4.6 Article

Molecule-like and lattice vibrations in metal clusters

期刊

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 22, 页码 13848-13859

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cp04708f

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资金

  1. University of Geneva
  2. Swiss National Science Foundation [200020_172511]
  3. Hasso Plattner Excellence Research Grant - Knowledge Transfer Center of the Lucian Blaga University of Sibiu [LBUS-HPI-ERG2020-07]
  4. MZ 2.0 mass spectrometry core facility at the Faculty of Sciences, University of Geneva

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We study distinct molecule-like and lattice vibrational properties of atomically precise, ligand-protected metal clusters using low-temperature Raman spectroscopy. Our results show the fingerprint Raman spectra of different metal clusters and how these spectra change with variations in metal atoms and/or ligands. This highlights the importance of low-frequency Raman spectroscopy in understanding the vibrational dynamics of other materials.
We report distinct molecule-like and lattice (breathing) vibrational signatures of atomically precise, ligand-protected metal clusters using low-temperature Raman spectroscopy. Our measurements provide fingerprint Raman spectra of a series of noble metal clusters, namely, Au-25(SR)(18), Ag-25(SR)(18), Ag24Au1(SR)(18), Ag-29(S2R)(12) and Ag-44(SR)(30) (-SR = alkyl/arylthiolate, -S2R = dithiolate). Distinct, well-defined, low-frequency Raman bands of these clusters result from the vibrations of their metal cores whereas the higher-frequency bands reflect the structure of the metal-ligand interface. We observe a distinct breathing vibrational mode for each of these clusters. Detailed analyses of the bands are presented in the light of DFT calculations. These vibrational signatures change systematically when the metal atoms and/or the ligands are changed. Most importantly, our results show that the physical, lattice dynamics model alone cannot completely describe the vibrational properties of ligand-protected metal clusters. We show that low-frequency Raman spectroscopy is a powerful tool to understand the vibrational dynamics of atomically precise, molecule-like particles of other materials such as molecular nanocarbons, quantum dots, and perovskites.

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