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Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-03-19 , DOI: 10.1021/acs.jpca.0c01943 Richard Thurston 1 , Matthew M. Brister 1 , Liang Z. Tan 2 , Elio G. Champenois 1, 3 , Said Bakhti 1 , Pavan Muddukrishna 1 , Thorsten Weber 1 , Ali Belkacem 1 , Daniel S. Slaughter 1 , Niranjan Shivaram 1
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-03-19 , DOI: 10.1021/acs.jpca.0c01943 Richard Thurston 1 , Matthew M. Brister 1 , Liang Z. Tan 2 , Elio G. Champenois 1, 3 , Said Bakhti 1 , Pavan Muddukrishna 1 , Thorsten Weber 1 , Ali Belkacem 1 , Daniel S. Slaughter 1 , Niranjan Shivaram 1
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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 third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S1 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 S1 state potential energy surface after three traversals of the intersystem crossing between the singlet S1 and triplet T2 states.
中文翻译：
超快瞬态极化光谱法测量硝基苯中激发态电子的超快动力学
我们使用超快速瞬态极化光谱技术研究了液态硝基苯中最低单重态激发电子态的超快动力学，将光学克尔效应光谱学的著名技术扩展到激发电子态。被激发的分子整体的三阶非线性响应是使用一对飞秒脉冲来测量的，该对飞秒脉冲紧随填充了S 1的第三飞秒脉冲之后兴奋的状态。通过测量对激发态特征和结构的细节高度敏感的响应，作为所涉及的三个脉冲之间的时间延迟的函数，我们提取出激发态下波包的移相时间。移相时间是泵激励后的时间延迟的函数，它显示出振荡，表明在激发态下振动波包的动态变化。从实验测量和支持的理论计算中，我们推论出在单重态S 1和三重态T 2态之间的系统间相交经过了三个遍历之后，波包完全离开了S 1状态势能面。
更新日期：2020-03-20
中文翻译：
超快瞬态极化光谱法测量硝基苯中激发态电子的超快动力学
我们使用超快速瞬态极化光谱技术研究了液态硝基苯中最低单重态激发电子态的超快动力学，将光学克尔效应光谱学的著名技术扩展到激发电子态。被激发的分子整体的三阶非线性响应是使用一对飞秒脉冲来测量的，该对飞秒脉冲紧随填充了S 1的第三飞秒脉冲之后兴奋的状态。通过测量对激发态特征和结构的细节高度敏感的响应，作为所涉及的三个脉冲之间的时间延迟的函数，我们提取出激发态下波包的移相时间。移相时间是泵激励后的时间延迟的函数，它显示出振荡，表明在激发态下振动波包的动态变化。从实验测量和支持的理论计算中，我们推论出在单重态S 1和三重态T 2态之间的系统间相交经过了三个遍历之后，波包完全离开了S 1状态势能面。
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