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Time-dependent partitioning theory of the control of radiationless transitions in 24-mode pyrazine

机译:基于时间的分配理论控制24模吡嗪的无辐射跃迁

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We consider the control of internal conversion between the S _2(~1B _(2u)) excited electronic state of pyrazine and the S _1(~1B _(3u)) state. The study is performed both during and after the femtosecond excitation of the ground electronic state S _0(~1A _g) to form the S _2 state. The dynamics is examined using the newly developed effective modes technique which enables the full computation of quantum dynamics in multi-dimensional spaces. Using this technique, we also investigate the coherent control of population transfer from S _0 to the S _2 and S _1 electronic states. We find that the use of shaped laser pulses enables a significant delay of the internal conversion. For example, after 60 fs, the S _2 population amounts to ~60 of the initial S _0 population, and remains at ~20 after 100 fs, in contrast to the S _0 electronic state which is completely depopulated within 75 fs.
机译:我们考虑了吡嗪的S _2(〜1B _(2u))激发电子态和S _1(〜1B _(3u))态之间的内部转换控制。在飞秒激发地面电子状态S _0(〜1A _g)以形成S _2状态期间和之后都进行了研究。使用新开发的有效模式技术对动力学进行了检查,该技术可以对多维空间中的量子动力学进行全面计算。使用这种技术,我们还研究了从S _0到S _2和S _1电子态的人口迁移的相干控制。我们发现,使用成形的激光脉冲可显着延迟内部转换。例如,在60 fs之后,S _2总数达到初始S _0种群的〜60,并在100 fs之后保持在〜20,而在75 fs内完全消失的S _0电子状态。

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