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ORIGINAL RESEARCH article

Front. Photonics
Sec. Plasmonics
Volume 6 - 2025 | doi: 10.3389/fphot.2025.1548555
This article is part of the Research Topic Nonlinear Optical Processes in Emerging Nanomaterials View all 3 articles

Large First Hyperpolarizability of the Au@Ag Core-Shell Nanoparticles as compared to the Corresponding Alloyed Nanoparticles resulting from Laser Annealing

Provisionally accepted
Isabelle Russier-Antoine Isabelle Russier-Antoine 1Christian Jonin Christian Jonin 2Emmanuel Benichou Emmanuel Benichou 1Franck Bertorelle Franck Bertorelle 3Pierre-Francois Brevet Pierre-Francois Brevet 1*
  • 1 Université Claude Bernard Lyon 1, Lyon, France
  • 2 Université de Montpellier, Montpellier, Languedoc-Roussillon, France
  • 3 Université de Nantes, Nantes, Pays de la Loire, France

The final, formatted version of the article will be published soon.

    In this work, the first hyperpolarizability of Au x @Ag 100-x core-shell nanoparticles with x the gold molar fraction in percent and the gold core of which is 12 nm in diameter, is determined and compared to that of their corresponding laser annealed nanoparticles using hyper Rayleigh scattering experiments. Laser annealing transforms the initially composite Au x @Ag 100-x core-shell nanoparticles into alloyed Au x Ag 100-x homogeneous nanoparticles, providing a reference for comparison. It is observed that the evolution with the relative molar ratio between gold and silver of the first hyperpolarizability magnitude of both the Au x @Ag 100-x core-shell and the alloyed Au x Ag 100-x nanoparticles is driven by the SPR resonance enhancement occurring at the harmonic wavelength due to red shifting of the SPR band away from the harmonic wavelength. Furthermore, the first hyperpolarizability magnitude of the Au x @Ag 100-x core-shell nanoparticles is found to be about three orders of magnitude larger than that of the annealed alloyed Au x Ag 100-x nanoparticles. This feature may be attributed to the existence of the two nonlinearities, namely the surface nonlinearity due to the surrounding medium -silver layer interface and the silver -gold metal -metal interface constructively contributing due to their close localization. The core-shell morphology is thus highly beneficial in view of applications as compared to the alloyed one.

    Keywords: Hyper Rayleigh scattering, Gold - Silver Core-Shell Nanoparticles, first hyperpolarizability, Laser Annealed Nanoparticles, resonance enhancement

    Received: 19 Dec 2024; Accepted: 03 Feb 2025.

    Copyright: © 2025 Russier-Antoine, Jonin, Benichou, Bertorelle and Brevet. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) or licensor are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms.

    * Correspondence: Pierre-Francois Brevet, Université Claude Bernard Lyon 1, Lyon, France

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