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Impulsive solvent heating probed by picosecond x-ray diffraction
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10.1063/1.2176617
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    Affiliations:
    1 European Synchrotron Radiation Facility, BP 220, Grenoble Cedex 38043, France; National Institute for the Physics of Matter, 16152 Genova, Italy; and Department of Physical and Astronomical Sciences, via Archirafi 36, Palermo, Italy
    2 European Synchrotron Radiation Facility, BP 220, Grenoble Cedex 38043, France
    3 Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea and School of Molecular Science (BK21), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea
    4 European Synchrotron Radiation Facility, BP 220, Grenoble Cedex 38043, France
    5 Dipartimento di Fisica, Università di Roma “La Sapienza,” I-00185 Roma, Italy and SOFT-INFM-CNR, Università di Roma “La Sapienza,” I-00185 Roma, Italy
    6 European Synchrotron Radiation Facility, BP 220, Grenoble Cedex 38043, France
    7 National Institute for the Physics of Matter, 16152 Genova, Italy and Department of Physical and Astronomical Sciences, via Archirafi 36, Palermo, Italy
    8 European Synchrotron Radiation Facility, BP 220, Grenoble Cedex 38043, France
    9 Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea and School of Molecular Science (BK21), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701, Republic of Korea
    a) Present address: Groupe Matiere Condensee et Materiaux UMR6626 CNRS, BAT11A Campus de Beaulieu, Universite de Rennes 1, 35042 Rennes Cedex, France.
    b) Author to whom correspondence should be addressed. Electronic mail: hyotcherl.ihee@kaist.ac.kr
    J. Chem. Phys. 124, 124504 (2006); http://dx.doi.org/10.1063/1.2176617
/content/aip/journal/jcp/124/12/10.1063/1.2176617
http://aip.metastore.ingenta.com/content/aip/journal/jcp/124/12/10.1063/1.2176617

Figures

Image of FIG. 1.
FIG. 1.

Absorption spectrum of dissolved in methanol in the range from UV to NIR. The optical density for the solute at is comparable to that for the solvent at 1500 and .

Image of FIG. 2.
FIG. 2.

Effect of the correction for the transient expansion of the liquid. Panel (A): pure methanol at time delay with an open-jet system. Panel (B): /methanol for time delay. The broken lines are uncorrected curves and the solid lines corrected ones. The differences are also shown.

Image of FIG. 3.
FIG. 3.

Transient heating of methanol resolved in as a function of time for selected time delays. Data at and were collected with a higher number of repetitions.

Image of FIG. 4.
FIG. 4.

Derivatives from the hydrodynamic equation of state for methanol. Panel (A): a comparison of the data (solid) multiplied by with (broken) determined experimentally from a series of static measurements at various temperatures. Panel (B): two principal solvent differentials (broken) and (solid) obtained in this work (see text).

Image of FIG. 5.
FIG. 5.

Time-resolved diffraction signal as a function of time delay for in methanol at a few selected time delays; difference maps in space. Panel (A): global fitting of all reaction components (solid) to experimental data (broken); the solvent components taken from MD simulation. Panel (B): like (A), but the solvent components are experimentally obtained from pure methanol excited by NIR pulses. The improvement is clear at low for data at time delays beyond .

Image of FIG. 6.
FIG. 6.

Real space representation of the curves in Fig. 5. The improvement is clear for entire for data at time delays beyond .

Image of FIG. 7.
FIG. 7.

Time-resolved structural dynamics of the solute and the solvent for in methanol. (A) The population change of the transient , the intermediate isomer , and the final product as a function of time delay. (B) The change in the solvent density and the solvent temperature as a function of time delay.

Tables

Generic image for table
Table I.

Comparison of the global fit results using MD solvent differentials and experimental solvent differentials.

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/content/aip/journal/jcp/124/12/10.1063/1.2176617
2006-03-23
2014-04-20
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Impulsive solvent heating probed by picosecond x-ray diffraction
http://aip.metastore.ingenta.com/content/aip/journal/jcp/124/12/10.1063/1.2176617
10.1063/1.2176617
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