Theory of Electronic and Nuclear Wavepacket Dynamic (Application to the structure deformation and electron transfer of molucular in laser field)

电子核波包动力学理论（在激光领域分子结构变形和电子转移中的应用）

基本信息

批准号：
12640484
负责人：
KONO Hirohiko
金额：
$ 2.18万
依托单位：
Tohoku University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2000
资助国家：
日本
起止时间：
2000 至 2001
项目状态：
已结题

项目摘要

To understand the ultrafast electronic dynamics in intense fields, we have been developing an efficient grid point method, the dual transformation method, for solving the time-dependent Schrodinger equation for the electronic degrees of freedom of a molecule. We have applied this method to small molecular systems such as H_2. The vibrational degree of freedom is also incorporated in the calculation of H^+_2 without resorting to the Born-Oppenheimer approximation.In a long wavelength case, for H_2, the localized ionic (bond) states H^+H^- and H^-H^+ appear alternately according to the optical cycle, through which tunnel ionization proceeds. After one-electron ionization from H_2, H^+_2 is prepared around the equilibrium internuclear distance of H_2. The bond distance of H^+_2 is then stretched by the applied field. With the help of ab initio molecular orbital calculations, we also demonstrate molecular structure deformations characteristic of intense-field dynamics such as symmetric two-bond stretching of CO_2 cations. The wave packet approach enables visualization of electron-nucleus correlation and two-electron dynamics in intense laser fields.Electronic motion can be controlled by adjusting the intensity, frequency, and pulse length. As an example, we have examined the electronic dynamics of H_2 in a short wavelength case (〜100 nm). Contrary to the long wavelength case, the electron pair is created near the proton at which the dipole interaction energy becomes higher. The nonstationary states H^+H^- and H^-H^+ appear alternately with a period inherent to the molecule even after the incident pulse has fully decayed. Ultrafast electron hopping between the nuclei can be controlled by a second pulse. Using this two-pulse scheme, we are able to enhance or suppress the ionization.

为了了解激烈场中的超快电子动力学，我们一直在开发一种有效的网格点方法，即双重变换方法，用于求解分子电子自由度的时间依赖性schrodinger方程。我们已经将此方法应用于诸如H_2之类的小分子系统。振动的自由度也包含在H^+_ 2的计算中，而无需诉诸于born-oppenheimer近似。在长的波长情况下，对于H_2而言，局部离子（键）h^+h^ - h^ - h^ - h^-h^+根据光学周期，通过隧道隧道离子的流动循环出现。从H_2进行一次电子电离后，围绕H_2的等效核对距离制备H^+_ 2。然后通过应用场拉伸H^+_ 2的键距离。借助从头算分子轨道计算，我们还展示了分子结构的变形，表征强场动力学，例如对称的两键co_2阳离子。波数据包方法可以通过调节强度，频率和脉冲长度来控制电子核核相关和两电子动力学的可视化。电子运动可以控制。例如，我们在短波长情况（〜100 nm）中检查了H_2的电子动力学。与长波长情况相反，电子对在偶极相互作用能量变得更高的质子附近产生。非平稳状态h^+ h^ - 和h^-h^+出现，即使在入射脉冲完全衰减之后，也会与分子遗传的周期相反。核之间的超快电子跳可以由第二个脉冲控制。使用这种两脉冲方案，我们能够增强或抑制电离。