over the Large High Altitude Air Shower Observatory(LHAASO),located at the Haizi Mountain,Daocheng County,China.To this end,we utilize the Longtin model,Mie scattering theory,and experimental data obtained by the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation(CALIPSO).Our theoretical calculations show that the total extinction coefficients of the atmospheric aerosol at the wavelength of 200-500 nm are inversely proportional to the laser wavelength,and influenced by the wind speed.From July 2015 to October 2016,the extinction coefficient of the surface atmospheric aerosols at 532 nm wavelength reached 0.04 km~(-1) with no wind,while it increased to 0.1 km~(-1) with gusts.In this period,the extinction coefficients of the surface atmospheric aerosol at 532 nm wavelength,obtained by the CALIPSO,change from 0.01 to 0.07 km~(-1),which is less than the values obtained the theoretical calculation and larger than the average of Tibetan Plateau in 2006-2016.These calculations and experimental evidence provide important arguments to the model of atmospheric aerosol to be applied in the calibration of LHAASO.Our results suggest that the extinction coefficients over LHAASO require further study,including research on the size distribution,shape,concentration of aerosols particles,wind dependence,relative humidity dependence,etc.     

相对湿度对大气气溶胶消光系数的影响

消光系数是气溶胶颗粒物光学性质的关键参数之一。基于Mie散射理论和气溶胶颗粒粒径及折射率的湿度增长模型,本文详细研究了气溶胶吸湿性对其消光系数的影响。计算结果表明:当入射光波长为808nm、相对湿度在60%~95%之间增加时,因颗粒粒径的增长及折射率的减小,导致颗粒物消光系数曲线右移且其波动性更加明显;而对于同一球形颗粒,小粒径颗粒的消光系数随相对湿度的增加呈指数规律增大,较大粒径颗粒的则表现为波动减小趋势。此外,在不同入射光条件下,小颗粒消光系数与相对湿度之间的关系保持不变。本文的计算结果对气溶胶光学性质与大气环境质量的研究具有一定的参考价值。     

两种按比例混合颗粒系的多次散射模拟

一种颗粒与其他种类的颗粒混合后, 会使其散射特性发生变化, 本文研究了水云中混有黑炭气溶胶后的散射特性变化. 根据Mie理论计算了水云和黑炭气溶胶散射相函数、单次散射反照率和不对称因子. 给出了混合颗粒系的蒙特卡罗模拟方法, 给出了颗粒碰撞类型抽样、自由程抽样和根据Mie相函数进行散射方向抽样的方法. 计算了光垂直入射时, 水云和黑炭气溶胶混合颗粒系的反射光强随观测角的变化, 并计算了平面反照率随入射角的变化, 讨论了黑炭气溶胶的有效半径、混合比例对整个混合颗粒系散射特性的影响. 计算结果表明, 水云中混合黑炭会加强其吸收, 且黑炭的比例和尺寸不同其散射特性差异较大.     

Linearized T-matrix and Mie scattering computations

We present a new linearization of T-Matrix and Mie computations for light scattering by non-spherical and spherical particles, respectively. In addition to the usual extinction and scattering cross-sections and the scattering matrix outputs, the linearized models will generate analytical derivatives of these optical properties with respect to the real and imaginary parts of the particle refractive index, and (for non-spherical scatterers) with respect to the “shape” parameter (the spheroid aspect ratio, cylinder diameter/height ratio, Chebyshev particle deformation factor). These derivatives are based on the essential linearity of Maxwell's theory. Analytical derivatives are also available for polydisperse particle size distribution parameters such as the mode radius. The T-matrix formulation is based on the NASA Goddard Institute for Space Studies FORTRAN 77 code developed in the 1990s. The linearized scattering codes presented here are in FORTRAN 90 and will be made publicly available.     

Visible light scattering study at 470, 550, and 660 nm of components of mineral dust aerosol: Hematite and goethite

Iron oxides, usually in the form of hematite or goethite, comprise an important component of atmospheric mineral dust aerosol. Because these minerals are strong visible absorbers they play a critical role in determining the overall impact of dust aerosol on climate forcing. In this work, results from light scattering measurements from hematite and goethite dust aerosol are presented for three visible wavelengths, λ=470, 550, and 660 nm. We observe important systematic differences in the scattering between these different iron oxide samples, as well as significant wavelength dependence across the visible region of the spectrum. Aerosol size distributions are measured simultaneously with the light scattering, enabling a rigorous comparison between theoretical light scattering models and experimental data. Theoretical simulations of the scattering are carried out using both Mie and T-Matrix theories. Simulations are in reasonably good agreement with experimental data for hematite; thus, our data offer a useful check on tabulated optical constants for hematite. However, simulations show very poor agreement for goethite. The poor agreement in the goethite case is likely the result of particle shape effects related to the rod-like morphology of the goethite particles. This study demonstrates how particle mineralogy and morphology play an important role in dictating the optical properties of mineral dust aerosol, a major component of tropospheric dust.     

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.     

