Regensburg 2022 – wissenschaftliches Programm

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O: Fachverband Oberflächenphysik

O 61: Plasmonics and Nanooptics 2

O 61.1: Topical Talk

Donnerstag, 8. September 2022, 10:30–11:00, H2

Single Molecule Nonlinearity in a Plasmonic Waveguide — •Markus Lippitz — Experimental Physics III, University of Bayreuth

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.