Selecting core-hole localization or delocalization in CS2 by photofragmentation dynamics
Open accessAbstract
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. Molecular core levels are localized around a single atomic site, but for indistinguishable atoms, photoionised core-holes can either be seen as localized or delocalized. Using a prototypical symmetric system, CS2, Guillemin et al. show that these states can be disentangled by fragmentation dynamics.
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
Vector momenta of ions and photoelectrons recorded in a multicoincidence COLTRIMS setup reveal fragmentation dependence of the localization/delocalization of a deep inner-shell hole in a symmetric molecule.
“The vector momenta of the ions and the photoelectrons have been recorded in a multicoincidence COLTRIMS setup revealing interesting features such as fragmentation dependence of the localization/ delocalization of a deep inner-shell hole in a symmetric molecule [27].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [27]
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
Cites
Henke, B. L., Gullikson, E. M., & Davis, J. C. (1993) · Atomic Data and Nuclear Data Tables · doi:10.1006/adnd.1993.1013 · Cited by 6,313 · see citing works
Die gegenw�rtige Situation in der Quantenmechanik
Schr�dinger, E. (1935) · Die Naturwissenschaften · doi:10.1007/bf01491891 · Cited by 3,392 · see citing works
WIDTHS OF THE ATOMIC K–N7 LEVELS
CAMPBELL, J. L., & Papp, T. (2001) · Atomic Data and Nuclear Data Tables · doi:10.1006/adnd.2000.0848 · Cited by 764 · see citing works
Applications ofB-splines in atomic and molecular physics
Bachau, H., Cormier, E., Decleva, P., Hansen, J. E., & Martı́n, F. (2001) · Reports on Progress in Physics · doi:10.1088/0034-4885/64/12/205 · Cited by 710 · see citing works
Self-citationAngular Distributions of 1sσ Photoelectrons from Fixed-in-Space N2 Molecules
Shigemasa, E., Adachi, J., Oura, M., et al. (1995) · Physical Review Letters · doi:10.1103/physrevlett.74.359 · Cited by 215 · see citing works
Single Photon-Induced Symmetry Breaking of H 2 Dissociation
Martı́n, F., Fernández, J., Havermeier, T., et al. (2007) · Science · doi:10.1126/science.1136598 · Cited by 199 · see citing works
Ultrafast Probing of Core Hole Localization in N 2
Schöffler, M. S., Titze, J., Petridis, N., Jahnke, T., Cole, K., Schmidt, L. P. H., Czasch, A., Akoury, D., Jagutzki, O., Williams, J., et al. (2008) · Science · doi:10.1126/science.1154989 · Cited by 195 · see citing works
Neumann, N., Hant, D., Schmidt, L. P. H., et al. (2010) · Physical Review Letters · doi:10.1103/physrevlett.104.103201 · Cited by 183 · see citing works
Decay of τ Mesons of Known Charge
Dalitz, R. H. (1954) · Physical Review · doi:10.1103/physrev.94.1046 · Cited by 175 · see citing works
Isotope-induced partial localization of core electrons in the homonuclear molecule N2
Rolles, D., Braune, M., Cvejanović, S., Geßner, O., Hentges, R., Korica, S., Langer, B., Lischke, T., Prümper, G., Reinköster, A., et al. (2005) · Nature · doi:10.1038/nature04040 · Cited by 167 · see citing works
Convergence of the multicenter B-spline DFT approach for the continuum
Toffoli, D., Stener, M., Fronzoni, G., et al. (2002) · Chemical Physics · doi:10.1016/s0301-0104(01)00549-3 · Cited by 155 · see citing works
Self-citationBjörneholm, O., Bässler, M., Ausmees, A., Hjelte, I., Feifel, R., Wang, H., Miron, C., Piancastelli, M. N., Svensson, S., Sorensen, S. L., et al. (2000) · Physical Review Letters · doi:10.1103/physrevlett.84.2826 · Cited by 127 · see citing works
Self-citationPhotoelectron spectroscopic studies of polyatomic molecules. I. Theory
Chandra, N. (1987) · Journal of Physics B Atomic and Molecular Physics · doi:10.1088/0022-3700/20/14/013 · Cited by 125 · see citing works
Localization and loss of coherence in molecular double-slit experiments
