Gold-seeded Lithium Niobate Nanoparticles: Influence of Gold Surface Coverage on Second Harmonic Properties

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.