Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics

• DOI: 10.1038/ncomms7166
• Publication Date: 2015-01-21T14:32:08Z
• Authors: R. Guillemin; P. Decleva; M. Stener; C. Bomme; T. Marin; L. Journel; T. Marchenko; R. K. Kushawaha; K. Jänkälä; N. Trcera; K. P. Bowen; D. W. Lindle; M. N. Piancastelli; M. Simon
• Keywords: Dynamics

Electronic core levels in molecules are highly localized around one atomic site. However, single-photon ionization of symmetric molecules, the question core-hole localization versus delocalization over two equivalent atoms has long been debated as answer lies at heart quantum mechanics. Here, using a joint experimental and theoretical study core-ionized carbon disulfide (CS2), we demonstrate that it is possible to experimentally select distinct molecular-fragmentation pathways which hole can be considered either on sulfur atom or delocalized between indistinguishable atoms. This feat accomplished by measuring photoelectron angular distributions within frame molecule, directly probing entanglement disentanglement function how molecule dissociates. Molecular single site, but for atoms, photoionised core-holes seen delocalized. Using prototypical system, CS2, Guillemin et al. show these states disentangled fragmentation dynamics.