Diabatic Hamiltonian construction in van der Waals heterostructure complexes

Abstract

A diabatization method is developed for the approximated description of the photoinduced charge separation/transfer processes in van der Waals (vdW) heterostructure complexes, and is based on the wavefunction projection approach using a plane wave basis set in the framework of the single-particle picture. We built a diabatic Hamiltonian to describe the interlayer photoinduced hole-transfer process of two-dimensional vdW MoS₂/WS₂ heterostructure complexes. The diabatic Hamiltonian gives the energies of the localized band states, located in the MoS₂ and WS₂ layers, respectively, as well as the diabatic couplings between them. The wavefunction projection method provides a practical and reasonable approach to construct a diabatic model to describe the photoinduced charge transfer processes in the vdW heterostructure complexes.