Revealing core-valence interactions in solution with femtosecond X-ray pump X-ray probe spectroscopy

Robert B. Weakly, Chelsea E. Liekhus-Schmaltz, Benjamin I. Poulter, Elisa Biasin, Roberto Alonso-Mori, Andrew Aquila, Sébastien Boutet, Franklin D. Fuller, Phay J. Ho, Thomas Kroll, Caroline M. Loe, Alberto Lutman, Diling Zhu, Uwe Bergmann, Robert W. Schoenlein, Niranjan Govind and Munira Khalil ()
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Robert B. Weakly: University of Washington
Chelsea E. Liekhus-Schmaltz: University of Washington
Benjamin I. Poulter: University of Washington
Elisa Biasin: SLAC National Accelerator Laboratory
Roberto Alonso-Mori: SLAC National Accelerator Laboratory
Andrew Aquila: SLAC National Accelerator Laboratory
Sébastien Boutet: SLAC National Accelerator Laboratory
Franklin D. Fuller: SLAC National Accelerator Laboratory
Phay J. Ho: Argonne National Laboratory
Thomas Kroll: SLAC National Accelerator Laboratory
Caroline M. Loe: University of Washington
Alberto Lutman: SLAC National Accelerator Laboratory
Diling Zhu: SLAC National Accelerator Laboratory
Uwe Bergmann: University of Wisconsin-Madison
Robert W. Schoenlein: SLAC National Accelerator Laboratory
Niranjan Govind: Pacific Northwest National Laboratory
Munira Khalil: University of Washington

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Femtosecond pump-probe spectroscopy using ultrafast optical and infrared pulses has become an essential tool to discover and understand complex electronic and structural dynamics in solvated molecular, biological, and material systems. Here we report the experimental realization of an ultrafast two-color X-ray pump X-ray probe transient absorption experiment performed in solution. A 10 fs X-ray pump pulse creates a localized excitation by removing a 1s electron from an Fe atom in solvated ferro- and ferricyanide complexes. Following the ensuing Auger–Meitner cascade, the second X-ray pulse probes the Fe 1s → 3p transitions in resultant novel core-excited electronic states. Careful comparison of the experimental spectra with theory, extracts +2 eV shifts in transition energies per valence hole, providing insight into correlated interactions of valence 3d with 3p and deeper-lying electrons. Such information is essential for accurate modeling and predictive synthesis of transition metal complexes relevant for applications ranging from catalysis to information storage technology. This study demonstrates the experimental realization of the scientific opportunities possible with the continued development of multicolor multi-pulse X-ray spectroscopy to study electronic correlations in complex condensed phase systems.

Date: 2023
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DOI: 10.1038/s41467-023-39165-2

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