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Register a new userUnconventional critical behaviour in a quasi-two-dimensional organic conductor
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Changing the interactions between particles in an ensemble-by varying the temperature or pressure, for example-can lead to phase transitions whose critical behaviour depends on the collective nature of the many-body system. Despite the diversity of ingredients, which include atoms, molecules, electrons and their spins, the collective behaviour can be grouped into several families (called universality classes) represented by canonical spin models1. One kind of transition, the Mott transition2, occurs when the repulsive Coulomb interaction between electrons is increased, causing wave-like electrons to behave as particles. In two dimensions, the attractive behaviour responsible for the superconductivity in high-transition temperature copper oxide3,4 and organic5-7 compounds appears near the Mott transition, but the universality class to which two-dimensional, repulsive electronic systems belongs remains unknown. Here we present an observation of the critical phenomena at the pressure-induced Mott transition in a quasi-two-dimensional organic conductor using conductance measurements as a probe. We find that the Mott transition in two dimensions is not consistent with known universality classes, as the observed collective behaviour has previously not been seen. This peculiarity must be involved in any emergent behaviour near the Mott transition in two dimensions.
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We investigated the effect of magnetic field on the highly correlated metal near the Mott transition in the quasi-two-dimensional layered organic conductor, $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, by the resistance measurements under control of temperature, pressure, and magnetic field. It was demonstrated that the marginal metallic phase near the Mott transition is susceptible to the field-induced localization transition of the first order, as was predicted theoretically. The thermodynamic consideration of the present results gives a conceptual pressure-field phase diagram of the Mott transition at low temperatures.
We study the electronic structure of the quasi-one-dimensional organic conductor TTF-TCNQ by means of density-functional band theory, Hubbard model calculations, and angle-resolved photoelectron spectroscopy (ARPES). The experimental spectra reveal significant quantitative and qualitative discrepancies to band theory. We demonstrate that the dispersive behavior as well as the temperature-dependence of the spectra can be consistently explained by the finite-energy physics of the one-dimensional Hubbard model at metallic doping. The model description can even be made quantitative, if one accounts for an enhanced hopping integral at the surface, most likely caused by a relaxation of the topmost molecular layer. Within this interpretation the ARPES data provide spectroscopic evidence for the existence of spin-charge separation on an energy scale of the conduction band width. The failure of the one-dimensional Hubbard model for the {it low-energy} spectral behavior is attributed to interchain coupling and the additional effect of electron-phonon interaction.
We have measured the high field magnetoresistence and magnetization of quasi-one- dimensional (Q1D) organic conductor (Per)2Pt(mnt)2 (where Per = perylene and mnt = maleonitriledithiolate), which has a charge density wave (CDW) ground state at zero magnetic field below 8 K. We find that the CDW ground state is suppressed with moderate magnetic fields of order 20 T, as expected from a mean field theory treatment of Pauli effects[W. Dieterich and P. Fulde, Z. Physik 265, 239 - 243 (1973)]. At higher magnetic fields, a new, density wave state with sub-phases is observed in the range 20 to 50 T, which is reminiscent of the cascade of field induced, quantized, spin density wave phases (FISDW) observed in the Bechgaard salts. The new density wave state, which we tenatively identify as a field induced charge density wave state (FICDW), is re-entrant to a low resistance state at even higher fields, of order 50 T and above. Unlike the FISDW ground state, the FICDW state is only weakly orbital, and appears for all directions of magnetic field. Our findings are substantiated by electrical resistivity, magnetization, thermoelectric, and Hall measurements. We discuss our results in light of theoretical work involving magnetic field dependent Q1D CDW ground states in high magnetic fields [D. Zanchi, A. Bjelis, and G. Montambaux, Phys. Rev. B 53, (1996)1240; A. Lebed, JETP Lett. 78,138(2003)].
Although the isotope effect in superconducting materials is well-documented, changes in the magnetic properties of antiferromagnets due to isotopic substitution are seldom discussed and remain poorly understood. This is perhaps surprising given the possible link between the quasi-two-dimensional (Q2D) antiferromagnetic and superconducting phases of the layered cuprates. Here we report the experimental observation of shifts in the N{e}el temperature and critical magnetic fields ($Delta T_{rm N}/T_{rm N}approx 4%$; $Delta B_{rm c}/B_{rm c}approx 4%$) in a Q2D organic molecular antiferromagnets on substitution of hydrogen for deuterium. These compounds are characterized by strong hydrogen bonds through which the dominant superexchange is mediated. We evaluate how the in-plane and inter-plane exchange energies evolve as the hydrogens on different ligands are substituted, and suggest a possible mechanism for this effect in terms of the relative exchange efficiency of hydrogen and deuterium bonds.
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.
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