期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 135, 期 48, 页码 18222-18228出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja409998j
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资金
- National Science Foundation (NSF) [CHE-1150249]
- Colorado State University
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1150249] Funding Source: National Science Foundation
Electronic energy relaxation of Au-144(SR)(60)(q) ligand-protected nanoclusters, where SR = SC6H13 and q = -1, 0, +1, and +2, was examined using femtosecond time-resolved transient absorption spectroscopy. The observed differential transient spectra contained three distinct components: (1) transient bleaches at 525 and 600 nm, (2) broad visible excited-state absorption (ESA), and (3) stimulated emission (SE) at 670 nm. The bleach recovery kinetics depended upon the excitation pulse energy and were thus attributed to electron-phonon coupling typical of metallic nanostructures. The prominent bleach at 525 nm was assigned to a core-localized plasmon resonance (CLPR). ESA decay kinetics were oxidation-state dependent and could be described using a metal-sphere charging model. The dynamics, emission energy, and intensity of the SE peak exhibited dielectric-dependent responses indicative of Superatom charge transfer states. On the basis of these data, the Au-144(SR)(60) system is the smallest-known nanocluster to exhibit quantifiable electron dynamics and optical properties characteristic of metals.
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