Single Molecule Nonlinearity in a Plasmonic Waveguide.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 32077703.
- Also identified by DOI 10.1021/acs.nanolett.0c00196.
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Abstract
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.