• Accepted Paper

Structure and thermodynamic stability of β-Ga2O3 surfaces

Konstantin Lion and Claudia Draxl

Phys. Rev. B - Accepted 22 September, 2026

DOI: https://doi.org/10.1103/ltwn-y8xf

Abstract

We present a comprehensive first-principles investigation of all symmetrically inequivalent low-index surfaces of β-Ga2O3, examining their structural properties and thermodynamic stability across experimentally relevant growth conditions. Using density-functional theory with both the semi-local functional PBEsol and a modified PBE0 hybrid functional with 26% exact exchange, denoted PBE0(0.26), we calculate surface free energies for the (010), (100), (001), (${2}01),(110),(111),and(11{1})orientations,includingtheeffectsofharmonicvibrationalcontributionsandvaryingoxygenchemicalpotentials.Wedemonstratethattheenergeticorderingremainsconsistentacrosscomputationalapproachesandthatthevibrationalcontributionsremainbelow0.2J/m^2$ up to temperatures of 1000 K. A coordination-based model that correlates surface stability with the density of under-coordinated atoms reveals that under-coordinated oxygen atoms and tetrahedral Ga sites substantially destabilize surfaces, while exposed under-coordinated octahedral Ga atoms serve as indicators of surface stability. Our thermodynamic analysis shows that stoichiometric terminations dominate over nearly the entire range of chemical potentials relevant for β-Ga2O3 stability, while non-stoichiometric terminations emerge only under extreme reducing or oxidizing conditions. Notably, we predict the formation of stable Ga-rich terminations resembling Ga adlayers for the (100) and (${2}$01) surfaces under highly reducing conditions.

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