Light absorption and scattering by aggregates: Application to black carbon and snow grains

A geometric-optics surface-wave approach has been developed for the computation of light absorption and scattering by nonspherical particles for application to aggregates and snow grains with external and internal mixing structures. Aggregates with closed- (internal mixing) and open-cell configurations are constructed by means of stochastic procedures using homogeneous and core-shell spheres with smooth or rough surfaces as building blocks. The complex aggregate shape and composition can be accounted for by using the hit-and-miss Monte Carlo geometric photon tracing method. We develop an integral expression for diffraction by randomly oriented aggregates based on Babinet's principle and a photon-number weighted geometric cross section. With reference to surface-wave contributions originally developed for spheres, we introduce a nonspherical correction factor using a non-dimensional volume parameter such that it is 1 for spheres and 0 for elongated particles. The extinction efficiency, single-scattering albedo, and asymmetry factor results for randomly oriented columns and plates compare reasonably well with those determined from the finite-difference time domain (FDTD) and the discrete dipole approximation (DDA) computer codes for size parameters up to about 20. The present theoretical approach covers all size ranges and is particularly attractive from the perspective of efficient light absorption and scattering calculations for complex particle shape and inhomogeneous composition.We show that under the condition of equal volume and mass, the closed-cell configuration has larger absorption than its open-cell counterpart for both ballistic and diffusion-limited aggregates. Because of stronger absorption in the closed-cell case, most of the scattered energy is confined to forward directions, leading to a larger asymmetry factor than the open-cell case. Additionally, light absorption for randomly oriented snowflakes is similar to that of their spherical counterparts under the condition of equal geometrical cross section area for both external and internal mixing states; however, nonspherical snowflakes scatter less light in forward directions than spheres, resulting in a substantial reduction of the asymmetry factor. We further demonstrate that small soot particles on the order of 1 μm internally mixed with snow grains could effectively reduce snow albedo by as much as 5-10%. Indeed, the depositions of black carbon would substantially reduce mountain-snow albedo, which would lead to surface warming and snowmelt, critical to regional climatic surface temperature amplification and feedback.     

Radiative transfer in finite volcanic eruption clouds

Radiation transfer through a volcanic aerosol medium has been studied. The radiation transfer properties of the medium as scattering, absorption and extinction coefficients are calculated using the Mie scattering theory. Average coefficients over the size parameter and the radiation wavelength are calculated. The radiation heat fluxes for volcanic eruption ash medium are calculated using the Variational Pomraning–Eddington approximation and compared with those obtained from the Galerkin method. The comparison showed very good agreement.     

随机取向气溶胶凝聚粒子光学特性研究

利用Cluster-cluster aggregation (CCA)模型,模拟了由64个球形原始微粒凝聚而成的四种随机取向气溶胶凝聚粒子。结合离散偶极子近似方法,分别得到了不同入射角和不同尺寸参数情况下气溶胶凝聚粒子的吸收、散射、消光效率因子和不对称因子的数值结果,并比较分析了四种形状气溶胶凝聚粒子吸收、散射、消光效率因子和不对称因子的差异。结果显示：对于相同数目原始微粒的气溶胶凝聚粒子,其光学特性明显依赖于入射光的入射角度和气溶胶凝聚粒子的形状;对于不同尺寸参数的气溶胶凝聚粒子,当入射光波长给定时,吸收、散射和消光效率因子最初随尺寸参数增大而快速增大,随后又随尺寸参数增大缓慢变小,但在尺寸参数变化过程中存在一个极大值;不对称因子则随尺寸参数的增大一直呈增大趋势,且随尺寸参数的增大趋近于1。     

Free carrier absorption in n-type CdTe

Experimental results for free carrier absorption at room temperature in lightly doped samples of n-type CdTe, including the λ³ dependence of the absorption coefficient on the photon wavelength, can be satisfactorily accounted for in terms of polar optical mode scattering with a very small contribution by impurity scattering. Use is made of the quantum theory of free carrier absorption initially developed for direct gap III–V semiconducting compounds, which utilizes the Kane band structure and includes nonparabolicity, arbitrary spin-orbit splitting values, overlap wave function factors, and intermediate states in other bands.     

