Chang Bo Y, Shin Seokmin, Engel Volker, Sola Ignacio R
School of Chemistry (BK21), Seoul National University , Seoul 08826, Republic of Korea.
Institut für Physikalische und Theoretische Chemie, Universität Würzburg , 97074 Würzburg, Germany.
J Phys Chem A. 2017 Nov 2;121(43):8280-8287. doi: 10.1021/acs.jpca.7b08767. Epub 2017 Oct 19.
We study laser-driven isomerization reactions through an excited electronic state using the recently developed Geometrical Optimization procedure. Our goal is to analyze whether an initial wave packet in the ground state, with optimized amplitudes and phases, can be used to enhance the yield of the reaction at faster rates, driven by a single picosecond pulse or a pair of femtosecond pulses resonant with the electronic transition. We show that the symmetry of the system imposes limitations in the optimization procedure, such that the method rediscovers the pump-dump mechanism.
我们使用最近开发的几何优化程序研究通过激发电子态的激光驱动异构化反应。我们的目标是分析具有优化幅度和相位的基态初始波包是否可用于在由与电子跃迁共振的单个皮秒脉冲或一对飞秒脉冲驱动时以更快的速率提高反应产率。我们表明系统的对称性在优化过程中施加了限制，使得该方法重新发现了泵浦-卸载机制。
