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用于气凝胶及类似软材料弹性和非弹性散射数据分析的时变层次模型。

A Time-Dependent Hierarchical Model for Elastic and Inelastic Scattering Data Analysis of Aerogels and Similar Soft Materials.

作者信息

Gommes Cedric J

机构信息

Department of Chemical Engineering, University of Liège, B6C, Allée du Six Août 3, B-4000 Liège, Belgium.

出版信息

Gels. 2022 Apr 12;8(4):236. doi: 10.3390/gels8040236.

Abstract

Soft nanomaterials like aerogels are subject to thermal fluctuations, so that their structure randomly fluctuates with time. Neutron elastic and inelastic scattering experiments provide unique structural and dynamic information on such systems with nanometer and nanosecond resolution. The data, however, come in the form of space- and time-correlation functions, and models are required to convert them into time-dependent structures. We present here a general time-dependent stochastic model of hierarchical structures, with scale-invariant fractals as a particular case, which enables one to jointly analyze elastic and inelastic scattering data. In order to describe thermal fluctuations, the model builds on time-dependent generalisations of the Boolean model of penetrable spheres, whereby each sphere is allowed to move either ballistically or diffusively. Analytical expressions are obtained for the correlation functions, which can be used for data fitting. The model is then used to jointly analyze previously published small-angle neutron scattering (SANS) and neutron spin-echo (NSE) data measured on silica aerogels. In addition to structural differences, the approach provides insight into the different scale-dependent mobility of the aggregates that make up the aerogels, in relation with their different connectivities.

摘要

像气凝胶这样的软纳米材料会受到热涨落的影响,以至于它们的结构会随时间随机波动。中子弹性和非弹性散射实验能以纳米和纳秒分辨率提供关于此类系统独特的结构和动态信息。然而,数据是以空间和时间关联函数的形式呈现的,需要模型将它们转换为随时间变化的结构。我们在此提出一种分层结构的通用随时间变化的随机模型,尺度不变分形作为一个特殊情况,它能够联合分析弹性和非弹性散射数据。为了描述热涨落,该模型基于可穿透球体布尔模型的随时间变化的推广,其中每个球体可以进行弹道运动或扩散运动。得到了关联函数的解析表达式,可用于数据拟合。然后该模型被用于联合分析先前发表的关于二氧化硅气凝胶的小角中子散射(SANS)和中子自旋回波(NSE)数据。除了结构差异外,该方法还能深入了解构成气凝胶的聚集体在不同尺度下与它们不同连通性相关的不同迁移率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0c2d/9025713/9fe740447b2c/gels-08-00236-g001.jpg

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