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Nat Commun. 2015 Jun 16;6:7469. doi: 10.1038/ncomms8469.

Quantum ferroelectricity in charge-transfer complex crystals.

Author information

1
1] National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba 305-8562, Japan [2] CREST, Japan Science and Technology Agency (JST), Tokyo 102-0076, Japan.
2
Condensed Matter Research Center (CMRC) and Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK), Tsukuba 305-0801, Japan.
3
1] CREST, Japan Science and Technology Agency (JST), Tokyo 102-0076, Japan [2] Condensed Matter Research Center (CMRC) and Photon Factory, Institute of Materials Structure Science, High Energy Accelerator Research Organization (KEK), Tsukuba 305-0801, Japan.
4
Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan.
5
1] CREST, Japan Science and Technology Agency (JST), Tokyo 102-0076, Japan [2] RIKEN Center for Emergent Matter Science (CEMS), Wako 351-0198, Japan.
6
1] Department of Applied Physics, The University of Tokyo, Tokyo 113-8656, Japan [2] RIKEN Center for Emergent Matter Science (CEMS), Wako 351-0198, Japan.

Abstract

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.

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