Angle-resolved second-harmonic light scattering from colloidal particles

We report angle-resolved second-harmonic generation (SHG) measurements from suspensions of centrosymmetric micron-size polystyrene spheres with surface-adsorbed dye (malachite green). The second-harmonic scattering profiles differ qualitatively from linear light scattering profiles of the same particles. We investigated these radiation patterns using several polarization configurations and particle diameters. We introduce a simple Rayleigh-Gans-Debye model to account for the SHG scattering anisotropy. The model compares favorably with our experimental data. Our measurements suggest scattering anisotropy may be used to isolate particle nonlinear optics from other bulk nonlinear optical effects in suspension.     

Backscattering of s-polarized light from a cloud of small particles above a dielectric substrate

The scattering of s-polarized electromagnetic waves by a cloud of small particles above an interface is numerically studied, accounting for multiple scattering. The backscattering effect is first observed without the interface and the influence of the index of the particles is shown. In the case of a dilute system of particles with a low index such that no backscattering peak appears without the interface, it is shown that the introduction of an interface restores the backscattering effect. A physical mechanism responsible for this peak is described. In conclusion, a comparison of this model with scattering by rough surfaces is made.     

Backscattering of s-polarized light from a cloud of small particles above a dielectric substrate

Abstract

The scattering of s-polarized electromagnetic waves by a cloud of small particles above an interface is numerically studied, accounting for multiple scattering. The backscattering effect is first observed without the interface and the influence of the index of the particles is shown. In the case of a dilute system of particles with a low index such that no backscattering peak appears without the interface, it is shown that the introduction of an interface restores the backscattering effect. A physical mechanism responsible for this peak is described. In conclusion, a comparison of this model with scattering by rough surfaces is made.     

Numerically exact computer simulations of light scattering by densely packed, random particulate media

Direct computer simulations of electromagnetic scattering by discrete random media have become an active area of research. In this progress review, we summarize and analyze our main results obtained by means of numerically exact computer solutions of the macroscopic Maxwell equations. We consider finite scattering volumes with size parameters in the range [20] and [59], composed of varying numbers of randomly distributed particles with different refractive indices. The main objective of our analysis is to examine whether all backscattering effects predicted by the low-density theory of coherent backscattering (CB) also take place in the case of densely packed media. Based on our extensive numerical data we arrive at the following conclusions: (i) all backscattering effects predicted by the asymptotic theory of CB can also take place in the case of densely packed media; (ii) in the case of very large particle packing density, scattering characteristics of discrete random media can exhibit behavior not predicted by the low-density theories of CB and radiative transfer; (iii) increasing the absorptivity of the constituent particles can either enhance or suppress typical manifestations of CB depending on the particle packing density and the real part of the refractive index. Our numerical data strongly suggest that spectacular backscattering effects identified in laboratory experiments and observed for a class of high-albedo Solar System objects are caused by CB.     

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.     

New effects in light scattering in disordered media and coherent backscattering cone: systems of magnetic particles

Single and multiple scattering of light by magnetic particles and their implications to the coherent backscattering effect are reported. Single scattering of light by small magnetic particles presents unusual features such as forward-backward asymmetry and resonance effects. In multiple scattering, this leads to a global decrease in the localization parameter kl(*), which exhibits an oscillatory dependence on the scatterer magnetic permeability. By considering magnetic scatterers following a Curie-Weiss susceptibility law, we suggest that kl(*) can be tuned by varying the temperature.     

Lidar observation of the bubble trace in the sea surface layer

The evolutions of the signals of the elastic (Mie) and Raman backscattering of the Nd:YAG laser second-harmonic radiation in the upper layer of the sea under cavitational perturbation induced by the passage of a high-speed boat are compared under the conditions of the outdoor experiment. It is shown that the signal of the elastic scattering on bubbles returns to the background level within the time of ∼10 min. The relaxation time of the spontaneous Raman scattering signal can be an order of magnitude larger than this value (the evaluated value under the particular conditions of this experiment is ∼120 min). Interpretation is given to this difference in attenuation time of the elastic and inelastic scattering signals at the cavitational perturbation of the sea.     

Coherence effects in scattering systems of two interacting dipoles at resonance

Coherence effects in the backward-scattering direction, such as enhanced backscattering (EBS) and the appearance of a negative polarization branch (NPB), are investigated for a simple scattering system composed of two dipolelike particles separated by a fixed distance. The influence on these effects of coupling resonances between the particles is analyzed. The appearance of these coherent phenomena (EBS and NPB) and their relationship as a function of the optical properties of the particles (polarizability) and particle separation are also studied.     

