Document Detail


Real-time Observation of Tight Au-Au Bond Formation and Relevant Coherent Motion upon Photoexcitation of [Au(CN)(2)(-)] Oligomers.
MedLine Citation:
PMID:  23273414     Owner:  NLM     Status:  Publisher    
Abstract/OtherAbstract:
Structural dynamics involving tight Au-Au bond formation of excited-state oligomers [Au(CN)(2)(-)](n) was studied using picosecond/femtosecond time-resolved emission and absorption spectroscopy. With selective excitation of the trimer ([Au(CN)(2)(-)](3)) in aqueous solutions, transient absorption due to the excited-state trimer was observed around 600 nm. This transient exhibited a significant intensity increase (τ = 2.1 ps) with a blue shift in the early picosecond time region. DFT/TDDFT calculations revealed that the observed spectral changes are ascribed to the structural change from the bent structures to linear staggered one in the triplet excited-state trimer. The transient absorption also exhibited a clear modulation of the peak position, reflecting coherent nuclear wavepacket motion induced by photoexcitation. The frequencies of the coherent motions are 66 and 87 cm(-1), which accorded very well with the frequencies of two Au-Au stretch vibrations in the excited state of the trimer calculated by DFT. Time-resolved emission spectra in the sub-nanosecond time region showed that association of the excited-state trimer with the ground-state monomer proceeds with τ = 2.0 ns, yielding the excited-state tetramer.
Authors:
Munetaka Iwamura; Koichi Nozaki; Satoshi Takeuchi; Tahei Tahara
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Publication Detail:
Type:  JOURNAL ARTICLE     Date:  2012-12-31
Journal Detail:
Title:  Journal of the American Chemical Society     Volume:  -     ISSN:  1520-5126     ISO Abbreviation:  J. Am. Chem. Soc.     Publication Date:  2012 Dec 
Date Detail:
Created Date:  2012-12-31     Completed Date:  -     Revised Date:  -    
Medline Journal Info:
Nlm Unique ID:  7503056     Medline TA:  J Am Chem Soc     Country:  -    
Other Details:
Languages:  ENG     Pagination:  -     Citation Subset:  -    
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