DOE OSTI · 3415758
Hybridization of Excited Interlayer Excitons with Intralayer Excitons in Transition-Metal Dichalcogenide Heterostructures: Interplay of Orbital and Structural Symmetry
Abstract
Hybridization between interlayer exciton (ILX) and intralayer excitons offers a powerful route to engineer light–matter interactions in transition-metal dichalcogenide (TMDC) heterostructures, yet the underlying mechanism and selection rules remain elusive. Here we probe exciton hybridization in MoTe2/MoSe2 heterobilayers under a tunable out-of-plane electric field and observe distinct avoided crossings in the electric-field dependent reflection spectra. We associate them with coupling between excited ILX states, including the 2p and 2s Rydberg states, and MoTe2 intralayer exciton. Supported by ab initio GW plus Bethe-Salpeter equation (GW-BSE) calculations, we identify the hybridizing states and establish optical selection rules based on the effective angular momentum of the exciton states. These findings highlight the role of excitonic binding in the observed hybridization, rather than that of simple band-mixing models, and provide a new pathway for brightening high-energy dark states.
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Yao, Helen [Department of Materials Science and Engineering; Stanford University; SLAC National Accelerator Laboratory] (ORCID:0009000497748994), Wang, Jierong [SLAC National Accelerator Laboratory; Department of Applied Physics; Stanford University] (ORCID:0009000074191442), Chen, Emily Y. [Department of Materials Science and Engineering; Stanford University] (ORCID:000000025972798X), Karni, Ouri [SLAC National Accelerator Laboratory; Department of Applied Physics; Stanford University; Physics & Informatics Laboratory, NTT Research Inc., 940 Stewart Dr., Sunnyvale, California 94085, United States] (ORCID:0000000301187033), Haber, Jonah B. [Department of Materials Science and Engineering; Stanford University], Watanabe, Kenji [Research Center for Electronic and Optical Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan] (ORCID:0000000337018119), Taniguchi, Takashi [Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan] (ORCID:0000000214673105), da Jornada, Felipe H. [Department of Materials Science and Engineering; Stanford University] (ORCID:0000000167127151), Heinz, Tony F. [SLAC National Accelerator Laboratory; Department of Applied Physics; Stanford University] (ORCID:0000000313659464). 2026-05-21. Hybridization of Excited Interlayer Excitons with Intralayer Excitons in Transition-Metal Dichalcogenide Heterostructures: Interplay of Orbital and Structural Symmetry. https://doi.org/10.1021/acs.nanolett.5c05898
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