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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy
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Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

机译：超快瞬态偏振光谱测量硝基苯中激发电子状态的超快动态

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摘要

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The thirdorder nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S-1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. From the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S-1 state potential energy surface after three traversals of the intersystem crossing between the singlet S-1 and triplet T-2 states.
机译：我们使用超快瞬态偏振光谱研究液态硝基苯中最低单线型激发电子状态的超快速动力学，延伸了众所周知的光学克尔效应光谱技术到激励的电子状态。使用填充S-1激发状态的第三飞秒脉冲之后的一对飞秒脉冲测量激发分子集合的三个非线性响应。通过测量对激发状态字符和结构的细节非常敏感的这种响应，作为所涉及的三个脉冲之间的时间延迟的函数，我们提取波包在激发状态下的去除时间。作为泵激励之后的时间延迟函数测量的去除时间，示出了指示激发状态上的振荡波分组动态的振荡。从实验测量和支持理论计算中，我们推断出在单个S-1和三重态T-2态之间的三个穿过三个穿透后，波包完全离开S-1状态电位能表面。

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