Ferroelectric phase transition, ionicity condensation, and multicriticality in charge-transfer organic complexes

IR

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Abstract

To elucidate a pressure-temperature phase diagram of the quasi-one-dimensional mixed-stack charge-transfer complex tetrathiafulvalene-P-chloranil (TTF-CA), we study the quasi-one-dimensional spin-1 Blume-Emery-Griffiths model. In addition to the local charge-transfer energy (Δ) and the inter-stack polar (dipole-dipole) interaction (J), we take account of the interstack electrostriction (Coulomb-lattice coupling). Using the self-consistent chain-mean-field theory, where the intra-stack degrees of freedom are exactly treated by the transfer-matrix method, we reproduce the gas-liquid-solid like phase diagram corresponding to the neutral (N), paraelectric ionic (Ipara), and ferroelectric ionic (Iferro) phases, respectively. Our classical model describes an essential point of the multicritical behavior of TTF-CA, i.e., the interchain electrostriction exclusively enhances the charge concentration (ionicity condensation), but does not affect the interchain ferroelectric coupling. This effect leads to appearance of the intermediate Ipara phase in between the N and Iferro phases on the -T phase diagram.

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