Hishikawa Akiyoshi, Ueyama Masakuni, Yamanouchi Kaoru
Institute for Molecular Science, National Institutes of Natural Sciences, Myodaiji, Okazaki, Aichi 444-8585, Japan.
J Chem Phys. 2005 Apr 15;122(15):151104. doi: 10.1063/1.1895745.
The temporal evolution of the nuclear wave packet of CS2 2+ formed in an intense laser field (60 fs, 0.13 PW/cm2) is traced in real time by the pump-and-probe technique combined with coincidence momentum imaging of the Coulomb explosion process, CS2 3+-->S+ + C+ + S+. The momentum correlations among the fragment ions obtained as a function of the pump-probe time delay between 133 fs to 3 ps reveal that the nuclear wave packet in CS2 2+ evolves not only along the anti-symmetric stretching coordinate to yield S+ and CS+ but also along the symmetric stretching coordinate leading to the simultaneous breaking of the two C-S bonds. The contribution from two different electronic states having bent and linear-type geometrical configurations is identified in the wave packet motion along the bending coordinate of CS2 2+.
通过泵浦-探测技术结合库仑爆炸过程CS2 3+→S+ + C+ + S+的符合动量成像，实时追踪了在强激光场（60飞秒，0.13 PW/cm2）中形成的CS2 2+核波包的时间演化。作为泵浦-探测时间延迟在133飞秒至3皮秒之间的函数获得的碎片离子之间的动量相关性表明，CS2 2+中的核波包不仅沿着反对称拉伸坐标演化以产生S+和CS+，而且还沿着对称拉伸坐标演化，导致两个C-S键同时断裂。在CS2 2+沿弯曲坐标的波包运动中，确定了具有弯曲和线性几何构型的两种不同电子态的贡献。
