Anomalous thermal transport in isotope-enriched germanium carbide

Abstract

Advances in modern electronics demand the dissipation of heat fluxes approaching 1000 W cm${}^{-2}$, which drives an urgent need for materials with thermal conductivity ($\kappa$) exceeding 1000 W m${}^{-1}$ K${}^{-1}$. Here, by solving the Boltzmann transport equation considering both three- and four-phonon interactions, we observe that isotopically pure cubic germanium carbide (GeC) exhibits a remarkable $\kappa$ of 1018 W m${}^{-1}$ K${}^{-1}$ at room temperature, which is further corroborated by state-of-the-art machine-learning molecular dynamics simulations. Two unique mechanisms underlie this anomalously high $\kappa$: a remarkably strong isotopic enhancement effect (289%) and a surprisingly modest suppression due to four-phonon scattering (22%)-despite the presence of a wide acoustic-optical phonon gap. Moreover, we find that GeC defies the conventional Leibfried-Schlomann formula and exhibits a non-monotonic variation of $\kappa$ with external hydrostatic pressure at elevated temperatures. Our findings establish isotope-enriched GeC as a material of ultrahigh $\kappa$ and an ideal platform for exploring exotic phonon physics.