Microscopic Origin of Temperature-Dependent Anisotropic Heat Transport in Ultrawide-Bandgap Rutile GeO2

TL;DR

This study combines experimental measurements and first-principles calculations to elucidate the microscopic mechanisms behind the temperature-dependent anisotropic heat transport in rutile GeO2, highlighting its potential for thermally robust electronics.

Contribution

It provides the first detailed microscopic analysis of anisotropic heat transport in rutile GeO2, linking phonon properties to temperature-dependent thermal conductivity.

Findings

Thermal conductivity at 295 K: 47.5 W/mK along [001], 32.5 W/mK along [110]

Thermal conductivity follows approximately T^(-1.4) dependence, indicating complex scattering

Anisotropy arises from phonon group velocities and direction-dependent phonon lifetimes

Abstract

Ultrawide-bandgap rutile GeO2 is emerging as a promising semiconductor for power electronics, where efficient heat dissipation is essential to suppress self-heating and ensure device reliability. However, the temperature dependence and microscopic origin of its anisotropic heat transport have remained experimentally unresolved. Here, temperature-dependent time-domain thermoreflectance measurements combined with first-principles phonon transport calculations are used to quantify the thermal conductivity of single-crystal rutile GeO2 from 80 to 350 K along [001] and [110]. At 295 K, the thermal conductivity reaches 47.5 W m^-1 K^-1 along [001] and 32.5 W m^-1 K^-1 along [110], corresponding to an anisotropy ratio of 1.46, in good agreement with theory. Rather than following a simple T^(-1) law, the thermal conductivity exhibits an approximate T^(-1.4) dependence, indicating additional scattering beyond purely three-phonon-limited transport. Mode-resolved analysis reveals that the room-temperature anisotropy originates from the combined effect of larger phonon group velocities along [001] and direction-dependent phonon lifetimes. Upon cooling, depopulation of high-frequency phonons progressively suppresses their contribution to heat transport and reduces the anisotropy. The temperature-dependent thermal boundary conductance of Al/rutile GeO2 interfaces is further resolved, and the scaled conductance indicates predominantly elastic interfacial transport. These findings establish the microscopic basis of bulk and interfacial heat transport in rutile GeO2 and position this material as a promising thermally robust platform for ultrawide-bandgap electronics.