Computational scheme for ab-initio predictions of chemical compositions interfaces realized by deposition growth

TL;DR

This paper introduces a new computational method to predict the chemical compositions of interfaces during growth processes, accounting for nonequilibrium conditions to better match real-world observations.

Contribution

The paper presents a novel computational scheme that predicts interface compositions during growth by incorporating nonequilibrium thermodynamics and growth conditions.

Findings

Predicts that strongly adhering interfaces are favored under realistic deposition conditions.

Shows equilibrium thermodynamics may not accurately predict interface adhesion.

Demonstrates the scheme on TiC/alumina interface, aligning predictions with experimental observations.

Abstract

We present a novel computational scheme to predict chemical compositions at interfaces as they emerge in a growth process. The scheme uses the Gibbs free energy of reaction associated with the formation of interfaces with a specific composition as predictor for their prevalence. It explicitly accounts for the growth conditions by rate-equation modeling of the deposition environment. The Bell-Evans-Polanyi principle motivates our emphasis on an effective nonequilibrium thermodynamic description inspired by chemical reaction theory. We illustrate the scheme by characterizing the interface between TiC and alumina. Equilibrium thermodynamics favors a nonbinding interface, being in conflict with the wear-resistant nature of TiC/alumina multilayer coatings. Our novel scheme predicts that deposition of a strongly adhering interface is favored under realistic conditions.