Coupled electron-nuclear wavepacket dynamics in potassium dimers
Coupled electron-nuclear wavepacket dynamics in potassium dimers
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DOI：
10.1088/0953-4075/47/12/124015
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发表时间：
2014-06-28
影响因子：
1.6
通讯作者：
Wollenhaupt, Matthias
中科院分区：
文献类型：
--
作者：
Braun, Hendrike;Bayer, Tim;Wollenhaupt, Matthias
最近，我们展示了分子价键激发的控制，这是由于诱导电荷振荡与驱动激光场的精确定制相位的相互作用(Bayer等人，2013物理)。莱特牧师。110 123003)。在这篇文章中，我们更详细地描述了双色实验--一个控制脉冲序列，然后是一个不同波长的电离探测脉冲。我们提供了为再现和分析实验结果而进行的量子动力学模拟的详细信息。对重现强场测量至关重要的相互作用区焦强分布平均化方法和取向平均化方法也作了详细的描述。对波包在相关势上的期望值的时间演化、分子中诱导的能量移动和电荷振荡中的调制的分析为进一步了解耦合核电子动力学的相互作用提供了更深的见解。由于测量的光电子能谱揭示了靶态的布居，我们描述了计算光电子能谱的量子力学方法，并用Mulliken的差势方法对结果进行了合理化。
Recently we have demonstrated control of valence-bond excitation of a molecule due to the interplay of the induced charge oscillation with the precisely tailored phase of the driving laser field (Bayer et al 2013 Phys. Rev. Lett. 110 123003). In this contribution we describe in more detail the two-colour experiment-a control pulse sequence followed by an ionizing probe pulse of a different wavelength. We provide details on the quantum dynamics simulations carried out to reproduce and to analyse the experimental results. The procedure for averaging over the focal intensity distribution in the interaction region and the method for orientation averaging, which are both crucial for the reproduction of our strong-field measurements, are also described in detail. The analysis of the temporal evolution of the expectation values of the wavepackets on the relevant potentials, the induced energetic shifts in the molecule and the modulation in the charge oscillation provides further insights into the interplay of the coupled nuclear-electron dynamics. Because the measured photoelectron spectra reveal the population of the target states we describe the quantum mechanical approach to calculate the photoelectron spectra and rationalize the results using Mulliken's difference potential method.