Jamming, relaxation, and crystallization of a supercooled fluid in a three-dimensional lattice

Abstract

Off-equilibrium dynamics of a three-dimensional lattice model with nearest- and next-nearest-neighbors exclusions is studied. At equilibrium, the model undergoes a first-order fluid-solid transition. Nonequilibrium filling, through random sequential adsorption with diffusion, creates amorphous structures and terminates at a disordered state with random closest packing density that lies in the equilibrium solid regime. The approach toward random closest packing is characterized by two distinct power-law regimes, reflecting the formation of small densely packed grains in the long-time regime of the filling process. We then study the fixed-density relaxation of these amorphous structures toward the solid phase. The route to crystallization for the high-density, deeply supercooled regime is shown to deviate from the simple grain growth proposed by classical nucleation theory. Our measurements suggest that relaxation in this regime is driven mainly by coalescence of neighboring crystallized grains which exist in the initial amorphous state.