Moiré quantum chemistry: charge transfer in transition metal dichalcogenide superlattices

Abstract

Transition metal dichalcogenide (TMD) bilayers have recently emerged as a robust and tunable moiré system for studying and designing correlated electron physics. In this work, by combining large-scale first principle calculation and continuum model approach, we provide an electronic structure theory that maps long-period heterobilayer TMD superlattices onto diatomic crystals with cations and anions. We find that the interplay between moiré potential and Coulomb interaction leads to filling-dependent charge transfer between MM and MX regions several nanometers apart. We show that the insulating state at half-filling found in recent experiments on WSe${}_2$/WS${}_2$ is a charge-transfer insulator rather than a Mott-Hubbard insulator. Our work reveals the richness of simplicity in moiré quantum chemistry.

4+3 pages, 4+5 figures