Abstract

Hybrid nanoparticles composed of an efficient nonlinear optical core and a gold shell can enhance and tune the nonlinear optical emission thanks to the plasmonic effect. However the influence of an incomplete gold shell, i.e., isolated gold nano-islands, is still not well studied. Here LiNbO3 (LN) core nanoparticles of 45 nm were coated with various densities of gold nano-seeds (AuSeeds). As both LN and AuSeeds bear negative surface charge, a positively-charged polymer was first coated onto LN. The number of polymer chains per LN was evaluated at 1210 by XPS and confirmed by fluorescence titration. Then, the surface coverage percentage of AuSeeds onto LN was estimated to a maximum of 30% using ICP-AES. The addition of AuSeeds was also accompanied with surface charge reversal, the negative charge increasing with the higher amount of AuSeeds. Finally, the first hyperpolarizability decreased with the increase of AuSeeds density while depolarization values for Au-seeded LN were close to the one of bare LN, showing a predominance of the second harmonic volumic contribution.

Highlights

  • The synthesis of functional, multi-material nanoparticles (NPs) has been of particular interest for over two decades, as it allows one to bring together or to enhance various physicochemical properties

  • According to the Au Seeds (AuSeeds):LN ratio, the percentage of the LN@Branched PolyEthylenImine (BPEI) surface that can be covered by the AuSeeds can be changed, with a maximum surface coverage of 31% as determined by inductive-coupled plasma atomic emission spectroscopy (ICP-AES) analysis

  • The quadratic nonlinear optical properties of the seeded and unseeded nanoparticles were determined from Hyper Rayleigh scattering (HRS) experiments

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Summary

Introduction

The synthesis of functional, multi-material nanoparticles (NPs) has been of particular interest for over two decades, as it allows one to bring together or to enhance various physicochemical properties. Several types of multi-material NPs with many different architectures and geometries have been reported such as Janus [1], core-shell [2] or hollow [3]. NPs. Gold-seeded NPs, i.e., NPs decorated with a non-continuous shell composed of gold nano-islands, have found application in various fields such as catalysis [4], sensing [5] or enhanced Raman scattering [6]. The present report focuses on the synthesis of lithium niobate core NPs decorated with gold seeds.

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