论文标题
飞秒的光电子圆形化学反应的二分法
Femtosecond photoelectron circular dichroism of chemical reactions
论文作者
论文摘要
了解分子反应途径的手性对于广泛的基本科学和应用科学至关重要。但是,当前在化学反应时间尺度上探测手性的能力仍然非常有限。在这里,我们展示了来自桌面源的时间分辨光电子圆形二色性(TRPECD),该光电二色性(TRPECD)具有超短圆极化的真空粉丝(VUV)脉冲。我们通过解决来自两个手性分子的原子碘的光解离时的手性变化来证明VUV-TRPECD的能力。我们确定了TRPECD的几个一般关键特征,其中包括沿完整的光化学反应路径探测动力学手性的能力,对不断发展的散射潜力的局部手性的敏感性以及电子散射在离解相处的影响。通过与分子光电离计算中瞬时pecd的新型高级AB-INITIO计算相比,我们的结果可以解释。我们的实验和理论技术定义了一种对女性病毒的一般方法。
Understanding the chirality of molecular reaction pathways is essential for a broad range of fundamental and applied sciences. However, the current ability to probe chirality on the time scale of chemical reactions remains very limited. Here, we demonstrate time-resolved photoelectron circular dichroism (TRPECD) with ultrashort circularly polarized vacuum-ultraviolet (VUV) pulses from a table-top source. We demonstrate the capabilities of VUV-TRPECD by resolving the chirality changes in time during the photodissociation of atomic iodine from two chiral molecules. We identify several general key features of TRPECD, which include the ability to probe dynamical chirality along the complete photochemical reaction path, the sensitivity to the local chirality of the evolving scattering potential, and the influence of electron scattering off dissociating photofragments. Our results are interpreted by comparison with novel high-level ab-initio calculations of transient PECDs from molecular photoionization calculations. Our experimental and theoretical techniques define a general approach to femtochirality.