颗粒系的可见消光光谱分析及最佳波长的选择

在光全散射法颗粒粒径测量中,被测颗粒系的消光光谱包含有颗粒粒径、折射率等信息。对常用的单峰及双峰R-R分布的可见消光光谱进行模拟,分析了可见消光光谱随粒径和相对折射率变化的规律。选取二阶微分可见消光光谱不连续点对应的波长作为测量波长,并将可见光边界波长同时作为测量波长,在非独立模式下,采用遗传优化算法反演粒径分布。仿真计算与实验验证结果表明,通过消光光谱分析,可以预先确定被测颗粒系的分布状况,缩小优化算法中反演参数的搜索范围。结合最佳波长选择方法,使测量的精度和可靠性明显提高。对测量光谱加入1%随机噪声时,单峰及多峰分布粒径反演均能得到满意的结果。     

动态光散射测量粒径分布的格雷码编码遗传算法反演运算

采用格雷码编码的遗传算法对动态光散射测量的粒径分布进行反演运算,数字测试结果表明,对于无噪声的分布,算法能精确的反演出各种粒子分布图像;对于加了一定噪声的分布,算法显示出较好的稳定性,能反演出主峰的分布图像.聚苯乙烯乳球的实验结果表明,该算法能反演双分布的粒径分布图像.与标准遗传算法和反演蒙特卡罗算法相比,该算法具有较高的搜索效率,能够用较少的计算时间快速搜索到最优解.格雷码编码遗传算法是一种更有效的随机反演算法.     

应用低相干动态光散射法测量悬浮液中的颗粒粒径分布

利用低相干动态光散射法测量不同浓度悬浮液中的颗粒粒径分布。由低相干光源和迈克尔逊干涉仪,结合传统的动态光散射技术组成低相干动态光散射装置,通过检测单次背散射光的能谱分布,利用CONTIN算法得到不同浓度悬浮液中颗粒的粒径分布。结果表明,对于1%～10%体积浓度范围内的单分散悬浮液羊品测量得到的颗粒粒径精确度在4%以内。     

Particle Size Distribution of Nanospheres by Monte Carlo Fitting of Small Angle X‐Ray Scattering Curves

A method for recovering the size distribution of spherical particles from small angle scattering data by using a Monte Carlo interference function fitting algorithm is presented. The method is based on the direct simulation of the small angle scattering data upon the assumption of non‐interacting hard sphere ensembles (“dilute” solution approximation). The algorithm for retrieving the particle size distribution does not require any additional parameters apart from the input of the scattering data. The fitting strategy necessarily implies positive particle size distributions, while preserving the advantage of the indirect transformation method for data desmearing. Furthermore, the present approach does not use any regularisation procedures of the best fit solution and favours smooth particle size distributions. The Monte Carlo procedure has been tested against several simulated cases with various types of mono‐ and bi‐modal size distributions and different noise levels. In the special case of non‐interacting spheres, the Monte Carlo fitting algorithm had the same retrieving ability as the well assessed indirect transformation, structure interference and maximum entropy methods. Finally, the algorithm was applied to retrieve the distribution of spherical nanopowders produced by gas‐to‐particle conversion both as free powder and as reinforcing second‐phase agent in polymer nanocomposites.     

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%。     

Fractal Character of Dynamic Light Scattering of Particles

Dynamic light scattering signals from particles, exhibit fractal characteristics. This feature can be used to determine the particle size. The use of the fractal dimension, as a quantitative method to analyze the properties of dynamic light scattering signals from submicron particles, is presented. The analysis is performed directly on the time‐resolved scattered intensity, and the Box Dimensions of light scattering signals of particles with diameters 100, 200, 500 and 1000 nm. The experimental results show that the fractal dimensions of light scattering signals correlate well with particle size. In the submicron size range, the smaller the particles, the larger their fractal dimensions. Compared with the PCS technique, only several hundreds of samples are required in the fractal method. Therefore, the data processing is easily accomplished. However, this method only provides the mean particle size, but not the particle size distribution.     

