Rydberg electron wavepacket dymanics in atoms and molecules
Rydberg electron wavepacket dymanics in atoms and molecules
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原子和分子中的里德伯电子波包动力学
DOI：
10.1098/rsta.1998.0170
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发表时间：
1998
期刊：
影响因子：
--
通讯作者：
H. H. Fielding
中科院分区：
文献类型：
--
作者：
J. Ramswell;V. Stavros;Q. Hong;H. H. Fielding
本文讨论了利用皮秒激光产生和探测里德伯电子波包的方法，并结合对自旋轨道自电离动力学的观测进行了讨论。基于对Ramsey干涉条纹的观测，采用了多光子（纳秒+皮秒）激发方案和双光子相敏探测。为了补充实验，时间相关的多通道量子亏损理论（TD-MQDT）的计算已经发展到研究Ar中的自旋轨道自电离里德堡波包的动力学。依赖于时间的部分光电离截面揭示了有趣的干涉图案的递归光谱占在自电离通道的量子缺陷。最后，利用TD-MQDT研究了H2中里德堡波包的振转和转动自电离动力学。结果表明，在时域中，旋转通道之间的组态相互作用可以用相互作用时间来定量描述。与由经典轨道周期（∞n3）确定的振转自电离寿命相反，旋转自电离寿命由与离子核碰撞后的电子波包的动能确定。
The generation and detection of Rydberg electron wavepackets using picosecond lasers is discussed with reference to the observation of the dynamics of spin–orbit autoionization in Xe. A multiphoton (nanosecond + picosecond) excitation scheme is employed with two–photon phase–sensitive detection, based on the observation of Ramsey interference fringes. To complement the experiment, time–dependent multichannel quantum–defect theory (TD–MQDT) calculations have been developed to investigate the dynamics of a spin–orbit autoionizing Rydberg wavepacket in Ar. The time–dependent partial photoionization cross–sections reveal interesting interference patterns in the recurrence spectra which are accounted for in terms of the quantum defects of the autoionizing channels. Finally, the rovibrational and rotational autoionization dynamics of a Rydberg wavepacket in H2 are investigated using TD–MQDT. It is demonstrated that, in the time–domain, the configuration interaction between rotational channels can be described quantitatively in terms of an interaction time. In contrast to the rovibrational autoionization lifetime, which is determined by the classical orbit period (∞n3, the rotational autoionization lifetime is determined by the kinetic energy of the electron wavepacket following collision with the ion core.