Moiré quantum chemistry: charge transfer in transition metal dichalcogenide superlattices (1910.14061v4)

Abstract: Transition metal dichalcogenide (TMD) bilayers have recently emerged as a robust and tunable moir\'e 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 moir\'e 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 moir\'e quantum chemistry.