FOM Institute for Atomic and Molecular Physics (AMOLF), Science Park 104, 1098 XG Amsterdam, The Netherlands.
Phys Chem Chem Phys. 2011 May 21;13(19):8647-52. doi: 10.1039/c1cp20058e. Epub 2011 Apr 11.
In the development of attosecond molecular science, a series of experiments have recently been performed where ionic fragment asymmetries in the dissociative ionization of H(2) into H(+) + H and that of D(2) into D(+) + D were used to uncover electron localization processes that occur on the attosecond and few-femtosecond timescale. Electron localization was observed both in strong-field dissociative ionization using carrier envelope phase-stable few-cycle laser pulses [Kling et al., Science, 2006, 312, 246] and in a two-color extreme ultra-violet + infrared attosecond pump-probe experiment [Sansone et al., Nature, 2010, 465, 763]. Here we show that the observed electron localization can be well understood using a semi-classical model that describes the dynamics in terms of quasi-static states that take the interaction of the molecule with the laser field instantaneously into account. The electron localization is shown to be determined by the passage of the dissociating molecule through a regime where the laser-molecule interaction is neither diabatic nor adiabatic.
在阿秒分子科学的发展过程中，最近进行了一系列实验，其中利用 H(2)解离电离为 H(+) + H 和 D(2)解离电离为 D(+) + D 中的离子碎片不对称性，揭示了在阿秒和飞秒时间尺度上发生的电子局域化过程。电子局域化现象既在使用载波包络相位稳定的少周期激光脉冲的强场解离电离中观察到[Kling 等人，Science，2006，312，246]，也在双色极端超紫外+红外阿秒泵浦探测实验中观察到[Sansone 等人，Nature，2010，465，763]。在这里，我们表明，使用半经典模型可以很好地理解观察到的电子局域化，该模型根据准静态状态来描述动力学，这些准静态状态即时考虑了分子与激光场的相互作用。电子局域化被证明是由通过一个既非非绝热也非绝热的激光分子相互作用区域的解离分子决定的。
