非绝热耦合分子光电子能谱及态布居延时依赖

Time delay dependence of photoelectron spectroscopy and state populations of nonadiabatic coupling molecules

利用三态模型和含时波包法,研究了强飞秒泵浦-探测激光场中延时对非绝热耦合NaI分子光电子能谱、备态布居的影响.结果表明波包在势能面上做周期性运动,周期约为1000 fs,延时为200 fs时波包第一次到达交叉区域并分裂成两部分,800 fs时波包再次返回交叉区域发生分裂。波包的周期性运动导致光电子能谱谱峰位置的周期性变化,波包在交叉区域的分裂情况影响了各态布居分布。调节泵浦-探测延时可实现对波包运动的控制及态布居的选择性分布,研究结果为实验上实现分子的光控制及量子操控过程提供了一定参考。

Influences of time delay on photoelectron spectra and state populations of nonadiabatic coupled NaI molecules in intense femtosecond pump-probe laser field are investigated by using three-state model and time-dependent wave packet method. Results show that the wave packet moves periodically on the potential energy surface with roundtrip time of 1000 fs. When time delay is 200 fs, the wave packet reaches the crossing region for the first time and splits into two parts again at 800 fs. The periodical motion of the wave The wave packet returns to the crossing region and splits packet results in the periodical variation of photoelectron spectra peak position. The splitting situation of wave packet in the cross region affects the distribution of state populations. The wave packet motion control and selective distribution of state populations can be achieved by adjusting pump-probe delay time. The results can provide some reference for realizing the optical control of molecules and quantum control process experimentally.