Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 25, Pages 5925-5931Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c01190
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Funding
- Chemical Sciences, Geosciences, and Biosciences division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DOE) [DE-SC0019484, KC-030103172684]
- National Science Foundation [CHE-1953045]
- Alexander von Humboldt foundation through the Feodor Lynen program
- Office of Biological and Environmental Research
- United States Department of Energy under DOE [DE-AC05-76RL1830]
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The study investigates the resonant stimulated X-ray Raman spectroscopy of a bimetallic manganese complex, revealing charge transfer processes and electron dynamics. A pump-probe sequence of resonant X-ray Raman excitations is employed to track electron wave packets. By using a two-color protocol and visualizing electron dynamics through natural orbital decomposition, the study provides insights into charge transfer in the molecule.
Resonant stimulated X-ray Raman spectroscopy of the bimetallic [(MnMnIV)-Mn-III(mu-O)(2)(mu-OAC)(tacn)(2)](2+) manganese complex is investigated in a simulation study. Essential biological processes, including water oxidation in photosynthesis, involve charge transfer between manganese sites of different oxidation states. We study a prototypical binuclear mixed- valence transition-metal complex with two Mn atoms in different oxidation states surrounded by ligand structures and employ a pump-probe sequence of resonant X-ray Raman excitations to follow the charge transfer occurring in the molecule. This allows us to generate and monitor valence-electron wave packets at selected regions in the molecule by exploiting element-specific core-excited states. A two-color protocol is presented, with pump and probe pulses tuned to the Mn and N K-edges. A natural orbital decomposition allows the visualization of the electron dynamics underlying the signal.
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