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

Vanko, G.; Bordage, A.; Glatzel, P.; Gallo, E.; Rovezzi, M.; Gawelda, W.; Galler, A.; Bressler, C.; Doumy, G.; March, A. M.; Kanter, E. P.; Young, L.; Southworth, S. H.; Canton, S. E.; Uhlig, J.; Smolentsev, G.; Sundstrom, V.; Haldrup, K.; van Driel, T. B.; Nielsen, M. M.; Kjaer, K. S.; Lemke, H. T.

doi:10.1016/j.elspec.2012.09.012

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

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Canton, S. E.
Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for Biophysical Chemistry, Max Planck Society;

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Vanko, G., Bordage, A., Glatzel, P., Gallo, E., Rovezzi, M., Gawelda, W., et al. (2013). Spin-state studies with XES and RIXS: From static to ultrafast. Journal of Electron Spectroscopy and Related Phenomena, 188, 166-171. doi:10.1016/j.elspec.2012.09.012.

Cite as: https://hdl.handle.net/11858/00-001M-0000-002D-8174-0

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) Fe-II 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 Is 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.