Interlayer Exciton-Phonon Coupling in MoSe 2 /WSe 2 Heterostructures.

Transition metal dichalcogenide heterostructures have garnered strong interest for their robust excitonic properties, mixed light-matter states such as exciton-polaritons, and tailored properties, vital for advanced device engineering. Two-dimensional heterostructures inherit their physics from monolayers with the addition of interlayer processes that have been particularly emphasized for their electronic and optical properties. Here, we demonstrate the interlayer coupling of the MoSe 2 phonons to WSe 2 excitons in a WSe 2 /MoSe 2 heterostructure using resonant Raman scattering. The WSe 2 monolayer induces an interlayer resonance in the Raman cross-section of the MoSe 2 A 1g phonons. Frozen-phonon calculations within density functional theory reveal a strong deformation-potential coupling between the A 1g MoSe 2 phonon and the electronic states of the close-by WSe 2 layer approaching 20% of the intralayer coupling to the MoSe 2 electrons. Understanding the vibrational properties of van der Waals heterostructures requires going beyond the sum of their constituents and considering cross-material coupling.