Effects of nondiffusive wave propagation upon coherent backscattering by turbid media

The nondiffusive contribution to the coherent backscattering intensity is calculated for the media with relatively large particles (size a is greater than wavelength λ). The results are in good agreement with the experimental data at the wings of the angular spectrum of the coherent backscattering. The shape of the backscattering peak is analyzed for strongly absorbing media. The correlation function of the intensity fluctuations is calculated for the scattering by Brownian particles at relatively large time shifts.     

Interference effects in backscattering of light by a layer of a discrete random medium

Multiple backscattering of light by a layer of a discrete random medium is considered. A brief derivation of equations for describing the coherent and incoherent components of scattered light is presented. These equations are solved numerically in the approximation of doubled scattering of light by a semi-infinite medium of spherical scatterers having a size comparable with the wavelength in order to study the effect of the properties of particles on the angular dependence of interference effects. Calculations show that the half-width of the interference peak decreases upon an increase in lateral scattering by particles and that the degree of polarization has a complex angular dependence on the properties of the particles. For an optically thin layer of the medium, the relations defining the interference peak half-width and the scattering angle upon extreme linear polarization as functions of the effective refractive index are given.     

双层散射介质的单次后向散射光谱分析

从上皮组织的结构特点出发,基于米氏(Mie)散射理论,建立了双层散射介质的单次后向散射光谱的理论模型,该模型通过偏振门屏蔽来自下层的噪声背景,只保留来自上层的单次散射光。计算分析了粒子的形态学参量如平均尺寸及其分布、相对折射率变化时,单次散射光谱的特征。并用傅里叶波形分析法研究了这些参量对单次后向散射光谱曲线形状及其谐波幅值的影响。结果表明,这些只经历了表层粒子单次散射的光谱信号对表层粒子的平均尺寸及其分布、相对折射率具有灵敏性。对光谱曲线波纹结构的幅值、频率,散射强度,光谱谐波的幅值有直接的影响。研究结果对早期癌症的散射光谱特征识别及其特征提取有重要的实用价值。     

Magnetic field effects on coherent backscattering of light

We have studied the influence of magneto-optical Faraday rotation on coherent backscattering of light experimentally, theoretically and by computer simulations of Monte-Carlo type. The consistency of these three approaches reveals new aspects of the propagation of vector waves in turbid media with and without Faraday rotation. Experimentally, we have demonstrated that the Faraday rotation may almost completely destroy the reciprocity of light paths. However, as shown by the simulations, the cone of coherent backscattering may not only be destroyed but also shifted off the exact backscattering direction, parallel to the magnetic field, as long as the amount of circular polarization is not completely destroyed by the multiple scattering. The relationship between coherent backscattering, depolarization and Faraday rotation are explained by a simple path model of vector waves. This leads to a new characteristic correlation length required to properly describe the influence of Faraday rotation on multiple light scattering. Received 28 January 2000     

Efficient second-harmonic generation by scattering from porous gallium phosphide

We experimentally study second-harmonic generation by femtosecond Cr: forsterite-laser radiation scattered on the surface of porous gallium phosphide with characteristic pore sizes and distances between the pores comparable with the second-harmonic wavelength. The intensity of the second-harmonic signal from samples with initial crystallographic surface orientations (110) and (111) is more than an order of magnitude higher than the intensity of the second harmonic generated in reflection from single-crystal gallium phosphide. The efficiency of second-harmonic generation by macroporous gallium phosphide substantially increases as the pump wave-length becomes shorter. The influence of light localization and scattering effects on the enhancement of second-harmonic generation and polarization properties of the second-harmonic is discussed.     

Incoherent and coherent backscattering of light by a layer of densely packed random medium

The problem of light scattering by a layer of densely packed discrete random medium is considered. The theory of light scattering by systems of nonspherical particles is applied to derive equations corresponding to incoherent (diffuse) and interference parts of radiation reflected from the medium. A solution of the system of linear equations describing light scattering by a system of particles is represented by iteration. It is shown that the symmetry properties of the T-matrices and of the translation coefficients for the vector Helmholtz harmonics lead to the reciprocity relation for an arbitrary iteration. This relation is applied to consider the backscattering enhancement phenomenon. Equations expressing the incoherent and interference parts of reflected light from statistically homogeneous and isotropic plane-parallel layer of medium are given. In the exact backscattering direction the relation between incoherent and interference parts is identical to that of sparse media.     

