Particle Size Distribution Retrieval from Elastic Light Scattering Measurements by a Modified Regularization Method

Retrieval of polymeric emulsions Particle Size Distribution (PSD) from Elastic Light Scattering (ELS) measurements requires the solution of an ill conditioned inverse problem. In this paper we compare the performance of classical regularization methods such as Truncated Singular Value Decomposition and Tikhonov's, to a regularization technique due to Pike that includes positivity constraints on the PSD. We also propose a new method that combines Tikhonov's approach with Pike's method. Simulated ELS measurements for two polymeric materials were generated under different experimental noise assumptions. Uncertainties on the polymer refractive index value were also considered. The PSD estimations obtained show that the implementation of the proposed more sophisticated algorithm is convenient for this very ill‐conditioned problem.     

Particle Size Distributions from Static Light Scattering with Regularized Non‐Negative Least Squares Constraints

Simulated data from static light scattering produced by several particle size distributions (PSD) of spherical particles in dilute solution is analyzed with a regularized non‐negative least squares method (r‐NNLS). Strong fluctuations in broad PSD's obtained from direct application of NNLS are supressed through an averaging procedure, as introduced long ago in the inversion problem in dynamic light scattering. A positive correlation between the best PSD obtained from several averaging schemes and the condition number of the respective data transfer matrices was obtained. The performance of the method is found to be similar to that of constrained regularization (CONTIN), which uses also NNLS as a starting solution, but incorporates another regularizing strategy.     

Determination of Soot Particle Size in a Premixed Flame: a Static and Dynamic Light Scattering Study

In this contribution we report upon our static and dynamic light scattering experiments to characterize soot particles in flames. We studied sooting laminar premixed flame with acetylene as fuel mixed with air as oxidizer. The air equivalence ratio of the combustion was larger than one. We used a Kaskan type burner with circular geometry and a stabilizing flow of nitrogen around the flame. We focused on the determination of the size of the soot particles in the center of the flame as a function of height above burner. In addition we investigated the influence of the mixing ratio of the gases on the size of the particles. Our results show that static light scattering is better suited than dynamic light scattering for a fast and reliable characterization of soot particles in flames. The latter needs detailed a priori information about the flame to allow the unique determination of sizes from the diffusion measurements. The soot particles grow monotonously with height above burner and with decreasing air equivalence ratio. The aggregates have a fractal dimension lower than two.     

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.     

光复散射对消光法粒径测量的影响:复散射模型与数值模拟

复散射效应在光散射颗粒测量中不仅重要．且尚未得到很好解决。采用蒙特卡罗方法,对不同的光波长,颗粒浓度以及收接器条件下的光复散射进行了数值模拟．数值算法程序经与四通量模型进行对比验证,数值结果与单散射条件的郎伯-比尔模型进行比较．进而讨论了复散射效应对消光法颗粒粒径测量影响。表明复散射对消光法颗粒测量的影响不仅取决于颗粒系自身的浓度．而且接收器的几何尺寸和接收位置起着非常重要的作用,减小颗粒介质层厚度和减小光接收器接收面积．增大接收距离以及减小接收角都能减小复散射效应对消光法粒径测量的影响。     

Sizing Polydisperse Dispersions by Focused Beam Reflectance and Small Angle Static Light Scattering

In this work, two different methods for particle characterization, namely focused beam reflectance and small angle static light scattering, are quantitatively compared. The results are presented in the form of moment ratios of the particle size distribution, i.e., the number weighted diameter, D_1/0, and the volume weighted diameter, D_4/3, for a broad range of particle size distributions ranging from 20 to 400 μm. Various aqueous dispersions including narrow, broad, and bimodal particle size distributions of spherical shaped ceramic beads were used in the comparison. It was found that the moment ratios obtained by focused beam reflectance measurements and small angle static light scattering correlate well, in the case of spherical particles. Furthermore, it was found that the D_1/0 values obtained by focused beam reflectance measurements are more sensitive to the presence of a small fraction of fine particles in a bimodal distribution than those obtained by small angle static light scattering.     

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.     

多角度动态光散射加权贝叶斯反演算法

研究加权贝叶斯算法在多角度动态光散射法测量单峰分布颗粒体系的颗粒粒度分布中的应用.采用颗粒粒度信息分布为底数、调节参数为指数的权重系数给各个角度下的光强自相关函数曲线加入不同的权重系数,再利用传统的贝叶斯算法反演.模拟与实验结果表明,加权后的贝叶斯算法能获得分布误差更小的反演结果,有效地抑制了数据噪声的影响,提高颗粒粒度分布反演的准确性.     

可见-红外波段光全散射法颗粒粒径测量范围的研究

在光全散射法颗粒粒径测量中,采用独立模式算法在可见-红外波段对粒径测量范围进行了深入的研究。通过对多种R-R分布函数反演结果进行分析,比较,以确定光全散射法颗粒粒径测量范围。同时在消光系数计算中,采用修正的消光系数代替原始的消光系数,以便得到更准确的粒径测量范围。仿真计算结果表明,在可见-红外光谱区,相对折射率m=1.235时的粒径测量范围为0.05～18 μm。在此区域内测量粒径分布,反演结果与真值基本吻合。随着颗粒相对折射率、波长范围的变化,粒径测量范围也随之发生改变。采用限制最小二乘算法能够最大限度地克服随机噪声对测量结果的影响,使测量的精度和可靠性明显提高。对测量的消光值加入±1%随机噪声时,颗粒粒径分布的反演均能得到满意的结果。     

