Multiple-scattering suppression in dilute and concentrated colloidal dispersions

Summary We describe the design and operation of an improved two-colour dynamic light scattering (TCDLS) equipment which effectively suppresses multiple scattering and allows the study of the Brownian dynamics of optically turbid samples. The technique operates by cross correlating scattered light of two different colours. With the appropriate scattering geometry, only singly scattered light contributes to the time-dependent part of the measured intensity cross-correlation function thus allowing straightforward interpretation of the data. To test the performance of the instrument we have studied several dilute colloidal suspensions, which, although dilute enough that free diffusion of the particles can be assumed, ranged from quite transparent to distinctly turbid. We have confirmed that the measured cross-correlation functions accurately reflect only single scattering even in the presence of strong multiple scattering. As a first application of the technique, we have performed light scattering measurements on concentrated suspensions of PMMA particles in cis-decalin. Paper presented at the I International Conference on Scaling Concepts and Complex Fluids, Copanello, Italy, July 4–8, 1994.     

单光束互相关法测量高浓度纳米颗粒粒径

针对光子相关光谱法不能测量高浓度纳米颗粒粒径和双光束互相关测量法装置结构过于复杂等问题,提出了一种基于范西特-泽尼克定理的单光束互相关法。首先分析了传统双光束互相关法存在的问题,然后根据范西特-泽尼克定理建立了单光束互相关测量法的模型,设计完成了单光束互相关颗粒粒度测量装置,最后对各种浓度不同粒径的颗粒进行了测量。实验证明,单光束互相关法能有效抑制多重散射的影响,适用于测量高浓度纳米颗粒粒径。     

Resolving Concentrated Particle Size Mixtures Using Dynamic Light Scattering

Dynamic light scattering (DLS) is a technique used for measuring the size of molecules and particles undergoing Brownian motion by observing time‐dependent fluctuations in the intensity of scattered light. The measurement of samples using conventional DLS instrumentation is limited to low concentrations due to the onset of a phenomenon called multiple scattering. The problems of multiple scattering have been addressed in a light scattering instrument incorporating non‐ invasive backscatter optics (NIBS). This novel optic arrangement maximizes the detection of scattered light while maintaining signal quality and allows for measurements of turbid samples. This paper discusses the ability of backscatter detection to accurately determine particle sizes at 1 %w/v sample concentrations and demonstrates the correct resolution of different size populations using a series of latex standard mixtures with known volume ratios. The concentration of 1 %w/v is much higher than can be measured on conventional dynamic light scattering instruments.     

Transport of quantum noise through random media

We present an experimental study of the propagation of quantum noise in a multiple scattering random medium. Both static and dynamic scattering measurements are performed: the total transmission of noise is related to the mean free path for scattering, while the noise frequency correlation function determines the diffusion constant. The quantum noise observables are found to scale markedly differently with scattering parameters compared to classical noise observables. The measurements are explained with a full quantum model of multiple scattering.     

旋转圆柱目标的动态散斑统计特性(英)

高斯光束照射以固定角速度旋转的粗糙圆柱体表面,反射空间形成随着被测表面运动变化的动态散斑。研究了照射面积大于圆柱曲面条件下在远场衍射区形成的动态散斑统计特性,得到了不同入射条件及不同圆柱时动态散斑强度起伏空间-时间归一化相关函数。结果表明:随着圆柱半径、旋转速度以及照射光斑有效面积的增大,动态散斑强度起伏相关性快速减小;当圆柱旋转速度恒定,动态散斑光强起伏相关函数的峰值随着探测点之间距离的增大而减小,但峰值的位置随之而增大;在近似点照射情况下随着圆柱半径的增大空间相关长度基本不变,而相关时间性明显增大。     

高散射媒质中的光程可分割动态光散射研究

为研究散射光强度随光子在散射媒质中散射光程的变化,基于单散射理论与扩散波光谱理论,采用了低相干动态光散射装置对不同粒径大小的聚苯乙烯悬浮液进行研究。将测量得到的背散射光光场强度谱的线宽与相应的理论计算结果相比较发现,在短光程区域,考虑容器壁附近拖曳效应的影响后,对于不同粒径的颗粒,光程为约5倍粒子平均自由程的区域可看成为单散射区域;对于光程大于225 m的区域可看成为扩散光波区域。实验结果表明低相干动态光散射法可实现高散射媒质从单散射区域到低次散射再到扩散区域的全光程的可分割的光场强度谱测量。     

Comparative Test of Methods to Determine Particle Size and Particle Size Distribution in the Submicron Range

