Long-Lived Interlayer Excitons and Type-II Band Alignment in Janus MoTe2/CrSBr van der Waals Heterostructures

TL;DR

This study uses first-principles calculations to reveal that MoTe2/CrSBr heterostructures exhibit stable type-II band alignment and host long-lived interlayer excitons, making them promising for advanced optoelectronic applications.

Contribution

It provides a detailed first-principles analysis of the electronic, optical, and excitonic properties of MoTe2/CrSBr heterostructures, highlighting their stability and potential for long-lived excitons.

Findings

Stable heterobilayers with type-II band alignment.

Interlayer excitons with lifetimes 18-45 ps.

Optical properties modulated by built-in electric field.

Abstract

Identifying two-dimensional heterostructures with exceptional electronic and optical properties remains an active area of research in advanced optoelectronics. Here, we present a comprehensive first-principles investigation of the electronic, optical, and excitonic properties of a MoTe2/CrSBr van der Waals heterostructure using density functional theory combined with fully relativistic GW and Bethe-Salpeter equation calculations. The close lattice matching between the two monolayers enables the formation of stable heterobilayers with two inequivalent interfaces (Te-S and Te-Br) arising from the Janus nature of CrSBr. Both interfaces are dynamically and thermally stable and exhibit type-II band alignment with a direct quasiparticle gap, promoting efficient spatial separation of electrons and holes. The heterostructure hosts interlayer excitons with lifetimes 18-45 ps significantly longer than those of the intralayer excitons in the isolated MoTe2, 3.6 ps, and CrSBr, 8.1 ps, monolayers. Moreover, the optical gap, exciton binding energy, and exciton lifetime of the heterostructure are strongly modulated by the built-in electric field associated with the Janus layer. These results establish the MoTe2/CrSBr heterostructure as a versatile platform for engineering long-lived interlayer excitons and highlight its potential for next-generation optoelectronic and light-harvesting applications.