Chaki Subhasish, Schweizer Kenneth S
Department of Materials Science, University of Illinois, Urbana, Illinois 61801 USA.
Materials Research Laboratory, University of Illinois, Urbana, Illinois 61801 USA.
J Chem Phys. 2024 Jan 28;160(4). doi: 10.1063/5.0177412.
Based on integrating microscopic statistical mechanical theories for structure and ideal kinetic arrest at the naive mode coupling level, we study dynamic localization, the linear elastic shear modulus, applied stress induced modulus softening, and the absolute yielding of simple biphasic binary mixtures composed of equal diameter hard and attractive spheres. The kinetic arrest map is a rich function of total packing fraction, strength of attraction, and mixture composition. The gel to attractive ideal glass transition, the degree of glass melting re-entrancy, and the crossover boundary separating repulsive glasses from attractive glasses vary with the mixture composition. Exponential and/or apparent (high) power law dependences of the elastic shear modulus on the total packing fraction are predicted with effective exponents or exponential prefactors that are sensitive to mixture composition and location in the kinetic arrest map. An analysis of the effective mean square force on a tagged particle that induces dynamic localization reveals a compensation effect between structural correlations and degree of particle localization, resulting in the emergence of a weaker dependence of the shear modulus on mixture composition at very high attraction strengths. Based on a microrheologically inspired formulation of how external stress weakens particle localization and the shear modulus, we analyze mechanical-induced modulus softening and absolute yielding, defined as a discontinuous solid-to-fluid stress-induced transition that can occur in either one or two steps. Estimates of the corresponding yield strains predict that the binary mixture becomes more brittle with increasing sticky particle composition and/or attraction strength.
基于在朴素模式耦合水平上整合结构的微观统计力学理论和理想动力学阻滞,我们研究了动态局域化、线性弹性剪切模量、外加应力诱导的模量软化以及由等直径硬球和吸引球组成的简单双相二元混合物的绝对屈服。动力学阻滞图是总堆积分数、吸引力强度和混合物组成的丰富函数。凝胶到吸引性理想玻璃转变、玻璃熔化再入程度以及将排斥性玻璃与吸引性玻璃分开的交叉边界随混合物组成而变化。预测弹性剪切模量对总堆积分数的指数和/或表观(高)幂律依赖性,其有效指数或指数前置因子对混合物组成和动力学阻滞图中的位置敏感。对诱导动态局域化的标记粒子上的有效均方力的分析揭示了结构相关性与粒子局域化程度之间的补偿效应,导致在非常高的吸引力强度下剪切模量对混合物组成的依赖性减弱。基于微观流变学启发的关于外部应力如何削弱粒子局域化和剪切模量的公式,我们分析了机械诱导的模量软化和绝对屈服,绝对屈服定义为可能以一步或两步发生的不连续固体到流体应力诱导转变。相应屈服应变的估计预测,随着粘性粒子组成和/或吸引力强度的增加,二元混合物变得更脆。