Second Harmonic Generation from a Single Plasmonic Nanorod Strongly Coupled to a WSe₂ Monolayer

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2009.08060.pdf (2.25 MB)

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https://pubs.acs.org/doi/10.1021/acs.nanolett.0c03757

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http://hdl.handle.net/11603/20079
 https://doi.org/10.1021/acs.nanolett.0c03757

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Author/Creator ORCID

https://orcid.org/0000-0002-1480-6959
 https://orcid.org/0000-0002-6370-8765

Date

2020-09-17

Type of Work

journal articles preprints
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Citation of Original Publication

Chentao Li, Xin Lu, Ajit Srivastava, S. David Storm, Rachel Gelfand, Matthew Pelton, Maxim Sukharev, and Hayk Harutyunyan. Chentao Li, Xin Lu, Ajit Srivastava, S. David Storm, Rachel Gelfand, Matthew Pelton, Maxim Sukharev, and Hayk Harutyunyan. Nano Letters 2021 21 (4), 1599-1605. DOI: 10.1021/acs.nanolett.0c03757

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This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Nano Letters, copyright © American Chemical Society after peer review. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.nanolett.0c03757

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Abstract

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.