雾霾粒子的紫外光散射特性研究

紫外光与雾霾粒子发生散射后,其散射信道特性能够反映雾霾粒子的相关物理信息,利用无线紫外光单次和多次散射信道模型,采用Mie散射和T矩阵理论分析了霾粒子在不同形态和浓度下的紫外光散射信道特性,以及散射角对散射光强的影响,并完成了紫外光在雾霾环境下的实测。通过理论及仿真分析,得到了不同霾粒子形态下的紫外光通信路径损耗以及光强分布。结果表明：紫外光直视通信方式下,路径损耗随着霾粒子浓度的增大而增大,且通信质量差于晴朗天。非直视通信方式中,在短距离通信时,高霾浓度下的路径损耗小于中低霾浓度,然而随着通信距离的继续增大,高雾霾浓度下的通信质量急剧下降,低霾浓度下通信质量最终达到最优,且距离为200 m时通信质量能优于晴朗环境。当通信距离相同时,三种雾霾浓度下的紫外光散射光强分布均随着散射角的增大而减小,当散射角继续增大并超过90°时,低霾浓度下的散射光强最大。主要原因是虽然散射角继续增大,但是有效散射体体积逐渐减小,因此低霾浓度下的散射光强较大。且当粒子粒径相同时,球形粒子的衰减较非球形粒子大。雾霾环境下实测结果与仿真结果相类似,证明了仿真结果的正确性,并在一定程度上证明了实际大气中雾霾非球形粒子多于球形粒子。     

Optical modeling of mineral dust particles: A review

Dust particles are uniquely and irregularly shaped, they can be inhomogeneous, form agglomerates, be composed of anisotropic materials, and have a preferred orientation. As such, modeling their light scattering is very challenging. This review takes a look at the advances in dust optical modeling over the last decade. It is obvious that our ability to model the single-scattering properties of dust particles accurately depends on the size parameter. Unfortunately, our ability to account realistically for all the relevant physical properties in light-scattering modeling is the best for small particles; whereas, the realistic treatment of the particles would be most important for large size parameters. When particles are not much larger than the wavelength, even simple model shapes such as homogeneous spheroids appear to perform well; practically any reasonable shape distribution of non-spherical model particles seems superior compared to the Mie theory. Our ability to model scattering by dust particles much larger than the wavelength is very limited: no method presently exists to predict reliably and accurately the single-scattering properties of such particles, although there are models that can be tuned to agree well with the laboratory-measured reference scattering matrices. The intermediate size parameters between the resonance domain and the geometric-optics domain appear to be almost uncharted territory and, consequently, very little can be said about the impact of different physical properties on scattering in this region. Despite the challenges, the use of Mie theory should be avoided: contrary to the popular belief, the use of Mie spheres is a major source of error even in radiation-budget considerations.     

Testing a new photocentrifuge for submicron particles with silica spheres

A theory has been developed for spectral photosedimentation in a centrifuge. The use of several wavelengths allows particle size analyses in the submicron range without a knowledge of the optical material properties and is not restricted to spherical particles. As a result of this theory the extinction efficiency and the particle size distribution of the analysed particles can be calculated even for non-spherical particles from an experiment. A photocentrifuge has been built according to the developed theory. The theory has been verified by the measurement of spherical particles for which Mie theory is applicable. The experimentally obtained extinction efficiency agrees well with computations according to Mie theory. The accuracy of measured particle size distributions is comparable to those measured with other sedimentometers.     

Light scattering properties of sea-salt aerosol particles inferred from modeling studies and ground-based measurements

Direct climate radiative forcing depends on the aerosol optical depth τ, the single scattering albedo ?, and the up-scatter fraction β; these quantities are functions of the refractive index of the particles, their size relative to the incident wavelength, and their shape. Sea-salt aerosols crystallize into cubic shapes or in agglomerates of cubic particles under low relative humidity conditions. The present study investigates the effects of the shape of dried sea-salt particles on the detection of light scattering from the particles. Ground-based measurements of scattering and backscattering coefficients have been performed with an integrating nephelometer instrument for a wavelength . The measurements are compared to two models: the Mie theory assuming a spherical shape for the particles and the Discrete Dipole Approximation (DDA) model for the hypothesis of cubic shape of the sea-salt aerosols. The comparison is made accurately by taking into account the actual range of the scattering angles measured by the nephelometer in both models that is from 7° to 170° for the scattering coefficient and from 90° to 170° for the backscattering coefficient. Modeled scattering and backscattering coefficients increase for nonspherical particles compared to spherical shape of particles with diameter larger than about 1 μm. However, the comparison of the modeling results with the measurements gives best agreement for particles diameter less than about 1 μm. The size distribution of the particles is measured with two instruments with different size bins: an electrical low-pressure impactor (ELPI) and an aerodynamic particle sizer (APS). It is found that the size of the bins of the instruments to determine the number concentration of the particles in accordance with their diameter is critical in the comparison of measurements with modeling.     

