Determination of melting temperature of hexagonal ice using Lee-Yang phase transition theory

TL;DR

This paper applies Lee-Yang phase transition theory to accurately determine the melting temperature of hexagonal ice using enhanced sampling techniques, demonstrating its practical applicability in realistic molecular systems.

Contribution

The authors extend a previous scheme to calculate Lee-Yang zeros, enabling efficient and accurate melting temperature estimation for ice Ih without prior phase transition knowledge.

Findings

Melting temperature of 248.15 K for TIP4P/2005 ice model.

Enhanced sampling is crucial for accurate Lee-Yang zeros.

Method achieves results comparable to coexistence simulations with lower computational cost.

Abstract

Lee-Yang phase transition theory is a milestone in statistical physics. Its applications in realistic systems, however, had been substantially hindered by availability of practical schemes to calculate the Lee-Yang zeros. In this manuscript, we extend the scheme we have designed earlier [Phys. Rev. E 109, 024118 (2024)] and report simulation results for the melting temperature (T) of ice Ih under ambient pressure. The enhanced sampling technique is shown to be crucial for accessing Lee-Yang zeros accurately. The real and imaginary parts of our Lee-Yang edges demonstrate linear scaling of sizes, which can lead to a melting T of 248.15 K for the TIP4P/2005 potential in the thermodynamic limit. This result is in close quantitative agreement with previous coexistence simulations, achieved with cheaper computational costs and without prior knowledge of the phase transition. With these, we demonstrate the applicability of Lee-Yang phase transition theory in realistic molecular systems, and provide a feasible scheme for high-throughput calculations in determining the phase transition temperature.