Diabatic Hamiltonian construction in van der Waals heterostructure complexes

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.