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Sub-100 nanometer silver doped gold–cysteine supramolecular assemblies with enhanced nonlinear optical properties

Abstract : The ability of gold(I) thiolates to self-assemble into supramolecular architectures opens the route for a new class of nanomaterials with a unique structure–optical property relationship. However, for a confirmed structure–optical property relationship, a control of the supramolecular architectures is required. In this work, we report a simple synthesis of sub-100 nanometer gold–cysteine and silver doped gold–cysteine supramolecular assemblies. We explore in particular silver-doping as a strategy to enhance the optical properties of these supramolecular assemblies. By an accurate characterization of as-synthesized supramolecular nanoparticles, we have been able to measure for the first time, their absolute two-photon absorption cross-section, two-photon excited fluorescence cross-section and first hyperpolarizabilities at different near-IR wavelengths. Huge values are obtained for silver doped gold–cysteine supramolecular assemblies, as compared to their corresponding undoped counterpart. In addition, we employ DFT and TD-DFT methods to study the geometric and electronic structures of model gold–cysteine and silver doped gold–cysteine compounds in order to address the structure−linear/nonlinear optical property relationship. The aim is to gain insights into the origin of the nonlinear optical enhancement of silver-doped gold supramolecular assemblies.
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Submitted on : Wednesday, October 28, 2020 - 3:59:12 PM
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Hussein Fakhouri, Martina Perić, Franck Bertorelle, Philippe Dugourd, Xavier Dagany, et al.. Sub-100 nanometer silver doped gold–cysteine supramolecular assemblies with enhanced nonlinear optical properties. Physical Chemistry Chemical Physics, Royal Society of Chemistry, 2019, 21 (23), pp.12091-12099. ⟨10.1039/c9cp00829b⟩. ⟨hal-02367612⟩

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