Layer sliding and twisting induced electronic transitions in correlated magnetic 1T-NbSe2 bilayers

Abstract: Correlated two-dimensional (2D) layers, like 1T-phases of TaS2, TaSe2 and NbSe2, exhibit rich tunability through varying interlayer couplings, which promotes the understanding of electron-correlation in the 2D limit. However, the coupling mechanism is, so far, poorly understood and was tentatively ascribed to interactions among the d_(z^2 ) orbitals of Ta or Nb atoms. Here, we theoretically show that the interlayer hybridization and localization strength of interfacial Se pz orbitals, rather than Nb d_(z^2 ) orbitals, govern the variation of electron-correlated properties upon interlayer sliding or twisting in correlated magnetic 1T-NbSe2 bilayers. Each of the both layers is in a star-of-David (SOD) charge-density-wave phase. Geometric and electronic structures, and magnetic properties of 28 different stacking configurations were examined and analyzed using density-functional-theory calculations. We found that the SOD contains a localized region (Reg-L), in which interlayer Se pz hybridization plays a paramount role in varying the energy levels of the two Hubbard bands. These variations lead to three electronic transitions among four insulating states, which demonstrated the effectiveness of interlayer interactions to modulate correlated magnetic properties in a prototypical correlated magnetic insulator.