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

Journal Article · · Nature Communications
 [1];  [2];  [3];  [4];  [4];  [4];  [5];  [5];  [5];  [5];  [5];  [5];  [4];  [5];  [4];  [4];  [6];  [5];  [7];  [8] more »;  [9] « less
  1. Argonne National Laboratory (ANL), Argonne, IL (United States); Paul-Scherrer Institute (PSI), Villigen (Switzerland); SLAC
  2. Universidad Autónoma de Madrid (Spain); École Polytechnique Fédérale de Lausanne (EPFL) (Switzerland)
  3. Universidad Autónoma de Madrid (Spain)
  4. Argonne National Laboratory (ANL), Argonne, IL (United States)
  5. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  6. Argonne National Laboratory (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility (ALCF)
  7. Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)
  8. Argonne National Laboratory (ANL), Argonne, IL (United States); Universidad Autónoma de Madrid (Spain)
  9. Argonne National Laboratory (ANL), Argonne, IL (United States); Paul-Scherrer Institute (PSI), Villigen (Switzerland); École Polytechnique Fédérale de Lausanne (EPFL) (Switzerland)
+ Show Author Affiliations
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.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
Swiss National Science Foundation (SNSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-06CH11357; AC02-76SF00515
OSTI ID:
2006555
Alternate ID(s):
OSTI ID: 2290334
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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