Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Tokyo 113-0033, Japan.
J Chem Phys. 2013 Mar 14;138(10):104304. doi: 10.1063/1.4794130.
Ionization of acetylene (C2H2) induced by an intense laser field whose polarization direction is parallel to the molecular axis is investigated by time-dependent Hartree-Fock calculations. It is found that, in the ionization process, the probability of the ejection of an electron from the two highest occupied orbitals of σ symmetry increases drastically as the C-H distance is symmetrically increased. On the contrary, the ejection probability of an electron in the two degenerate π orbitals is much less influenced by the bond elongation. The laser-induced dynamics of the time-dependent orbitals are interpreted by projecting them onto time-independent orbitals, which are eigenfunctions of the time-independent Fock operator.
采用与分子轴平行的强激光场电离乙炔（C2H2），通过含时 Hartree-Fock 计算进行研究。发现，在电离过程中，随着 C-H 距离的对称增加，来自于 σ 对称的两个最高占据轨道的电子的逐出几率急剧增加。相反，在两个简并的π轨道中电子的逐出几率受键长伸长的影响要小得多。通过将时间相关轨道投影到时间无关轨道上，即时间无关 Fock 算符的本征函数上，对时间相关轨道的激光诱导动力学进行解释。
