College of Physics and Information Engineering, Shanxi Normal University, Linfen, 041004, China.
College of Chemistry and Materials Science, Shanxi Normal University, Linfen, 041004, China.
Sci Rep. 2017 Sep 4;7(1):10359. doi: 10.1038/s41598-017-10667-6.
A pump-probe scheme for monitoring the electron dynamics of the excited state has been investigated by numerically solving the two-state time-dependent Schrödinger equation based on the non-Born-Oppenheimer approximation. By adjusting the delay time between a mid-infrared probe pulse and an ultra violet pump pulse, an obvious minimum can be seen in the higher-order harmonic region. With electron probability density distribution, ionization rate and classical simulation, the minimum can be ascribed to the electron localization around one nucleus at larger delay time and represents the electron dynamics of the excited state at the time of ionization. Moreover, the position of the minimum is much more sensitive to the nuclear motion.
我们通过数值求解基于非玻恩-奥本海默近似的双态含时薛定谔方程，研究了一种用于监测激发态电子动力学的泵浦-探测方案。通过调整中红外探测脉冲和紫外泵浦脉冲之间的延迟时间，可以在高次谐波区域观察到明显的最小值。通过电子概率密度分布、离化率和经典模拟，可以将最小值归因于在较大延迟时间下围绕一个原子核的电子局域化，代表了离化时激发态的电子动力学。此外，最小值的位置对核运动更为敏感。
