Molecular-frame photoelectron angular distributions during double core-hole generation in and molecules

Abstract

Angular distributions of photoelectrons emitted upon double core-hole (DCH) generation in nitrogen and oxygen molecules are studied theoretically in the frame of a molecular reference. The respective electronic structure calculations are performed by the single center method for photoelectron kinetic energies up to 40 eV in the relaxed-core Hartree–Fock approximation. The molecular frame photoelectron angular distributions are computed for single-site and two-site DCH creation processes and further analyzed for different orientations of the molecular axis with respect to the electric field vector of linearly polarized incident light and for localized or delocalized emitting atomic site scenarios. The present theoretical results provide reliable predictions for future experiments with high-repetition free-electron lasers.