Optical frequency- and vibrational time-resolved two-dimensional spectroscopy by real-time impulsive resonant coherent Raman scattering in polydiacetylene
Optical frequency- and vibrational time-resolved two-dimensional spectroscopy by real-time impulsive resonant coherent Raman scattering in polydiacetylene
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DOI：
10.1103/physreva.70.023811
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发表时间：
2004-08-01
影响因子：
2.9
通讯作者：
Kobayashi, T
中科院分区：
文献类型：
--
作者：
Ishii, N;Tokunaga, E;Kobayashi, T
利用多通道锁相放大器对4-fs超短激光脉冲诱导的实时脉冲共振拉曼散射进行了光谱分辨。引入了光学和振动二维谱来分离振动功率谱中电子和振动展宽的影响。光谱分辨的实时振荡可以识别与聚合物聚二乙炔的碳-碳双键和三键的拉伸振动模式相关的波包运动。考虑到基态波包的非线性极化计算可以很好地再现观测到的动力学。证实了基态振动和激发态振动在远低于吸收边缘的波包动力学中起着重要的作用。
Real-time impulsive resonant Raman scattering induced by a 4-fs ultrashort laser pulse was spectrally resolved with a multichannel lock-in amplifier. An optical and vibrational two-dimensional spectrum was introduced to separate the effects of electronic and vibrational broadening in the power spectrum of the vibrations. Spectrally resolved real-time oscillations can identify the wave packet motion associated with the stretching vibrational mode of the carbon-carbon double and triple bonds of the polymer polydiacetylene. Calculated nonlinear polarizations which take into account the ground-state wave packets reproduced the observed dynamics fairly well. It is confirmed that the ground-state vibrations play a significant role in the dynamics of the wave packet even far below the absorption edge, as well as the excited-state vibrations.