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首页> 外文期刊>Physical Review, A. Atomic, molecular, and optical physics >Unified treatment of field-induced and intrinsic nonadiabatic transitions with a generalized Floquet Hamiltonian method
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Unified treatment of field-induced and intrinsic nonadiabatic transitions with a generalized Floquet Hamiltonian method

机译：广义Floquet哈密顿量方法统一处理场致和固有非绝热跃迁

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摘要

We propose a generalized Floquet Hamiltonian method that is applicable to laser-induced molecular dynamics including nonperiodicity arising from time dependence of laser parameters and nuclear kinematic effects. Effects from these two types of nonperiodicity are formulated as generalized nonadiabatic transitions and treated in a unified manner. In this unified treatment, the field-induced dynamics of a molecule is mapped onto an effective nonadiabatic dynamics. An analog of the gradient approximation to the field-free nonadiabatic dynamics thus naturally follows and the relevant validity conditions are also formulated. Full-quantum-type numerical implementation of this method is applied first to the field-induced dynamics of H_2~+/D_2~+ within a two-state model and second to that of LiF based on the ab initio potential-energy surfaces.With the H_2~+/D_2~+ calculations, we confirm the validity of our formalism by reproducing the previously reported dissociation probabilities, which represent the phenomena of bond softening and bond hardening, including the "inverse bond-hardening effect" that has been identified in the present study. In the calculations of LiF, we realize full generalized ab initio Floquet analysis including the intrinsic nuclear derivative coupling. The effects of nuclear derivative couplings are assessed by directly comparing the calculations with and without the couplings. The present method, giving a simple and clear view of field-induced and kinematically induced nonadiabatic transitions, appears to be promising for the study of ab initio laser-induced dynamics of a system with nuclear derivative couplings.
机译：我们提出了一种通用的Floquet Hamiltonian方法，该方法适用于激光诱导的分子动力学，包括由激光参数的时间依赖性和核运动学效应引起的非周期性。这两种非周期性的影响被表述为广义的非绝热转变，并以统一的方式进行处理。在这种统一的处理中，分子的场诱导动力学被映射到有效的非绝热动力学上。因此，自然会遵循无场非绝热动力学的梯度近似模拟，并制定了相关的有效性条件。该方法的全量子型数值实现首先应用于两态模型中H_2〜+ / D_2〜+的场致动力学，其次基于从头算势能面应用于LiF的动力学。在H_2〜+ / D_2〜+计算中，我们通过重现先前报道的解离概率来证实我们形式主义的有效性，该解离概率代表了键软化和键硬化的现象，包括已在本文中确定的“逆键硬化效应”。本研究。在LiF的计算中，我们实现了完全的从头算起的Floquet分析，包括本征核导数耦合。通过直接比较带和不带耦合的计算，可以评估核导数耦合的影响。本方法给出了场致和运动学引起的非绝热跃迁的简单清晰视图，对于研究具有核导数耦合的系统从头开始激光诱导的动力学似乎很有希望。

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