Energetics of intrinsic point defects in ZrSiO$_4$

TL;DR

This study uses first principles calculations to analyze the formation energies, structures, and electronic effects of intrinsic point defects in zircon, relevant for nuclear waste immobilization and electronic device applications.

Contribution

It provides detailed atomic and electronic characterizations of various intrinsic defects in zircon, including their formation energies and effects on electronic properties.

Findings

Charged defects influence zircon's electronic levels.

Radiation-induced swelling affects defect concentrations.

Defects impact zircon's suitability in electronic devices.

Abstract

Using first principles calculations we have studied the formation energies, electron and hole affinities, and electronic levels of intrinsic point defects in zircon. The atomic structures of charged interstitials, vacancies, Frenkel pairs and anti-site defects are obtained. The limit of high concentration of point defects, relevant for the use of this material in nuclear waste immobilization, was studied with a variable lattice relaxation that can simulate the swelling induced by radiation damage. The limit of low concentration of defects is simulated with larger cells and fixed lattice parameters. Using known band offset values at the interface of zircon with silicon, we analyze the foreseeable effect of the defects on the electronic properties of zircon used as gate in metal-oxide-semiconductor devices.