Thermal History-Dependent Current Relaxation in hBN/MoS₂ van der Waals Dimers

Combining atomically thin layers of van der Waals (vdW) materials in a chosen vertical sequence is an emerging route to create devices with desired functionalities. While this method aims to exploit the individual properties of partnering layers, strong interlayer coupling can significantly alter their electronic and optical properties. Here we explored the impact of the vdW epitaxy on electrical transport in atomically thin molybdenum disulfide (MoS₂) when it forms a vdW dimer with crystalline films of hexagonal boron nitride (hBN). We observe a thermal history-dependent long-term (over ∼40 h) current relaxation in the overlap region of MoS₂/hBN heterostructures, which is absent in bare MoS₂ layers (or homoepitaxial MoS₂/MoS₂ dimers) on the same substrate. Concurrent relaxation in the low-frequency Raman modes in MoS₂ in the heterostructure region suggests a slow structural relaxation between trigonal and octahedral polymorphs of MoS₂ as a likely driving mechanism that also results in inhomogeneous charge distribution in the MoS₂ layer. Our experiment yields an aspect of vdW heteroepitaxy that can be generic to electrical devices with atomically thin transition-metal dichalcogenides.