Conducting Metal Dithiolene Complexes:  Structural and Electronic Properties

Kato, Reìzo

doi:10.1021/cr030655t

Cited by 470 publications

(357 citation statements)

References 180 publications

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“…This behaviour is explainable only by the effect of frustration, which efficiently suppresses the growth of antiferromagnetic correlation. Similar behaviour has been found in κ-(BEDT-TTF) 2 Cu 2 (CN) 3 [4] and a few other materials [7][8][9]. Most Z [Pd(dmit) 2 ] 2 salts exhibit antiferromagnetic ordering at lower temperatures [2], while no magnetic phase transition is detected in κ-(BEDT-TTF) 2 Cu 2 (CN) 3 down to very low temperatures, which is viewed as the first evidence for a gapless spin-liquid state realised in κ-(BEDT-TTF) 2 Cu 2 (CN) 3 [4].…”

Section: Introductionsupporting

confidence: 83%

“…Two classes of compounds have been hitherto known to give 2D triangular antiferromagnets: the Z [Pd(dmit) 2 ] 2 salts [2] (for a comprehensive review article see [3]) and κ-(BEDT-TTF) 2 X salts [4] (for review see [5,6]), where BEDT-TTF = bis(ethylenedithio)tetrathiafulvalene, and Z and X are monovalent cation and anion, respectively (scheme 1 shows their chemical structures). Characteristic behaviour of frustrated spins has been observed through the temperature dependence of magnetic susceptibility χ in several Z [Pd(dmit) 2 ] 2 salts [2].…”

Section: Introductionmentioning

confidence: 99%

“…Some of the observed phenomena [13][14][15] can never be expected for the single-level systems such as the conventional TTF-based conductors. From a quantum chemical viewpoint, the HOMO-LUMO interchange is based not only on the strong dimerization but also on the symmetries of HOMO and LUMO, which are characteristic of the metal-dithiolene complexes [3]. The material design inspired by these features has been developed; it leads to the single-component molecular metals based on Ni(tmdt) 2 (tmdt = trimethylenetetrathiafulvalenedithiolate) [27].…”

Section: Introductionmentioning

confidence: 99%

“…In this article, only typical experimental data are explicitly referred to. The structural and electrical data for a wide range of related compounds can be found in the comprehensive review [3] and references therein. …”

Section: Introductionmentioning

confidence: 99%

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Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Tamura

Kato

2009

Science and Technology of Advanced Materials

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Recent studies on the physical properties of the triangular system based on the Pd(dmit) 2 salts (dmit = 1,3-dithiole-2-thione-4,5-dithiolate) are reviewed. Quantum chemical architectures of the Pd(dmit) 2 molecule and its dimer are introduced with emphasis on the strong dimerization of a two-level system, which provides unique physical properties of the salts. The magnetic properties are outlined in view of the magneto-structural correlation specific to the frustrated spin systems. Some newly discovered ground states and their origins are discussed, for which the valence bond formation plays a key role. Among them, the two-level structure is crucial for the novel charge-separated state found in two salts. The valence bond ordering, similar to the spin-Peierls transition, has been found in a two-dimensional frustrated spin system. The physical aspects and possible relation to the pressure-induced superconductivity are discussed.

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Section: Introductionsupporting

confidence: 83%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Tamura

Kato

2009

Science and Technology of Advanced Materials

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“…The ground state is, however, settled into a spin-gapped phase by the lattice distortion via the spin-phonon coupling at 25 K, as shown in Fig. 1 inset [8,10], while most of the Pd(dmit) 2 salts having anisotropic triangular lattice (0.55 < t ′ /t < 0.85) show antiferromagnetic order [9]. Application of hydrostatic pressure, which increases the bandwidth, induces a superconducting transition at T c = 5 K [8].…”

