Time-resolved X-ray absorption spectroscopy: Watching atoms dance

Chris J. Milne, Van Thai Pham, Wojciech Gawelda, Renske M. Van Der Veen, Amal ElNahhas, Steven L. Johnson, Paul Beaud, Gerhard Ingold, Frederico Lima, Dimali A. Vithanage, Maurizio Benfatto, Daniel Grolimund, Camelia Borca, Maik Kaiser, Andreas Hauser, Rafael Abela, Christian Bressler, Majed Chergui

Research output: Contribution to journalArticlepeer-review

Abstract

The introduction of pump-probe techniques to the field of X-ray absorption spectroscopy (XAS) has allowed the monitoring of both structural and electronic dynamics of disordered systems in the condensed phase with unprecedented accuracy, both in time and in space. We present results on the electronically excited high-spin state structure of an Fe(II) molecular species, [Fe II(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 . In addition an analysis technique using the reduced χ2 goodness of fit between FEFF EXAFS simulations and the experimental transient absorption signal in energy space has been successfully tested as a function of excited state population and chemical shift, demonstrating its applicability in situations where the fractional excited state population cannot be determined through other measurements. Finally by using a novel ultrafast hard X-ray 'slicing' source the question of how the molecule relaxes after optical excitation has been successfully resolved using femtosecond XANES.

Original languageEnglish (US)
Article number012052
JournalJournal of Physics: Conference Series
Volume190
DOIs
StatePublished - 2009
Externally publishedYes

ASJC Scopus subject areas

  • Physics and Astronomy(all)

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