First-Principles Phase-Field Modeling

Abstract: Phase-field methods offer a versatile computational framework for simulating large-scale microstructure evolution. However, the applicability and predictability of phase-field models are inherently limited by their ad hoc nature, and there is currently no bottom-up theory available that enables truly first-principles predictive modeling of large-scale non-equilibrium processes. Here, we present a bottom-up framework that provides a route to the construction of mesoscopic phase-field models entirely based on atomistic information. By introducing a molecular coarse-grained system as an intermediate step, we demonstrate the approach on the example of ice nucleation dynamics, with a spatiotemporal scale-up of nearly $10^8$ times compared to the microscopic model. Our framework offers a unique approach for incorporating atomistic details into mesoscopic models, systematically bridging the gap between microscopic particle-based simulations and field-theoretic models.