Femtosecond time-resolved observation of butterfly vibration in electronically excited o-fluorophenol.
Femtosecond time-resolved observation of butterfly vibration in electronically excited o-fluorophenol.
复制标题
电子激发邻氟苯酚中蝶形振动的飞秒时间分辨观察
DOI：
10.1038/s41598-017-14483-w
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发表时间：
2017-11-10
影响因子：
4.6
通讯作者：
Zhang B
中科院分区：
文献类型：
--
作者：
Ling F;Li S;Song X;Wang Y;Long J;Zhang B
利用飞秒时间分辨离子产额谱结合时间分辨光电子成像技术，对电子激发态邻氟苯酚中氢隧穿过程中的蝶形振动进行了真实的观测.在第一激发电子态（S1）中准备了离面C-F蝴蝶运动的相干叠加。当C-F键相对于芳香环振动时，核几何形状周期性地变化，导致光电离通道的相应变化。通过与里德伯态共振，非平面最小值的电离概率更有利，振动波包的演化表现为母离子瞬态中的叠加拍频。此外，时间分辨的光电子能谱提供了平面几何和非平面最小值之间的振荡蝴蝶振动的直接映射。来自平面几何的光电子峰的拍频与来自非平面最小值的拍频异相。我们的研究结果提供了一个物理上直观的和完整的图片的振荡流的能量负责的相干振动运动的激发态表面。
The butterfly vibration during the hydrogen tunneling process in electronically excited o-fluorophenol has been visualized in real time by femtosecond time-resolved ion yield spectroscopy coupled with time-resolved photoelectron imaging technique. A coherent superposition of out-of-plane C–F butterfly motions is prepared in the first excited electronic state (S1). As the C–F bond vibrates with respect to the aromatic ring, the nuclear geometry varies periodically, leading to the corresponding variation in the photoionization channel. By virtue of the more favorable ionization probability from the nonplanar minimum via resonance with the Rydberg states, the evolution of the vibrational wave packet is manifested as a superimposed beat in the parent-ion transient. Moreover, time-resolved photoelectron spectra offer a direct mapping of the oscillating butterfly vibration between the planar geometry and nonplanar minimum. The beats for the photoelectron peaks originating from the planar geometry are out of phase with those from the nonplanar minimum. Our results provide a physically intuitive and complete picture of the oscillatory flow of energy responsible for the coherent vibrational motion on the excited state surface.
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影响因子：
64.8
作者：
DANTUS, M;BOWMAN, RM;ZEWAIL, AH
通讯作者：
ZEWAIL, AH
影响因子：
4.4
作者：
Davies, Julia A.;Reid, Katharine L.
通讯作者：
Reid, Katharine L.
影响因子：
2.3
作者：
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通讯作者：
Klaeboe, Peter
影响因子：
5.7
作者：
Midgley, Jonathan;Davies, Julia A.;Reid, Katharine L.
通讯作者：
Reid, Katharine L.
影响因子：
56.9
作者：
ROSKER, MJ;DANTUS, M;ZEWAIL, AH
通讯作者：
ZEWAIL, AH