Direct Observation of the Pressure-Induced Structural Variation in Gold Nanoclusters and the Correlated Optical Response

Qi Li*, Charles J. Zeman, Bora Kalkan, Kristin Kirschbaum, Christopher G. Gianopoulos, Abhinav Parakh, David Doan, Andrew C. Lee, John Kulikowski, George C. Schatz, Guoyin Shen, Martin Kunz, X. Wendy Gu*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

The ability to gradually modify the atomic structures of nanomaterials and directly identify such structural variation is important in nanoscience research. Here, we present the first example of a high-pressure single-crystal X-ray diffraction analysis of atomically precise metal nanoclusters. The pressure-dependent, subangstrom structural evolution of an ultrasmall gold nanoparticle, Au25S18, has been directly identified. We found that a 0.1 Å decrease of the Au-Au bond length could induce a blue-shift of 30 nm in the photoluminescence spectra of gold nanoclusters. From theoretical calculations, the origins of the blue-shift and enhanced photoluminescence under pressure are investigated, which are ascribed to molecular orbital symmetry and conformational locking, respectively. The combination of the high-pressure in situ X-ray results with both theoretical and experimental optical spectra provides a direct and generalizable avenue to unveil the underlying structure-property relations for nanoclusters and nanoparticles which cannot be obtained through traditional physical chemistry measurements.

Original languageEnglish (US)
Pages (from-to)132-139
Number of pages8
JournalNano letters
Volume23
Issue number1
DOIs
StatePublished - Jan 11 2023

Keywords

  • High-Pressure
  • Luminescence
  • Nanoclusters
  • Single-Crystal X-ray Diffraction

ASJC Scopus subject areas

  • Condensed Matter Physics
  • Mechanical Engineering
  • Bioengineering
  • General Chemistry
  • General Materials Science

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