聚芴共轭聚合物在稀薄溶液中形态变化的静态光散射研究

PF8聚芴共轭高分子材料是应用于制作蓝色光激发光器件的一种有潜力功能材料, 故本文利用静态光散射技术研究了PF8聚芴共轭高分子在稀薄甲苯溶液中的形态结构变化特点。研究结果显示, PF8共轭高分子在甲苯稀薄溶液中单一分子链的持续长度与Kuhn链结长度均明显受到温度的影响。这表明在较高温度下高分子与溶剂间的相互作用力较大, 导致其呈现较伸展的虫状形态结构; 而在较低温度下高分子与溶剂间相互作用力较小, 导致其呈现收缩的结构形态。因此在较高温度状态下PF8共轭高分子应该具有比较刚硬的特征。     

利用低相干光纤动态光散射法测量浓悬浮液中多分散颗粒粒径分布

本文针对高浓度散射介质,用低相干光纤动态光散射技术测量浓悬浮液中多分散颗粒系的粒径及其粒径分布。利用迭代CONTIN算法对实验数据进行反演运算,得到多分散颗粒系的粒径分布结果。结果表明,浓悬浮液中多分散颗粒系的峰值粒径测量值与给定的两种标准粒径值相吻合,其误差在4%之内,粒径分布曲线中各散射颗粒所反映的散射体光强分布与根据Mie散射计算得到的理论值相吻合。实验结果证明低相干光纤动态光散射实验系统能准确测量浓悬浮液中多分散颗粒粒径及粒径分布。     

动态光散射技术的角度依赖性

与单角度动态光散射技术相比,多角度动态光散射(MDLS)颗粒测量技术能够提高颗粒粒度分布的测量准确性。但在MDLS技术中,测量角度的选择常常与被测颗粒体系的分布有关。对100nm、500nm的单峰模拟分布和300nm与600nm混合的双峰模拟分布的颗粒体系,分别在1、3、6、9个散射角条件下进行了测量。颗粒粒度反演结果表明,随着散射角个数的增大,颗粒粒度分布更趋于真实的颗粒粒度分布。对数量比为5:1的100nm与503nm双峰分布的聚苯乙烯颗粒,分别在1、3、5、10个散射角条件下进行了测量,实测结果表明采用单角度测量只能得到单峰分布,3个及更多散射角可得到双峰分布,并且双峰的数量比随散射角数量的增加逐渐趋近真实的数量比。因此,MDLS颗粒测量技术能够改善颗粒粒度分布的测量结果,但这种改善程度会随散射角的增多逐渐降低。由于散射角个数的增多会增加散射角的校准噪声和光强相关函数的测量噪声,因而会导致在有些情况下颗粒粒度分布的测量结果反而变差。     

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.     

分段自相关动态光散射法测量亚微米粒度

介绍了动态光散射法测量微粒尺度的原理，通过对相关函数相对的分析，提出了分段自相关的方法，该方法解决了高速，大数据量采集的困难，又不显著影响相关函数的精度，给出了实验装置及实验结果，测量结果与标准样品的标称值相符。     

颗粒溶液颗粒尺寸及浓度的差分偏振弹性散射光谱在线分析方法

偏振弹性散射光谱技术的基本原理为在偏振光入射条件下,根据出射光的偏振特性不同可以筛选出浅表层组织的单次散射光信息和深层组织的漫散射光信息。该研究的创新点在于将这种方法应用于颗粒溶液检测,目的是在颗粒溶液原始状态下实现对颗粒尺寸及浓度的同时检测。设计了一个共轴笼式光学系统,测量了聚苯乙烯微球颗粒溶液某一角度的背向散射信号,通过控制入射端和收集端偏振片的偏振方向获得了颗粒溶液的偏振平行光谱与偏振垂直光谱,两者之差即偏振差分光谱对应颗粒的单次散射信息,将该单次散射信息与Mie散射数据库进行比对获得颗粒的尺寸,然后在颗粒尺寸作为已知的条件下进一步分析偏振垂直光谱,将该垂直光谱对应的颗粒溶液的漫散射信息代入光漫散射下的近似表达式拟合得到颗粒的浓度信息。将实验结果与样品提供值进行了比对,并进一步分析了在获取颗粒数浓度时,颗粒直径的方差分布对结果的影响,最终验证了该实验方法的可行性。该方法的潜在应用包括对标准颗粒制造厂商的产品在线检测以及对牛奶制品中脂肪和蛋白质的浓度检测研究。     

微粗糙面上方球形粒子的光散射及其散射截面的计算

基于互易定理研究了光波入射时微粗糙面与其上方球形粒子复合模型的光散射。根据粗糙表面电流积分方程并利用表面微扰展开，得到了微粗糙面表面极化电流的迭代解，给出了耦合电场的计算方法。结合散射耦合场散射矩阵和已有的微粗糙面及球形粒子的散射矩阵，给出了复合模型散射截面的计算公式，数值计算了复合模型的后向散射截面并进行了详细讨论。     

一种扩大动态光散射颗粒法可测溶液浓度的改进方法

针对传统动态光散射颗粒测量法测量溶液浓度范围较小的问题，通过模型和实验研究了传统DLS系统双孔结构中测量区大小对测量结果的影响，发现可通过改变测量区大小控制散射体体积，从而扩大测量溶液浓度的范围。并基于传统DLS系统双孔结构光路，通过使用可调狭缝，并增加透镜，扩大了DLS测量溶液浓度范围，实验结果表明了该方法的有效性。     

后向动态光散射测量中样品池的影响及校正

针对后向动态光散射高浓度颗粒测量中样品池产生的影响,本文对负球差进行了分析,提出了采用ZEMAX确定聚焦透镜的光学参数校正球差的方案,对由于样品池表面反射引起的二次散射进行计算,提出了削弱二次散射的方法。     

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。