Role of phonon scattering and bonding in resolving lattice thermal conductivity ambiguities of β-Ga2O3

Understanding the lattice thermal conductivity (kappa(l)) of beta-Ga2O3 is very intriguing owing to its advantages in high-voltage and high-temperature applications. Despite several attempts, the underlying mechanism and causes of the notable discrepancies found in the kappa(l) values of beta-Ga2O3 along [100] and [001] directions calculated using first principles remained unresolved. We demonstrate that the understanding of the nature of chemical bonding is crucial to overcome the inconsistency in theoretically reported kappa(l) values. In low-symmetry structures such as beta-Ga2O3, the nature of the interactions is primarily long-range; therefore, a sufficiently large supercell inclusive of various bonding characteristics is required to capture relevant phonon wavelengths. Bonding nature-aware structure modeling allows precise estimation of acoustic and optical mode contributions towards kappa(l). Additionally, phonon mean free path analysis confirms that considering only third-order interaction terms is adequate to determine the kappa(l) of beta-Ga2O3. The calculated kappa(l) values are in excellent agreement with experimentally reported values in all three directions. Our results establish that the bonding nature and its influence on phonon scattering are essential to consider in calculating kappa(l) accurately.