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Quantum ferroelectricity in charge-transfer complex crystals #MMPMID26076656
Quantum phase transition achieved by fine tuning the continuous phase transition down to zero kelvin is a challenge for solid state science. Critical phenomena distinct from the effects of thermal fluctuations can materialize when the electronic, structural or magnetic long-range order is perturbed by quantum fluctuations between degenerate ground states. Here we have developed chemically pure tetrahalo-p-benzoquinones of n iodine and 4?n bromine substituents (QBr4?nIn, n=0?4) to search for ferroelectric charge-transfer complexes with tetrathiafulvalene (TTF). Among them, TTF?QBr2I2 exhibits a ferroelectric neutral?ionic phase transition, which is continuously controlled over a wide temperature range from near-zero kelvin to room temperature under hydrostatic pressure. Quantum critical behaviour is accompanied by a much larger permittivity than those of other neutral?ionic transition compounds, such as well-known ferroelectric complex of TTF?QCl4 and quantum antiferroelectric of dimethyl?TTF?QBr4. By contrast, TTF?QBr3I complex, another member of this compound family, shows complete suppression of the ferroelectric spin-Peierls-type phase transition.