Published June 2, 2023 | Version v1
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Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS₂ bilayers

  • 1. Department of Physics and Astronomy, The University of Sheffield, Sheffield S3 7RH, UK
  • 2. Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci, 32, Milano, 20133, Italy
  • 3. Department of Physics, University of Exeter, Stocker Road, Exeter, EX4 4PY, UK
  • 4. RIKEN Center for Emergent Matter Science, Wako, Saitama, 351-0198, Japan
  • 5. Department of Physics and Mathematics, University of Hull, Rober Blackburn, Hull HU6 7RX, UK
  • 6. National Graphene Institute, University of Manchester, Manchester, UK
  • 7. Department of Physics and Astronomy, University of Manchester, Manchester, UK
  • 8. Research Center for Electronic and Optical Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
  • 9. Research Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan

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Description

Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS₂ to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons (dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS₂ monolayers, both hIX and dipolaritons exhibit approximately 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This provides access to an unusual nonlinear regime which we describe theoretically as a mixed effect of Pauli exclusion and exciton-exciton interactions enabled through charge tunnelling. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.

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References

Preprint
Louca C., Genco A. et al. "Nonlinear interactions of dipolar excitons and polaritons in MoS2 bilayers." arXiv preprint arXiv:2204.00485 (2022)., doi: 10.48550/arXiv.2204.00485