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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Laser-polarization effects on coherent vibronic excitation of molecules with quasi-degenerate electronic states
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Laser-polarization effects on coherent vibronic excitation of molecules with quasi-degenerate electronic states

机译：激光极化对准简并电子态分子的相干振动激发的影响

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摘要

The laser-polarization effects on nonadiabatically coupled π-electron rotation (ring current) and molecular vibration have been theoretically analyzed for aromatic molecules with quasi-degenerate excited states irradiated by an ultrashort laser pulse of arbitrary polarization. We first derived general formulations of the coherent electronic wave packet and expectation value of electronic angular momentum within a frozen-nuclei model. The relative quantum phase of the superposed quasi-degenerate states, which determines the oscillating behavior of angular momentum, can be manipulated by the ellipticity and orientation of the incident laser. Nuclear wave packet simulations with a model molecule confirmed the controllability of π-electron rotation, although the angular momentum is gradually reduced by nonadiabatic couplings. The amplitude of molecular vibration depends prominently on the orientation of linear polarization vectors rather than the helicity of circular polarization. The characteristic feature in vibrational amplitudes is attributed to the interference in nonadiabatic transition governed by the relative quantum phase between nuclear wave packets. This offers a new strategy for laser control of molecular vibrations through the wave packet interference in nonadiabatic transition.
机译：理论上已经分析了由任意极化的超短激光脉冲辐照的准简并激发态的芳族分子对非绝热耦合π电子旋转（环电流）和分子振动的激光偏振效应。我们首先推导了相干电子波包的一般公式以及冻结核模型中电子角动量的期望值。叠加准退化态的相对量子相位决定了角动量的振荡行为，可以通过入射激光的椭圆率和取向对其进行控制。尽管通过非绝热耦合逐渐减小了角动量，但是使用模型分子进行的核波包模拟证实了π电子旋转的可控性。分子振动的幅度主要取决于线性极化矢量的方向，而不是圆形极化的螺旋度。振动幅度的特征归因于非绝热跃迁中的干扰，该干扰由核波包之间的相对量子相位决定。这为非绝热跃迁中的波包干涉提供了一种激光控制分子振动的新策略。

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