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Réseaux ordonnés de nanoparticules étudiés par la combinaison de microscopie STM et spectroscopie SFG

Abstract : This manuscript describes the development of a dense and ordered network of epitaxially grown nanoparticles on an oxide thin-film (Al₂O₃) prepared on a Ni₃Al (111) crystal. Pd nanoparticles, and nanoparticles with palladium core and gold shell, were made with a narrow size distribution, thanks to the fact that the nucleation centers are regularly spaced. The thin oxide layer and then the nanoparticle network are studied by STM microscopy according to the substrate oxidation and Pd deposition parameters, in particular the oxidation and annealing temperatures, and the flow of palladium atoms. Beyond 1 ML of Pd and 1 ML of gold, the network becomes progressively disordered.In addition to STM microscopy, the small size distribution makes it possible to study the nanoparticles by means of overall spectroscopic measurements: the sum frequency generation (SFG) vibrational spectroscopy is used to characterize the distribution of the adsorption sites according to the size and chemical nature of the nanoparticles; differential reflectance spectroscopy (DRS) is used to characterize plasmonic properties. SFG discriminates between facet and edge sites, allowing to show that the nanoparticles grow rapidly in height. On core-shell particles, SFG allows to observe the segregation of Pd atoms across the gold shell, with Pd and gold sites distinguished by CO frequency. CO is selectively adsorbed on Pd atoms at moderate pressure (less than 10-3 mbar), then also on Au atoms at high pressures (1 mbar). Moreover, at high pressure CO induces the thermally reversible segregation of a large number of Pd atoms.The DRS makes it possible to observe the appearance of a plasmon resonance for a shell wider than 3 ML of gold. The resonance is more intense as the core of Pd is small, and the shell thick. But only becomes really intense in the vicinity of the coalescence of NPs.These experiments pave the way for finer experiments, in particular to probe more precisely the properties as a function of size, or the adsorption of CO in the presence of oxygen. They also open the way for the subsequent study of the adsorption of organic molecules on the nanoparticle network. The adsorption of molecules in bridge between nanoparticles will be sought. The electron transfer in the hybrid network thus formed will be studied using pump-probe experiments where electrons will be excited in the nanoparticles. SFG will probe the transient state of molecules under the effect of charge transfer.
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Abdoul Mouize Zakaria. Réseaux ordonnés de nanoparticules étudiés par la combinaison de microscopie STM et spectroscopie SFG. Chimie-Physique [physics.chem-ph]. Université Paris-Saclay, 2018. Français. ⟨NNT : 2018SACLS143⟩. ⟨tel-01827439⟩

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