The reflection and polarization properties of non-spherical aerosol particles

In this paper, we investigate the capability of multi-angle TOA reflectance and polarized reflectance for the retrieval of aerosol properties including aerosol mode (fine mode and coarse mode), aerosol shape (sphere and non-spherical), and aerosol optical thickness. Single-scattering parameters and phase-matrix elements were computed for randomly oriented non-spherical aerosol particles. Sensitivity indices were introduced to quantify the sensitivity of the TOA total reflectance and polarized reflectance to aerosol parameters. Finally, on the basis of the sensitivity study, this paper presents a conceptual approach toward the remote sensing of non-spherical aerosol three parameters (aerosol mode, aerosol shape, and aerosol optical thickness) using the TOA total reflectance and TOA polarized reflectance for the 0.865 μm spectral bands measured at multiple viewing angles.     

Mass concentration calculation with the pulse height distribution of aerosols and system calibration

The pulse height distribution of aerosols, which was measured by an optical particle counter, was applied to inverse aerosol mass concentration. Using the conceptions of equivalent diameters, the feasibility that the pulse height distribution was used to inverse mass concentration was verified theoretically, and then the definition of average mass was introduced. According to the Mie scattering theory, considering particle shape and non-uniformity of intensity distribution in the optical sensing volume, a novel algorithm for mass concentration was proposed based on the theoretical analysis. In this algorithm, we only need to calibrate two coefficients. The Gauss-Newton and the two-step calibration methods were presented. The former method revealed that calibration coefficients calculated with nonlinear regression are related to the range of mass concentration, leading to the instability of the calibration coefficients. Furthermore, though detailed analysis of the problem, the latter method was put forward. The experimental results indicate mass concentrations inversed by the algorithm have high precision.     

基于平均质量的悬浮颗粒物的质量密度算法

基于米氏(Mie)散射理论得到了粒子计数器测量球形颗粒物质量密度的计算公式。考虑非球形颗粒,从颗粒群粒度分布概念出发,提出了统计意义上的平均质量概念,推导了非球形颗粒物质量密度的理论公式。运用理论公式证明了粒子计数器测量非球形颗粒物质量密度计算公式的合理性,进而给出了基于平均质量的悬浮颗粒物的质量密度算法,该算法只需对两个系数进行标定。实验表明,该算法的质量密度计算值与实际值十分吻合,两者拟合直线的斜率为0.9713,相关系数为0.9998。该算法为实现粒子计数器在线测量悬浮颗粒物的质量密度提供了一种可行途径。     

测量气溶胶单粒子折射率方法研究

设计了一种粒子计数器,它可以测量粒子的动力学粒径和两个散射角下的散射光强度,而粒子的散射强度可以根据Mie散射理论从光学等效粒径和粒子折射率出发计算出来。当可以近似认为动力学粒径与光学等效粒径相同时,利用上述测量结果可以反演计算单个粒子的折射率。     

A Review of Elastic Light Scattering Theories

Mie scattering is an important tool for diagnosing microparticles or aerosol particles in technical or natural environments. Mie theory is restricted to spherical, homogeneous, isotropic and non-magnetic particles in a non-absorbing medium. However, as microparticles are hardly ever spherical or homogeneous, there is much interest in more advanced scattering theories. During recent decades, scattering methods for non-spherical and non-homogeneous particles have been developed and even some computer codes are readily available. Extension of Mie theory covers coated spheres, stratified spheres and clustered spheres. For homogeneous non-spherical particles such as spheroids, ellipsoids and finite cylinders, surface discretization methods have been developed. Scattering by inhomogeneous particles may be computed by volume discretization methods.     

近红外波段气溶胶的衰减特性研究

在已知大气气溶胶折射率和气溶胶谱分布的基础上, 对近红外波段的气溶胶衰减特性进行了研究。利用Mie散射理论计算并讨论了气溶胶的消光、散射、吸收效率因子随尺度参数的变化和消光系数随半径和波长的变化, 并且在MATLAB中对各种变化情况进行了仿真。结果表明, 三种气溶胶粒子的消光和散射能力依次为沙尘性粒子, 水溶性粒子, 烟煤。消光系数在粒子半径和入射波长相近时达到最大, 并且粒子半径对消光、散射、吸收系数的影响比入射波长更明显。这些结论可以为红外辐射在大气中的衰减计算和分析提供依据。     

非球形椭球粒子参数变化对光偏振特性的影响

针对自然界中多数沙尘、烟煤粒子的非球形问题, 在球形粒子偏振特性的基础上, 进一步研究非球形椭球粒子的折射率、有效半径、粒子形状等参数变化对光偏振特性的影响, 采用基于T矩阵的非球形粒子仿真方法, 模拟非偏振光经椭球粒子传输后光的偏振特性及其与球形粒子间的差异, 并以实际沙尘、海洋、烟煤三种气溶胶粒子为例说明结果的正确性. 结果表明: 当折射率实部越小, 虚部越大时, 球形粒子与非球形粒子的偏振差异越不明显; 当粒子有效半径增加时, 球形粒子偏振度的变化比非球形粒子更为明显, 且最大值分别出现在散射角为150°和120°的位置; 当粒子形状不同时, 不同形状椭球及球形粒子的差异在散射角小于60° 时并不明显, 且当椭球粒子纵横比互为倒数时, 两种粒子的偏振特性近似相同. 通过以上分析可知, 在光传输过程中, 椭球粒子多数情况下无法被近似为球形粒子进行计算.