含噪动态光散射测量数据反演中正则化算法与Chahine算法的比较

采用两种常用的粒度反演方法——正则化和Chahine算法,对90nm与250nm单峰分布、50nm与200nm双峰分布、100nm与300nm双峰分布的模拟动态光散射数据,以及105nm、300nm标准颗粒的实测动态光散射数据进行了反演分析.结果表明:噪声水平的高低是影响粒度分布反演准确性的关键因素之一,反演结果的准确性随噪声水平的增加而降低,噪声水平超过某一阈值后,将无法得到有意义的反演结果;不同反演方法具有不同的抗噪能力,在低噪声水平下反演结果无显著差别,随着噪声水平的增加,反演结果表现出很大差异;正则化方法通过正则参数的选择可以有效抑制噪声影响,表现出强于Chahine算法的抗噪能力;与Chahine算法相比,正则化方法不需要假定初始分布,因此,在噪声较大的实验或生产过程中进行颗粒分布测量时,宜采用正则化方法.     

双峰分布颗粒体系的多角度动态光散射数据反演

采用多角度动态光散射和加权正则化反演方法,对4组模拟的双峰分布颗粒体系(100/600 nm,200/600 nm,300/600 nm和350/600 nm)分别选取1、3、6和10个散射角进行测量.粒度反演结果表明,采用加权正则化方法反演双峰颗粒体系的多角度动态光散射测量数据,可获得峰值位置比小于2∶1且含有大粒径(＞350 nm)颗粒的双峰颗粒粒度分布.采用标准聚苯乙烯乳胶颗粒进行实测的结果验证了这一结论.得到含大粒径颗粒的双峰粒度分布反演结果的原因在于,多角度动态光散射能提供更多的大粒径颗粒的粒度信息,加权正则化反演方法能减少测量数据中的噪声,因而多角度动态光散射测量数据的加权反演能实现峰值位置比小于2∶1且含有大粒径颗粒的双峰颗粒体系的测量.     

Determination of Particle Size Distribution Parameters using a Laser-Scattered Light Spectrometer

A method based on the measurement of scattered light intensity distributions is demonstrated to be able to determine directly the particle size of monodisperse supermicron-size particles. In all other cases of a particle cloud, information about the size distribution can be acquired from comparison of measured and calculated intensities as a function of scattering angle. This indirect method is only applicable if the assumptions made in the theory used for comparison are fulfilled. Therefore, the method is limited to spherical particles with known refractive index. The type of size distribution also has to be known. In the cases considered a log-normal size distribution was assumed. The uncertainty of the result increases with increase in the number of parameters that have to be determined. The method seems to be limited to unimodal distributions described with two parameters.     

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.     

Ultrasonic Measurement of Sub-Micron Particles

Based on technology described in a Du Pont patent for an offline system, we have developed a prototype in-line ultrasonic cell for measuring particle size distribution. We have used this cell to verify the Allegra-Hawley model of ultrasonic attenuation in dilute (< 5 % vol) slurries of sub-micron ceramic particles, and we are developing a model that can cope with the multiple scattering effects occuring at higher concentrations. In this paper we present the results of attenuation measurements for ultrasound (2–50 MHz) in slurries with concentrations ranging from 0.5 010 to 38 010 (vol). The attenuation is proportional to slurry concentration up to 5 010 (vol) and is predicted by single scattering models. Above approximately 100% concentration, the attenuation is actually lower than expected. For the dilute slurries we find excellent agreement between our measurements and the Allegra-Hawley calculations, and the effects of the particle size distribution are evident in the ultrasonic attenuation spectrum. These ultrasonic data can be inverted to determine the particle size and concentration in aqueous slurries of sub-micron particles.     