Zimmermann, B., Rolles, D., Langer, B., Hentges, R., Braune, M., Cvejanović, S., Geßner, O., Heiser, F., Korica, S., Lischke, T., et al. (2008) · Nature Physics · doi:10.1038/nphys993 · Cited by 122 · see citing works
Stener, M., Fronzoni, G., & Decleva, P. (2005) · The Journal of Chemical Physics · doi:10.1063/1.1937367 · Cited by 101 · see citing works
Self-citationCarlson, T. A., & Krause, M. O. (1972) · The Journal of Chemical Physics · doi:10.1063/1.1677680 · Cited by 80 · see citing works
Hishikawa, A., Hasegawa, H., & Yamanouchi, K. (2002) · Chemical Physics Letters · doi:10.1016/s0009-2614(02)00880-1 · Cited by 76 · see citing works
Localization of inner-shell photoelectron emission and interatomic Coulombic decay in Ne 2
Kreidi, K., Jahnke, T., Weber, T., et al. (2008) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/41/10/101002 · Cited by 51 · see citing works
Adachi, J., Hosaka, K., Teramoto, T., et al. (2007) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/40/20/f01 · Cited by 40 · see citing works
Decay of and OCS after sulphur 1s photoexcitation: II. Dissociation channels and kinematics
Ankerhold, U., Esser, B., & Busch, F. (1997) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/30/5/015 · Cited by 35 · see citing works
Laksman, J., Månsson, E. P., Grunewald, C., et al. (2012) · The Journal of Chemical Physics · doi:10.1063/1.3692293 · Cited by 29 · see citing works
Nenner, I., Reynaud, C., Schmelz, H. C., et al. (1996) · Zeitschrift für Physikalische Chemie · doi:10.1524/zpch.1996.195.part_1_2.043 · Cited by 29 · see citing works
Miyabe, S., McCurdy, C. W., Orel, A. E., et al. (2009) · Physical Review A · doi:10.1103/physreva.79.053401 · Cited by 27 · see citing works
Double momentum spectrometer for ion-electron vector correlations in dissociative photoionization
Bomme, C., Guillemin, R., Marin, T., et al. (2013) · Review of Scientific Instruments · doi:10.1063/1.4824194 · Cited by 24 · see citing works
Self-citationComplex decay patterns in atomic core photoionization disentangled by ion-recoil measurements
Guillemin, R., Bomme, C., Marin, T., et al. (2011) · Physical Review A · doi:10.1103/physreva.84.063425 · Cited by 24 · see citing works
Self-citationPhotoelectron and Auger-electron angular distributions of fixed-in-space CO2
Sturm, F. P., Schöffler, M. S., Lee, S. M., et al. (2009) · Physical Review A · doi:10.1103/physreva.80.032506 · Cited by 23 · see citing works
Multicoincidence mass spectrometry of core excited molecules
Simon, M., Lavollée, M., Meyer, M., et al. (1996) · Journal of Electron Spectroscopy and Related Phenomena · doi:10.1016/0368-2048(96)02881-2 · Cited by 22 · see citing works
Self-citationKrishnamurthi, V., Krishamurthy, M., Marathe, V. R., et al. (1992) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/25/23/018 · Cited by 20 · see citing works
Alkemper, U., Hornig, R., & Busch, F. (1996) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/29/1/009 · Cited by 17 · see citing works
Stener, M., Decleva, P., Mizuno, T., et al. (2014) · The Journal of Chemical Physics · doi:10.1063/1.4862267 · Cited by 13 · see citing works
Self-citationCorrelation and coherence phenomena studied by photoelectron spectroscopy
Becker, U., & Langer, B. (2008) · Nuclear Instruments and Methods in Physics Research Section A Accelerators Spectrometers Detectors and Associated Equipment · doi:10.1016/j.nima.2008.12.105 · Cited by 12 · see citing works
Molecular-frame photoelectron angular distribution imaging studies of OCS S1s photoionization
Bomme, C., Guillemin, R., Marin, T., et al. (2012) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/45/19/194005 · Cited by 12 · see citing works
Self-citationLucchese, R. R., Fukuzawa, H., Liu, X. J., et al. (2012) · Journal of Physics B Atomic Molecular and Optical Physics · doi:10.1088/0953-4075/45/19/194014 · Cited by 10 · see citing works
