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

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, Stefan Moeller, Stephen T. Pratt, Dipanwita Ray, Ron Shepard, Stephen H. Southworth, Álvaro Vázquez-Mayagoitia, Peter Walter, Linda Young, Antonio Picón () and Christoph Bostedt ()
Additional contact information
Andre Al-Haddad: Chemical Sciences and Engineering Division, Argonne National Laboratory
Solène Oberli: Universidad Autónoma de Madrid
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
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
Antonio Picón: Chemical Sciences and Engineering Division, Argonne National Laboratory
Christoph Bostedt: Chemical Sciences and Engineering Division, Argonne National Laboratory

Nature Communications, 2022, vol. 13, issue 1, 1-7

Abstract: 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.

Date: 2022
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DOI: 10.1038/s41467-022-34670-2

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