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

Milne, Chris J. ; Pham, Van-Thai LU ; Gawelda, Wojciech ; Van Der Veen, Renske M. ; ElNahhas, Amal ; Johnson, Steven L. ; Beaud, Paul ; Ingold, Gerhard ; Lima, Frederico and Vithanage, Dimali A. LU , et al. (2009) In Journal of Physics: Conference Series 190.
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... (More)

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.

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publishing date
type
Contribution to journal
publication status
published
in
Journal of Physics: Conference Series
volume
190
article number
012052
publisher
IOP Publishing
external identifiers
  • scopus:73349090928
ISSN
1742-6588
DOI
10.1088/1742-6596/190/1/012052
language
English
LU publication?
no
id
8890c9a7-68af-4cdd-9c30-42417e62e1e6
date added to LUP
2019-06-30 09:59:06
date last changed
2020-10-27 02:58:46
@article{8890c9a7-68af-4cdd-9c30-42417e62e1e6,
  abstract     = {<p>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 <sup>II</sup>(bpy)<sub>3</sub>]<sup>2+</sup>, in aqueous solution, resolving the Fe-N bond distance elongation as 0.2 . In addition an analysis technique using the reduced χ<sup>2</sup> 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.</p>},
  author       = {Milne, Chris J. and Pham, Van-Thai and Gawelda, Wojciech and Van Der Veen, Renske M. and ElNahhas, Amal and Johnson, Steven L. and Beaud, Paul and Ingold, Gerhard and Lima, Frederico and Vithanage, Dimali A. and Benfatto, Maurizio and Grolimund, Daniel and Borca, Camelia and Kaiser, Maik and Hauser, Andreas and Abela, Rafael and Bressler, Christian and Chergui, Majed},
  issn         = {1742-6588},
  language     = {eng},
  month        = {01},
  publisher    = {IOP Publishing},
  series       = {Journal of Physics: Conference Series},
  title        = {Time-resolved X-ray absorption spectroscopy : Watching atoms dance},
  url          = {http://dx.doi.org/10.1088/1742-6596/190/1/012052},
  doi          = {10.1088/1742-6596/190/1/012052},
  volume       = {190},
  year         = {2009},
}