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Observation of site-selective chemical bond changes via ultrafast chemical shifts

Author

Listed:
  • Andre Al-Haddad

    (Chemical Sciences and Engineering Division, Argonne National Laboratory
    Paul-Scherrer Institute)

  • Solène Oberli

    (Universidad Autónoma de Madrid
    LUXS Laboratory for Ultrafast X-ray Sciences, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL)
    Laboratory of Theoretical Physical Chemistry, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL))

  • Jesús González-Vázquez

    (Universidad Autónoma de Madrid)

  • Maximilian Bucher

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Gilles Doumy

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Phay Ho

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Jacek Krzywinski

    (SLAC National Accelerator Laboratory)

  • Thomas J. Lane

    (SLAC National Accelerator Laboratory)

  • Alberto Lutman

    (SLAC National Accelerator Laboratory)

  • Agostino Marinelli

    (SLAC National Accelerator Laboratory
    Stanford PULSE Institute, SLAC National Accelerator Laboratory)

  • Timothy J. Maxwell

    (SLAC National Accelerator Laboratory)

  • Stefan Moeller

    (SLAC National Accelerator Laboratory)

  • Stephen T. Pratt

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Dipanwita Ray

    (SLAC National Accelerator Laboratory)

  • Ron Shepard

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Stephen H. Southworth

    (Chemical Sciences and Engineering Division, Argonne National Laboratory)

  • Álvaro Vázquez-Mayagoitia

    (Argonne Leadership Computing Facility)

  • Peter Walter

    (SLAC National Accelerator Laboratory)

  • Linda Young

    (Chemical Sciences and Engineering Division, Argonne National Laboratory
    Department of Physics and James Franck Institute, The University of Chicago)

  • Antonio Picón

    (Chemical Sciences and Engineering Division, Argonne National Laboratory
    Universidad Autónoma de Madrid)

  • Christoph Bostedt

    (Chemical Sciences and Engineering Division, Argonne National Laboratory
    Paul-Scherrer Institute
    LUXS Laboratory for Ultrafast X-ray Sciences, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL))

Abstract

The concomitant motion of electrons and nuclei on the femtosecond time scale marks the fate of chemical and biological processes. Here we demonstrate the ability to initiate and track the ultrafast electron rearrangement and chemical bond breaking site-specifically in real time for the carbon monoxide diatomic molecule. We employ a local resonant x-ray pump at the oxygen atom and probe the chemical shifts of the carbon core-electron binding energy. We observe charge redistribution accompanying core-excitation followed by Auger decay, eventually leading to dissociation and hole trapping at one site of the molecule. The presented technique is general in nature with sensitivity to chemical environment changes including transient electronic excited state dynamics. This work provides a route to investigate energy and charge transport processes in more complex systems by tracking selective chemical bond changes on their natural timescale.

Suggested Citation

  • Andre Al-Haddad & Solène Oberli & Jesús González-Vázquez & Maximilian Bucher & Gilles Doumy & Phay Ho & Jacek Krzywinski & Thomas J. Lane & Alberto Lutman & Agostino Marinelli & Timothy J. Maxwell & S, 2022. "Observation of site-selective chemical bond changes via ultrafast chemical shifts," Nature Communications, Nature, vol. 13(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34670-2
    DOI: 10.1038/s41467-022-34670-2
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    References listed on IDEAS

    as
    1. C. Behrens & F.-J. Decker & Y. Ding & V. A. Dolgashev & J. Frisch & Z. Huang & P. Krejcik & H. Loos & A. Lutman & T. J. Maxwell & J. Turner & J. Wang & M.-H. Wang & J. Welch & J. Wu, 2014. "Few-femtosecond time-resolved measurements of X-ray free-electron lasers," Nature Communications, Nature, vol. 5(1), pages 1-7, September.
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