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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >New Strategy for Optimal Control of Femtosecond Pump-Dump Processes
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New Strategy for Optimal Control of Femtosecond Pump-Dump Processes

机译：飞秒抽水过程最优控制的新策略

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摘要

We propose a new strategy for optimal control with tailored pump-dump pulses which drive a system of moderate complexity via electronically excited states to a desired objective in the ground state with a maximal yield. It is based on the concept of the intermediate target in the excited state which selects the appropriate Franck-Condon window at a given time delay between the two pulses mandatory for reaching optimally the objective. The existence of the intermediate target ensures the connective pathway between the initial state and the objective in the ground state, necessary for the controllability of multidimensional systems involving two electronic states. We show that scope of this concept by optimizing and analyzing the pump and dump pulses for driving the isomerization process in the Na_3F_2 cluster to the second isomer by suppressing radiationless transition through the conical intersection between the first excited and the ground state. This has been realized by employing our ab initio Wigner distribution approach.
机译：我们提出了一种新的策略，可通过量身定制的泵浦突降脉冲进行最佳控制，该脉冲可以通过电激发态将具有中等复杂度的系统驱动到基态，并以最大的产量达到所需的目标。它基于处于激发态的中间目标的概念，该目标在两个脉冲之间的给定时间延迟内选择适当的Franck-Condon窗口，以强制达到最佳目标。中间目标的存在确保了初始状态和基态目标之间的连接路径，这对于涉及两个电子状态的多维系统的可控性是必需的。通过优化和分析用于抑制Na_3F_2团簇向第二异构体的异构化过程的泵浦和卸载脉冲，通过抑制通过第一激发态和基态之间的圆锥形交点的无辐射跃迁，我们证明了该概念的范围。这是通过采用我们的从头开始的威格纳分配方法实现的。

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