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.
The switching of electric polarization induced by electric fields, a fundamental functionality of ferroelectrics, is closely associated with the motions of the domain walls that separate regions with distinct polarization directions. Therefore, understanding domain-walls dynamics is of essential importance for advancing ferroelectric applications. In this Letter, we show that the topology of the multidomain structure can have an intrinsic impact on the degree of switchable polarization. Using a combination of polarization hysteresis measurements and piezoresponse force microscopy on a uniaxial organic ferroelectric, α-6,6′-dimethyl-2,2′-bipyridinium chloranilate, we found that the head-to-head (or tail-to-tail) charged domain walls are strongly pinned and thus impede the switching process; in contrast, if the charged domain walls are replaced with electrically neutral antiparallel domain walls, bulk polarization switching is achieved. Our findings suggest that manipulation of the multidomain topology can potentially control the switchable polarization.
Ferroelectric domain walls are typically stationary because of the presence of a pinning potential. Nevertheless, thermally activated, irreversible creep motion can occur under a moderate electric field, thereby underlying rewritable and non-volatile memory applications. Conversely, as the temperature decreases, the occurrence of creep motion becomes less likely and eventually impossible under realistic electric-field magnitudes. Here we show that such frozen ferroelectric domain walls recover their mobility under the influence of quantum fluctuations. Nonlinear permittivity and polarization-retention measurements of an organic charge-transfer complex reveal that ferroelectric domain-wall creep occurs via an athermal process when the system is tuned close to a pressure-driven ferroelectric quantum critical point. Despite the heavy masses of material building blocks such as molecules, the estimated effective mass of the domain wall is comparable to the proton mass, indicating the realization of a ferroelectric domain wall with a quantum-particle nature near the quantum critical point.
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