Angular Distribution of ICD Electrons in Rare Gas Dimers

传统上，原子间库仑衰变（ICD）的实验依赖于探测由库仑爆炸产生的带电粒子（电子和离子碎片）。对这些粒子的同步检测提供了直接获取ICD期间发射角分布的相关信息。发射粒子的角分布对出射部分电子连续波的相位及其干涉非常敏感，为光致弛豫动力学提供了重要的补充信息，这些信息在总光谱中可能无法获得。目前，对ICD电子的角分布所知甚少。因此，在这个DFG研究单元FOR-1789的第二阶段，两个实验项目提出了在角分辨模式下对ICD进行全面研究。本建议的主要目的是为计划的ICD角度分辨实验提供准确可靠的理论解释。该小组的首席研究员已经开发了一种强大的工具，用于角度分辨电离分子的研究，这被称为单中心（SC）方法。固定式SC法最早用于研究双原子分子。最近，它已成功地扩展到多原子分子。目前，我们正在实施SC方法的时间依赖公式来研究任意辐射脉冲下多原子分子的角分辨多光子电离。在本项目中，SC方法将应用于稀有气体二聚体在内价电离或共振激发后发射的ICD电子的实验室和分子框架角分布的理论研究。

Traditionally, experiments on the interatomic Coulombic decay (ICD) relay on the detection of charged particles (electrons and ionic fragments) produced by Coulomb explosions. Coincident detections of those particles provide a direct access to the relevant information on the emission angular distributions during ICD. Being very sensitive to the phases of the outgoing partial electron continuum waves and to their interferences, angular distributions of emitted particles afford important complementary information on the photoinduced relaxation dynamics which may not be accessible in the total spectra. At present, only little is known about the angular distribution of ICD electrons. Therefore, two experimental projects have proposed a comprehensive investigation of ICD in the angle-resolved mode during the second period of this DFG research unit FOR-1789. The main aim of the present proposal is to provide accurate and reliable theoretical interpretation for planned angle-resolved experiments on ICD. The group of the principal investigator has developed a powerful tool for angle-resolved ionization studies of molecules, which is known as the Single Center (SC) method. The stationary SC method was first developed to study diatomic molecules. Recently, it has been successfully extended to polyatomic molecules. Currently, we are implementing the time-dependent formulation of the SC method to study angle-resolved multiphoton ionization of polyatomic molecules by arbitrary radiation pulses. In the present project, the SC method will be applied to the theoretical investigation of the laboratory and molecular frame angular distributions of the ICD electrons emitted after inner-valence ionization or resonant excitation of rare gas dimers.