Fast crystal growth in deeply undercooled ZrTi melts

Abstract

We investigate the growth of crystals in Zr50Ti50 melts by classical molecular-dynamics simulations with an embedded atom method and a Stillinger–Weber potential model. Both models display fast solidification rates that can be captured by the transition state theory or the Ginzburg–Landau theory at small undercoolings. Fast crystal-growth rates are found to be affected by the pre-existing ordering in liquids, such as the body-centered cubic-like and icosahedral-like structures. The interface-induced ordering unveiled by the crystal-freezing method can explain the rate difference between these two models. However, these orderings fail to rationalize the temperature evolution of the growth rate at deep undercoolings. We correlate the growth kinetics with the detailed dynamical processes in liquids, finding the decoupling of hierarchic relaxation processes when collective motion emerges in supercooled liquids. We find that the growth kinetics is nondiffusive, but with a lower activation barrier corresponding to the structural relaxation or the cage-relative motion in ZrTi melts. These results explore a new relaxation mechanism for the fast growth rate in deeply undercooled liquids.