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

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 and M. Simon
Additional contact information
R. Guillemin: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
P. Decleva: Università di Trieste
M. Stener: Università di Trieste
C. Bomme: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
T. Marin: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
L. Journel: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
T. Marchenko: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
R. K. Kushawaha: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
K. Jänkälä: University of Oulu
N. Trcera: Synchrotron SOLEIL, l'Orme des Merisiers, Saint-Aubin
K. P. Bowen: University of Nevada
D. W. Lindle: University of Nevada
M. N. Piancastelli: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement
M. Simon: Sorbonne Universités, UPMC Univ Paris 06, UMR 7614, Laboratoire de Chimie Physique Matière et Rayonnement

Nature Communications, 2015, vol. 6, issue 1, 1-6

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

Date: 2015
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DOI: 10.1038/ncomms7166

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