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Register a new userFerroelectric properties of charge-ordered alpha-(BEDT-TTF)2I3
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A detailed investigation of the out-of-plane electrical properties of charge-ordered alpha-(BEDT-TTF)2I3 provides clear evidence for ferroelectricity. Similar to multiferroic alpha-(BEDT-TTF)2Cu[N(CN)2]Cl, the polar order in this material is ascribed to the occurrence of bond- and site-centered charge order. Dielectric response typical for relaxor ferroelectricity is found deep in the charge-ordered state. We suggest an explanation in terms of the existence of polar and nonpolar stacks of the organic molecules in this material, preventing long-range ferroelectricity. The results are discussed in relation to the formation or absence of electronic polar order in related charge-transfer salts.
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Electric-field-dependent pulse measurements are reported in the charge-ordered state of alpha-(BEDT-TTF)2I3. At low electric fields up to about 50 V/cm only negligible deviations from Ohmic behavior can be identified with no threshold field. At larger electric fields and up to about 100 V/cm a reproducible negative differential resistance is observed with a significant change in shape of the measured resistivity in time. These changes critically depend whether constant voltage or constant current is applied to the single crystal. At high enough electric fields the resistance displays a dramatic drop down to metallic values and relaxes subsequently in a single-exponential manner to its low-field steady-state value. We argue that such an electric-field induced negative differential resistance and switching to transient states are fingerprints of cooperative domain-wall dynamics inherent to two-dimensional bond-charge density wave with ferroelectric-like nature.
The charge response of charge-ordered state in the organic conductor alpha-(BEDT-TTF)2I3 is characterized by dc resistivity, dielectric and optical spectroscopy in different crystallographic directions within the two-dimensional conduction layer. Two dielectric modes are detected. The large mode is related to the phason-like excitation of the 2kF bond-charge density wave which forms in the ab plane. The small dielectric mode is associated with the motion of domain-wall pairs along the a- and b-axes between two types of domains which are created due to inversion symmetry breaking.
We report on the anisotropic response, the charge and lattice dynamics of normal and charge-ordered phases with horizontal stripes in single crystals of the organic conductor alpha-(BEDT-TTF)2I3 determined by dc resistivity, dielectric and optical spectroscopy. An overdamped Drude response and a small conductivity anisotropy observed in optics is consistent with a weakly temperature dependent dc conductivity and anisotropy at high temperatures. The splitting of the molecular vibrations nu27(Bu) evidences the abrupt onset of static charge order below TCO=136 K. The drop of optical conductivity measured within the ab plane of the crystal is characterized by an isotropic gap that opens of approximately 75 meV with several phonons becoming pronounced below. Conversely, the dc conductivity anisotropy rises steeply, attaining at 50 K a value 25 times larger than at high temperatures. The dielectric response within this plane reveals two broad relaxation modes of strength Deltaepsilon_LD ~= 5000 and Deltaepsilon_SD ~= 400, centered at 1 kHz < f_LD < 100 MHz and f_SD ~= 1 MHz. The anisotropy of the large-mode (LD) mean relaxation time closely follows the temperature behavior of the respective dc conductivity ratio. We argue that this phason-like excitation is best described as a long-wavelength excitation of a 2kF bond-charge density wave expected theoretically for layered quarter-filled electronic systems with horizontal stripes. Conversely, based on the theoretically expected ferroelectric-like nature of the charge-ordered phase, we associate the small-mode (SD) relaxation with the motion of domain-wall pairs, created at the interface between two types of domains, along the a and b axes. We also consider other possible theoretical interpretations and discuss their limitations.
The effects of electron correlation in the quasi-two-dimensional organic conductor alpha-(BEDT-TTF)2I3 are investigated theoretically by using an extended Hubbard model with on-site and nearest-neighbor Coulomb interactions. A variational Monte Carlo method is applied to study its ground-state properties. We show that there appears a nonmagnetic horizontal-stripe charge order in which nearest-neighbor correlation functions indicate a tendency toward a spin-singlet formation on the bonds with large transfer integrals along the charge-rich stripe. Under uniaxial pressure, a first-order transition from the nonmagnetic charge order to a zero-gap state occurs. Our results on a spin correlation length in the charge-ordered state suggest that a spin gap is almost unaffected by the uniaxial pressure in spite of the suppression of the charge disproportionation. The relevance of these contrasting behaviors in spin and charge degrees of freedom to recent experimental observations is discussed.
$alpha$-(BEDT-TTF)$_2$I$_3$ is a prominent example of charge ordering among organic conductors. In this work we explore the details of transport within the charge-ordered as well as semimetallic phase at ambient pressure. In the high-temperature semimetallic phase, the mobilities and concentrations of both electrons and holes conspire in such a way to create an almost temperature-independent conductivity as well as a low Hall effect. We explain these phenomena as a consequence of a predominantly inter-pocket scattering which equalizes mobilities of the two types of charge carriers. At low temperatures, within the insulating charge-ordered phase two channels of conduction can be discerned: a temperature-dependent activation which follows the mean-field behavior, and a nearest-neighbor hopping contribution. Together with negative magnetoresistance, the latter relies on the presence of disorder. The charge-ordered phase also features a prominent dielectric peak which bears a similarity to relaxor ferroelectrics. Its dispersion is determined by free-electron screening and pushed by disorder well below the transition temperature. The source of this disorder can be found in the anion layers which randomly perturb BEDT-TTF molecules through hydrogen bonds.
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