In-operando control of sum-frequency generation in tip-enhanced nanocavities

Philippe Roelli; Isabel Pascual Robledo; Iris Niehues; Javier Aizpurua; Rainer Hillenbrand

doi:10.1038/s41377-025-01855-5

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In-operando control of sum-frequency generation in tip-enhanced nanocavities

Original Articles

- In-operando control of sum-frequency generation in tip-enhanced nanocavities
- Light: Science & Applications Vol. 14, Issue 8, Pages: 2152-2162(2025)
- Affiliations：
  
  1.CIC nanoGUNE BRTA, 20018 Donostia-San Sebastián, Spain
  2.Materials Physics Center, CSIC-UPV/EHU, 20018 Donostia-San Sebastián, Spain
  3.Institute of Physics, University of Münster, 48149 Münster, Germany
  4.Donostia International Physics Center (DIPC), 20018 Donostia-San Sebastián, Spain
  5.IKERBASQUE, Basque Foundation for Science, 48013 Bilbao, Spain
  6.Department of Electricity and Electronics, University of the Basque Country (UPV/EHU), 48940 Leioa, Spain
- Author bio：
  
  Philippe Roelli (p.roelli@nanogune.eu)
  Rainer Hillenbrand (r.hillenbrand@nanogune.eu)
- Funds：
- DOI：10.1038/s41377-025-01855-5
  CLC：
- Received：29 October 2024，
  
  Revised：26 March 2025，
  
  Accepted：31 March 2025，
  
  Published Online：22 May 2025，
  
  Published：31 August 2025
- Accepted：
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Roelli, P. et al. In-operando control of sum-frequency generation in tip-enhanced nanocavities. Light: Science & Applications, 14, 2152-2162 (2025).
DOI：

Roelli, P. et al. In-operando control of sum-frequency generation in tip-enhanced nanocavities. Light: Science & Applications, 14, 2152-2162 (2025). DOI： 10.1038/s41377-025-01855-5.

摘要

Abstract

Sum-frequency generation (SFG) is a second-order nonlinear process widely used for characterizing surfaces and interfaces with monolayer sensitivity. Recently

optical field enhancement in plasmonic nanocavities has enabled SFG with continuous wave (CW) lasers from nanoscale areas of molecules

promising applications like nanoscale SFG spectroscopy and coherent upconversion for mid-infrared detection at visible frequencies. Here

we demonstrate CW SFG from individual nanoparticle-on-mirror (NPoM) cavities

which are resonant at visible frequencies and filled with a monolayer of molecules

when placed beneath a metal scanning probe tip. The tip acts as an efficient broadband antenna

focusing incident CW infrared illumination onto the nanocavity. The cascaded near-field enhancement within the NPoM nanocavity yields nonlinear optical responses across a broad range of infrared frequencies

achieving SFG enhancements of up to 14 orders of magnitude. Further

nanomechanical positioning of the tip allows for in-operando control of SFG by tuning the local field enhancement rather than the illumination intensities. The versatility of tip-enhanced nanocavities allows for SFG studies of a wide range of molecular species in the few-molecule regime without the need for complex nanofabrication. Our results also promise SFG nanoimaging with tips providing strong visible and IR field enhancement at their apex

offering a robust platform for future applications in nonlinear nanooptics.

关键词

Keywords

references

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