光散射法测量微粒粒径分布的一种反演遗传算法

本文提出一种基于改进遗传算法的随机及演方法,该方法具有更强的全局收敛性,同时也具有对粒径分布形状不敏感、抗噪声能力强等优点,适合于工业现场应用．     

Anomalous diffraction approximation method for retrieval of spherical and spheroidal particle size distributions in total light scattering

Using total light scattering technique to measure the particle size distribution has advantages of simplicity in measurement principle and convenience in the optical arrangement. However, the calculation of extinction efficiency based on Mie theory for a spherical particle is expensive in both time and resources. Thus, a simple but accurate approximation formula for the exact extinction efficiency may be very desirable. The accuracy and limitations of using the anomalous diffraction approximation (ADA) method for calculating the extinction efficiency of a spherical particle are investigated. Meanwhile, the monomodal and bimodal particle size distributions of spherical particles are retrieved using the genetic algorithm in the dependent model. Furthermore, the spheroidal model in the retrieval of non-spherical particle size distribution is also discussed, which verifies the non-sphericity has a significant effect on the retrieval of particle size distribution compared with the assumed homogeneous isotropic sphere. Both numerical computer simulations and experimental results illustrate that the ADA can be successfully applied to retrieve the particle size distributions for spherical and spheroidal particles with high stability even in the presence of random noise. The method has advantages of simplicity, rapidity, and suitability for in-line particle size measurement.     

基于超声波测量技术的颗粒尺寸分布模型的研究

提出了一种利用单颗粒背向散射信号来进行粒径分布估算的超声波测量技术,系统阐述了其 理论基础及基本工作原理。被测颗粒的散射信号幅度与它在探测区中的位置、颗粒尺寸和形状有关。 通过理论分析,建立了一个可用于描述散射信号幅度概率分布与颗粒系尺寸分布之间关系的数学模 型,对该模型的反演计算便可得到颗粒系的尺寸分布信息。为了避免求解过程中的病态系数矩阵问 题,将模型求解转化成了易于解决的最优化问题。仿真实例结果验证了该技术的可行性。     

生物组织的可见光与近红外光散射模型

对生物组织光学模型尤其是光散射特性进行了研究, 发现可以利用等效粒子数密度的粒度分布更精确地了解生物组织的光散射性质。在夫琅和费衍射近似下, 散射系数和散射相函数可以由等效粒子数密度的粒度分布得到。基于粒子粒度光散射测量技术, 所得结果可给出一种新的可行的测量生物组织光学性质参数的方法。     

Inversion of visible optical extinction data for spheroid particle size distribution based on PCA

The problem of light scattering properties of spheroid particles is studied, and a general approach is presented for calculating the single particle light scattering of spheroids. In this approach, the extinction efficiency of spheroid particles can be calculated by combining the spline interpolation of T matrix method and ADA (anomalous diffraction approximation) theory. Furthermore, the retrieval of spheroid particle size distribution is performed in the dependent mode and a selection method about the optical extinction data is proposed based on PCA (principle component analysis) of first derivative corresponding to the raw optical extinction. By calculating the contribution rate of first derivative corresponding to the raw optical extinction, the optical extinction with more significant features can be selected as the inversion optical extinction data. In this way, the selected optical extinction has less information redundancy and higher capacity of resisting noise disturbance. Simulation experiments indicate that the spheroid particle size distributions obtained with the proposed method coincide fairly well with the given distributions, which provides a simple, reliable and efficient method to retrieve the spheroid particle size distribution using the optical extinction data.     

非独立模式算法下粒径分布反演及分类的研究

在光全散射法颗粒粒径测量中,提出一种非独立模式算法下粒径分布反演及分类的方法。对被测颗粒系分别按照不同的粒径分布函数同时进行反演,并依据反演误差大小判断被测颗粒系符合哪种分布函数。仿真实验结果表明,在非独立模式下,完全可以利用已知的不同分布函数的反演误差作为分类依据,从而更准确地确定被测颗粒系的粒径分布。采用的遗传反演算法能够在3个可见光波长下得到较准确的粒径分布,反演结果稳定可靠,最大限度地减少了多个波长的使用,从而对光源有更大的选择余地。对透射消光测量结果加入5%随机噪声时,单峰分布颗粒系的反演误差小于5%,多峰分布颗粒系的反演误差小于10%。整个算法运行时间小于2 s。该方法具有原理简单,计算速度快等优点,能够满足颗粒粒径在线测量的要求。     

