Collective Motion of Repulsive Brownian Particles in Single-File Diffusion with and without Overtaking

摘要

Subdiffusion is commonly observed in liquids with high density or in restricted geometries, as the particles are constantly pushed back by their neighbors. Since this “cage effect” emerges from many-body dynamics involving spatiotemporally correlated motions, the slow diffusion should be understood not simply as a one-body problem but as a part of collective dynamics, described in terms of space–time correlations. Such collective dynamics are illustrated here by calculations of the two-particle displacement correlation in a system of repulsive Brownian particles confined in a (quasi-)one-dimensional channel, whose subdiffusive behavior is known as the single-file diffusion (SFD). The analytical calculation is formulated in terms of the Lagrangian correlation of density fluctuations. In addition, numerical solutions to the Langevin equation with large but finite interaction potential are studied to clarify the effect of overtaking. In the limiting case of the ideal SFD without overtaking, correlated motion with a diffusively growing length scale is observed. By allowing the particles to overtake each other, the short-range correlation is destroyed, but the long-range weak correlation remains almost intact. These results describe nested space–time structure of cages, whereby smaller cages are enclosed in larger cages with longer lifetimes.