Interlayer excitons in bilayer MoS2 with strong oscillator strength up to room temperature

Abstract

Coulomb bound electron-hole pairs, excitons, govern the optical properties of semi-conducting transition metal dichalcogenides like MoS${}_2$ and WSe${}_2$. We study optical transitions at the K-point for 2H homobilayer MoS${}_2$ in Density Functional Theory (DFT) including excitonic effects and compare with reflectivity measurements in high quality samples encapsulated in hexagonal BN. In both calculated and measured spectra we find a strong interlayer exciton transition in energy between A and B intralayer excitons, observable for T$=4-300$ K, whereas no such transition is observed for the monolayer in the same structure in this energy range. The interlayer excitons consist of an electron localized in one layer and a hole state delocalized over the bilayer, which results in the unusual combination of high oscillator strength and a static dipole moment. We also find signatures of interlayer excitons involving the second highest valence band (B) and compare absorption calculations for different bilayer stackings. For homotrilayer MoS${}_2$ we also observe interlayer excitons and an energy splitting between different intralayer A-excitons originating from the middle and outer layers, respectively.

arXiv comment9 pages, 6 figures

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