Concerted effects of local and nonlocal plasmons on the broadband nonlinear optical response in tip-enhanced nanophotonics

10 April 2023, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

We report critical impacts of local and nonlocal geometries of plasmonic tips on the broadband nonlinear optical responses in tip-substrate nanocavities. Using gold tips with varied geometries, we demonstrated for the first time that not only the nanometer-scale sharpness of tip apexes but also the micrometer-scale geometry of tip shafts directly affects the enhancement properties of second-harmonic generation over the visible-to-infrared wavelength range. Numerical simulations of the tip-substrate plasmonic field revealed concerted contributions from spatially nonlocal and local plasmonic modes. Micrometer-scale tip shafts enable the excitation of nonlocal plasmonic modes throughout the tip, enhancing near-to-mid-infrared incoming light. Subsequent radiation of visible-to-near-infrared second harmonics is boosted by localized plasmons at the nanogap. Based on the agreement between experiments and calculations, our results indicate the importance of nanometer- and micrometer-scale geometrical engineering of plasmonic tips and provide a firm basis to understand and finely manipulate nonlinear optical phenomena in tip-substrate nanocavities.

Keywords

tip-enhanced second harmonic generation
near-field optics
plasmonic nanocavity
nonlinear nanophotonics
plasmonics

Supplementary materials

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Title
Supporting information: Concerted effects of local and non-local plasmons on the broadband nonlinear optical response in tip-enhanced nanophotonics
Description
Section 1. Method; section 2. Threshold of excitation intensity; and section 3. Discussion on the non-local effects of tip shafts.
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