Abstract

The nonlinear properties of hybrid metallic-dielectric systems are attracting great interest due to their potential for the enhancement of frequency conversion processes at nanoscale dimensions. In this work, we theoretically and experimentally address the correlation between the near field distribution of hexagonal plasmonic necklaces of silver nanoparticles formed on the surface of a LiNbO3 crystal and the second harmonic generation (SHG) produced by this nonlinear crystal in the vicinities of the necklaces. The spectral response of the hexagonal necklaces does not depend on the polarization direction and is characterized by two main modes, the absorptive high-energy mode located in the UV spectral region and the lower energy mode, which is strongly radiant and extends from the visible to the near infrared region. We show that the spatial distribution of the enhanced SHG is consistent with the local field related to the low energy plasmon mode, which spectrally overlaps the fundamental beam. The results are in agreement with the low absorption losses of this mode and the two-photon character of the nonlinear process and provide deeper insight in the connection between the linear and nonlinear optical properties of the hybrid plasmonic-ferroelectric system. The study also highlights the potential of hexagonal necklaces as useful plasmonic platforms for enhanced optical processes at the nanoscale.

Highlights

  • Over the last few years, the study of plasmon enhanced nonlinear optical processes at the nanoscale has been receiving significant attention due to their potential applications in a diversity of disciplines such as molecular sensing, advanced spectroscopies or integrated photon sources for optical circuits [1,2,3,4,5]

  • We theoretically and experimentally address the correlation between the near field distribution of hexagonal plasmonic necklaces of silver nanoparticles formed on the surface of a LiNbO3 crystal and the second harmonic generation (SHG) produced by this nonlinear crystal in the vicinities of the necklaces

  • The spectral response of the hexagonal necklaces does not depend on the polarization direction and is characterized by two main modes, the absorptive high-energy mode located in the UV spectral region and the lower energy mode, which is strongly radiant and extends from the visible to the near infrared region

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Summary

Introduction

Over the last few years, the study of plasmon enhanced nonlinear optical processes at the nanoscale has been receiving significant attention due to their potential applications in a diversity of disciplines such as molecular sensing, advanced spectroscopies or integrated photon sources for optical circuits [1,2,3,4,5]. Most of these functionalities rely on the capability of nonlinear frequency converters to operate in a broad spectral range (from the UV down to the mid-infrared spectral region) with a controlled polarization state and high frequency stability. The mechanism responsible for this intensification has been mainly related to the local field enhancement of the fundamental beam, which participates with two photons in the SHG process

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