Journal
NATURE COMMUNICATIONS
Volume 7, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms13240
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Funding
- Air Force Office of Scientific Research under AFOSR [FA9550-11-1-9999 (FA9550-11-1-0147)]
- Camille Dreyfus Teacher-Scholar Awards Program
- NSFC [21372006, U1532141, 21631001]
- Ministry of Education
- US Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]
- Education Department of Anhui Province
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The evolution from the metallic (or plasmonic) to molecular state in metal nanoparticles constitutes a central question in nanoscience research because of its importance in revealing the origin of metallic bonding and offering fundamental insights into the birth of surface plasmon resonance. Previous research has not been able to probe the transition due to the unavailability of atomically precise nanoparticles in the 1-3 nm size regime. Herein, we investigate the transition by performing ultrafast spectroscopic studies on atomically precise thiolate-protected Au-25, Au-38, Au-144, Au-333, Au-similar to 520 and Au-similar to 940 nanoparticles. Our results clearly map out three distinct states: metallic (size larger than Au-333, that is, larger than 2.3 nm), transition regime (between Au-333 and Au-144, that is, 2.3-1.7 nm) and non-metallic or excitonic state (smaller than Au-144, that is, smaller than 1.7 nm). The transition also impacts the catalytic properties as demonstrated in both carbon monoxide oxidation and electrocatalytic oxidation of alcohol.
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