Dynamic Heterogeneity of Gelatin Study by Probe Particle Tracking Microrheology

Wei Hong; Guo-zhi Xu; Wei-xiang Sun; Zhen Tong

doi:10.11777/j.issn1000-3304.2017.17071

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Dynamic Heterogeneity of Gelatin Study by Probe Particle Tracking Microrheology

Research Article | 更新时间：2021-01-27

- Dynamic Heterogeneity of Gelatin Study by Probe Particle Tracking Microrheology
- Acta Polymerica Sinica Issue 9, Pages: 1488-1496(2017)
- 作者机构：
  
  华南理工大学材料科学研究所广州 510640
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2017.17071
  CLC：
- Published：20 September 2017，
  
  Received：1 April 2017，
  
  Revised：11 May 2017，
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Wei Hong, Guo-zhi Xu, Wei-xiang Sun, Zhen Tong. Dynamic Heterogeneity of Gelatin Study by Probe Particle Tracking Microrheology. [J]. Acta Polymerica Sinica (9):1488-1496(2017)
DOI：

Wei Hong, Guo-zhi Xu, Wei-xiang Sun, Zhen Tong. Dynamic Heterogeneity of Gelatin Study by Probe Particle Tracking Microrheology. [J]. Acta Polymerica Sinica (9):1488-1496(2017) DOI： 10.11777/j.issn1000-3304.2017.17071.

摘要

利用探针粒子示踪微流变法对明胶溶液等温凝胶化过程的动态不均匀性进行了观测.通过向体系中引入探针粒子，利用广义的Stokes-Einstein关系由探针粒子的位移建立了体系结构的空间分布.进而利用van Hove函数和非高斯因子描述了凝胶化转变前后动态不均匀性的变化，结果表明在凝胶化后体系动态在空间和时间尺度上都是不均匀的，与凝胶化前相比，凝胶化后的快动态有更高的贡献.为了进一步探究这种动态不均匀性在空间和时间上相关的变化，本工作在粒子示踪技术的基础上，实现了四点相关函数和极化率的测量.实验结果表明，凝胶化前体系的快松弛可以原位独立完成，而慢松弛则需要周围的结构单元协同完成；凝胶化后体系的快松弛和慢松弛均需要协同完成.

Abstract

Vitrification and gelation are two main paths for matters to transform from liquid to solid in nature. During these transition processes

the dynamics of the systems becomes slower

and there appears a relatively fast and slow dynamics

which finally results in the heterogeneous distribution of dynamics in the space and time. This dynamic heterogeneity in the space and time has been reported to diverge following the power law when approaching to the glass transition. However

it is still unclear for the dynamic heterogeneity evolution when approaching to the gelation. In this work

the dynamic heterogeneity in a gelatin solution during isothermal gelation at 22℃ was monitored by the probe particle tracking microrheology. The gel point was determined as the waiting time

=8 min through the ensemble averaged dynamic modulus

which was obtained from the mean square displacement of the particles using the generalized Stokes-Einstein relation (GSER). The spatial distribution of the loss angle tan

was established from the particle trajectories to represent heterogeneous viscoelasticity in the gelatin during the gelation. Then

the dynamic heterogeneity change during the gelation was quantitatively evaluated by the van Hove function and the non-Gaussian parameter

. The dynamics was found to be heterogeneous after gelation in both respects of space and time

and the fast dynamics contributed more after gelation when compared with that before gelation. To further investigate the spatial and time correlation for this dynamic heterogeneity

the 4-point correlation function and 4-point susceptibility were measured on the base of particle tracking statistics. The results indicated that

before gelation of the gelatin solution

the fast relaxation proceeded independently

while the slow relaxation occurred with a large spatial correlation containing more surrounding units. On the other hand

after gelation both the fast and slow relaxations processed correlatively and cooperatively with more surrounding units. This was consistent with the result from molecular dynamics simulation for the chemically crosslinked polymer gels.

关键词

凝胶化动态不均匀性van Hove函数四点极化率

Keywords

GelationDynamic heterogeneityvan Hove function4-Point susceptibility

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