Silver-island films probed by hyper-Rayleigh scattering and atomic force microscopy

Incoherent second-harmonic generation, or hyper-Rayleigh scattering (HRS), and atomic force microscopy (AFM) are proposed as a combined probe of nonlinear optical and structural properties of silver-island films. HRS and linear (Rayleigh) scattering indicatrices are measured. The correlation function, deduced from the HRS indicatrices and characterising spatial fluctuations of the total polarisation at second-harmonic frequency, has a length scale significantly larger than that of the correlation functions that are obtained from the AFM data and characterise spatial fluctuations of quadratic optical susceptibilities of the dipole and quadrupole types. This difference is interpreted as indicating that the HRS indicatrix shape is determined by the long-range fluctuations of the local-field factors. Received: 16 October 2001 / Revised version: 16 April 2002 / Published online: 6 June 2002     

球形粒子在聚焦拉盖尔-高斯光束中的散射特性研究

研究了球形粒子在聚焦拉盖尔-高斯光束中的散射特性. 根据广义Mie理论, 推导出球形粒子在聚焦拉盖尔-高斯光束中散射系数的解析公式. 针对光束的电场分布及粒子散射强度进行了数值仿真, 讨论了散射强度随散射角、散射球粒子半径和拓扑荷的变化特性, 并通过散射系数解释了散射强度分布的振荡现象. 结果表明, 在聚焦拉盖尔-高斯光束照射下, 球形粒子的后向散射强度随着粒子半径的增大而逐渐增大; 后向散射强度开始增大时对应的粒子半径与拓扑荷有关. 通过与高斯光束的对比, 可以看出球形粒子在聚焦拉盖尔-高斯光束中散射特性的差异, 使其在粒径测量、光通信和大气后向散射探测等方面具有潜在应用价值.     

Monte Carlo Simulation of Optical Properties of Wake Bubbles

Based on Mie scattering theory and the theory of multiple light scattering, the light scattering properties of air bubbles in a wake are analysed by Monte Carlo simulation. The results show that backscattering is enhanced obviously due to the existence of bubbles, especially with the increase of bubble density, and that it is feasible to use the Monte Carlo method to study the properties of light scattering by air bubbles.     

Light scattering by a sphere with variable optical properties of the intermediate layer

A two-parameter model of a scattering spherical particle with a layer of a variable thickness (the first parameter), inside which the refractive index is specified by an arbitrary continuous function (the second parameter), is proposed. An algorithm for calculating the extinction and backscattering efficiency factors with the help of a developed piecewise-hyperbolic approximation of the scattering coefficients is presented. A correct choice of the parameters allowed us to obtain good agreement between the experimental and calculated data on the extinction and backscattering efficiency for typical polydisperse systems of particles of irregular shape.     

Optical properties of aggregate particles comparable in size to the wavelength

The angular dependence of brightness and linear polarization of randomly oriented aggregates has been investigated in order to find rules connecting their scattering properties with their structure, packing density, complex refractive index, and number and size of the spheres forming the aggregate. Our study is based on an interpretation in terms of successive orders of scattering, in particular on the analysis of the contribution of the interference and near-field effects. Such an approach allowed us to explain and interrelate the main peculiarities of the angular dependence of the intensity and polarization displayed by aggregates. Of special interest are the aggregates showing a so-called negative branch of linear polarization of light scattered into angles close to the backscattering direction. It has been shown that the enhancement of intensity and the negative polarization in this angular range are mainly caused by the interference of multiply scattered waves as well as by near-field effects. If the number of particles in the aggregate is large enough and its size is comparable to the wavelength, the backscattering enhancement is caused by the particles in the surface layers of the aggregate, where the radiation field is mostly homogeneous, while the negative branch is mainly generated by the deeper layers of particles, where the radiation field is inhomogeneous with chaotic changes of amplitudes and phases. This results in a rather weak dependence of the negative polarization on particle location in the deeper layers of the aggregate and on particle number but not on packing density.     

Multiscattering effects in the far-field region for two small particles on a flat conducting substrate

Abstract

The scattered field in the far-field region for two small metallic particles on a conducting substrate is analysed as a function of both their separation and the angle of incidence. Special attention is paid to multiple scattering, which appears when the particles are very close, as well as to its related effects such as its influence on the enhanced backscattering phenomenon and depolarization of the incident beam in the plane of incidence.