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The optical spectra of vertically stackedMoSe   2    /WSe   2heterostructures contain additional “interlayer” excitonic peaks that are absent in the individual monolayer materials and exhibit a significant spatial charge separation in out‐of‐plane direction. A many‐body perturbation theory approach is used to simulate the excitonic spectra ofMoSe   2    /WSe   2heterobilayers with three stacking orders, considering both momentum‐direct and momentum‐indirect excitons. The small oscillator strengths and the optical responses of the interlayer excitons are significantly stacking‐dependent and give rise to high radiative lifetimes in the range of 5–200 ns at low temperature for the “bright” interlayer excitons. Solving the finite‐momentum Bethe–Salpeter Equation (BSE), the lowest energy excitation is predicted to be an exciton over the fundamental indirect band gap, with a binding energy of 220 meV. However, in agreement with recent magneto‐optics experiments and previous theoretical studies, the simulations of the effective excitonic  g ‐factors suggest that the low energy momentum‐indirect excitons are not experimentally observed. The existence of “interlayer”  C  excitons with significant exciton binding energies and optical oscillator strengths is further revealed, which are analogous to the prominent band nesting excitons in mono‐ and few‐layer transition‐metal dichalcogenides.

Interlayer Excitonic Spectra of Vertically Stacked MoSe 2 /WSe 2 Heterobilayers