Abstract

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Femtosecond X-ray Spectroscopy in Catalysis?

I-33

Femtosecond X-ray Spectroscopy in Catalysis?


Frank de Groot1

1Debye Institute of Nanomaterials Science, Utrecht University, Universiteitsweg 99, 3584 CG Utrecht, Netherlands

Time-resolved x-ray spectroscopy experiments are well-developed to probe the time-evolution of laser-excited states. It is possible to perform such experiments with synchrotrons [1], x-ray FEL’s [2] and laboratory sources [3]. As yet, most (excitonic) electronic state calculations for such experiments are based on fixed configurations for the initial, intermediate and final states. A second topic I will discuss is the potential application of time-resolved experiments to track chemical reactions in a catalytic system at work. Using a dispersive monochromator one can in principle measure an x-ray (emission) spectrum momentarily, allowing fs time-resolved spectroscopy. It remains to be seen how one can couple this to chemical reactions on timescales from fs to ns, μs, ms and seconds. A complication for fast experiments is the realization of a trigger that is not optical or electromagnetic. A last topic is the dynamics of core excitation and decay processes by using the energy domain instead of the time-domain. For example using x-ray Raman scattering, one can probe the exact lifetime of excited states.

References:

[1] N. Huse et al. J. Phys. Chem. Lett. 2, 880 (2011)

[2] R. Mitzner, et al. J. Phys. Chem. Lett. 4, 3641 (2013)

[3] J. Vura-Weis, et al. J. Phys. Chem. Lett. 4, 3667 (2013)