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Single Molecule Nonlinearity in a Plasmonic Waveguide

Cite this: Nano Lett. 2020, 20, 3, 2152–2156
Publication Date (Web):February 20, 2020
https://doi.org/10.1021/acs.nanolett.0c00196
Copyright © 2020 American Chemical Society

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    Abstract

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    Plasmonic waveguides offer the unique possibility to confine light far below the diffraction limit. Past room temperature experiments focused on efficient generation of single waveguide plasmons by a quantum emitter. However, only the simultaneous interaction of the emitter with multiple plasmonic fields would lead to functionality in a plasmonic circuit. Here, we demonstrate the nonlinear optical interaction of a single molecule and propagating plasmons. An individual terrylene diimide (TDI) molecule is placed in the nanogap between two single-crystalline silver nanowires. A visible wavelength pump pulse and a red-shifted depletion pulse travel along the waveguide, leading to stimulated emission depletion (STED) in the observed fluorescence. The efficiency increases by up to a factor of 50 compared to far-field excitation. Our study thus demonstrates remote nonlinear four-wave mixing at a single molecule with propagating plasmons. It paves the way toward functional quantum plasmonic circuits and improved nonlinear single-molecule spectroscopy.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.0c00196.

    • Sample fabrication; optical setup; pump and depletion spot size; depletion statistics of TDI; lifetime histogram of TDI; quantifying the background emission; propagation of the depletion pulses; propagation loss with PMMA cover; supplementary note 1: numerical simulations; supplementary note 2: model for fluorescence suppression (PDF)

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    This article is cited by 15 publications.

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