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Register a new userOnsager phase factor of quantum oscillations in the organic metal theta-(BEDT-TTF)4CoBr4(C6H4Cl2)
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Authors
Alain Audouard
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De Haas-van Alphen oscillations are studied for Fermi surfaces illustrating the Pippards model, commonly observed in multiband organic metals. Field- and temperature-dependent amplitude of the various Fourier components, linked to frequency combinations arising from magnetic breakdown between different bands, are considered. Emphasis is put on the Onsager phase factor of these components. It is demonstrated that, in addition to the usual Maslov index, field-dependent phase factors must be considered to precisely account for the data at high magnetic field. We present compelling evidence of the existence of such contributions for the organic metal theta-(BEDT-TTF)4CoBr4(C6H4Cl2).
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Interlayer magnetoconductance of the quasi-two dimensional organic metal (BEDT-TTF)8Hg4Cl12(C6H5Cl)2 has been investigated in pulsed magnetic fields extending up to 36 T and in the temperature range from 1.6 to 15 K. A complex oscillatory spectrum, built on linear combinations of three basic frequencies only is observed. These basic frequencies arise from the compensated closed hole and electron orbits and from the two orbits located in between. The field and temperature dependencies of the amplitude of the various oscillation series are studied within the framework of the coupled orbits model of Falicov and Stachowiak. This analysis reveals that these series result from the contribution of either conventional Shubnikov-de Haas effect (SdH) or quantum interference (QI), both of them being induced by magnetic breakthrough. Nevertheless, discrepancies between experimental and calculated parameters indicate that these phenomena alone cannot account for all of the data. Due to its low effective mass, one of the QI oscillation series - which corresponds to the whole first Brillouin zone area - is clearly observed up to 13 K.
The critical cooling rate $R_{rm c}$ above which charge ordering is kinetically avoided upon cooling, which results in charge-glass formation, was investigated for the geometrically frustrated system $theta$-(BEDT-TTF)$_2X$. X-ray diffraction experiments revealed that $theta$-(BEDT-TTF)$_2$TlCo(SCN)$_4$ exhibits a horizontally charge-ordered state, and kinetic avoidance of this state requires rapid cooling of faster than 150 K/min. This value is markedly higher than that reported for two other isostructural $theta$-type compounds, thus demonstrating the lower charge-glass-forming ability of $X$ $=$ TlCo(SCN)$_4$. In accounting for the systematic variations of $R_{rm c}$ among the three $theta$-(BEDT-TTF)$_2X$, we found that stronger charge frustration leads to superior charge-glass former. Our results suggest that charge frustration tends to slow the kinetics of charge ordering.
The dielectric constant and ac conductivity have been measured for the layered organic conductor theta-(BEDT-TTF)_2CsZn(SCN)_4 along the out-of-plane direction, which show a relaxation behavior similar to those in the charge-density-wave conductor. Most unexpectedly, they exhibit a large bias dependence with a hysteresis, and changes in magnitude by 100-1000 times at a threshold. These findings are very similar to the collective excitation of the charge density wave. theta-$(BEDT-TTF)_2CsZn(SCN)_4 has collective excitations associated with charge ordering, though it shows no clear indication of long range order.
Using the Lanczos exact-diagonalization and density-matrix renormalization group methods, we study the extended Hubbard model at quarter filling defined on the anisotropic triangular lattice. We focus on charge ordering (CO) phenomena induced by onsite and intersite Coulomb interactions. We determine the ground-state phase diagram including three CO phases, i.e., diagonal, vertical, and three-fold CO phases, based on the calculated results of the hole density and double occupancy. We also calculate the dynamical density-density correlation functions and find possible coexistence of the diagonal and three-fold charge fluctuations in a certain parameter region where the onsite and intersite interactions compete. Furthermore, the characteristic features of the optical conductivity for each CO phase are discussed.
The organic charge-transfer salt $kappa$-(BEDT-TTF)$_{2}$Hg(SCN)$_{2}$Br is a quasi two-dimensional metal with a half-filled conduction band at ambient conditions. When cooled below $T=80$ K it undergoes a pronounced transition to an insulating phase where the resistivity increases many orders of magnitude. In order to elucidate the nature of this metal-insulator transition we have performed comprehensive transport, dielectric and optical investigations. The findings are compared with other dimerized $kappa$-(BEDT-TTF) salts, in particular the Cl-analogue, where a charge-order transition takes place at $T_{rm CO}=30$ K.
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