Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy.
Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy.
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通过超快瞬态偏振光谱测量硝基苯中激发电子态的超快动力学。
DOI：
10.1021/acs.jpca.0c01943
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
N. Shivaram
中科院分区：
文献类型：
--
作者：
Richard L. Thurston;M. Brister;Liang Z. Tan;E. Champenois;S. Bakhti;P. Muddukrishna;T. Weber;A. Belkacem;D. Slaughter;N. Shivaram
我们利用超快瞬态偏振光谱研究了液体硝基苯中最低单线态激发态的超快动力学，将著名的光学克尔效应光谱技术扩展到激发态。受激分子系综的三阶非线性响应是用两个飞秒脉冲跟随一个填充S1激发态的第三个飞秒脉冲测量的。通过测量这种对激发态特征和结构细节高度敏感的响应，将其作为三个脉冲之间的时间延迟的函数，我们提取了激发态上波包的消相时间。减相时间作为泵浦激励后时滞的函数，显示振荡，表明激发态上的振荡波包动力学。从实验测量和支持的理论计算中，我们推断波包在单重态S1和三重态T2之间的系统间穿越三次后完全离开S1态势能面。
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 two 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 inter-system crossing between the singlet S1 and triplet T2 states.
影响因子：
16.6
作者：
H. Timmers;Xiaolei Zhu;Zheng Li;Yuki Kobayashi;M. Sabbar;M. Hollstein;Maurizio Reduzzi;T. Martínez;D. Neumark;S. Leone
通讯作者：
H. Timmers;Xiaolei Zhu;Zheng Li;Yuki Kobayashi;M. Sabbar;M. Hollstein;Maurizio Reduzzi;T. Martínez;D. Neumark;S. Leone