Interlayer excitons in MoSe${}_2$/WSe${}_2$ heterostructures from first-principles

Abstract

Based on \emph{ab initio} theoretical calculations of the optical spectra of vertical heterostructures of MoSe${}_2$ (or MoS${}_2$) and WSe${}_2$ sheets, we reveal two spin-orbit-split Rydberg series of excitonic states below the \textsl{A} excitons of MoSe${}_2$ and WSe${}_2$ with a significant binding energy on the order of 250\,meV for the first excitons in the series. At the same time, we predict crystalographically aligned MoSe${}_2$/WSe${}_2$ heterostructures to exhibit an indirect fundamental band gap. Due to the type-II nature of the MoSe${}_2$/WSe${}_2$ heterostructure, the indirect transition and the exciton Rydberg series corresponding to a direct transition exhibit a distinct interlayer nature with spatial charge separation of the coupled electrons and holes. The experimentally observed long-lived states in photoluminescence spectra of MoX${}_2$/WY${}_2$ heterostructure are attributed to such interlayer exciton states. Our calculations further suggest an effect of stacking order on the peak energy of the interlayer excitons and their oscillation strengths.

8 pages main manuscript, 12 pages supplementary information

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