Transition metal dichalcogenides (TMDs) constitute a versatile platform for atomically thin optoelectronics devices and spin–valley memory applications. In monolayer TMDs the optical absorption is strong, but the transition energy cannot be tuned as the neutral exciton has essentially no out-of-plane static electric dipole1,2. In contrast, interlayer exciton transitions in heterobilayers are widely tunable in applied electric fields, but their coupling to light is substantially reduced. In this work, we show tuning over 120 meV of interlayer excitons with a high oscillator strength in bilayer MoS2 due to the quantum-confined Stark effect3. We optically probed the interaction between intra- and interlayer excitons as they were energetically tuned into resonance. Interlayer excitons interact strongly with intralayer B excitons, as demonstrated by a clear avoided crossing, whereas the interaction with intralayer A excitons is substantially weaker. Our observations are supported by density functional theory (DFT) calculations, which include excitonic effects. In MoS2 trilayers, our experiments uncovered two types of interlayer excitons with and without in-built electric dipoles. Highly tunable excitonic transitions with large in-built dipoles and oscillator strengths will result in strong exciton–exciton interactions and therefore hold great promise for non-linear optics with polaritons.
The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request.
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N.L., L.S. and R.J.W. acknowledge funding from the PhD School Quantum Computing and Quantum Technology, SNF (project no. 200020_156637), Swiss Nanoscience Institute and NCCR QSIT. S.S., I.P., C.R., D.L., A.B., X.M., I.C.G. and B.U. acknowledge funding from ANR 2D-vdW-Spin, ANR VallEx, ANR MagicValley, ITN 4PHOTON Marie Sklodowska Curie grant agreement no. 721394 and the Institut Universitaire de France. K.W. and T.T. acknowledge support from the Elemental Strategy Initiative conducted by the MEXT, Japan, grant no. JPMXP0112101001, JSPS KAKENHI grant no. JP20H00354 and the CREST(JPMJCR15F3), JST. I.C.G. thanks the CALMIP initiative for the generous allocation of computational time, through the project p0812, as well as GENCI-CINES and GENCI-IDRIS for grant A006096649. We thank J.-M. Poumirol for the atomic force microscopy measurements and J. G. Roch for crucial help at early stages of this work.
The authors declare no competing interests.
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Leisgang, N., Shree, S., Paradisanos, I. et al. Giant Stark splitting of an exciton in bilayer MoS2. Nat. Nanotechnol. 15, 901–907 (2020). https://doi.org/10.1038/s41565-020-0750-1
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