Collective motion and its connection to the energy landscape in 2D soft crystals†

Abstract

We examine the collective motion in computational models of a two-dimensional dusty plasma crystal and a charged colloidal suspension as they approach their respective melting transitions. To unambiguously identify rearrangement events in the crystal, we map the trajectory of configurations from an equilibrium molecular dynamics simulation to the corresponding sequence of configurations of local potential energy minima (“inherent structures”). This inherent structure (IS) trajectory eliminates the ambiguity that arises from localized vibrational motion. We find that the evolution of the IS trajectory in the crystal can be split into comparatively longer-lived ground states and shorter-lived discrete excited states. These discrete excited energy levels are a consequence of discrete numbers of defect clusters in the crystal. We find that the collective rearrangement occurs through different mechanisms: (i) small closed-loop motion in the ground states without the facilitation of defects, and (ii) much larger and complex open-ended particle motions in excited states that are facilitated by clusters of defects. In both cases, clusters of displacing particles can be separated into much smaller groups of replacing particles with a loop-like structure. In contrast to glass-forming liquids, the mass of the rearranging groups grows on heating towards the melting temperature rather than cooling. We find that crystal melting in these systems can be anticipated by the merging of the average time the crystal spends in the ground state with the average time in the excited states.