Cooperative activated dynamics in dense mixtures of hard and sticky spheres

作     者：Douglas C. Viehman Kenneth S. Schweizer 

作者机构：[]Department of Chemical and Biomolecular Engineering and Department of Materials Science Frederick Seitz Materials Research Laboratory University of Illinois 1304 West Green Street Urbana Illinois 61801 USA 

出 版 物：《Physical Review E》 (物理学评论E辑：统计、非线性和软体物理学)

年 卷 期：2008年第78卷第5期

页      面：051404-051404页

核心收录：

学科分类：07[理学] 070203[理学-原子与分子物理] 0702[理学-物理学] 

基　　金：National Science Foundation [DMR-0642573] 

主　　题：Mixtures 

摘      要：The coupled activated dynamics in dense mixtures of repulsive and sticky hard spheres is studied using stochastic nonlinear Langevin equation theory. The effective free energy surface, barriers, saddle point trajectories, and mean first passage times depend in a rich manner on mixture composition, (high) total volume fraction, and attractive interaction strength. In general, there are three types of saddle point trajectories or relaxation pathways: a pure sticky or pure repulsive particle displacement keeping the other species localized, and a cooperative motion involving repulsive and attractive particle displacements. The barrier for activated hopping usually increases with the ratio of sticky to repulsive particle displacement. However, at intermediate values of the displacement ratio it can attain a broad plateau value, and can even exhibit a local maximum, and hence nonmonotonic behavior, at high sticky particle mixture compositions if the attraction strength is modest. The mean first passage, or hopping, times are computed using multidimensional Kramers theory. In most cases the hopping time trends reflect the behavior of the barrier height, especially as the sticky particle attraction strengths become large. However, there are dramatic exceptions associated with cooperative repulsive and attractive particle trajectories where the barriers are high but a greatly enhanced number of such trajectories exist near the saddle point.