Surface Dynamics and Ligand-Core Interactions of Quantum Sized Photoluminescent Gold Nanoclusters

Yiyang Lin, Patrick Charchar, Andrew J. Christofferson, Michael R. Thomas, Nevena Todorova, Manuel M. Mazo, Qu Chen, James Doutch, Robert Richardson, Irene Yarovsky*, Molly M. Stevens

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)

12 Citations (Scopus)

Abstract

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 surface-bound water molecules. These findings provide key design principles for understanding the surface dynamics of peptide-protected nanoparticles and maximizing the photoluminescence of metallic clusters through the exploitation of biologically relevant ligand properties.

Original languageEnglish
Pages (from-to)18217-18226
Number of pages10
JournalJournal of the American Chemical Society
Volume140
Issue number51
DOIs
Publication statusPublished - 26 Dec 2018

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    Lin, Y., Charchar, P., Christofferson, A. J., Thomas, M. R., Todorova, N., Mazo, M. M., Chen, Q., Doutch, J., Richardson, R., Yarovsky, I., & Stevens, M. M. (2018). Surface Dynamics and Ligand-Core Interactions of Quantum Sized Photoluminescent Gold Nanoclusters. Journal of the American Chemical Society, 140(51), 18217-18226. https://doi.org/10.1021/jacs.8b04436