Spatially Resolved Nonlinear Plasmonics.

Johannes Schust, Florian Mangold, Florian Sterl, Niklas Metz, Thorsten Schumacher, Markus Lippitz, Mario Hentschel, Harald Giessen
Author Information
  1. Johannes Schust: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany. ORCID
  2. Florian Mangold: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany.
  3. Florian Sterl: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany. ORCID
  4. Niklas Metz: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany.
  5. Thorsten Schumacher: Experimental Physics III, University of Bayreuth, Universitätstr. 30, 95440 Bayreuth, Germany.
  6. Markus Lippitz: Experimental Physics III, University of Bayreuth, Universitätstr. 30, 95440 Bayreuth, Germany. ORCID
  7. Mario Hentschel: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany.
  8. Harald Giessen: 4th Physics Institute and Research Center SCoPE, University of Stuttgart, Pfaffenwaldring 57, 70569 Stuttgart, Germany.

Abstract

Nonlinear optical plasmonics investigates the emission of plasmonic nanoantennas with the aid of nonlinear spectroscopy. Here we introduce nonlinear spatially resolved spectroscopy (NSRS) which is capable of imaging the k-space as well as spatially resolving the THG signal of gold nanoantennas and investigating the emission of individual antennas by wide-field illumination of entire arrays. Hand in hand with theoretical simulations, we demonstrate our ability of imaging various oscillation modes inside the nanostructures and therefore spatial emission hotspots. Upon increasing intensity of the femtosecond excitation, an individual destruction threshold can be observed. We find certain antennas becoming exceptionally bright. By investigating those samples taking structural SEM images of the nanoantenna arrays afterward, our spatially resolved nonlinear image can be correlated with this data proving that antennas had deformed into a peanut-like shape. Thus, our NSRS setup enables the investigation of a nonlinear self-enhancement process of nanoantennas under critical laser excitation.

Keywords

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