Static and dynamic order of cooperative multi-electron transfer

¹ Institute of Physical and Theoretical Chemistry, Technical University of Wrocław PL-50370 Wrocław, Poland
² Groupe Matière Condensée et Matériaux, UMR 6626 CNRS, Université de Rennes 1 F-35042 Rennes, France
³ Kanagawa Academy of Science and Technology (KAST) Takatsu-ku, Kawasaki JP-213-0012, Japan
⁴ Department of Materials Science, Tokyo Institute of Technology Meguro-ku, Tokyo JP-152-8551, Japan
⁵ Laboratoire Leon Brillouin, CEA/Saclay - F-91191 Gif-sur-Yvette, France
⁶ Department of Applied Physics, University of Tokyo Bunkyo-ku, Tokyo JP-113-8656, Japan
⁷ Joint Research Center for Atom Technology Tsukuba JP-305-0046, Japan
⁸ Institute Laue Langevin - F-38042 Grenoble, France

Received: 2 May 2002
Accepted: 31 May 2002

Abstract

We report on high correlation and ordering of multi-electron transfer at neutral-ionic transformation in quasi–one-dimensional prototype crystal of tetrathiafulvalene-chloranil (TTF-CA). We present experimental evidences that the ordering of lattice-relaxed charge-transfer strings, which are nano-scale objects, occurs under static thermal equilibrium condition and non-equilibrium one achieved by femto-second laser irradiation. We suggest that the transformation is a profound example of self-organized, cooperative electron transfer with tendency for phase separation driven by energetics of inter-chain interaction and ferroelectric ordering.