Universal Character of Atomic Motions at the Liquid-Solid Transition

Jerome Daligault

Published 2020-09-30Version 1

We show evidence from computer simulations of a universal feature in the atoms dynamics of simple liquids that heralds the freezing transition. We develop a physically transparent model to shed light on the physics responsible for the precursory effect. We find that the freezing point is concomitant with the crossover of two characteristic time scales, namely the average period of oscillation of the liquid configuration in a minimum of the potential energy surface, and the average time separating transits between potential energy minima as a result of the continuous dynamical rearrangement of particles. When entering the undercooled regime, the transit time becomes smaller than the period of oscillation, and the delicate balance between the disordering effects of thermal agitation and the ordering effects of interactions can be destabilized in favor of the periodic order. Finally, we demonstrate that the discovered precursory feature gives rise to a new efficient method for determining the liquid-solid coexistence line of real materials from atomistic simulations, which, unlike other methods commonly used in materials science, does not require knowing the crystalline structure of the solid phase.