Angular Distribution of ICD Electrons in Rare Gas Dimers

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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.