Among the most important characteristic properties of disperse systems such as latices, pigments, ceramic materials or drug formulations are the particle size and the particle size distribution. To measure these quantities, several methods and measuring instruments based on different physical principles are available. These include turbidimetry, dynamic and static light scattering, electron microscopy with image analysis, ultra- and disc centrifugation, light diffraction and the electrical sensing zone method. All these measuring techniques are doubtless necessary because of the large product variety and the broad particle size range. However, some problems arise if different techniques are used and the results are compared uncritically without considering to the application range and the resolution of the methods. An extensive comparative test was therefore carried out using seven latices in the submicron range with defined monomodal, bimodal and hexamodal particle size distributions. The most important methods of determining average particle size values and particle size distributions were tested and compared. Of the methods to determine only average particle sizes, turbidimetry is the most efficient, followed by dynamic light scattering with cumulants evaluation. Static light scattering only yields accurate results for small particles with narrow particle size distributions. Of the methods to determine particle size distributions, ultracentrifugation and, somewhat less, disc centrifugation and electron microscopy with image analysis are the most efficient. Dynamic light scattering only yields reliable results in the case of small particles with narrow distribution curves. Light diffraction and the electrical sensing zone method are less suitable for the submicron range.     

Kinetics of colloidal fractal aggregation by differential dynamic microscopy

We study the kinetics of an aggregation process induced by adding salt to a stable colloidal suspension of 73 nm (diameter) particles. Despite the subdiffraction size of the colloidal particles, the process is monitored via optical microscopy, which is used here to obtain time-resolved scattering information about the colloidal aggregates. The radius of the aggregates is determined as a function of time and their fractal dimension is extracted. Our results are compatible with a diffusion limited aggregation process, as independently confirmed by spectral turbidimetry measurements on the same sample.     

The Estimation of Multiple Light Scattering in Turbid Colloidal Suspensions using a 2-Probe Detector

This paper describes a detector for the direct measurement of multiple scattering in moderately turbid colloidal suspensions. The detector uses two optical fibers aligned so that one of the fibers measures the total signal (single and multiple scattering) and the other measures multiple scattering only. We report the results of preliminary investigations, and show how such a detector can be used to aid both static and dynamic light scattering investigations. In the former case we show how this information can be used to correct for low level multiple scattering. The utility and limitations of the technique are discussed.     

Microrheology from rotational diffusion of colloidal particles

The microrheology of viscoelastic fluids is obtained from rotational diffusion of optically anisotropic spherical colloidal probes, measured by depolarized dynamic light scattering. The storage and loss moduli obtained from the rotational mean squared displacement is in excellent agreement with those obtained from translational diffusion and by mechanical measurements. We also show that this method is applicable to samples with strong light scattering components. This extends the capabilities of the microrheological methods based on the diffusional motion of colloidal probes.     

Measurement of elastic light scattering from two optically trapped microspheres and red blood cells in a transparent medium

Optical tweezers can be used to manipulate small objects and cells. A trap can be used to fix the position of a particle during light scattering measurements. The places of two separately trapped particles can also be changed. In this Letter we present elastic light scattering measurements as a function of scattering angle when two trapped spheres are illuminated with a He-Ne laser. This setup is suitable for trapping noncharged homogeneous spheres. We also demonstrate measurement of light scattering patterns from two separately trapped red blood cells. Two different illumination schemes are used for both samples.     

Diffusive mobility of fractal aggregates over the entire Knudsen number range

We determine the effective mobility radius for fractal aggregate particles. Our method is to use static light scattering to measure the radius of gyration R(g) of the aggregates, and dynamic light scattering to measure the diffusion coefficient hence the mobility radius R(m). The range of our results can be specified by the Knudsen number Kn, which is the mean free path of the medium molecules divided by the radius of the aggregate. Our results apply to the entire range of Kn from the continuum limit (Kn=0) to the free molecular limit (Kn>1). In the continuum regime we find R(m)/R(g)=0.97+/-0.05 when the aggregate fractal dimension is D(f) approximately 2.15, and 0.70+/-0.05 when D(f) approximately 1.75. The latter result is independent of Kn for Kn < or approximately 1.3. The free molecular mobility goes as R(m)=aN(0.44+/-0.03), where a is the monomer radius and N is the number of monomers per aggregate. Since R(g) approximately aN(1/D(f)), R(m)/R(g) is not a constant when Kn is large. We find for all Kn that the functionality of R(m)/R(g) must always begin with the correct N-->1 limit, and this affects experimental observation.     

Measurement of optical constants for dense media by low-coherence dynamic light scattering

We perform the optical constants measurements for different absorption dense media by low-coherence dynamic light scattering (DLS) technique. The estimated particle size is used to calculate the scattering coefficient of particles suspended in dense media. The path-length resolved intensity distributions of light backscattered from the absorbing dense media are investigated experimentally by virtue of path-length resolved performance in low-coherence DLS measurements. The absorption coefficient can be obtained by applying the measured path-length resolved intensity distributions to the modified Lambert-Beer law. As a result, we proposed a new low-coherence DLS technique in simultaneous measurement of the scattering and absorption coefficients of absorbing dense media.     

