期刊
NANO LETTERS
卷 21, 期 4, 页码 1599-1605出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c03757
关键词
plasmon-exciton polaritons; strong coupling; transition metal dichalcogenides; nonlinear optics; second harmonic generation; Rabi splitting
类别
资金
- Department of Energy [DESC0020101]
- NSF through the EFRI [EFMA-1741691]
- NSF DMR Award [1905809]
- U.S. National Science Foundation [DMR-1905135]
- Air Force Office of Scientific Research [FA9550-19-1-0009]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1905809] Funding Source: National Science Foundation
This study presents the first experimental investigation of the nonlinear properties of monolayer transition metal dichalcogenides coupled to metal plasmonic nanocavities, showing a pronounced splitting in the pump-frequency dependence of the second-harmonic signal. Numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results.
Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light-matter interactions. These systems are expected to have nonlinear-optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here, we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe2 monolayer strongly coupled to a single gold nanorod. The pump-frequency dependence of the second-harmonic signal displays a pronounced splitting that can be explained by a coupled-oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.
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