Yamada Yuji, Kayano Masakazu, Mikami Naohiko, Ebata Takayuki
Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578 Japan.
J Phys Chem A. 2006 May 18;110(19):6250-5. doi: 10.1021/jp0571832.
Picosecond time-resolved IR-UV pump-probe spectroscopy has been performed to study intracluster vibrational energy redistribution (ICVR) and vibrational predissociation (VP) for the OH and CH stretch vibrations of phenol-ethylene hydrogen-bonded cluster. The transient UV spectra after the picosecond IR pulse excitation of these modes were observed by 1+1 REMPI via S(1) with a picosecond UV pulse. We have focused on the difference of the energy flow routes and their rates between the donor (phenol) and the acceptor (ethylene) site. Though the transient UV spectra showed a similar broad feature for all the vibrations examined, the time profiles exhibited a remarkable site dependence, as well as substantial mode dependence. Especially, we found a large difference in the early stage of the IVR evolution and the rates, whereas the VP rates were very similar.
已进行皮秒时间分辨红外 - 紫外泵浦 - 探测光谱研究苯酚 - 乙烯氢键簇中OH和CH伸缩振动的团簇内振动能量再分布（ICVR）和振动预解离（VP）。通过1 + 1共振增强多光子电离（REMPI）经由S(1)，利用皮秒紫外脉冲观测了这些模式在皮秒红外脉冲激发后的瞬态紫外光谱。我们关注了供体（苯酚）和受体（乙烯）位点之间能量流动路径及其速率的差异。尽管对于所有检测的振动，瞬态紫外光谱显示出相似的宽带特征，但时间轮廓表现出显著的位点依赖性以及明显的模式依赖性。特别是，我们发现在内振动能量再分布（IVR）演化的早期阶段和速率上存在很大差异，而振动预解离（VP）速率非常相似。
