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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Pronounced non-condon effect as the origin of the quantum beat observed in the time-resolved absorption signal from excited-state cis-stilbene
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Pronounced non-condon effect as the origin of the quantum beat observed in the time-resolved absorption signal from excited-state cis-stilbene

机译：明显的非密码子效应是在激发态顺式二苯乙烯的时间分辨吸收信号中观察到的量子拍的起源

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摘要

We carried out wavelength-dispersed time-resolved absorption measurements of cis-stilbene to investigate the mechanism of the appearance of the similar to 220 cm(-1) oscillation, which has been assigned to the nuclear wavepacket motion of the S, state. The observed oscillatory pattern showed almost same amplitude and phase across the absorption peak at 645 nm, which indicates that the modulation of the transition intensity gives rise to the quantum beat. We also carried out a semiquantitative numerical simulation of the time-resolved absorption spectra based on the effective linear response theory, in which we newly incorporated the Herzberg-Teller coupling model by introducing a coordinate-dependence of the transition moment. The results of these experiments and simulation clearly showed that the intensity of the quantum beat arises from a significant coordinate dependence of the S-n <- S-1 transition moment, i.e., non-Condon effect. It was concluded that the vibronic coupling of the S-n state with other electronic, states is so large that the Herzberg-Teller coupling predominantly contributes to the intensity of the quantum beat of the totally symmetric similar to 220 cm(-1) vibration. The present work suggests a general importance of the non-Condon effect in spectroscopy involving highly excited electronic states.
机译：我们进行了顺-二苯乙烯的波长分散的时间分辨吸收测量，以研究类似于220 cm（-1）振荡的出现机理，该振荡已分配给S状态的核波包运动。观察到的振荡模式在645 nm处的吸收峰上显示出几乎相同的幅度和相位，这表明跃迁强度的调制引起了量子拍。我们还基于有效的线性响应理论对时间分辨的吸收光谱进行了半定量数值模拟，其中我们通过引入跃迁矩的坐标相关性，将赫兹伯格-泰勒耦合模型重新引入。这些实验和模拟的结果清楚地表明，量子拍的强度源自S-n ＜-S-1跃迁矩的显着坐标依赖性，即非康登效应。结论是，S-n状态与其他电子状态的振动耦合非常大，以至于Herzberg-Teller耦合主要对类似于220 cm（-1）振动的完全对称量子拍的强度作出贡献。本工作表明非康登效应在涉及高激发电子态的光谱学中的一般重要性。

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