Influence of surface roughness on the elastic-light scattering patterns of micron-sized aerosol particles

The relation between the surface roughness of aerosol particles and the appearance of island-like features in their angle-resolved elastic-light scattering patterns is investigated both experimentally and with numerical simulation. Elastic scattering patterns of polystyrene spheres, Bacillus subtilis spores and cells, and NaCl crystals are measured and statistical properties of the island-like intensity features in their patterns are presented. The island-like features for each class of particle are found to be similar; however, principal-component analysis applied to extracted features is able to differentiate between some of the particle classes. Numerically calculated scattering patterns of Chebyshev particles and aggregates of spheres are analyzed and show qualitative agreement with experimental results.     

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。     

空间垂直方向气溶胶消光特性的研究

在已知大气气溶胶折射率和气溶胶谱分布的基础上,对空间垂直方向的气溶胶消光特性进行了研究。文章利用Mie散射理论计算讨论了气溶胶的消光、散射、吸收系数随各参数的变化,并在MATLAB中对变化情况进行了仿真。结果表明,粒子半径与入射波长大小相近时气溶胶的消光最强,并且随着能见度的增大,气溶胶衰减系数减小。这些结论可以为红外辐射的大气衰减计算和分析提供依据。     

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.     

Light scattering by multilayer ellipsoids in the Rayleigh approximation

A problem of light scattering by multilayer confocal ellipsoids is solved in the Rayleigh approximation. The electric field of a light wave is assumed constant and a set of Laplace equations with the corresponding boundary conditions is considered. The final expression for the polarizability of a particle is represented in the matrix form (2×2 matrices) in terms of parameters of a nucleus and subsequent layers. Numerical calculations of the scattering and absorption efficiencies of small multilayer spheres obtained using the exact (the generalization of the Mie theory) and approximate solutions well agree with each other.     

光散射和消光参量对气溶胶折射系数的敏感性分析

利用米氏理论，对满足不同Ｊｕｎｇｅ谱型气溶胶的后向散射、消光以及两者之比对其折射系数实部和虚部的敏感性进行了数值计算，得出了有益的结论．     

利用DDA方法计算大气气溶胶粒子光学特性

大气气溶胶是大气的重要组成部分,其光学特性是研究大气辐射传输特性的重要参量。本文基于DDA方法,对不同形状气溶胶粒子的光学特性进行计算,得到气溶胶粒子的消光因子、吸收因子随波长变化的数值结果。结合Muller散射矩阵,给出了气溶胶粒子散射强度和极化度的角分布,为研究大气辐射传输提供了有效的方法。     

The effect of the size,shape, and structure of metal nanoparticles on the dependence of their optical properties on the refractive index of a disperse medium

The effect of the size, shape, and structure of gold and silver nanoparticles on the dependence of their extinction and integral scattering spectra on the dielectric environment has been investigated. Calculations were performed using the Mie theory for spheres and nanoshells and the T-matrix method for chaotically oriented bispheres, spheroids, and s cylinders with hemispherical ends. The sensitivity of plasmon resonances to variations in the refractive index of the environment in the range 1.3–1.7 for particles of different equivolume size, as well as to variations in the thickness of the metal layer of nanoshells, was studied. For nanoparticles with an equivolume diameter of 15 nm, the maximal shifts of plasmon resonances due to variation in the refractive index of the environment are observed for bispheres and the shifts decrease in the series nanoshells, s cylinders or spheroids, and spheres. For particles 60 nm in diameter, the largest shifts of plasmon resonances occur for nanoshells and the shifts decrease in the series bispheres, s cylinders or spheroids, and spheres. All other conditions being the same, silver nanoparticles are more sensitive to the resonance tuning due to a change in the dielectric environment.     

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.     

