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Guest-Host Interact...
Guest-Host Interactions Investigated by Time-Resolved X-ray Spectroscopies and Scattering at MHz Rates: Solvation Dynamics and Photoinduced Spin Transition in Aqueous Fe(bipy)(3)(2+)
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Haldrup, K. (author)
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Vanko, G. (author)
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Gawelda, W. (author)
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Galler, A. (author)
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Doumy, G. (author)
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March, A. M. (author)
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Kanter, E. P. (author)
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Bordage, A. (author)
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Dohn, A. (author)
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van Driel, T. B. (author)
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Kjaer, K. S. (author)
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Lemke, H. T. (author)
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- Canton, Sophie (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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Uhlig, J. (author)
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- Sundström, Villy (author)
- Lund University,Lunds universitet,Kemisk fysik,Enheten för fysikalisk och teoretisk kemi,Kemiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,Chemical Physics,Physical and theoretical chemistry,Department of Chemistry,Departments at LTH,Faculty of Engineering, LTH
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Young, L. (author)
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Southworth, S. H. (author)
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Nielsen, M. M. (author)
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Bressler, C. (author)
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(creator_code:org_t)
- 2012-10-03
- 2012
- English.
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In: The Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory. - : American Chemical Society (ACS). - 1520-5215. ; 116:40, s. 9878-9887
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Abstract
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- We have studied the photoinduced low spin (LS) to high spin (HS) conversion of [Fe(bipy)(3)](2+) in aqueous solution. In a laser pump/X-ray probe synchrotron setup permitting simultaneous, time-resolved X-ray diffuse scattering (XDS) and X-ray spectroscopic measurements at a 3.26 MHz repetition rate, we observed the interplay between intramolecular dynamics and the intermolecular caging solvent response with better than 100 ps time resolution. On this time scale, the initial ultrafast spin transition and the associated intramolecular geometric structure changes are long completed, as is the solvent heating due to the initial energy dissipation from the excited HS molecule. Combining information from X-ray emission spectroscopy and scattering, the excitation fraction as well as the temperature and density changes of the solvent can be closely followed on the subnanosecond time scale of the HS lifetime, allowing the detection of an ultrafast change in bulk solvent density. An analysis approach directly utilizing the spectroscopic data in the XDS analysis effectively reduces the number of free parameters, and both combined permit extraction of information about the ultrafast structural dynamics of the caging solvent, in particular, a decrease in the number of water molecules in the first solvation shell is inferred, as predicted by recent theoretical work.
Subject headings
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
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- art (subject category)
- ref (subject category)
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- By the author/editor
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Haldrup, K.
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Vanko, G.
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Gawelda, W.
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Galler, A.
-
Doumy, G.
-
March, A. M.
-
show more...
-
Kanter, E. P.
-
Bordage, A.
-
Dohn, A.
-
van Driel, T. B.
-
Kjaer, K. S.
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Lemke, H. T.
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Canton, Sophie
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Uhlig, J.
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Sundström, Villy
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Young, L.
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Southworth, S. H ...
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Nielsen, M. M.
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Bressler, C.
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show less...
- About the subject
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- NATURAL SCIENCES
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NATURAL SCIENCES
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and Physical Science ...
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and Atom and Molecul ...
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The Journal of P ...
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Lund University