Striking Generic Impact of Light-Induced Non-Adiabaticity in Polyatomic Molecules.,The Journal of Physical Chemistry Letters

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Striking Generic Impact of Light-Induced Non-Adiabaticity in Polyatomic Molecules.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-06-12 , DOI: 10.1021/acs.jpclett.0c01574
Csaba Fábri _{1,

2} , Benjamin Lasorne ₃ , Gábor J Halász ₄ , Lorenz S Cederbaum ₅ , Ágnes Vibók _{6,

7}

Affiliation

Non-adiabaticity, i.e., the effect of mixing electronic states by nuclear motion, is a central phenomenon in molecular science. The strongest nonadiabatic effects arise due to the presence of conical intersections of electronic energy surfaces. These intersections are abundant in polyatomic molecules. Laser light can induce in a controlled manner new conical intersections, called light-induced conical intersections, which lead to strong nonadiabatic effects similar to those of the natural conical intersections. These effects are, however, controllable and may even compete with those of the natural intersections. In this work we show that the standard low-energy vibrational spectrum of the electronic ground state can change dramatically by inducing non-adiabaticity via a light-induced conical intersection. This generic effect is demonstrated for an explicit example by full-dimensional high-level quantum calculations using a pump-probe scheme with a moderate-intensity pump laser and a weak probe laser.

中文翻译：

在多原子分子中光诱导的非绝热的惊人通用影响。

非绝热性，即通过核运动混合电子态的效应，是分子科学中的中心现象。最强的非绝热效应是由于电子能表面的圆锥形相交的存在而产生的。这些交点富含多原子分子。激光可以以受控的方式诱发新的圆锥形交叉点，称为光诱导圆锥形交叉点，从而产生类似于自然圆锥形交叉点的强非绝热效应。但是，这些效果是可控的，甚至可以与自然交叉路口的效果相抗衡。在这项工作中，我们表明，电子基态的标准低能量振动谱可以通过通过光诱导的圆锥形交点引起非绝热性而发生巨大变化。

更新日期：2020-07-02

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