Sub-100 nanometer silver doped gold–cysteine supramolecular assemblies with enhanced nonlinear optical properties. Issue 23 (13th May 2019)

• Record Type: Journal Article
• Authors: Fakhouri, Hussein; Perić, Martina; Bertorelle, Franck; Dugourd, Philippe; Dagany, Xavier; Russier-Antoine, Isabelle; Brevet, Pierre-François; Bonačić-Koutecký, Vlasta; Antoine, Rodolphe
• Is Part Of: Physical chemistry chemical physics. Volume 21:Issue 23(2019)
• Page Start: 12091
• Page End: 12099
• Publication Date: 2019-05-13
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/c9cp00829b
• Languages: English
• ISSNs: 1463-9076

Abstract

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. 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.