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Picosecond calorimetry : time-resolved x-ray diffraction studies of liquid CH2Cl2

Georgiou, Panayiotis ; Vincent, Jonathan ; Andersson, Magnus ; Wöhri, Annemarie B ; Gourdon, Pontus LU ; Poulsen, Jens ; Davidsson, Jan and Neutze, Richard (2006) In Journal of Chemical Physics 124(23). p.1-9
Abstract

Liquid phase time-resolved x-ray diffraction with 100 ps resolution has recently emerged as a powerful technique for probing the structural dynamics of transient photochemical species in solution. It is intrinsic to the method, however, that a structural signal is observed not only from the photochemical of interest but also from the embedding solvent matrix. To experimentally characterize the x-ray diffraction signal deriving from the solvent alone we performed time-resolved diffraction studies of a pure liquid sample over a time domain from -250 ps to 2.5 micros. Multiphoton excitation was used to rapidly heat liquid CH(2)Cl(2) using UV pulses of 100 fs duration. A significant x-ray diffraction signal is visible prior to the onset of... (More)

Liquid phase time-resolved x-ray diffraction with 100 ps resolution has recently emerged as a powerful technique for probing the structural dynamics of transient photochemical species in solution. It is intrinsic to the method, however, that a structural signal is observed not only from the photochemical of interest but also from the embedding solvent matrix. To experimentally characterize the x-ray diffraction signal deriving from the solvent alone we performed time-resolved diffraction studies of a pure liquid sample over a time domain from -250 ps to 2.5 micros. Multiphoton excitation was used to rapidly heat liquid CH(2)Cl(2) using UV pulses of 100 fs duration. A significant x-ray diffraction signal is visible prior to the onset of thermal expansion, which characterizes a highly compressed superheated liquid. Liquid CH(2)Cl(2) then expands as a shock wave propagates through the sample and the temporal dependence of this phenomenon is in good agreement with theory. An unexpectedly slow initial release of energy into the liquid as heat is observed from multiphoton excited CH(2)Cl(2), revealing the presence of a metastable state of multiphoton excited CH(2)Cl(2).

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author
; ; ; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
keywords
Journal Article
in
Journal of Chemical Physics
volume
124
issue
23
article number
234507
pages
1 - 9
publisher
American Institute of Physics (AIP)
external identifiers
  • pmid:16821929
  • scopus:33745304378
ISSN
0021-9606
DOI
10.1063/1.2205365
language
English
LU publication?
no
id
5ad87af5-129e-45fd-8189-8275668da436
date added to LUP
2017-04-29 15:32:43
date last changed
2024-01-28 17:04:41
@article{5ad87af5-129e-45fd-8189-8275668da436,
  abstract     = {{<p>Liquid phase time-resolved x-ray diffraction with 100 ps resolution has recently emerged as a powerful technique for probing the structural dynamics of transient photochemical species in solution. It is intrinsic to the method, however, that a structural signal is observed not only from the photochemical of interest but also from the embedding solvent matrix. To experimentally characterize the x-ray diffraction signal deriving from the solvent alone we performed time-resolved diffraction studies of a pure liquid sample over a time domain from -250 ps to 2.5 micros. Multiphoton excitation was used to rapidly heat liquid CH(2)Cl(2) using UV pulses of 100 fs duration. A significant x-ray diffraction signal is visible prior to the onset of thermal expansion, which characterizes a highly compressed superheated liquid. Liquid CH(2)Cl(2) then expands as a shock wave propagates through the sample and the temporal dependence of this phenomenon is in good agreement with theory. An unexpectedly slow initial release of energy into the liquid as heat is observed from multiphoton excited CH(2)Cl(2), revealing the presence of a metastable state of multiphoton excited CH(2)Cl(2).</p>}},
  author       = {{Georgiou, Panayiotis and Vincent, Jonathan and Andersson, Magnus and Wöhri, Annemarie B and Gourdon, Pontus and Poulsen, Jens and Davidsson, Jan and Neutze, Richard}},
  issn         = {{0021-9606}},
  keywords     = {{Journal Article}},
  language     = {{eng}},
  month        = {{06}},
  number       = {{23}},
  pages        = {{1--9}},
  publisher    = {{American Institute of Physics (AIP)}},
  series       = {{Journal of Chemical Physics}},
  title        = {{Picosecond calorimetry : time-resolved x-ray diffraction studies of liquid CH2Cl2}},
  url          = {{http://dx.doi.org/10.1063/1.2205365}},
  doi          = {{10.1063/1.2205365}},
  volume       = {{124}},
  year         = {{2006}},
}