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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Electronic Dynamics by Ultrafast Pump Photoelectron Detachment Probed by Ionization: A Dynamical Simulation of Negative?Neutral?Positive in LiH~?
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Electronic Dynamics by Ultrafast Pump Photoelectron Detachment Probed by Ionization: A Dynamical Simulation of Negative?Neutral?Positive in LiH~?

机译：电离探测超快泵浦光电子脱附的电子动力学：LiH〜-中负负中性的动力学模拟

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摘要

The control of electronic dynamics in the neutral electronic states of LiH before the onset of significant nuclei motion is investigated using a negative?neutral? positive (NeNePo) ultrafast IR pump?attoescond pulse train (APT) probe scheme. Starting from the ground state of the anion (LiH~?), multiphoton ultrafast electron detachment and subsequent excitation of the neutral by a few femtosecond intense IR pulse produces a non-equilibrium electronic density in neutral LiH. The coherent electronic wave packet is then probed by angularly resolved photoionization to the cation by an APT generated from a replica of the pump IR pulse at several time delays. Realistic parameters for the pump and the APT are used. Several NeNePo schemes are simulated using different IR carrier frequencies, showing that the delay between the successive attosecond pulses in the train can be used as a filter to probe the different pairs of states present in the coherent electronic wave packet produced by the pump pulse. The dynamical simulations include the pump and the probe pulses to all orders by solving the time-dependent Schr?dinger equation using a coupled equation scheme for the manifolds of the anion, neutral, and cation subspaces. We show that an incomplete molecular orientation of the molecule in the laboratory frame does not prevent probing the electronic density localization by angularly resolved photoelectron maps.
机译：使用负“中性粒子”研究了在显着核运动开始之前LiH处于中性电子态的电子动力学控制。正（NeNePo）超快红外泵浦？脚秒脉冲序列（APT）探针方案。从阴离子的基态（LiH〜）开始，多光子超快电子脱离以及随后通过几个飞秒的强IR脉冲激发中性离子，在中性LiH中产生了非平衡电子密度。然后，通过从泵浦IR脉冲的副本在几个时间延迟处生成的APT，通过角度分辨的光电离对阳离子进行相干电子波包探测。使用泵和APT的实际参数。使用不同的IR载波频率对几种NeNePo方案进行了仿真，显示出序列中连续的阿秒脉冲之间的延迟可以用作滤波器，以探测由泵浦脉冲产生的相干电子波包中存在的不同状态对。通过对阴离子，中性和阳离子子空间的流形使用耦合方程式求解时间相关的薛定er方程，动力学仿真包括泵浦和探测脉冲到所有阶数。我们表明，在实验室框架内分子的不完全分子取向不会阻止通过角度解析的光电子图来探测电子密度局部化。

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