Klamroth Tillmann
Theoretische Chemie, Institut für Chemie, Universität Potsdam, Golm, Germany.
J Chem Phys. 2006 Apr 14;124(14):144310. doi: 10.1063/1.2185633.
We report time-dependent configuration interaction singles calculations for the ultrafast laser driven many-electron dynamics in a polyatomic molecule, N-methyl-6-quinolone. We employ optimal control theory to achieve a nearly state-selective excitation from the S(0) to the S(1) state, on a time scale of a few ( approximately 6) femtoseconds. The optimal control scheme is shown to correct for effects opposing a state-selective transition, such as multiphoton transitions and other, nonlinear phenomena, which are induced by the ultrashort and intense laser fields. In contrast, simple two-level pi pulses are not effective in state-selective excitations when very short pulses are used. Also, the dependence of multiphoton and nonlinear effects on the number of states included in the dynamical simulations is investigated.
我们报告了对多原子分子N-甲基-6-喹诺酮中超快激光驱动的多电子动力学进行含时组态相互作用单激发计算。我们采用最优控制理论，在几（约6）飞秒的时间尺度上实现从S(0)态到S(1)态的近态选择性激发。结果表明，最优控制方案能够校正超短强激光场诱导的诸如多光子跃迁和其他非线性现象等不利于态选择性跃迁的效应。相比之下，当使用极短脉冲时，简单的二能级π脉冲在态选择性激发中无效。此外，还研究了多光子和非线性效应与动力学模拟中所包含的态数的关系。
