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Science 25 April 2003:
Vol. 300. no. 5619, pp. 612 - 615
DOI: 10.1126/science.1082001
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Reports

Laser-Induced Ferroelectric Structural Order in an Organic Charge-Transfer Crystal

Eric Collet,1,2* Marie-Hélene Lemée-Cailleau,1 Marylise Buron-Le Cointe,1 Hervé Cailleau,1 Michael Wulff,3 Tadeusz Luty,4 Shin-Ya Koshihara,5 Mathias Meyer,6 Loic Toupet,1 Philippe Rabiller,1 Simone Techert3,7

We report the direct observation by x-ray diffraction of a photoinduced paraelectric-to-ferroelectric structural phase transition using monochromatic 100-picosecond synchrotron pulses. It occurs in tetrathiafulvalene-p-chloranil, a charge-transfer molecular material in which electronic and structural changes are strongly coupled. An optical 300-femtosecond laser pulse switches the material from a neutral to an ionic state on a 500-picosecond time scale and, by virtue of intrinsic cooperativity, generates self-organized long-range structural order. The x-ray data indicate a macroscopic ferroelectric reorganization after the laser irradiation. Refinement of the structures before and after laser irradiation indicates structural changes at the molecular level.

1 Groupe Matière Condensée et Matériaux, UMR CNRS 6626, Universite Rennes 1, 35042 Rennes Cedex, France.
2 Laboratoire Léon Brillouin, Commissariat á l'Energie Atomique, Saclay, 91191 Gif-sur-Yvette, France.
3 European Synchrotron Radiation Facility, Boîte Postale 220, 38043 Grenoble, France.
4 Institute of Physical and Theoretical Chemistry, Technical University of Wroclaw, 50-370 Wroclaw, Poland.
5 Department of Materials Science, Tokyo Institute of Technology, 2-12-1 Oh-okayama, Meguro-ku, Tokyo 152-8551, and Kanagawa Academy of Science and Technology, 3-2-1 Sakado, Takatsu-ku, Kawasaki 213-0012, Japan.
6 Oxford Diffraction Poland Sp. z.o.o., ul. Rogowska 127A, 54-440 Wroclaw, Poland.
7 Max Planck Institut for Biophysical Chemistry, Department 010, 37070 Göttingen, Germany.

* To whom correspondence should be addressed. E-mail: Eric.Collet{at}univ-rennes1.fr

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