Non-Gaussian, transiently anomalous, and ergodic self-diffusion of flexible dumbbells in crowded two-dimensional environments: Coupled translational and rotational motions
【Abstract】 We employ Langevin-dynamics simulations to unveil non-Brownian and non-Gaussian center-of-mass self-diffusion of massive flexible dumbbell-shaped particles in crowded two-dimensional solutions. We study the intradumbbell dynamics of the relative motion of the two constituent elastically coupled disks. Our main focus is on effects of the crowding fraction ϕ and of the particle structure on the diffusion characteristics. We evaluate the time-averaged mean-squared displacement (TAMSD), the displacement probability-density function (PDF), and the displacement autocorrelation function (ACF) of the dimers. For the TAMSD at highly crowded conditions of dumbbells, e.g., we observe a transition from the short-time ballistic behavior, via an intermediate subdiffusive regime, to long-time Brownian-like spreading dynamics. The crowded system of dimers exhibits two distinct diffusion regimes distinguished by the scaling exponent of the TAMSD, the dependence of the diffusivity on ϕ, and the features of the displacement-ACF. We attribute these regimes to a crowding-induced transition from viscous to viscoelastic diffusion upon growing ϕ. We also analyze the relative motion in the dimers, finding that larger ϕ suppress their vibrations and yield strongly non-Gaussian PDFs of rotational displacements. For the diffusion coefficients D(ϕ) of translational and rotational motion of the dumbbells an exponential decay with ϕ for weak and a power-law variation D(ϕ)∝(ϕ−ϕ★)2.4 for strong crowding is found. A comparison of simulation results with theoretical predictions for D(ϕ) is discussed and some relevant experimental systems are overviewed.
【Author】 Kolja Klett, Andrey G. Cherstvy, Jaeoh Shin, Igor M. Sokolov, Ralf Metzler
【Journal】 Physical Review E(IF：2.4) Time：2021-12-05