Interspecies exciton interactions lead to enhanced nonlinearity of dipolar excitons and polaritons in MoS2 homobilayers

Charalambos Louca (), Armando Genco (), Salvatore Chiavazzo, Thomas P. Lyons, Sam Randerson, Chiara Trovatello, Peter Claronino, Rahul Jayaprakash, Xuerong Hu, James Howarth, Kenji Watanabe, Takashi Taniguchi, Stefano Dal Conte, Roman Gorbachev, David G. Lidzey, Giulio Cerullo, Oleksandr Kyriienko and Alexander I. Tartakovskii ()
Additional contact information
Charalambos Louca: The University of Sheffield
Armando Genco: Politecnico di Milano
Salvatore Chiavazzo: University of Exeter
Thomas P. Lyons: The University of Sheffield
Sam Randerson: The University of Sheffield
Chiara Trovatello: Politecnico di Milano
Peter Claronino: The University of Sheffield
Rahul Jayaprakash: The University of Sheffield
Xuerong Hu: The University of Sheffield
James Howarth: University of Manchester
Kenji Watanabe: National Institute for Materials Science
Takashi Taniguchi: National Institute for Materials Science
Stefano Dal Conte: Politecnico di Milano
Roman Gorbachev: University of Manchester
David G. Lidzey: The University of Sheffield
Giulio Cerullo: Politecnico di Milano
Oleksandr Kyriienko: University of Exeter
Alexander I. Tartakovskii: The University of Sheffield

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract 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 ≈ 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.

Date: 2023
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DOI: 10.1038/s41467-023-39358-9

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