Heat transport properties of PbTe1−xSex alloys using equivariant graph neural network interatomic potential

Abstract

The suppression of heat transport in disordered crystals arises from a competition between mass fluctuations and bond disorder, but their relative contributions remain difficult to disentangle. We address this challenge using a machine-learned interatomic potential trained on ab initio data across the PbTe_1−xSe_x alloy series. Molecular dynamics simulations with the trained machine-learned interatomic potential reproduce experimental lattice thermal conductivities and density-functional theory phonon dispersions while enabling frequency-resolved analysis of heat transport from 300 to 800 K. We find a narrow window near 1.7–2.0 THz dominates heat transport across all compositions, where heat is primarily carried by mixed longitudinal acoustic and optical modes. Alloying dramatically reduces spectral diffusivity near 2 THz leading to the deterioration of thermal conductivity. For the parent compounds both the spectral diffusivity and overall thermal conductivity decrease at elevated temperatures. However, the thermal degradation is weaker for the mid-range composition (x = 0.5) due to the greater thermal occupation of vibrational modes and increased heat capacity. Alchemical simulations show that force–constant disorder, not mass contrast, plays the dominant role in this suppression. These results highlight the microscopic mechanisms underlying thermal transport breakdown in alloys and demonstrate how machine-learned interatomic potentials now offer a tractable path toward predictive, physics-rich thermal transport modeling in complex disordered solids.