论文标题
通过时间分辨X射线衍射探测分子结构对超快电荷迁移的影响
Probing the Effect of Molecular Structure Saddling on Ultrafast Charge Migration via Time-Resolved X-ray Diffraction
论文作者
论文摘要
金属 - 摩尔斯是具有许多实际应用的大环有机分子。尤其是，铜矿表现出有趣的鞍形几何形状，多年来，它引起了理论家和实验家的重大关注。目前的工作致力于了解铜矿中结构鞍座对通过成像超快相干电子动力学的潜在探针信号的影响。线性极化脉冲用于触发电子动力学，并使用时间分辨的X射线衍射来对触发的动力学进行成像。发现在超快电荷迁移期间，时间分辨衍射信号和电子通量密度的对称性降低是铜孔洛尔中鞍座的标志。此外，对电子通量密度的分析表明，对角氮原子通过中央铜原子介导它们之间的相干电荷迁移。通量密度和衍射信号的相关性表明电荷迁移的特征是在时间分辨衍射信号中编码的。在其基态中，比较了非饰面平面铜卟啉和鞍形非平面铜孔洛的静态衍射信号的比较。
Metal-corroles are macrocycle organic molecules with numerous practical applications. In particular, copper corroles exhibit an interesting saddled geometry, which has attracted significant attention from theoreticians and experimentalists over the years. The present work is dedicated to understand the effect of structural saddling in a copper corrole on potential probe signals via imaging ultrafast coherent electron dynamics. A linearly polarized pulse is used to trigger the electron dynamics and time-resolved x-ray diffraction is employed to image the triggered dynamics. It is found that the symmetry reduction in the time-resolved diffraction signals and electronic flux densities is a signature of the saddling in a copper corrole during ultrafast charge migration. Moreover, analysis of the electronic flux density reveals that the diagonal nitrogen atoms mediate coherent charge migration between them via a central copper atom. Correlation of the flux densities and the diffraction signals indicates that the signature of the charge migration is encoded in time-resolved diffraction signals. A comparison of the static diffraction signals of nonsaddled planar copper porphyrin and saddled nonplanar copper corrole in their ground states is made.
