Spin-state studies with XES and RIXS: From static to ultrafast

György Vankó, Amélie Bordage, Pieter Glatzel, Erik Gallo, Mauro Rovezzi, Wojciech Gawelda, Andreas Galler, Christian Bressler, Gilles Doumy, Anne Marie March, Elliot P. Kanter, Linda Young, Stephen H. Southworth, Sophie E. Canton, Jens Uhlig, Grigory Smolentsev, Villy Sundström, Kristoffer Haldrup, Tim Brandt van Driel, Martin Meedom NielsenKasper S. Kjaer, Henrik T. Lemke

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Abstract

We report on extending hard X-ray emission spectroscopy (XES) along with resonant inelastic X-ray scattering (RIXS) to study ultrafast phenomena in a pump-probe scheme at MHz repetition rates. The investigated systems include low-spin (LS) FeII complex compounds, where optical pulses induce a spin-state transition to their (sub)nanosecond-lived high-spin (HS) state. Time-resolved XES clearly reflects the spin-state variations with very high signal-to-noise ratio, in agreement with HS–LS difference spectra measured at thermal spin crossover, and reference HS–LS systems in static experiments, next to multiplet calculations. The 1s2p RIXS, measured at the Fe 1s pre-edge region, shows variations after laser excitation, which are consistent with the formation of the HS state. Our results demonstrate that X-ray spectroscopy experiments with overall rather weak signals, such as RIXS, can now be reliably exploited to study chemical and physical transformations on ultrafast time scales.

Original languageEnglish
JournalJournal of Electron Spectroscopy and Related Phenomena
Volume188
Pages (from-to)166-171
ISSN0368-2048
DOIs
Publication statusPublished - 2013

Keywords

  • Molecular switching
  • Time-resolved spectroscopy
  • X-ray spectroscopy
  • Spin transition
  • Photoinduced transition
  • Ultrafast phenomena
  • Pump-probe experiments

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