Theory of pion-nucleus scattering lengths

We calculate the scattering lengths for pions on light nuclei, in a multiple scattering theory given earlier. We include all effects through second order in the pion-nucleon scattering amplitudes, using a simple nuclear model. We show how to calculate the binding corrections (BC) consistently, and find large cancellations between differentBC terms. The resulting scattering lengths are smaller than those obtained from measurements of pi-atomic level shifts. The size of the difference is consistent with the contribution of pion absorption, which we estimate.     

蒙特卡罗法计算无序激光器的阈值

提出了计算无序激光器阈值增益的模型,提出了已知平均自由程和散射强度分布得到分布函数及相应的随机变量的方法.对各向同性的光散射,导出了各分布函数,并在每次散射中得到相应的随机变量.运用蒙特卡罗法模拟光子在无序介质中的随机行走,得到了无序激光器的阈值.讨论了阈值增益与光子平均自由程、增益区半径、增益区深度、非增益区光吸收系数的关系,提出了降低阈值的方法.理论结果与实验数据是符合的. 关键词： 激光物理 阈值 蒙特卡罗 散射     

Investigation of interface roughness cross-correlation properties of optical thin films from total scattering losses

The interface roughness and interface roughness cross-correlation properties affect the scattering losses of high-quality optical thin films. In this paper, the theoretical models of light scattering induced by surface and interface roughness of optical thin films are concisely presented. Furthermore, influence of interface roughness cross-correlation properties to light scattering is analyzed by total scattering losses. Moreover, single-layer TiO₂ thin film thickness, substrate roughness of K9 glass and ion beam assisted deposition (IBAD) technique effect on interface roughness cross-correlation properties are studied by experiments, respectively. A 17-layer dielectric quarter-wave high reflection multilayer is analyzed by total scattering losses. The results show that the interface roughness cross-correlation properties depend on TiO₂ thin film thickness, substrate roughness and deposition technique. The interface roughness cross-correlation properties decrease with the increase of film thickness or the decrease of substrates roughness. Furthermore, ion beam assisted deposition technique can increase the interface roughness cross-correlation properties of optical thin films. The measured total scattering losses of 17-layer dielectric quarter-wave high reflection multilayer deposited with IBAD indicate that completely correlated interface model can be observed, when substrate roughness is about 2.84 nm.     

Probing a nonequilibrium einstein relation in an aging colloidal glass

We present a direct experimental measurement of an effective temperature in a colloidal glass of laponite, using a micrometric bead as a thermometer. The nonequilibrium fluctuation-dissipation relation, in the particular form of a modified Einstein relation, is investigated with diffusion and mobility measurements of the bead embedded in the glass. We observe an unusual nonmonotonic behavior of the effective temperature: starting from the bath temperature, it is found to increase up to a maximum value, and then decrease back, as the system ages. We show that the observed deviation from the Einstein relation is related to the relaxation times previously measured in dynamic light scattering experiments.     

Time-dependent strength of colloidal gels

Colloidal silica gels are shown to stiffen with time, as demonstrated by both dynamic light scattering and bulk rheological measurements. Their elastic moduli increase as a power law with time, independent of particle volume fraction; however, static light scattering indicates that there are no large-scale structural changes. We propose that increases in local elasticity arising from bonding between neighboring colloidal particles can account for the strengthening of the network, while preserving network structure.     

Scattering of Polarized and Natural Light by a Monolayer of Spherical Homogeneous Spatially Ordered Particles under Normal Illumination

We consider distortions of the shapes of absorption bands of strongly scattering samples in the spectra of molecules adsorbed on the surface of dispersed solids. We show that the influence of the scattering on IR spectra of dispersed samples is not reduced merely to a weakening of the intensity of the transmitted light, but, rather, the scattering affects the contour of a spectral band due to changes in the refractive index of the substance in the range of the absorption band. Using carbon dioxide adsorbed on a NaX zeolite as an example, we demonstrate two methods for taking into account the contribution of the scattering to the spectra of surface compounds: the registration of the “diffuse-transmission” spectrum and placing a sample into an immersion liquid, for which liquid oxygen is used. The obtained spectra indicate that, if the zeolite is saturated with the adsorbate, the band of the antisymmetric stretching vibration of CO₂ molecules broadens and reveals a complex structure as a result of the resonant dipole–dipole interaction between adsorbed molecules.     

基于后向散射的高浓度纳米颗粒粒度分布测量方法研究

传统的动态光散射法通常采集侧向散射进行纳米颗粒粒度分布的测量,由于多次散射的影响,利用侧向散射不能准确测量高浓度样品的颗粒粒度分布。针对该问题,对后向散射测量方法进行了研究,在实验基础上提出了后向散射最佳光程的判断准则。在不同样品浓度下,用侧向散射和后向散射方法对标称粒径分别为110 nm、220 nm的聚苯乙烯乳胶球颗粒进行了测量。实验结果表明,对于高浓度的待测样品,后向散射测量方法通过自适应调整光程,在最优光程处进行测量,能够有效得到高浓度纳米颗粒的粒径及粒度分布,测量结果相对误差为2.72%。