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  Observing solvation dynamics with simultaneous femtosecond X-ray emission spectroscopy and X-ray scattering.

Haldrup, K., Gawelda, W., Abela, R., Alonso-Mori, R., Bergmann, U., Bordage, A., et al. (2016). Observing solvation dynamics with simultaneous femtosecond X-ray emission spectroscopy and X-ray scattering. Journal of Physical Chemistry B, 120(6), 1158-1168. doi:10.1021/acs.jpcb.5b12471.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-5FAE-5 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-002B-5FB1-C
Genre: Journal Article

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 Creators:
Haldrup, K., Author
Gawelda, W., Author
Abela, R., Author
Alonso-Mori, R., Author
Bergmann, U., Author
Bordage, A., Author
Cammarata, M., Author
Canton, S. E.1, Author              
Dohn, A. O., Author
Brandt van Driel, T., Author
Fritz, D. M., Author
Galler, A., Author
Glatzel, P., Author
Harlang, T., Author
Kjær, K. S., Author
Lemke, H. T., Author
Møller, K. B., Author
Németh, Z., Author
Pápai, M., Author
Sas, N., Author
Uhlig, J., AuthorZhu, D., AuthorVankó, G., AuthorSundström, V., AuthorNielsen, M. M., AuthorBressler, C., Author more..
Affiliations:
1Research Group of Structural Dynamics of (Bio)Chemical Systems, MPI for Biophysical Chemistry, Max Planck Society, ou_578564              

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 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 previous ab initio molecular dynamics simulations. Structural changes in the aqueous solvent associated with density and temperature changes occur with ∼1 ps time constants, characteristic for structural dynamics in water. This slower time scale of the solvent response allows us to directly observe the structure of the excited solute molecules well before the solvent contributions become dominant.

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Language(s): eng - English
 Dates: 2016-01-192016
 Publication Status: Published in print
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 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpcb.5b12471
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Title: Journal of Physical Chemistry B
Source Genre: Journal
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Pages: - Volume / Issue: 120 (6) Sequence Number: - Start / End Page: 1158 - 1168 Identifier: -