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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Dynamics of nonadiabatic chemical reactions
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Dynamics of nonadiabatic chemical reactions

机译：非绝热化学反应的动力学

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摘要

New methods are proposed to treat nonadiabatic chemical dynamics in realistic large molecular systems by using the Zhu-Nakamura (ZN) theory of curve-crossing problems. They include the incorporation of the ZN formulas into the Herman-Kluk type semiclassical wave packet propagation method and the trajectory surface hopping (TSH) method, formulation of the nonadiabatic transition state theory, and its application to the electron transfer problem. Because the nonadiabtic coupling is a vector in multidimensional space, the one-dimensional ZN theory works all right. Even the classically forbidden transitions can be correctly treated by the ZN formulas. In the case of electron transfer, a new formula that can improve the celebrated Marcus theory in the case of normal regime is obtained so that it can work nicely in the intermediate and strong electronic coupling regimes. All these formulations mentioned above are demonstrated to work well in comparison with the exact quantum mechanical numerical solutions and are expected to be applicable to large systems that cannot be treated quantum mechanically numerically exactly. To take into account another quantum mechanical effect, namely, the tunneling effect, an efficient method to detect caustics from which tunneling trajectories emanate is proposed. All the works reported here are the results of recent activities carried out in the author's research group. Finally, the whole set of ZN formulas is presented in Appendix.
机译：提出了一种新的方法，通过使用朱-中村（ZN）曲线交叉问题理论来处理现实的大分子系统中的非绝热化学动力学。它们包括将ZN公式合并到Herman-Kluk型半经典波包传播方法和轨迹表面跳变（TSH）方法中，拟定非绝热过渡态理论，并将其应用于电子转移问题。由于非绝热耦合是多维空间中的向量，因此一维ZN理论行之有效。 ZN公式甚至可以正确处理经典禁止的跃迁。在电子转移的情况下，获得了一个可以在正常状态下改进著名的马库斯理论的新公式，从而可以在中等和强电子耦合状态下很好地工作。与精确的量子力学数值解相比，上面提到的所有这些公式都被证明可以很好地工作，并且有望适用于无法对量子力学进行精确数值处理的大型系统。考虑到另一种量子力学效应，即隧道效应，提出了一种有效的方法来检测从中产生隧道轨迹的焦散。这里报告的所有作品都是作者研究小组近期活动的结果。最后，附录中介绍了整个ZN公式。

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