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Multiplet lines in seeded stimulated Mn Kα1 x-ray emission

Thomas Kroll1,*, Margaret Doyle2, Aliaksei Halavanau3, Thomas M. Linker4,5, Joshua Everts1,6, Yurina Michine7, Franklin D. Fuller8, Clemens Weninger9, Roberto Alonso-Mori8 et al.

Claudio Pellegrini3, Andrei Benediktovitch10, Makina Yabashi11,12, Ichiro Inoue11,13, Yuichi Inubushi11,12, Taito Osaka11, Toru Hara11, Jumpei Yamada11, Jan Kern2, Junko Yano2, Vittal K. Yachandra2, Nina Rohringer10,14, Hitoki Yoneda7, and Uwe Bergmann4,†

  • *Contact author: tkroll@slac.stanford.edu
  • †Contact author: ubergmann@wisc.edu

Phys. Rev. Applied 25, L051006 – Published 22 May, 2026

DOI: https://doi.org/10.1103/b13n-djsx

Abstract

We report the successful resolution of the multiplet structure of Kα1 x-ray emission in manganese (Mn) complexes through seeded stimulated x-ray emission spectroscopy (seeded S-XES). Using a femtosecond pump pulse above the Mn K edge to generate simultaneous 1s core holes, and a second-color tunable seed pulse to initiate the stimulated emission process, we were able to enhance individual lines within the Kα1 emission. This approach allows to resolve the fine multiplet features that are obscured by lifetime broadening in conventional (spontaneous) Mn Kα XES. The work builds on our previous observation that S-XES from Mn(II) and Mn(VII) complexes pumped at high intensities can exhibit stimulated emission without sacrificing the chemical sensitivity to oxidation states. This technique opens the door to controlled high-resolution electronic structure spectroscopy in transition-metal complexes beyond the core-hole lifetime, with potential applications in catalysis, inorganic chemistry, and materials science.

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