mentioning

confidence: 99%

Mott Transition in a Valence-Bond Solid Insulator with a Triangular Lattice

et al. 2007

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We have investigated the Mott transition in a quasi-two-dimensional Mott insulator EtMe3P[Pd(dmit)2]2 with a spin-frustrated triangular lattice in hydrostatic pressure and magnetic field. In the pressure-temperature (P -T ) phase diagram, a valence bond solid phase is found to neighbor the superconductor and metal phases at low temperatures. The profile of the phase diagram is common to those of Mott insulators with antiferromagnetic order. In contrast to the antiferromagnetic Mott insulators, the resistivity in the metallic phase exhibits anomalous temperature dependence, ρ = ρ0 + AT 2.5 .PACS numbers: 71.20. Rv, 71.30.+h, 74.25.Nf, 74.70.Kn The Mott transition has been one of the fundamental issues in condensed matter physics [1]. Much attention has been paid on the superconducting state near the Mott transition in transition metal compounds [2] and in organic materials [3]. Mott insulators so far studied usually exhibit antiferromagnetic long-range order, and the relation between the existence of the ordered state and the appearance of superconducting states has been widely discussed [2] [7], in which the metal-insulator transition has not been accessible. Thus the Mott transition and superconductivity appearing from the quantum disordered state have been longed for the last few decades.Here we show that an organic material is a good playground of the quantum spin physics on the frustrated lattice accessible to Mott physics. An anion radical salt EtMe 3 P[Pd(dmit) 2 ] 2 is the 2D VBS Mott insulator synthesized recently [8], where Et and Me denote C 2 H 5 and CH 3 respectively, and Pd(dmit) 2 (dmit = 1,3-dithiole-2-thione-4,5-dithiolate, C 3 S 2− 5 ) is an electron-acceptor molecule. Its crystal structure consists of two layers: the Pd(dmit) 2 layer that involves in conduction and magnetism, and the insulating closed-shell EtMe 3 P + layer. In the conduction layer, pairs of Pd(dmit) 2 molecules form dimers arranged in a triangular lattice in terms of transfer integrals, t and t ′ (t ′ /t = 1.05) [see Fig. 1 inset]. The conduction band is half filling, consisting of an anitibonding combination of the highest-occupied molecular orbital of Pd(dmit) 2 [9]. The large onsite Coulomb interaction in the dimer, compared with the bandwidth, produces a Mott-Hubbard insulating state with a spin-1/2 at each dimer site. The magnetic susceptibility behaves in accordance with the triangular-lattice antiferromagnetic Heisenberg model over a wide temperature range (60 K < T < 300 K) with J = 250 K [10], indicating the presence of spin frustration and hence highly degenerate ground states. The ground state is, however, settled into a spin-gapped phase by the lattice distortion via the spin-phonon coupling at 25 K, as shown in Fig. 1 inset [8,10], while most of the Pd(dmit) 2 salts having anisotropic triangular lattice (0.55 < t ′ /t < 0.85) show antiferromagnetic order [9]. Application of hydrostatic pressure, which increases the bandwidth, induces a superconducting transition at T c = 5 K [8]. However, the nature of the ins...

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Structure and Properties of d ⁸ Metal–Dithiolene Complexes

Deplano

Mercuri

Serpe

et al. 2010

Patai's Chemistry of Functional Groups

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Conducting Metal Dithiolene Complexes: Structural and Electronic Properties

Cited by 470 publications

References 180 publications

Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Mott Transition in a Valence-Bond Solid Insulator with a Triangular Lattice

Structure and Properties of d ⁸ Metal–Dithiolene Complexes

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Conducting Metal Dithiolene Complexes: Structural and Electronic Properties

Cited by 470 publications

References 180 publications

Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)2

Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)2

Mott Transition in a Valence-Bond Solid Insulator with a Triangular Lattice

Structure and Properties of d 8 Metal–Dithiolene Complexes

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Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Variety of valence bond states formed of frustrated spins on triangular lattices based on a two-level system Pd(dmit)₂

Structure and Properties of d ⁸ Metal–Dithiolene Complexes