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

Chris J Milne1, Van-Thai Pham1, Wojciech Gawelda3, Renske M van der Veen1,2, Amal El Nahhas1, Steven L Johnson2, Paul Beaud2, Gerhard Ingold2, Frederico Lima1, Dimali A Vithanage1, Maurizio Benfatto4, Daniel Grolimund2, Camelia Borca2, Maik Kaiser2, Andreas Hauser5, Rafael Abela2, Christian Bressler6 and Majed Chergui1

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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, [FeII(bpy)3]2+, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 Å. 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.


PACS

78.70.Dm X-ray absorption spectra

61.25.Em Molecular liquids

78.47.-p Spectroscopy of solid state dynamics

Subjects

Soft matter, liquids and polymers

Condensed matter: electrical, magnetic and optical

Dates

Issue 1 (2009)



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