“…In particular, (DMe-DCNQI) 2 Ag (R 1 = R 2 = Me) presents high-temperature 4k F and 2k F structural instabilities, diverging successively into a 4k F order just followed by a 2k F SP-like transition. [40][41][42] The compound (DI-DCNQI) 2 Ag (R 1 = R 2 = I) exhibits also a high-temperature 1D 4k F structural instability diverging into a 4k F order 43 but stabilizes an AF ground state at lower temperature. [44][45][46] However, a recent synchrotron study 33 has revealed the occurrence of a complex 4k F modulation pattern consisting of three types of 4k F order: one with charges on the sites (CO), one with charges on the bonds (DM), and one chain with the presence of charges on both sites and bonds.…”
The 2:1 family of organic salts (o-DMTTF) 2 X (X = Cl, Br, I) exhibits regular stacks and a high-symmetry structure, which provide a perfect three-quarter-filling-band system allowing a rich phase diagram in the presence of strong electronic correlations. In this paper, we present a detailed study of this series combining complementary experimental techniques such as resistivity, thermopower, electron spin resonance, static magnetic measurements, and x-ray diffraction. In particular, we show that at ambient pressure (o-DMTTF) 2 X with X = Br and Cl undergoes two successive phase transitions setting successively a 4k F charge density and bond order wave order, then a spin-Peierls (SP) ground state. We discuss the symmetry of these phases and its relationship with the transport and magnetic properties. These phases are also followed under pressure by transport experiments, allowing the establishment of a generic phase diagram for this series of salts, where, with the onset of a one-dimensional to three-dimensional deconfinement transition, the 4k F order vanishes and the SP ground state transforms into a Peierls one. Interestingly, this phase diagram differs significantly from the one previously reported in other three-quarter-filled systems such as (TMTTF) 2 X and δ-(EDT-TTF-CONMe 2 ) 2 X.
“…In particular, (DMe-DCNQI) 2 Ag (R 1 = R 2 = Me) presents high-temperature 4k F and 2k F structural instabilities, diverging successively into a 4k F order just followed by a 2k F SP-like transition. [40][41][42] The compound (DI-DCNQI) 2 Ag (R 1 = R 2 = I) exhibits also a high-temperature 1D 4k F structural instability diverging into a 4k F order 43 but stabilizes an AF ground state at lower temperature. [44][45][46] However, a recent synchrotron study 33 has revealed the occurrence of a complex 4k F modulation pattern consisting of three types of 4k F order: one with charges on the sites (CO), one with charges on the bonds (DM), and one chain with the presence of charges on both sites and bonds.…”
The 2:1 family of organic salts (o-DMTTF) 2 X (X = Cl, Br, I) exhibits regular stacks and a high-symmetry structure, which provide a perfect three-quarter-filling-band system allowing a rich phase diagram in the presence of strong electronic correlations. In this paper, we present a detailed study of this series combining complementary experimental techniques such as resistivity, thermopower, electron spin resonance, static magnetic measurements, and x-ray diffraction. In particular, we show that at ambient pressure (o-DMTTF) 2 X with X = Br and Cl undergoes two successive phase transitions setting successively a 4k F charge density and bond order wave order, then a spin-Peierls (SP) ground state. We discuss the symmetry of these phases and its relationship with the transport and magnetic properties. These phases are also followed under pressure by transport experiments, allowing the establishment of a generic phase diagram for this series of salts, where, with the onset of a one-dimensional to three-dimensional deconfinement transition, the 4k F order vanishes and the SP ground state transforms into a Peierls one. Interestingly, this phase diagram differs significantly from the one previously reported in other three-quarter-filled systems such as (TMTTF) 2 X and δ-(EDT-TTF-CONMe 2 ) 2 X.
