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二维玻璃态胶体中的多尺度非均匀动力学

Multiscale heterogeneous dynamics in two-dimensional glassy colloids.

作者信息

Pastore Raffaele, Giavazzi Fabio, Greco Francesco, Cerbino Roberto

机构信息

Department of Chemical, Materials and Production Engineering, University of Naples Federico II, P.le Tecchio 80, Napoli 80125, Italy.

Department of Medical Biotechnology and Translational Medicine, University of Milan, Via F.lli Cervi 93, Segrate (MI) 20090, Italy.

出版信息

J Chem Phys. 2022 Apr 28;156(16):164906. doi: 10.1063/5.0087590.

Abstract

On approaching the glass transition, a dense colloid exhibits a dramatic slowdown with minute structural changes. Most microscopy experiments directly follow the motion of individual particles in real space, whereas scattering experiments typically probe the collective dynamics in reciprocal space at variable wavevector q. Multiscale studies of glassy dynamics are experimentally demanding and, thus, seldom performed. By using two-dimensional hard-sphere colloids at various area fractions ϕ, we show here that Differential Dynamic Microscopy (DDM) can be effectively used to measure the collective dynamics of a glassy colloid in a range of q within a single experiment. As ϕ is increased, the single decay of the intermediate scattering functions is progressively replaced by a more complex relaxation that we fit to a sum of two stretched-exponential decays. The slowest process, corresponding to the long-time particle escapes from caging, has a characteristic time τ = 1/(Dq) with diffusion coefficient D∼(ϕ-ϕ), and ϕ ≃ 0.81. The fast process exhibits, instead, a non-Brownian scaling of the characteristic time τ(q) and a relative amplitude a(q) that monotonically increases with q. Despite the non-Brownian nature of τ(q), we succeed in estimating the short-time diffusion coefficient D, whose ϕ-dependence is practically negligible compared to the one of D. Finally, we extend DDM to measure the q-dependent dynamical susceptibility χ(q, t), a powerful yet hard-to-access multiscale indicator of dynamical heterogeneities. Our results show that DDM is a convenient tool to study the dynamics of colloidal glasses over a broad range of time and length scales.

摘要

在接近玻璃化转变时,致密胶体表现出显著的减速,同时伴随着微小的结构变化。大多数显微镜实验直接跟踪单个粒子在实空间中的运动,而散射实验通常在可变波矢q下探测倒易空间中的集体动力学。玻璃态动力学的多尺度研究对实验要求很高,因此很少进行。通过使用不同面积分数ϕ的二维硬球胶体,我们在此表明,差分动态显微镜(DDM)可以有效地用于在单个实验中测量一系列q范围内玻璃态胶体的集体动力学。随着ϕ的增加,中间散射函数的单一衰减逐渐被更复杂的弛豫所取代,我们将其拟合为两个拉伸指数衰减的总和。最慢的过程对应于长时间粒子从笼中逸出,其特征时间τ = 1/(Dq),扩散系数D∼(ϕ - ϕ),且ϕ ≃ 0.81。相反,快速过程表现出特征时间τ(q)的非布朗标度以及相对振幅a(q)随q单调增加。尽管τ(q)具有非布朗性质,但我们成功估计了短时间扩散系数D,与D相比,其对ϕ的依赖性实际上可以忽略不计。最后,我们扩展DDM以测量q依赖的动态磁化率χ(q, t),它是动态不均匀性的一个强大但难以获取的多尺度指标。我们的结果表明,DDM是研究广泛时间和长度尺度范围内胶体玻璃动力学的便捷工具。

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