Observing Solvation Dynamics with Simultaneous Femtosecond X-ray Emission Spectroscopy and X-ray Scattering

The Journal of Physical Chemistry. B
K HaldrupChristian Bressler

Abstract

In liquid phase chemistry dynamic solute-solvent interactions often govern the path, ultimate outcome, and efficiency of chemical reactions. These steps involve many-body movements on subpicosecond time scales and thus ultrafast structural tools capable of capturing both intramolecular electronic and structural changes, and local solvent structural changes are desired. We have studied the intra- and intermolecular dynamics of a model chromophore, aqueous [Fe(bpy)3](2+), with complementary X-ray tools in a single experiment exploiting intense XFEL radiation as a probe. We monitored the ultrafast structural rearrangement of the solute with X-ray emission spectroscopy, thus establishing time zero for the ensuing X-ray diffuse scattering analysis. The simultaneously recorded X-ray diffuse scattering patterns reveal slower subpicosecond dynamics triggered by the intramolecular structural dynamics of the photoexcited solute. By simultaneous combination of both methods only, we can extract new information about the solvation dynamic processes unfolding during the first picosecond (ps). The measured bulk solvent density increase of 0.2% indicates a dramatic change of the solvation shell around each photoexcited solute, confirming previ...Continue Reading

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Citations

Oct 5, 2016·Inorganic Chemistry·Asmus O DohnKlaus B Møller
Apr 5, 2017·Annual Review of Physical Chemistry·Hosung KiHyotcherl Ihee
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May 3, 2020·Nature Communications·Grigory SmolentsevMatthias Vogt
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Sep 16, 2019·The Journal of Chemical Physics·Mátyás PápaiKlaus B Møller
Aug 15, 2017·Chemical Reviews·Carlito S PonsecaVilly Sundström

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