论文标题
通过高阶谐波捕获分子中圆锥形交集周围的几何相效应
Catching the geometric phase effect around conical intersection in molecules by high order harmonic spectroscopy
论文作者
论文摘要
在大多数多原子分子的光诱导过程中，避免越过或圆锥形交集周围的非绝热动力学起着至关重要的作用。目前的工作表明，圆锥形交集中的拓扑阶段使泵探针高阶谐波光谱法的行为与避免越过的情况不同。当系统越过避免交叉时，建立的连贯性将导致光谱的振荡行为，而在圆锥形相交的情况下，几何相侵蚀了这些振荡。此外，动态蓝光和时间分辨光谱的分裂允许使用子段分辨率捕获快照动力学。
Nonadiabatic dynamics around an avoid crossing or a conical intersection play a crucial role in the photoinduced processes of most polyatomic molecules. The present work shows that the topological phase in conical intersection makes the behavior of pump-probe high-order harmonic spectroscopy different from the case of avoid crossing. The coherence built up when the system crosses the avoid crossing will lead to the oscillatory behavior of the spectrum, while the geometric phase erodes these oscillations in the case of conical intersection. Additionally, the dynamical blueshift and the splitting of time-resolved spectrum allow capturing the snapshot dynamics with sub-femtosecond resolution.
