Variable-spot-size laser-flash Raman method to measure in-plane and interfacial thermal properties of 2D van der Waals heterostructures

Abstract

Stacked layers of different atomically thin 2D materials is called the van der Waals (vdW) heterostructure, which has become a rapidly developing research field due to its extraordinary and tunable properties. In this paper, we develop a variable-spot-size laser-flash Raman method to in-situ measure the thermal properties as well as the laser absorption in the supported 2D vdW heterostructure with arbitrary layers. The extracted thermal properties include the in-plane thermal conductivity and diffusivity of each layer, and interfacial thermal conductance between every two adjacent layers. A three-dimensional transient heat conduction model is developed and analytically solved to describe the process of pulsed Gaussian laser heating supported n-layer heterostructure. The temperature of each atomic layer can be simultaneously non-contact detected from their distinct Raman peaks whose positions are temperature dependent. The laser spot sizes and pulse durations are varied to generate multiple temperature curves. The multiple thermal properties as well as the laser absorption can be extracted by simultaneously fitting these temperature curves into the analytical solutions at multiple spot sizes or/and pulse durations. We also establish the approach of sensitivity and uncertainty analysis for the multi-response multi-parameter least-square fitting in our proposed measurement methods. Case studies show that the transient temperature curves are generally more sensitive to the thermal properties than the steady-state temperatures at variable spot sizes. All the unknown thermal properties and laser absorption can be extracted with sufficiently high accuracy if multiple transient temperature curves at multiple spot sizes are simultaneously fitted into the analytical solution. The measurement method and uncertainty analysis approach presented here are useful for investigating the thermal transport in the emerging 2D materials and vdW heterostructures.