Doppler effect in fragment autoionization following core-to-valence excitation in O2
Guillemin, R., Simon, M., & Shigemasa, E. (2010) · Physical Review A · doi:10.1103/physreva.82.051401 · Cited by 10 · see citing works
Self-citationCore localization and σ∗ delocalization in the O 1s core-excited sulfur dioxide molecule
Lindgren, A., Kosugi, N., Gisselbrecht, M., et al. (2008) · The Journal of Chemical Physics · doi:10.1063/1.2844808 · Cited by 6 · see citing works
Recoil frame photoemission in inner-shell photoionization of small polyatomic molecules
Dowek, D., Haouas, A., Guillemin, R., et al. (2009) · The European Physical Journal Special Topics · doi:10.1140/epjst/e2009-00977-8 · Cited by 5 · see citing works
Self-citationTsuru, S., Kazama, M., Fujikawa, T., et al. (2014) · Chemical Physics Letters · doi:10.1016/j.cplett.2014.05.086 · Cited by 5 · see citing works
Localization of inner shell photoelectron emission and interatomic Coulombic decay in neon dimers
Kreidi, K., Jahnke, T., Weber, T. H., et al. (2010) · Journal of Physics Conference Series · doi:10.1088/1742-6596/212/1/012007 · Cited by 3 · see citing works
Flagged first, then by citations
Cited by
Sorted by citations
Roadmap of ultrafast x-ray atomic and molecular physics
Young, L., Ueda, K., Gühr, M., Bucksbaum, P. H., Simon, M., Mukamel, S., Rohringer, N., Prince, K. C., Masciovecchio, C., Meyer, M., et al. (2018) · Journal of Physics B: Atomic, Molecular and Optical Physics · doi:10.1088/1361-6455/aa9735 · Cited by 337 · see citing works
Self-citationHetero-site-specific X-ray pump-probe spectroscopy for femtosecond intramolecular dynamics
Picón, A., Lehmann, C. S., Bostedt, C., Rudenko, A., Marinelli, A., Osipov, T., Rolles, D., Berrah, N., Bomme, C., Bucher, M., et al. (2016) · Nature Communications · doi:10.1038/ncomms11652 · Cited by 88 · see citing works
Self-citationPiancastelli, M. N., Guillemin, R., Marchenko, T., Journel, L., Travnikova, O., Marin, T., Goldsztejn, G., de Miranda, B. C., Ismail, I., & Simon, M. (2017) · Journal of Physics B: Atomic, Molecular and Optical Physics · doi:10.1088/1361-6455/aa52e8 · Cited by 11 · see citing works
Self-citation
- Authors
- Guillemin, R., Decleva, P., Stener, M., Bomme, C., Marin, T., Journel, L., Marchenko, T., Kushawaha, R. K., Jänkälä, K., Trcera, N., Bowen, K. P., Lindle, D. W., Piancastelli, M. N., & Simon, M.
- Affiliations
- Centre National de la Recherche Scientifique (FR)
- University of Trieste (IT)
- University of Oulu (FI)
- Synchrotron SOLEIL (FR)
- University of Nevada, Las Vegas (US)
- Uppsala University (SE)
- Corresponding author
- Guillemin, R.
- ORCID
- Venue
- Nature Communications
- Published
- 2015-01-21
- Volume
- 6
- Issue
- 1
- Pages
- 6166-6166
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W2070304978
- Cited by
- 78
- References
- 38
- Citations by year
- 2026: 3 · 2025: 8 · 2024: 4 · 2023: 8 · 2022: 11 · 2021: 5 · 2020: 7 · 2019: 7 · 2018: 12 · 2017: 5 · 2016: 3 · 2015: 5
- FWCI
- 4.23
- Type
- journal article
- Language
- en
- Open access
- gold
- doi.org
- Licence
- Locations
- Nature Communications (publishedVersion)
- PubMed (publishedVersion)
- RePEc: Research Papers in Economics (submittedVersion)
- ArTS Archivio della ricerca di Trieste (University of Trieste https://www.units.it/) (submittedVersion)
- INFM-OAR (INFN Catania) (submittedVersion, other-oa)
- Funders
- Agence Nationale de la Recherche (ANR-11-LABX-0062)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Atomic and Molecular Physics
- Physical Sciences › Physics and Astronomy › Radiation › X-ray Spectroscopy and Fluorescence Analysis
- Keywords
- core-hole localization, carbon disulfide, single-photon ionization, photoelectron angular distributions, quantum entanglement, disentanglement, core ionization
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
