期刊
NANO LETTERS
卷 12, 期 11, 页码 5989-5994出版社
AMER CHEMICAL SOC
DOI: 10.1021/nl303488m
关键词
Plasmonics; surface-enhanced Raman scattering; femtosecond stimulated Raman spectroscopy; vibrational coherence lifetimes; molecule-plasmon interactions
类别
资金
- National Science Foundation [CHE-0802913, CHE-0911145, CHE-1152547, DMR-1121262, DGE-0824162]
- AFOSR/DARPA Project [BAA07-61, FA9550-08-1-0221]
- Department of Energy Basic Energy Sciences [DE-FG02-09ER16109, DE-FG02-03ER15457]
- NSF-NSEC
- NSF-MRSEC
- Keck Foundation
- State of Illinois
- Northwestern University
- Direct For Mathematical & Physical Scien [0802913] Funding Source: National Science Foundation
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1152547] Funding Source: National Science Foundation
- Division Of Chemistry [0802913] Funding Source: National Science Foundation
We examine ultrafast dynamics in a coupled molecule-Plasmon system.:Using a new ultrafast Raman technique called surface enhanced-femtosecond stimulated Raman Spectroscopy (SE-FSRS), we prove that plasmonic nanoparticles and adsorbed molecules are coupled by the appearance of Fano-like lineshapes, which arise from the interaction of narrowband vibrational coherences and the broadband plasmon resonance. We probe the effect of plasmon energy on the vibrational lineshapes and observe changes in the phase of the line shape dispersion. Finally, we examine the effect of plasmon-molecule coupling on the molecular Vibrational coherence lifetime. Surprisingly, coupling of the molecular vibration to the plasmon does not significantly shorten: the ::vibrational: coherence dephasing time Better understanding of the ultrafast dynamics of excited vibrational states and vibrational coherences in coupled molecular-plasmonic systems should assist in developing a mechanism based view of plasmonically enhanced photovoltaic and photocatalytic systems.
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