Moire excitons in MoSe2-WSe2 heterobilayers and heterotrilayers

Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moire interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe2-WSe2 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 moire excitons in different spin and valley configurations. We conclude that the photoluminescence of MoSe2-WSe2 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 moire 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. Here, the authors show that the photoluminescence of MoSe2/WSe2 heterobilayers is dominated by valley-direct excitons, whereas, in heterotrilayers, interlayer hybridization turns momentum-indirect interlayer excitons into energetically lowest states with phonon-assisted emission.

Automated summary

The authors studied excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides, finding different optical signatures. In heterobilayers, the photoluminescence is dominated by valley-direct excitons, while in heterotrilayers, interlayer hybridization transforms momentum-indirect interlayer excitons into energetically lowest states with phonon-assisted emission.