Abstract

Abstract Highly sensitive characterization of surface plasmon resonance (SPR) modes lays the solid foundation for wide SPR-related applications. Herein, we discover that these SPR modes based on all-metal nanostructures without any probed molecule can be characterized with ultrahigh sensitivities at both excitation and emission wavelengths by utilizing plasmon-enhanced sum frequency generation (PESFG) spectroscopy. The theory of PESFG for sensitively characterizing SPR modes is first validated experimentally. Moreover, we have elaborately demonstrated that PESFG strongly depends on both the resonant wavelengths of SPR modes and spatial mode distributions when azimuthal angles of excitations are varied. Our study not only enhances the understanding of the mechanism that governs PESFG, but also offers a potentially new method for exploring new-style SPR modes (e.g. plasmon-induced magnetic resonance and bound states in the continuum) by PESFG.

Highlights

  • Plasmonic nanostructures, based on surface plasmon resonance (SPR) [1, 2], have prompted intense interests in various areas exemplified by solar cell [3], strong coupling [4, 5], super-resolution imaging [6], and so on

  • Highly sensitive characterization of surface plasmon resonance (SPR) modes lays the solid foundation for wide SPR-related applications. We discover that these SPR modes based on all-metal nanostructures without any probed molecule can be characterized with ultrahigh sensitivities at both excitation and emission wavelengths by utilizing plasmon-enhanced sum frequency generation (PESFG) spectroscopy

  • SPR-sensitive SFG spectroscopy has been demonstrated by (a) propagating surface plasmon polaritons (SPPs) excited in the grating and attenuated total internal reflection configurations [29, 30] or by (b) localized SPR [31, 32]

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Summary

Introduction

Plasmonic nanostructures, based on surface plasmon resonance (SPR) [1, 2], have prompted intense interests in various areas exemplified by solar cell [3], strong coupling [4, 5], super-resolution imaging [6], and so on. SPR-sensitive SFG spectroscopy has been demonstrated by (a) propagating surface plasmon polaritons (SPPs) excited in the grating and attenuated total internal reflection configurations (such as Langmuir–Blodgett layers covered on a silver film, organic films covered on silver gratings) [29, 30] or by (b) localized SPR (e.g. monolayers of octadecanethiol and dodecanethiol adsorbed on nanospheres and nanopillars, respectively) [31, 32] These studies indicate that plasmon-enhanced SFG (PESFG) is capable of characterizing SPR modes by introducing probed molecules to the nanostructures. Validated excellently by the phase-matching equation, we experimentally demonstrate the dependence of PESFG on resonant wavelengths of SPR modes and modes’ spatial distributions

Design and experimental setups
Validation of SFG signals
A greement between reflectance spectra and PESFG signals
D ispersion relation and field distributions
Conclusions
Sample preparation
SFG measurements
Reflectance calculations using FEM

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