论文标题
几何阶段在圆锥交叉处电子相干形成中的作用
The role of geometric phase in the formation of electronic coherences at conical intersections
论文作者
论文摘要
直接观察圆锥形交集的非绝热动力学是分子物理学的长期目标。已经提出了新型的时间分辨光谱法对激发态波袋通过锥形交叉区域引起的电子相干敏感。在这里，我们证明了几何阶段效应及其表现形式对于正确描述可能发展或可能不会发展的瞬态电子相干至关重要。对于不同对称性的电子状态，电子相干被几何相抑制。相反，对于相同对称性的状态，可能具有明显的电子相干，但它们的幅度取决于锥形交叉路口方法的地形和方向。这些一般结果对圆锥形交叉处的所有电子相干研究都有后果。
The direct observation of non-adiabatic dynamics at conical intersections is a long-standing goal of molecular physics. Novel time-resolved spectroscopies have been proposed which are sensitive to electronic coherences induced by the passage of an excited state wavepacket through a region of conical intersection. Here we demonstrate that inclusion of the geometric phase effect, and its manifestations, is essential for the correct description of the transient electronic coherences that may or may not develop. For electronic states of different symmetry, electronic coherences are suppressed by the geometric phase. Conversely, for states of the same symmetry, appreciable electronic coherences are possible, but their magnitude depends on both the topography of and direction of approach to the conical intersection. These general results have consequences for all studies of electronic coherences at conical intersections.
