標題: Real-Time Vibrational Dynamics in Chlorophyll a Studied with a Few-Cycle Pulse Laser
作者: Du, Juan
Teramoto, Takahiro
Nakata, Kazuaki
Tokunaga, Eiji
Kobayashi, Takayoshi
電子物理學系
Department of Electrophysics
公開日期: 17-Aug-2011
摘要: We use a 6.8-fs laser as the light source for broad-band femtosecond pump-probe real-time vibrational spectroscopy to investigate both electronic relaxation and vibrational dynamics of the Q(y)-band of Chl-a at 293 K. More than 25 vibrational modes coupled to the Q(y) transition are observed. Eleven of them have been clarified predominantly due to the excited state, and six of them are concluded to be nearly exclusively resulting from the ground-state wave-packet motion. Moreover, thanks to the broad-band detection over 5000 cm(-1), the modulated signals due to the excited state vibrational coherence are observed on both sides of the 0-0 transition with equal separation. The corresponding nonlinear process has been studied using a three-level model, from which the probe wavelength dependence of the phase of the periodic modulation can be calculated. The probe wavelength dependence of the vibrational amplitude is interpreted in terms of the interaction between the "pump" or "laser," Stokes, and anti-Stokes field intermediated by the molecular vibrations. In addition, an excited state absorption peak at similar to 709 nm has been observed. To the best of our knowledge, this is the first study of broad-band real-time vibrational spectroscopy in Chl-a.
URI: http://hdl.handle.net/11536/20167
ISSN: 0006-3495
期刊: BIOPHYSICAL JOURNAL
Volume: 101
Issue: 4
起始頁: 995
結束頁: 1003
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