On the Non-Metallicity of 2.2 nm Au (SR) Nanoclusters.

Authors:
Meng Zhou
Meng Zhou
Harbin Medical University
China
Chenjie Zeng
Chenjie Zeng
Carnegie Mellon University
Pittsburgh | United States
Yongbo Song
Yongbo Song
Wuhan University
China
Jonathan W Padelford
Jonathan W Padelford
Georgia State University
Gangli Wang
Gangli Wang
Georgia State University
United States
Matthew Y Sfeir
Matthew Y Sfeir
Columbia University
United States
Tatsuya Higaki
Tatsuya Higaki
Carnegie Mellon University
Pittsburgh | United States
Rongchao Jin
Rongchao Jin
Carnegie Mellon University
United States

Angew Chem Int Ed Engl 2017 12 22;56(51):16257-16261. Epub 2017 Nov 22.

Department of Chemistry, Carnegie Mellon University, Pittsburgh, PA, 15213, USA.

The transition from molecular to plasmonic behaviour in metal nanoparticles with increasing size remains a central question in nanoscience. We report that the giant 246-gold-atom nanocluster (2.2 nm in gold core diameter) protected by 80 thiolate ligands is surprisingly non-metallic based on UV/Vis and femtosecond transient absorption spectroscopy as well as electrochemical measurements. Specifically, the Au nanocluster exhibits multiple excitonic peaks in transient absorption spectra and electron dynamics independent of the pump power, which are in contrast to the behaviour of metallic gold nanoparticles. Moreover, a prominent oscillatory feature with frequency of 0.5 THz can be observed in almost all the probe wavelengths. The phase and amplitude analysis of the oscillation suggests that it arises from the wavepacket motion on the ground state potential energy surface, which also indicates the presence of a small band-gap and thus non-metallic or molecular-like behaviour.

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December 2017
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