Surface Dynamics and Ligand−Core Interactions of Quantum Sized Photoluminescent Gold Nanoclusters
Issue Date: 
American Chemical Society
Yiyang, L. (Lin); Charchar, P, (Patrick); Christofferson, A.J. (Andrew J.); et al. "Surface Dynamics and Ligand−Core Interactions of Quantum Sized Photoluminescent Gold Nanoclusters". J. Am. Chem. Soc.. 140, 2018, 18217 - 18226
Quantum-sized metallic clusters protected by biological ligands represent a new class of luminescent materials; yet the understanding of structural information and photoluminescence origin of these ultrasmall clusters remains a challenge. Herein we systematically study the surface ligand dynamics and ligand−metal core interactions of peptide-protected gold nanoclusters (AuNCs) with combined experimental characterizations and theoretical molecular simulations. We show that the peptide sequence plays an important role in determining the surface peptide structuring, interfacial water dynamics and ligand−Au core interaction, which can be tailored by controlling peptide acetylation, constituent amino acid electron donating/withdrawing capacity, aromaticity/hydrophobicity and by adjusting environmental pH. Specifically, emission enhancement is achieved through increasing the electron density of surface ligands in proximity to the Au core, discouraging photoinduced quenching, and by reducing the amount of surfacebound water molecules. These findings provide key design principles for understanding the surface dynamics of peptideprotected nanoparticles and maximizing the photoluminescence of metallic clusters through the exploitation of biologically relevant ligand properties.

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