Abstract
Mixed-stack organic charge-transfer complexes which undergo a neutral-to-ionic transition are model systems to study strong cooperative effects between lattice-relaxed electronic excitations. An overview is given on structural and dynamical properties associated with this electronic-structural phase transformation which can be photo-induced. The analysis of the structural changes allows to underline the respective parts taken by the ionicity, which is a totally symmetric order parameter, and the dimerization which is the symmetry-breaking order parameter. The cooperative mechanism and the thermodynamics of the neutral-to-ionic transition are discussed on the basis of pressure effects, in particular with the observation of the tendency towards a tricritical point at high-pressure. This uncommon phase transition can be viewed as resulting from the condensation and the ordering of ionic dimers. However it needs to take into account quantum effects which are of great importance. Two types of characteristic excitation exist, on the one hand a polar vibrational soft mode of dimerization, on the other hand lattice-relaxed charge-transfer excitations which can be thermally- or photo- induced. Pretransitional dynamics is discussed in order to give a consistent view on the different results, recent and earlier.
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Cailleau, H., Cointe, M.L., Lemée-Cailleau, M.H. (1997). Structural Properties, Dynamics and Pressure Effects at the Neutral-to-Ionic Transition. In: Nasu, K. (eds) Relaxations of Excited States and Photo-Induced Structural Phase Transitions. Springer Series in Solid-State Sciences, vol 124. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-60702-8_14
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DOI: https://doi.org/10.1007/978-3-642-60702-8_14
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