“…These systems are members of DCNQI 2 X (X: monovalent metal cation X + , e.g., Ag and Li) 38,39 and TM 2 X (X: monovalent anion X − , e.g., PF 6 , AsF 6 , SCN, and Br), 23 respectively, both having quasi-1D structures. DC-NQI stands for the R 1 R 2 -DCNQI molecule where R 1 , R 2 are sustituents such as CH 3 , Br, I, etc.…”
Esta es la versión de autor del artículo publicado en: This is an author produced version of a paper published in: El acceso a la versión del editor puede requerir la suscripción del recurso Access to the published version may require subscription (Received February 4, 2008) Theoretical studies on charge ordering phenomena in quarter-filled molecular (organic) conductors are reviewed. Extended Hubbard models including not only the on-site but also the inter-site Coulomb repulsion are constructed in a straightforward way from the crystal structures, which serve for individual study on each material as well as for their systematic understandings. In general the inter-site Coulomb interaction stabilizes Wigner crystal-type charge ordered states, where the charge localizes in an arranged manner avoiding each other, and can drive the system insulating. The variety in the lattice structures, represented by anisotropic networks in not only the electron hopping but also in the inter-site Coulomb repulsion, brings about diverse problems in low-dimensional strongly correlated systems. Competitions and/or co-existences between the charge ordered state and other states are discussed, such as metal, superconductor, and the dimer-type Mott insulating state which is another typical insulating state in molecular conductors. Interplay with magnetism, e.g., antiferromagnetic state and spin gapped state for example due to the spin-Peierls transition, is considered as well. Distinct situations are pointed out: influences of the coupling to the lattice degree of freedom and effects of geometrical frustration which exists in many molecular crystals. Some related topics, such as charge order in transition metal oxides and its role in new molecular conductors, are briefly remarked.
“…Meanwhile, (DI-DCNQI) 2 Ag has a considerable conductivity in the transverse direction and it is an insulator already at room temperature. From the activation plot, the charge gap is estimated to be 490K [10]. (DMe-DCNQI) 2 Ag becomes a spin-Peierls state at about 80K so that it has a finite spin gap at zero temperature.…”
Section: E Effects Of a Cutoff In The Logarithmic Singularitymentioning
confidence: 99%
“…(DMe-DCNQI) 2 Ag becomes a spin-Peierls state at about 80K so that it has a finite spin gap at zero temperature. Meanwhile, (DI-DCNQI) 2 Ag becomes antiferromagnetic below 5.5K [10] so that the spin excitation spectrum is gapless. The Mott insulator in the present study is expected to become an antiferromagnetic [or spin-density-wave (SDW)] state when weak three-dimensionality is taken into account because the repulsive interaction would produce an effective antiferromagnetic coupling in the transverse direction.…”
Section: E Effects Of a Cutoff In The Logarithmic Singularitymentioning
confidence: 99%
“…[9] At low temperatures, (DMe-DCNQI) 2 Ag becomes a spin-Peierls state, while (DI-DCNQI) 2 Ag becomes an antiferromagnet. [10] Thus electron correlation in the π band also plays an essential role to determine the ground-state phases.…”
Metal-insulator transitions and different ground-state phases in quasi-one-dimensional materials, (R1R2-DCNQI)2M (R1=R2=CH3, I and M=Ag, Cu), are studied with a renormalization-group method. We use one-dimensional continuum models with backward scatterings, umklapp processes and couplings with 2kF and 4kF phonons (not static lattice distortion). We take a quarter-filled band for M=Ag and a sixth-filled band coupled with a third-filled band for M=Cu. Depending on electron-electron and electron-phonon coupling strengths, the ground-state phase becomes a Tomonaga-Luttinger liquid or a state with a gap(s). For M=Ag, there appear a spin-gap state with a dominant 2kF charge-density-wave correlation, a Mott insulator with a dominant 4kF chargedensity-wave correlation, or a spin-Peierls state with different magnitudes of spin and charge gaps. Three-dimensionality is taken into account by cutting off the logarithmic singularity in either the particle-particle channel or the particle-hole channel. The difference between the ground-state phase of the R1=R2=CH3 salt (spin-Peierls state) and that of the R1=R2=I salt (antiferromagnetic state) is qualitatively explained by a difference in the cutoff energy in the particle-particle channel. For M=Cu, there appear a Mott insulator with a charge density wave of period 3 and a Peierls insulator with a charge density wave of period 6. The conditions for the experimentally observed, Mott insulator phase are strong correlation in the sixth-filled band, moderate electron-phonon couplings, and finite electron-4kF phonon coupling. Resistance is calculated as a function of temperature with a memory-function approximation in both cases above. It qualitatively reproduces the differences among the M=Ag and M=Cu cases as well as the R1=R2=CH3 and R1=R2=I cases.
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