Twist-Dependent Anisotropic Thermal Conductivity in Homogeneous MoS₂ Stacks

Thermal transport property of homogeneous twisted molybdenum disulfide (MoS$_2$) is investigated using non-equilibrium molecular dynamics simulations with the state-of-art force fields. The simulation results demonstrate that the cross-plane thermal conductivity strongly depends on the interfacial twist angle, while it has only a minor effect on the in-plane thermal conductivity, exhibiting a highly anisotropic nature. A frequency-decomposed phonon analysis showed that both the cross-plane and in-plane thermal conductivity of MoS$_2$ are dominated by the low-frequency phonons below 15 THz. As the interfacial twist angle increases, these low-frequency phonons significantly attenuate the phonon transport across the interface, leading to impeded cross-plane thermal transport. However, the in-plane phonon transport is almost unaffected, which allows for maintaining high in-plane thermal conductivity. Additionally, our study revealed the strong size dependence for both cross-plane and in-plane thermal conductivities due to the low-frequency phonons of MoS$_2$. The maximum in-plane to cross-plane thermal anisotropy ratio is estimated as 400 for twisted MoS$_2$ from our simulation, which is in the same order of magnitude as recent experimental results (~900). Our study highlights the potential of twist engineering as a tool for tailoring the thermal transport properties of layered materials.