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首页> 外文期刊>The Journal of Chemical Physics >Theory of ultrafast nonresonant multiphoton transitions in polyatomic molecules: Basics and application to optimal control theory
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Theory of ultrafast nonresonant multiphoton transitions in polyatomic molecules: Basics and application to optimal control theory

机译：多原子分子中超快非共振多光子跃迁的理论：基础及其在最优控制理论中的应用

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摘要

A systematic approach is presented to describe nonresonant multiphoton transitions, i.e., transitions between two electronic states without the presence of additional intermediate states resonant with the single-photon energy. The method is well suited to describe femtosecond spectroscopic . experiments and, in particular, attempts to achieve laser pulse control of molecular dynamics. The obtained effective time-dependent Schrodinger equation includes effective couplings to the radiation field which combine powers of the field strength and effective transition dipole operators between the initial and final states. To arrive at time-local equations our derivation combines the well-known rotating wave approximation with the approximation of slowly varying amplitudes. Under these terms, the optimal control formalism can be readily extended to also account for nonresonant multiphoton events. Exemplary, nonresonant two- and three-photon processes, similar to those occurring in the recent femtosecond pulse-shaping experiments on CpMn(CO)3, are treated using related ab initio potential energy surfaces.
机译：提出了一种系统的方法来描述非共振多光子跃迁，即两个电子状态之间的跃迁，而没有其他与单光子能量共振的中间态的存在。该方法非常适合描述飞秒光谱。实验，尤其是尝试实现分子动力学的激光脉冲控制。所获得的有效的随时间变化的薛定inger方程包括与辐射场的有效耦合，该耦合将场强的功率与初始状态和最终状态之间的有效跃迁偶极算子结合在一起。为了得出时间局部方程，我们的推导将众所周知的旋转波近似与缓慢变化的振幅近似结合在一起。在这些术语下，可以轻松扩展最佳控制形式，以解决非共振多光子事件。示例性的非共振两光子和三光子过程，类似于最近在CpMn（CO）3上飞秒脉冲成形实验中发生的过程，使用相关的从头算势能面进行处理。

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