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Instantaneous nonvertial electronic transitions with shaped femtosecond laser pulses: Is is possible?

机译:具有成形飞秒激光脉冲的瞬时非垂直电子跃迁:可能吗?

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摘要

In molecular electronic transitions, a vertical transition c an be induced by an ultrashort laser pulse. That is, a replica of the initial nuclear state-times the transition dipole moment of the electronic transition-can be created instantaneously (on the time scale of nuclear motion) in the excited electronic state. Now, applying pulse shaping via the modulation of the phases of each spectral component of an ultrashort pulse, it is tempting to ask whether it is also possible to induce instantaneous nonvertical transitions to bound electronic states, provided that the phases of each spectral component of the pulse are set to appropriate values at the discrete frequencies corresponding to the energy levels of the potential. We analyze the problem in the weak-field limit, and show that such a phase requirement cannot be encoded into an ultrashort pulse. This result is equivalent to the statement that it is not possible to move matter faster than the time associated with the natural (field-free) dynamics of the system.
机译:在分子电子跃迁中,垂直跃迁可以由超短激光脉冲引起。也就是说,可以在受激电子状态下瞬间(在核运动的时间尺度上)创建初始核态的副本(即电子跃迁的跃迁偶极矩)。现在,通过调制超短脉冲的每个频谱分量的相位来应用脉冲整形,很想问一问,是否还可以诱导瞬时非垂直跃迁到绑定的电子态,前提是该信号的每个频谱分量的相位都可以。在对应于电势能级的离散频率处将脉冲设置为适当的值。我们分析了弱场限制中的问题,并表明这种相位要求无法被编码为超短脉冲。该结果等同于这样的陈述:物质的移动不可能快于与系统自然(无场)动力学相关的时间。

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