Moir\'e excitons in MoSe$_2$-WSe$_2$ heterobilayers and heterotrilayers

TL;DR

This study investigates moiré excitons in twisted MoSe₂-WSe₂ heterostructures, revealing how interlayer hybridization influences optical properties and exciton behavior in bilayer and trilayer configurations.

Contribution

It provides experimental and theoretical insights into moiré excitons in twisted TMD heterostructures, highlighting the role of interlayer hybridization and spin-valley configurations.

Findings

Photoluminescence in heterobilayer includes valley-direct and phonon-assisted emissions.

Heterotrilayer emission is dominated by momentum-dark interlayer excitons.

Interlayer hybridization significantly affects optical signatures in TMD heterostructures.

Abstract

Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moir\'e interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe$_2$-WSe$_2$ stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlayer moir\'e excitons in different spin and valley configurations. We conclude that the photoluminescence of MoSe$_2$-WSe$_2$ heterobilayer is consistent with joint contributions from radiatively decaying valley-direct interlayer excitons and phonon-assisted emission from momentum-indirect reservoirs that reside in spatially distinct regions of moir\'e supercells, whereas the heterotrilayer emission is entirely due to momentum-dark interlayer excitons of hybrid-layer valleys. Our results highlight the profound role of interlayer hybridization for transition metal dichalcogenide heterostacks and other realizations of multi-layered semiconductor van der Waals heterostructures.