Terminal polydispersity in the crystallization of polydisperse Lennard-Jones liquid

TL;DR

This study uses computer simulations to identify a terminal polydispersity in Lennard-Jones liquids where the volume change on freezing vanishes, revealing insights into the nature of crystallization and amorphous phases.

Contribution

It demonstrates the existence of a terminal polydispersity at 0.11 where the volume change on freezing approaches zero, and characterizes the energetic transition between crystalline and amorphous phases.

Findings

Fractional volume change decreases with polydispersity.

Terminal polydispersity is approximately 0.11.

Inherent structure energy increases quadratically with polydispersity.

Abstract

We find through computer simulations that the fractional volume change on freezing of polydisperse Lennard-Jones liquid decreases with increasing polydispersity and approaches zero near a terminal polydispersity of 0.11, independent of temperature. The transition however remains first order at terminal polydispersity. Average inherent structure (IS) energy of the crystalline phase increases nearly quadratically with polydispersity indices ({\delta}) and marked by a crossover to nearly constant IS energy in the amorphous phase.