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Phys. Rev. Lett. 101, 037402 (2008) [4 pages]

Excited-State Molecular Vibration Observed for a Probe Pulse Preceding the Pump Pulse by Real-Time Optical Spectroscopy

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Takayoshi Kobayashi1,2,3,4,*, Juan Du1,2, Wei Feng5, and Katsumi Yoshino6
1Department of Applied Physics and Chemistry and Institute for Laser Science, the University of Electro-communications, 1-5-1 Chofugaoka, Chofu, Tokyo, 182-8585, Japan
2JST, ICORP, Ultrashort Pulse Laser Project, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
3Department of Electrophysics, National Chiao Tung University, 1001 Ta Hsueh Road, Hsin-Chu 3005, Taiwan
4Institute of Laser Engineering, Osaka University, 2-6 Yamada-Oka, Suita, Osaka 565-0971, Japan
5School of Materials Science and Engineering, Tianjin University, Tianjin 300072, P.R.China
6Shimane Institute for Industrial Technology, 1 Hokuryo-cho, Matsue, Shimane 690-0816, Japan

Received 19 December 2007; published 18 July 2008

It is shown experimentally that the absorbance change observed in the “negative” time range, where probe pulse precedes pump pulse in real-time vibrational spectroscopy is induced only by the excited-state wave-packet motion as theoretically expected. Coherent molecular vibration of a polymer in the excited state was observed in the real-time trace without the effect of wave-packet motion in the ground state, which usually makes it difficult to ascribe the signal either to the ground state or to the excited state.

© 2008 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.101.037402
DOI:
10.1103/PhysRevLett.101.037402
PACS:
78.47.−p, 42.65.−k, 78.47.J−, 78.40.Me

*kobayashi@ils.uec.ac.jp

 
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