降雨粒子的无线紫外光散射特性

紫外光与降雨粒子相互作用发生散射,散射光特性改变能够反映降雨粒子的相关物理特性（如粒子尺寸参数、浓度、形态）,因此研究粒子的物理参数对散射光特性的影响对有效提高光谱法定量探测降水的精度有很大意义。由于雨滴在非球形降水粒子中具有代表性,以群雨滴粒子为例,采用T矩阵理论,利用紫外光直视和非直视单次散射模型,分析了入射光波长、群雨滴粒子形态、降雨强度、粒径大小与散射光强之间的关系。并用蒙特卡洛方法仿真分析了非球形群雨滴粒子在不同降雨强度和粒径下散射角与散射光强之间的关系,以及降雨环境中的风切变对紫外光散射特性的影响。通过理论及仿真分析,得到了不同群雨滴粒子形态下的路径损耗,不同降雨强度、风切变率和粒径下的散射光强分布。仿真结果表明：在紫外光直视与非直视通信方式下,降雨环境中的通信质量比晴天条件下的通信质量差,即路径损耗增大。当粒径分布已知时,随着降雨强度的增大,衰减系数增大,路径损耗增加,且直视通信方式的路径损耗比非直视降低7 dB左右。随着降雨强度、风切变率和粒子粒径的增大,散射光强曲线整体呈下降趋势,其中,降雨强度的变化对散射光强分布影响程度最大。相同通信距离时,不同降雨强度下的紫外光散射光强分布均随着散射角的增大而减小,当散射角继续增大到90°时,有效散射体体积逐渐减小,接收到的光子能量减小,暴雨中的散射光强衰减程度最大。相同降雨强度下考虑风切变时,相比较无风时的路径损耗增大5 dB左右。除此之外,还研究了椭球形和切比雪夫形粒子对紫外光散射光强的影响,结果表明当粒子粒径分布相同时,椭球形粒子的散射光强衰减较广义切比雪夫形粒子大。根据散射粒子的散射光强分布以及路径损耗能够区分雨滴粒子是否由相同粒径及形态组成,为粒子测量提供理论基础。分析降水中群雨滴粒子的光散射特性,为提高光谱法评估降水衰减的数值模拟方面提供理论依据,为光学技术在探测识别降水现象等气象领域的广泛应用提供了设计参考。     

Determining particle size distribution and refractive index in a two-layer tissue phantom by linearly polarized light

We report a new method for measuring particle size distribution (PSD) and refractive index of the top layer in a two-layer tissue phantom simulated epithelium tissue by varying the azimuth angle of incident linearly polarized light. The polarization gating technique is used to decouple the single and multiple scattering components in the returned signal. The theoretical model based on Mie theory is presented and a nonlinear inversion method - floating genetic algorithm - is applied to inverting the azimuth dependence of component of polarization light backscattered. The experiment results demonstrate that the size distribution and refractive index of the scatters of the top layer can be determined by measuring and analyzing the differential signal of the parallel and perpendicular components from a two-layer tissue phantom. The method implies to detect precancerous changes in human epithelial tissue.     

A V-curve criterion for the parameter optimization of the Tikhonov regularization inversion algorithm for particle sizing

The regularization parameter plays an important role in applying the Tikhonov regularization method to recover the particle size distribution from dynamic light scattering experiments. The so-called V-curve, which is a plot of the product of the residual norm and the norm of the recovered distribution versus all valid regularization parameters, can be used to estimate the result of inversion. Numerical simulation demonstrated that the resultant V-curve can be applied to optimize the regularization parameter. The regularization parameter is optimized corresponding to the minimum value of the V-curve. Simulation and experimental results show that stable distributions can be retrieved using the Tikhonov regularization with optimum parameter for unimodal particle size distributions.