Tuning magnitude and direction of lattice thermal conductivity in transition metal dichalcogenide heterobilayers

TL;DR

This study uses first-principles calculations to analyze and suggest ways to tune the lattice thermal conductivity in transition metal dichalcogenide heterobilayers through doping and structural modifications.

Contribution

It introduces a comprehensive analysis protocol linking phonon properties to thermal conductivity, enabling targeted tuning in 2D heterostructures.

Findings

Pristine heterobilayers show isotropic in-plane LTC with temperature stability.

Doping reduces and makes LTC anisotropic, affecting phonon scattering.

Layer localization and mass contrast influence thermal transport properties.

Abstract

We investigate the nanoscale mechanisms determining lattice thermal conductivity (LTC) of pristine and W-doped MX$_2$-M$^\prime$X$^\prime_2$ transition metal dichalcogenide heterobilayers from first principles, using the exact solution of the linearised Boltzmann transport equation in both phonon and relaxon bases. Pristine heterobilayers exhibit isotropic in-plane LTC with preserved ordering across temperature. Relaxon analysis identifies descriptors linking LTC to phonon properties such as the phonon group velocity and layer localisation. While systems with lighter atoms generally favour higher LTC, a sufficiently large mass contrast is required to induce layer localisation of the transport-relevant vibrational modes. Further, we show through the thermal viscosity that the relative distribution of vibrational states between metal/non-metal sublattices influences the balance between Normal and Umklapp scattering processes. On the other hand, doped systems exhibit reduced and anisotropic in-plane LTC, retain a well-defined layer character, but are strongly affected by enhanced phonon-phonon scattering due to mass disorder. Notably, we find that both configuration and temperature dictate the direction of maximum thermal transport, which opens the possibility to tune the direction of maximum (and minimum) conductivity via doping in novel 2D functional materials. Thanks to its general formulation, the analysis protocol can be readily extended to other van der Waals heterostructures, and the descriptors may be implemented in high-throughput engines to identify promising layered materials with tailored thermal transport characteristics.