首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >'Stirred, Not Shaken': Vibrational Coherence Can Speed Up Electronic Absorption
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'Stirred, Not Shaken': Vibrational Coherence Can Speed Up Electronic Absorption

机译:“搅拌而不晃动”:振动相干性可以加快电子吸收

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We have recently proposed a laser control scheme for ultrafast absorption in multilevel systems by parallel transfer (J. Phys. Chem. Lett. 2015, 6, 1724). In this work we develop an analytical model that better takes into account the main features of electronic absorption in molecules. We show that the initial vibrational coherence in the ground electronic state can be used to greatly enhance the rate and yield of absorption when ultrashort pulses are used, provided that the phases of the coherences are taken into account. On the contrary, the initial coherence plays no role in the opposite limit, when a single long pulse drives the optical transition. The theory is tested by numerical simulations in the first absorption band of Na-2.
机译:我们最近提出了一种通过并行转移在多级系统中实现超快吸收的激光控制方案(J. Phys。Chem。Lett。2015,6,1724)。在这项工作中,我们开发了一个分析模型,可以更好地考虑分子中电子吸收的主要特征。我们表明,在使用超短脉冲的情况下,只要考虑了相干的相位,就可以使用基态电子态的初始振动相干性来大大提高吸收速率和产率。相反,当单个长脉冲驱动光学跃迁时,初始相干性在相反的范围内不起作用。该理论通过数值模拟在Na-2的第一个吸收带中进行了测试。

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