| Summary: | Although the Neutral-Ionic transition in mixed stack charge-transfer crystals was discovered almost forty years ago, many features of this intriguing phase transition, as well as open questions, remain at the heart of today’s science. First of all, there is the most spectacular manifestation of electronic ferroelectricity, in connection with a high degree of covalency between alternating donor and acceptor molecules along stacks. In addition, a charge-transfer instability from a quasi-neutral to a quasi-ionic state takes place concomitantly with the stack dimerization, which breaks the inversion symmetry. Moreover, these systems exhibit exceptional one-dimensional fluctuations, with an enhancement of the effects of electron-lattice interaction. This may lead to original physical pictures for the dynamics of pre-transitional phenomena, as the possibility of a pronounced Peierls-type instability and/or the generation of unconventional non-linear excitations along stacks. Last but not least, these mixed stack charge-transfer systems constitute a valuable test bed to explore some of the key questions of ultrafast photo-induced phenomena, such as multiscale dynamics, selective coherent excitations and non-linear responsiveness. These different aspects will be discussed through the structural and dynamical features of the neutral-ionic transition, considering old and recent results, open questions and future opportunities. In particular, we revisit the structural changes and symmetry considerations, the pressure-temperature phase diagrams and conclude by their interplay with the photo-induced dynamics.
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