Pump and probe ultrafast electron dynamics in LiH: a computational study
Pump and probe ultrafast electron dynamics in LiH: a computational study
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LiH 中的泵浦和探测超快电子动力学：计算研究
DOI：
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发表时间：
2008
期刊：
影响因子：
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通讯作者：
R. Levine
中科院分区：
文献类型：
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作者：
M. Nest;F. Remacle;R. Levine
采用含时多组态方法计算了LiH中所有电子对几个周期的强泵浦场和探测脉冲的响应。超短泵浦脉冲激发了稳态电子态的相干叠加，并且通过改变泵浦参数，例如强度、持续时间、偏振和载波频率的相位，可以操纵电子的运动。特别注意的是由偏振和相位提供的控制。例如，极化的变化用于选择在垂直于键的平面中旋转或在包含键的平面中旋转的电子波包。电子波包可以通过延迟的第二脉冲来探测。这个延迟的探测脉冲也包括在哈密顿量中，结果是频率分散的探测光谱可以被计算并显示为二维图。
A time-dependent multiconfiguration method with a large electronic basis set is used to compute the response of all the electrons of LiH to a few-cycle intense pump field followed by a probe pulse. The ultrashort pump pulse excites a coherent superposition of stationary electronic states and, by changing the pump parameters such as intensity, duration, polarization and phase of carrier frequency, one can steer the motion of the electrons. Particular attention is given to the control provided by the polarization and by the phase. For example, a change in polarization is used to select an electronic wave packet that is rotating in a plane perpendicular to the bond or rotation in a plane containing the bond. The electronic wave packet can be probed by a delayed second pulse. This delayed probe pulse is also included in the Hamiltonian with the result that the frequency dispersed probe spectrum can be computed and displayed as a two-dimensional plot.