Kutscher Eric, Artemyev Anton N, Demekhin Philipp V
Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Str. 40, 34132 Kassel, Germany.
Struct Dyn. 2025 Apr 18;12(2):024102. doi: 10.1063/4.0000300. eCollection 2025 Mar.
Photoelectron circular dichroism (PECD) in the ionization of chiral molecules by circularly polarized radiation is a well-established tool for chiral recognition in the gas phase. The effect consists in a forward-backward asymmetry in angular emission distributions of photoelectrons with respect to the light propagation direction, which survives averaging over molecular orientations. Its magnitude is governed by the ability of the outgoing photoelectron to probe an asymmetry of the ionic potential by multiple scattering effects, and it can be significantly enhanced by fixing molecular orientation in space. Even achiral fixed-in-space molecules can exhibit such a forward-backward asymmetry in the photoemission. In the present work, we establish a qualitative correspondence between the PECD in one-photon ionization of fixed-in-space molecules and a degree of the asymmetry of their ionic potential. For this purpose, we introduce an enantiosensitive dichroic characteristic of the ionic potential, which describes a physical mechanism behind the forward-backward asymmetry in the photoemission from fixed-in-space molecules ionized by circularly polarized light. This characteristic, as a function of molecular orientation angles, can be compared to the respective PECD landscape. The present findings are exemplified by several applications to achiral and chiral species.
圆偏振辐射对手性分子进行电离时产生的光电子圆二色性(PECD)是气相中用于手性识别的一种成熟工具。这种效应表现为光电子角发射分布相对于光传播方向的前后不对称性,这种不对称性在分子取向平均化后依然存在。其大小取决于出射光电子通过多重散射效应探测离子势不对称性的能力,并且通过固定分子在空间中的取向可以显著增强这种效应。即使是空间固定的非手性分子在光发射中也能表现出这种前后不对称性。在本工作中,我们建立了空间固定分子单光子电离中的PECD与其离子势不对称程度之间的定性对应关系。为此,我们引入了离子势的对映体敏感二色性特征,它描述了由圆偏振光电离的空间固定分子光发射中前后不对称性背后的物理机制。作为分子取向角的函数,这一特征可以与相应的PECD图谱进行比较。本文通过对几种非手性和手性物种的应用举例说明了这些发现。