Diabatic Hamiltonian Construction in van der Waals heterostructure complexes

TL;DR

This paper develops a wavefunction projection-based diabatization method to construct diabatic Hamiltonians for describing photoinduced charge transfer in van der Waals heterostructures, specifically MoS2/WS2.

Contribution

It introduces a practical approach to build diabatic Hamiltonians for interlayer charge transfer in vdW heterostructures using wavefunction projection.

Findings

Successfully constructs diabatic Hamiltonian for MoS2/WS2 heterostructure

Provides energies of localized valence band states and their couplings

Demonstrates the method's applicability to charge transfer processes

Abstract

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