Controlling Exciton and Valley Dynamics in Two-Dimensional Heterostructures with Atomically Precise Interlayer Proximity.

Abstract

Two-dimensional (2D) materials and heterostructures with strong excitonic effect and spin/valley properties have emerged as an exciting platform for optoelectronic and spin/valleytronic applications. There, precise control of the exciton transformation process (including intralayer to interlayer exciton transition and recombination) and valley polarization process <i>via</i> structural tuning is crucial but remains largely unexplored. Here, using hexagonal boron nitride (BN) as an intermediate layer, we show the fine-tuning of exciton and valley dynamics in 2D heterostructures with atomic precision. Both interfacial electron and hole transfer rates decrease exponentially with increasing BN thickness, which can be well-described with quantum tunneling model. The increased spatial separation with BN intercalation weakens the electron-hole Coulomb interaction and significantly prolongs the interlayer exciton population and valley polarization lifetimes in van der Waals (vdW) heterostructures. For example, WSe₂/WS₂ heterostructures with monolayer BN intercalation exhibit a hole valley polarization lifetime of ∼60 ps at room temperature, which is approximately threefold and 3 orders of magnitude longer than that in WSe₂/WS₂ heterobilayer without BN and WSe₂ monolayer, respectively. Considering a large family of layered materials, this study suggests a general approach to tailor and optimize exciton and valley properties in vdW heterostructures with atomic precision.