Third-order polarizability of interlayer excitons in hetero-bilayers

Abstract: In this paper, we employ a fully microscopic approach to the study of interlayer excitons in hetero-bilayers. We use Fowler's and Karplus' method to access the dynamical polarizability of non--interacting interlayer excitons in a $\mathrm{WSe}{2}/\mathrm{WS}{2}$--based van der Waals heterostructure. Following from the calculation of the linear polarizability, we consider Svendsen's variational method to the calculation of the dynamic third--order polarizability. With this variational method, we study both two--photon absorption and third--harmonic generation processes for interlayer excitons in a $\mathrm{WSe}{2}/\mathrm{WS}{2}$ hetero--bilayer, discussing the various selection rules of intra--excitonic energy level transitions.