Thermodynamics of the Neutral-to-Ionic Transition as Condensation and Crystallization of Charge-Transfer Excitations

M. H. Lemée-Cailleau, M. Le Cointe, H. Cailleau, T. Luty, F. Moussa, J. Roos, D. Brinkmann, B. Toudic, C. Ayache, and N. Karl
Phys. Rev. Lett. 79, 1690 – Published 1 September 1997
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Abstract

The pressure-temperature phase diagram of tetrathiafulvalene-p-chloranil, prototype for the neutral-to-ionic transition, is determined by neutron diffraction and nuclear quadrupole resonance and discussed in relation to thermally induced charge-transfer (CT) excitations. The respective role of ionicity and dimerization is highlighted. Supported by theoretical considerations taking into account the interplay between quantum and thermal effects, the experimental results show that this uncommon electronic-structural transition can be described in terms of condensation and crystallization of CT excitations with a solid-liquid-gas–like phase diagram.

  • Received 5 May 1997

DOI:https://doi.org/10.1103/PhysRevLett.79.1690

©1997 American Physical Society

Authors & Affiliations

M. H. Lemée-Cailleau1, M. Le Cointe1, H. Cailleau1, T. Luty1,2, F. Moussa3, J. Roos4, D. Brinkmann4, B. Toudic1, C. Ayache5, and N. Karl6

  • 1Groupe Matière Condensée et Matériaux, UMR au CNRS 6626, Université Rennes 1, F-35042 Rennes Cedex, France
  • 2Institute of Physical and Theoretical Chemistry, Technical University, PL-50-370 Wroclaw, Poland
  • 3Laboratoire Léon Brillouin, CEA-CNRS Saclay, F-91191 Gif sur Yvette Cedex, France
  • 4Physik Institut der Universität Zürich, CH-8057 Zürich, Switzerland
  • 5Laboratoire de Cryophysique, CEN Grenoble, F-38041 Grenoble Cedex, France
  • 6Physikalisches Institut, Universität Stuttgart, D-70550 Stuttgart, Germany

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Vol. 79, Iss. 9 — 1 September 1997

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