Standard

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)32+. / Haldrup, Martin Kristoffer; Vanko, G.; Gawelda, W.; Galler, A.; Doumy, G.; March, A.M.; Kanter, E.P.; Bordage, A.; Dohn, Asmus Ougaard; Brandt van Driel, Tim; Kjær, K. S.; Lemke, H.T.; Canton, S.E.; Uhlig, J.; Sundstrom, V.; Young, L.; Southworth, S.H.; Nielsen, Martin Meedom; Bressler, C.

In: Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, Vol. 116, No. 40, 2012, p. 9878-9887.

Publication: Research - peer-reviewJournal article – Annual report year: 2012

Harvard

APA

CBE

MLA

Vancouver

Author

Haldrup, Martin Kristoffer; Vanko, G.; Gawelda, W.; Galler, A.; Doumy, G.; March, A.M.; Kanter, E.P.; Bordage, A.; Dohn, Asmus Ougaard; Brandt van Driel, Tim; Kjær, K. S.; Lemke, H.T.; Canton, S.E.; Uhlig, J.; Sundstrom, V.; Young, L.; Southworth, S.H.; Nielsen, Martin Meedom; Bressler, C. / 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)32+.

In: Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, Vol. 116, No. 40, 2012, p. 9878-9887.

Publication: Research - peer-reviewJournal article – Annual report year: 2012

Bibtex

@article{f2ce516f7c2a4267b5c54bff74a58eb0,
title = "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)32+",
publisher = "American Chemical Society",
author = "Haldrup, {Martin Kristoffer} and G. Vanko and W. Gawelda and A. Galler and G. Doumy and A.M. March and E.P. Kanter and A. Bordage and Dohn, {Asmus Ougaard} and {Brandt van Driel}, Tim and Kjær, {K. S.} and H.T. Lemke and S.E. Canton and J. Uhlig and V. Sundstrom and L. Young and S.H. Southworth and Nielsen, {Martin Meedom} and C. Bressler",
year = "2012",
doi = "10.1021/jp306917x",
volume = "116",
number = "40",
pages = "9878--9887",
journal = "Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory",
issn = "1089-5639",

}

RIS

TY - JOUR

T1 - Guest–Host Interactions Investigated by Time-Resolved X-ray Spectroscopies and Scattering at MHz Rates

T2 - Solvation Dynamics and Photoinduced Spin Transition in Aqueous Fe(bipy)<sub>3</sub><sup>2+</sup>

A1 - Haldrup,Martin Kristoffer

A1 - Vanko,G.

A1 - Gawelda,W.

A1 - Galler,A.

A1 - Doumy,G.

A1 - March,A.M.

A1 - Kanter,E.P.

A1 - Bordage,A.

A1 - Dohn,Asmus Ougaard

A1 - Brandt van Driel,Tim

A1 - Kjær,K. S.

A1 - Lemke,H.T.

A1 - Canton,S.E.

A1 - Uhlig,J.

A1 - Sundstrom,V.

A1 - Young,L.

A1 - Southworth,S.H.

A1 - Nielsen,Martin Meedom

A1 - Bressler,C.

AU - Haldrup,Martin Kristoffer

AU - Vanko,G.

AU - Gawelda,W.

AU - Galler,A.

AU - Doumy,G.

AU - March,A.M.

AU - Kanter,E.P.

AU - Bordage,A.

AU - Dohn,Asmus Ougaard

AU - Brandt van Driel,Tim

AU - Kjær,K. S.

AU - Lemke,H.T.

AU - Canton,S.E.

AU - Uhlig,J.

AU - Sundstrom,V.

AU - Young,L.

AU - Southworth,S.H.

AU - Nielsen,Martin Meedom

AU - Bressler,C.

PB - American Chemical Society

PY - 2012

Y1 - 2012

N2 - <p>We have studied the photoinduced low spin (LS) to high spin (HS) conversion of [Fe(bipy)<sub>3</sub>]<sup>2+ </sup>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.</p>

AB - <p>We have studied the photoinduced low spin (LS) to high spin (HS) conversion of [Fe(bipy)<sub>3</sub>]<sup>2+ </sup>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.</p>

U2 - 10.1021/jp306917x

DO - 10.1021/jp306917x

JO - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

JF - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

SN - 1089-5639

IS - 40

VL - 116

SP - 9878

EP - 9887

ER -