Pattern formation during nonequilibrium crystallization by classical-density-functional-based approach

TL;DR

This paper introduces a classical-density-functional-theory-based model to simulate nonequilibrium crystal growth patterns at the atom scale, capturing complex microstructures like dendrites and spherulites, and highlighting seed distribution's role in the CET.

Contribution

It presents a novel minimal model for nonequilibrium crystallization that incorporates elastic relaxation, enabling simulation of diverse patterns and growth stages at the atom scale.

Findings

Seed distribution influences the CET.

Two-stage growth process identified: diffusion-controlled and GFN-dominated.

Dislocation increments explain amorphous nucleation precursor.

Abstract

Solidification pattern during nonequilibrium crystallization is among the most important microstructures in the nature and technical realms. Phase field crystal (PFC) model could simulate the pattern formation during equilibrium crystallization at atom scale, but cannot grasp the nonequilibrium ones due to the absence of proper elastic-relaxation time scale. In this work, we propose a minimal classical-density-functional-theory-based model for crystal growth in supercooled liquid. Growth front nucleation (GFN) and various nonequilibrium patterns, including the faceting growth, spherulite, dendrite and the columnar-to-equiaxed transition (CET) among others, are grasped at atom scale. It is amazing that, except for undercooling and seed spacing, seed distribution is key factor that determines the CET. Overall, two-stage growth process, i.e., the diffusion-controlled growth and the GFN-dominated growth, are identified. But, compared with the second stage, the first stage becomes too short to be noticed under the high undercooling. The distinct feature for the second stage is the dramatic increments of dislocations, which explains the amorphous nucleation precursor in the supercooled liquid. Transition time between the two stages at different undercooling are investigated. Crystal growth of BCC structure further confirms our conclusions.