Defect Healing and Charge Transfer-Mediated Valley Polarization in MoS₂/MoSe₂/MoS₂ Trilayer van der Waals Heterostructures

Abstract

Monolayer transition metal dichalcogenides (TMDCs) grown by chemical vapor deposition (CVD) are plagued by a significantly lower optical quality compared to exfoliated TMDCs. In this work, we show that the optical quality of CVD-grown MoSe 2 is completely recovered if the material is sandwiched in MoS 2 /MoSe 2 /MoS 2 trilayer van der Waals heterostructures. We show by means of density functional theory that this remarkable and unexpected result is due to defect healing: S atoms of the more reactive MoS 2 layers are donated to heal Se vacancy defects in the middle MoSe 2 layer. In addition, the trilayer structure exhibits a considerable charge-transfer mediated valley polarization of MoSe 2 without the need for resonant excitation. Our fabrication approach, relying solely on simple flake transfer technique, paves the way for the scalable production of large-area TMDC materials with excellent optical quality.