随机取向非球形沙尘气溶胶粒子的光学特性

利用离散偶极子近似法分析了一种随机取向旋转椭球体沙尘气溶胶粒子模型在尺度参数变化范围为0.1~23时(波长0.55!m对应有效半径为0.01~2!m)的光学特性,研究了沙尘粒子非球形性程度对其光学特性的影响,并考察了非球形粒子的随机取向能否用等体积球体来代替。就随机取向单分散和多分散旋转椭球体沙尘气溶胶而言,粒子非球形特征越明显,消光效率因子、不对称因子和单次散射反照率基本上偏离其等体积球体越大;对于相同的非球形,不对称因子偏离其等体积球体的相对偏差要比消光效率因子和单次散射反照率要大。非球形粒子的随机取向并不能使其光学特性严格等效为其等体积球体的光学特性。如果粒子形状偏离球体较小,则非球形粒子的随机取向的平均效果能使其消光效率因子、不对称因子和单次散射反照率近似用等体积球体的对应光学参量来等效;而如果粒子形状偏离球形较大,仅有单次散射反照率可以近似用等体积球体的单次散射反照率来等效,例如,轴半径比为16的旋转椭球体沙尘粒子的单次散射反照率偏离其等体积球体仅在3%以内。     

Influence of an intense pulsed electromagnetic field on nonresonant scattering of a photon by an electron for the nonrelativistic energy

The theory of nonresonant scattering of a photon by an electron in the field of an intense pulsed light wave is developed. The approximation when a pulse width is considerably greater than the characteristic time of wave oscillation is considered. The nonresonant kinematic region is determined. The general relativistic expression for the nonresonant cross-section is derived for the range of the external field intensities if η ₀ ? 1, η₀ ² ? 1 (see Eq. (12)) is valid. The obtained differential cross-section of the process has form of a sum over partial differential cross-sections. Each of them corresponds to the process with emission (absorption) of a certain number of wave photons. It is shown, that for nonrelativistic energy the cross-section summed over all possible partial processes differs considerably from the cross-section of Compton scattering if the external field is absent and may exceed the latter over than 200%.     

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。     

Optical switching based on the manipulation of microparticles in a colloidal liquid using strong scattering force

This paper demonstrates the realization of an optical switch by optically manipulating a large number of polystyrene spheres contained in a capillary.The strong scattering force exerted on polystyrene spheres with a large diameter of 4.3 μm is employed to realize the switching operation.A transparent window is opened for the signal light when the polystyrene spheres originally located at the beam centre are driven out of the beam region by the strong scattering force induced by the control light.The switching dynamics under different incident powers is investigated and compared with that observed in the optical switch based on the formation of optical matter.It is found that a large extinction ratio of ～ 30 dB and fast switching-on and switching-off times can be achieved in this type of switch.     

双光路DOAS系统获取大气颗粒物粒谱分布方法研究

当前大气复合污染日趋严重,造成大气氧化性增强,气体向颗粒物的转化加快。大气颗粒物粒径大小及谱分布决定其在大气中的行为,以差分吸收光谱法（DOAS）为基础,结合双光路设计技术,开展实时、在线、获取近地面大气气溶胶颗粒物的粒谱分布的光谱方法研究。首先构建低噪声性能稳定的宽带氙弧灯为光源的双光路差分吸收光谱系统,基于干净天气条件下大气的能见度数据对系统进行校准,通过两个不同光路获得的光谱信号强度之比获取近地面紫外-近红外波段的大气总宽波段消光系数。基于宽波段消光系数,在去除瑞利散射以及气体吸收对消光系数的影响后,解析出气溶胶颗粒物的消光系数。基于核函数准则,利用均匀球型粒子的电磁场Mie理论来反演气溶胶物理特性,获得气溶胶粒子在该测量谱段的体积谱分布,利用体积谱与数密度谱的关系,反演出气溶胶粒子的数密度谱分布。开展利用直方图方法来表现颗粒物的粒谱分布方法研究,首先将DOAS测量波段近似等分为若干谱段,利用谱段处平均值,获取气溶胶粒谱直方分布图。最后把该系统和方法应用于外场实验,获得了气溶胶颗粒物在300～650 nm范围内的消光系数,将测量波段等分为11个谱段,反演了颗粒物的在0.1～1.25 μm粒径范围的数密度谱分布。该研究为整治我国灰霾天气,研究大气气相/粒子非均相化学反应提供科学依据。同时将推动DOAS技术的进一步发展和应用。