Direct Spectroscopic Observation of Cross-Plane Heat Transfer in a Two-Dimensional Van der Waals Heterostructure

Two-dimensional (2D) transition metal chalcogenides (TMDs) have drawn significant attention in recent years due to their extraordinary optical and electronic properties. As heat transfer plays an important role in device performance, various methods such as optothermal Raman spectroscopy and time-domain thermoreflectance have been developed to measure the thermal conductivity and interfacial thermal conductance in 2D van der Waals (vdW) heterostructures. Here, we employ the vibrational-pump-visible-probe (VPVP) spectroscopy to directly visualize the heat transfer process in a heterostructure of multilayer h-BN and monolayer WS₂. Following an impulsive vibrational excitation of h-BN in the mid-infrared, we probe the heat transfer from h-BN through WS₂ and finally to the substrate from the subpicosecond to the submicrosecond timescale. The interfacial thermal conductance of the h-BN/WS₂ and WS₂/SiO₂ interfaces is obtained by corroborating the experiments with heat transfer calculations based on the Fourier’s law of heat conduction. Our study demonstrates an alternative, time-resolved optical method to measure cross-plane heat dissipation and opens up a new pathway to investigate the interlayer electron–phonon and phonon–phonon interactions in vdW heterostructures.