Baer Michael
The Fritz Haber Research Center for Molecular Dynamics, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
J Phys Chem A. 2006 May 25;110(20):6571-8. doi: 10.1021/jp0617266.
A few years ago, we developed an approach to treat molecular systems exposed to an external, intense, time-dependent field (J. Phys. Chem. A 2003, 107, 4724; J. Chem. Phys. 2003, 119, 6998). Within this study, we encountered two novel concepts: the dressed (namely, field affected) time-dependent nonadiabatic coupling term and the space-time contours. In the present article, we analyze the newly introduced nonadiabatic coupling term and discuss its importance for dynamical studies. We also refer to the just mentioned space-time contour and present the more efficient contour for realistic situations. The scope of the above-mentioned articles is extended with the aim of defining quasi-adiabatic states for such situations. Strictly speaking, molecular systems exposed to intense, fast oscillating fields are not expected to form adiabatic states. Still we consider such a situation and end up with three possibilities for quasi-adiabatical time-dependent states eventually to be used within the Born-Oppenheimer approximation.
几年前，我们开发了一种方法来处理暴露于外部强时变场的分子系统（《物理化学杂志A》2003年，第107卷，4724页；《化学物理杂志》2003年，第119卷，6998页）。在这项研究中，我们遇到了两个新概念：修饰（即场影响）的含时非绝热耦合项和时空轮廓。在本文中，我们分析新引入的非绝热耦合项，并讨论其在动力学研究中的重要性。我们还提及刚刚提到的时空轮廓，并给出适用于实际情况的更有效轮廓。上述文章的范围得以扩展，目的是为这种情况定义准绝热态。严格来说，暴露于强快速振荡场的分子系统预计不会形成绝热态。尽管如此，我们仍考虑这种情况，并最终得到三种准绝热含时状态的可能性，最终将在玻恩-奥本海默近似中使用。
