Reproducible capillary fluctuation analysis of solid-liquid interfaces for stiffness and anisotropy calculations

Abstract

The capillary fluctuation method (CFM) is widely used to compute solid–liquid interfacial properties from atomistic simulations, but its accuracy depends on choices in interface construction, wave-vector selection, sampling, and simulation geometry. Here, we develop a diagnostics-driven workflow for reproducible CFM calculations using pure Al as a representative system. Employing both ribbon models and thick two-dimensional references, we show that the apparent linearity of the fluctuation spectrum alone does not guarantee reliable estimates of stiffness or anisotropy. Instead, a reliable CFM analysis requires a fitting window consistent with both temporal sampling and continuum capillary-wave assumptions, systematic sensitivity tests of the interface identification procedure, explicit propagation of replica variability, and independent verification of model-thickness convergence. We further propose a practical thickness-selection rule based on coexistence-temperature consistency, which enables control of finite-size effects while retaining the substantial computational efficiency of ribbon geometries. By making the main sources of uncertainty explicit and diagnosable, the proposed workflow improves the reliability of the CFM as a quantitative tool and provides a foundation for its broader application to complex solid–liquid interfaces.