Quasi-ballistic thermal transport across MoS$_2$ thin films

TL;DR

This study reveals unexpectedly long c-axis phonon mean free paths in MoS2 thin films, showing quasi-ballistic heat transport that influences thermal resistance and has implications for optoelectronic and thermoelectric devices.

Contribution

It provides the first experimental and theoretical evidence of long c-axis phonon MFPs in MoS2, challenging previous assumptions of low cross-plane thermal conductivity in layered 2D materials.

Findings

Over 50% of heat is carried by phonons with MFP >200 nm.

Thermal conductivity scales with film thickness due to quasi-ballistic effects.

Volumetric thermal resistance asymptotes to ~10 m^2K/W in thin films.

Abstract

Layered two-dimensional (2D) materials have highly anisotropic thermal properties between the in-plane and cross-plane directions. In general, it is thought that cross-plane thermal conductivities ($\kappa_z$) are low, and therefore c-axis phonon mean free paths (MFPs) are small. Here, we measure $\kappa_z$ across MoS$_2$ films of varying thickness (20 to 240 nm) and uncover evidence of very long c-axis phonon MFPs at room temperature in these layered semiconductors. Experimental data obtained using time-domain thermoreflectance (TDTR) are in good agreement with first-principles density functional theory (DFT). These calculations reveal that ~50% of the heat is carried by phonons with MFP >200 nm, exceeding kinetic theory estimates by nearly two orders of magnitude. Because of quasi-ballistic effects, the $\kappa_z$ of nanometer thin films of MoS$_2$ scales with their thickness and the volumetric thermal resistance asymptotes to a non-zero value, ~10 m$^{2}$KGW$^{-1}$. This contributes as much as 30% to the total thermal resistance of a 20 nm thick film, the rest being limited by thermal interface resistance with the SiO$_2$ substrate and top-side aluminum transducer. These findings are essential for understanding heat flow across nanometer-thin films of MoS$_2$ for optoelectronic and thermoelectric applications.