Finite-temperature surface elasticity of crystalline solids

TL;DR

This paper introduces a Gaussian phase packets method to compute surface energies and elastic properties of crystalline solids at finite temperatures, enabling more accurate nanoscale material modeling.

Contribution

The paper presents a novel GPP-based technique for finite-temperature surface property calculations, improving over traditional zero-temperature or thermodynamic integration methods.

Findings

Surface energies decrease with temperature for studied metals.

Elastic constants vary non-uniformly with temperature across materials.

Validation confirms the accuracy of the GPP method against molecular dynamics.

Abstract

Surface energies and surface elasticity largely affect the mechanical response of nanostructures as well as the physical phenomenon associated with surfaces such as evaporation and adsorption. Studying surface energies at finite temperatures is therefore of immense interest for nanoscale applications. However, calculating surface energies and derived quantities from atomistic ensembles is usually limited to zero temperature or involve cumbersome thermodynamic integration techniques at finite temperature. Here, we illustrate a technique to identify the energy and elastic properties of surfaces of solids at non-zero temperature based on a Gaussian phase packets (GPP) approach (which in the isothermal limit coincides with a maximum-entropy formulation). Using this setup, we investigate the effect of temperature on the surface properties of different crystal faces for six pure metals -- copper, nickel, alumimum, iron, tungsten and vanadium -- thus covering both FCC and BCC lattice structures. While the obtained surface energies and stresses usually show a decreasing trend with increasing temperature, the elastic constants do not show such a consistent trend across the different materials and are quite sensitive to temperature changes. Validation is performed by comparing the obtained surface energy densities of selected BCC and FCC materials to those calculated via molecular dynamics.