Nature of Long-Lived Moiré Interlayer Excitons in Electrically Tunable MoS2/MoSe2 Heterobilayers

Nano Lett. 2024 Sep 11;24(36):11232-11238. doi: 10.1021/acs.nanolett.4c02635. Epub 2024 Aug 30.

Abstract

Interlayer excitons in transition-metal dichalcogenide heterobilayers combine high binding energy and valley-contrasting physics with a long optical lifetime and strong dipolar character. Their permanent electric dipole enables electric-field control of the emission energy, lifetime, and location. Device material and geometry impact the nature of the interlayer excitons via their real- and momentum-space configurations. Here, we show that interlayer excitons in MoS2/MoSe2 heterobilayers are formed by charge carriers residing at the Brillouin zone edges, with negligible interlayer hybridization. We find that the moiré superlattice leads to the reversal of the valley-dependent optical selection rules, yielding a positively valued g-factor and cross-polarized photoluminescence. Time-resolved photoluminescence measurements reveal that the interlayer exciton population retains the optically induced valley polarization throughout its microsecond-long lifetime. The combination of a long optical lifetime and valley polarization retention makes MoS2/MoSe2 heterobilayers a promising platform for studying fundamental bosonic interactions and developing excitonic circuits for optical information processing.

Keywords: Stark shift; interlayer excitons; layered materials heterostructures; moiré superlattice; photoluminescence; transition-metal dichalcogenides; valley polarization.