Extending SLUSCHI for Automated Diffusion Calculations

TL;DR

This paper extends the SLUSCHI computational package to automate diffusion calculations from first-principles molecular dynamics, enabling efficient evaluation of transport properties like diffusivity and viscosity in various materials.

Contribution

The authors adapt SLUSCHI for diffusion analysis, integrating post-processing tools and validation across multiple material systems, broadening its application scope beyond melting point estimation.

Findings

Validated diffusion calculations in Al-Cu alloys and oxides.

Automated diagnostic plots for diffusive regimes.

Linking viscosity and diffusivity via Stokes-Einstein relation.

Abstract

We present an extension of the SLUSCHI package (Solid and Liquid in Ultra Small Coexistence with Hovering Interfaces) to enable automated diffusion calculations from first-principles molecular dynamics. While the original SLUSCHI workflow was designed for melting temperature estimation via solid-liquid coexistence, we adapt its input and output handling to isolate the volume search stage and generate one production trajectory suitable for diffusion analysis. Post-processing tools parse VASP outputs, compute mean-square displacements (MSD), and extract tracer diffusivities using the Einstein relation with robust error estimates through block averaging. Diagnostic plots, including MSD curves, running slopes, and velocity autocorrelations, are produced automatically to help identify diffusive regimes. The method has been validated through representative case studies: self- and inter-diffusion in Al-Cu liquid alloys, sublattice melting in Li_7La_3Zr_2O_12 and Er_2O_3, interstitial oxygen transport in bcc and fcc Fe, and oxygen diffusivity in Fe-O liquids with variable Si and Al contents. Viscosity and diffusivity are linked through the Stokes-Einstein relation, with composition dependence assessed via simple linear mixing. This capability broadens SLUSCHI from melting-point predictions to transport property evaluation, enabling high-throughput, fully first-principles datasets of diffusion coefficients and viscosities across metals and oxides.