Quantum simulations of defects near the (0001) surface of $\alpha$-Al$_2$O$_3$

TL;DR

This study employs quantum simulations and defect embedding theory to accurately analyze the electronic structure of surface vacancies in $ ext{Al}_2 ext{O}_3$, revealing insights into corrosion initiation mechanisms.

Contribution

It introduces a quantum computational approach combined with defect embedding theory to study surface defects in $ ext{Al}_2 ext{O}_3$, achieving high accuracy and demonstrating error mitigation on quantum hardware.

Findings

Quantum simulations match exact solutions within chemical accuracy.

Defect electronic states are strongly localized at the surface.

Hydration influences defect properties related to corrosion.

Abstract

Defects in materials are ubiquitous and one of their adverse effects in $\alpha$-Al$_2$O$_3$ is the initiation of corrosion. While this process starts near the surface, the defects involved and their electronic structure need to be elucidated with high accuracy. Since point defects are confined to a small spatial region, defect embedding theory allows the definition of an active space, comprising of the defect electronic states, that is coupled to the environment of the host material. The active space Hamiltonian is of small rank, enabling access to its electronic properties using a high-level or even exact quantum theory. In this paper we use these techniques and first-principles simulations to compute the structural and electronic properties of near-surface vacancies for the (0001) surface of $\alpha$-Al$_2$O$_3$, and investigate the influence of defects and hydration on the initiation and propagation of corrosion. We report the defect electronic structure for strongly localized ground and excited states of the surface O vacancy and compare results obtained using full configuration interaction and a variational quantum eigensolver on a quantum computer. Error mitigation techniques are explored and shown to reduce the error due to the hardware noise to the point where the quantum result agrees with the exact solution within chemical accuracy.