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Register a new userDimer-Mott and charge-ordered insulating states in the quasi-one-dimensional organic conductors $delta_{P}$- and $delta_{C}$-(BPDT-TTF)$_2$ICl$_2$
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Added by
Kenichiro Hashimoto
Publication date
2017
fields
Physics
and research's language is
English
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We investigated the electronic states of the quasi-one-dimensional organic conductors $delta_{P}$-(BPDT-TTF)$_2$ICl$_2$ and $delta_{C}$-(BPDT-TTF)$_2$ICl$_2$, both of which are insulating at room temperature owing to strong electron correlations. Through measurements of electrical resistivity, optical conductivity, and magnetic susceptibility, as well as band-structure calculations, we have revealed that the two materials possess completely different ground states, even though they have the same chemical composition and stacking configuration of the donor molecules. We have found that the $delta_P$-type salt with an effective half-filled band behaves as a dimer-Mott (DM) insulator and exhibits a nonmagnetic transition at 25 K, whereas the $delta_C$-type salt with a 3/4-filled band shows a charge ordering (CO) transition just above room temperature and becomes nonmagnetic below 20 K. The optical spectra of the $delta_P$-type salt are composed of two characteristic bands due to intra- and interdimer charge transfers, supporting the DM insulating behavior arising from the strong on-site Coulomb interaction. By contrast, in the $delta_C$-type salt, a single band characterizing the formation of CO arising from the off-site Coulomb interactions is observed. Upon lowering the temperature, the shape of the optical spectra in the $delta_C$-type salt becomes asymmetric and shifts to much lower frequencies, suggesting the emergence of domain-wall excitations with fractional charges expected in a one-dimensional CO chain. The temperature dependence of the magnetic susceptibility of the $delta_P$-type salt is well described by a 2D spin-1/2 Heisenberg AFM model on an anisotropic square lattice in the dimerized picture, while in the $delta_C$-type salt, it can be explained by a 2D spin-1/2 Heisenberg AFM model on an anisotropic honeycomb lattice formed in the CO state.
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To elucidate the pressure evolution of the electronic structure in an antiferromagnetic dimer-Mott (DM) insulator ${beta}^{prime}$-(BEDT-TTF)$_2$ICl$_2$, which exhibits superconductivity at 14.2 K under 8 GPa, we measured the polarized infrared (IR) optical spectra under high pressure. At ambient pressure, two characteristic bands due to intra- and interdimer charge transfers have been observed in the IR spectra, supporting that this salt is a typical half-filled DM insulator at ambient pressure. With increasing pressure, however, the intradimer charge transfer excitation shifts to much lower energies, indicating that the effective electronic state changes from half-filled to 3/4-filled as a result of weakening of dimerization. This implies that the system approaches a charge-ordered state under high pressure, in which charge degrees of freedom emerge as an important factor. The present results suggest that charge fluctuation inside of dimers plays an important role in the high-temperature superconductivity.
The recently proposed multiferroic state of the charge-transfer salt {kappa}-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl [P. Lunkenheimer et al., Nature Mater., vol. 11, pp. 755-758, Sept. 2012] has been studied by dc-conductivity, magnetic susceptibility and measurements of the dielectric constant on various, differently prepared single crystals. In the majority of crystals we confirm the existence of an order-disorder-type ferroelectric state which coincides with antiferromagnetic order. This phenomenology rules out scenarios which consider an inhomogeneous, short-range-ordered ferroelectric state. Measurements of the dielectric constant and the magnetic susceptibility on the same crystals reveal that both transitions lie very close to each other or even collapse, indicating that both types of order are intimately coupled to each other. We address issues of the frequency dependence of the dielectric constant {epsilon} and the dielectric loss {epsilon} and discuss sample-to-sample variations.
The quasi-one-dimensional organic conductors (TMTTF)$_2X$ with non-centrosymmetric anions commonly undergo charge- and anion-order transitions upon cooling. While for compounds with tetrahedral anions ($X$ = BF$_4^-$, ReO$_4^-$, and ClO$_4^-$) the charge-ordered phase is rather well understood, the situation is less clear in the case of planar triangular anions, such as (TMTTF)$_2$NO$_3$. Here we explore the electronic and structural transitions by transport experiments, optical and magnetic spectroscopy. This way we analyze the temperature dependence of the charge imbalance 2$delta$ and an activated behavior of $rho(T)$ with $Delta_{rm CO}approx 530$~K below $T_{rm CO} = 250$~K. Since (TMTTF)$_2$NO$_3$ follows the universal relation between charge imbalance 2$delta$ and size of the gap $Delta_{rm CO}$, our findings suggest that charge order is determined by TMTTF stacks with little influence of the anions. Clear signatures of anion ordering are detected at $T_{rm AO}=50$~K. The tetramerization affects the dc transport, the vibrational features of donors and acceptors, and leads to formation of spin singlets.
We review some properties of quasi-one-dimensional organic conductors, such as the Bechgaard salts, with an emphasis on aspects related to the crossovers between a Mott insulating state to a metallic state, and crossovers between different metallic behaviors. We discuss why a theoretical description of these issues is a particularly challenging problem, and describe a recent non-perturbative approach designed to deal with systems of coupled chains. This method, dubbed chain-DMFT, is a generalization of dynamical mean field theory that treats both, one-dimensional and higher dimensional physics, in a unified manner. We present numerical results for a system of coupled Hubbard chains. Chain-DMFT indeed captures the metal-insulator transition and the dimensional crossover from a high temperature Luttinger liquid to a low temperature Fermi liquid phase, and allows to access the properties of these phases. Based on these results perspectives for a theoretical understanding of the physics of the Bechgaard salts are discussed.
Low-dimensional organic conductors could establish themselves as model systems for the investigation of the physics in reduced dimensions. In the metallic state of a one-dimensional solid, Fermi-liquid theory breaks down and spin and charge degrees of freedom become separated. But the metallic phase is not stable in one dimension: as the temperature is reduced, the electronic charge and spin tend to arrange themselves in an ordered fashion due to strong correlations. The competition of the different interactions is responsible for which broken-symmetry ground state is eventually realized in a specific compound and which drives the system towards an insulating state. Here we review the various ordering phenomena and how they can be identified by optic and magnetic measurements. While the final results might look very similar in the case of a charge density wave and a charge-ordered metal, for instance, the physical cause is completely different. When density waves form, a gap opens in the density of states at the Fermi energy due to nesting of the one-dimension Fermi surface sheets. When a one-dimensional metal becomes a charge-ordered Mott insulator, on the other hand, the short-range Coulomb repulsion localizes the charge on the lattice sites and even causes certain charge patterns. We try to point out the similarities and conceptional differences of these phenomena and give an example for each of them. Particular emphasis will be put on collective phenomena which are inherently present as soon as ordering breaks the symmetry of the system.
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