Spectroscopic evidence for the low-temperature charge-separated state of [Pd(dmit)2] salts

Tamura, Masafumi; Takenaka, K.; Takagi, H.; Sugai, S.; Tajima, Akiko; Kato, Reìzo

doi:10.1016/j.cplett.2005.06.026

Cited by 50 publications

(52 citation statements)

References 13 publications

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“…More sophisticated calculations support this conclusion [24][25][26]. A novel phase transition is driven by this effect in some Z [Pd(dmit) 2 ] 2 salts [13][14][15]. Some of the observed phenomena [13][14][15] can never be expected for the single-level systems such as the conventional TTF-based conductors.…”

Section: Introductionmentioning

confidence: 55%

“…The calculations predict 1 : 2 splitting of the bonding-antibonding photo-excitation appearing in the near-IR region [14]. In fact, the reflectivity spectra exhibit the expected splitting of the near-IR peak at low temperatures [14].…”

Section: A Novel Charge Separation In the Et 2 Me 2 Sb Saltmentioning

confidence: 90%

“…Like in the BEDT-TTF salts, a 2D band structure based on Pd(dmit) 2 HOMO plays a significant role in the Z [Pd(dmit) 2 ] 2 series. The band calculations [3,[24][25][26] [14,[21][22][23]. It is also noticeable that the bonding-anti-bonding splitting of HOMOs and LUMOs are nearly the same.…”

Section: Quantum Chemical Background: Molecular Characteristics Of Pdmentioning

confidence: 92%

“…For example, the χ behaviour showing strong frustration effect is commonly observed in many Z [Pd(dmit) 2 ] 2 salts [2], whereas, among the κ-(BEDT-TTF) 2 X salts, only the Cu 2 (CN) 3 salt exhibits such behaviour [4], the other κ-salts being metals or paramagnetic insulators with significant antiferromagnetic correlation [5,6]. In the Z [Pd(dmit) 2 ] 2 series, in contrast, a variety of unconventional valence bond states [13][14][15][16][17] appear around the spin-frustrated state depending on the cation and pressure. For this reason, the Z [Pd(dmit) 2 ] 2 series occupy a unique position in molecular materials.…”

Section: Introductionmentioning

confidence: 99%

“…A novel phase transition is driven by this effect in some Z [Pd(dmit) 2 ] 2 salts [13][14][15]. 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].…”

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: Introductionmentioning

confidence: 55%

Section: A Novel Charge Separation In the Et 2 Me 2 Sb Saltmentioning

confidence: 90%

Section: Quantum Chemical Background: Molecular Characteristics Of Pdmentioning

confidence: 92%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

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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Crystal structure and band parameters of mixed crystals derived from quantum spin liquid β′‐EtMe₃Sb[Pd(dmit)₂]₂ (dmit = 1,3‐dithiol‐2‐thione‐4,5‐dithiolate)

Kato

Fukunaga

Yamamoto

et al. 2012

Physica Status Solidi (b)

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altering its crystal symmetry. The mixing ratio and lattice parameters of these mixed crystals can be continuously tuned. We calculated intermolecular transfer integrals between highest occupied molecular orbitals (HOMOs) based on structural data. Increasing the number of ethyl groups at the cation site reduces the anisotropy of the triangular lattice, and the dimer units form an almost regular triangular lattice in pure Et 2 Me 2 Sb salt. In this process, the Pd(dmit) 2 molecule is slightly curved to exhibit a crescent shape. This distortion plays an important role in tuning the interdimer transfer integrals.

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Rich variety in the ground states of [Pd(dmit)₂]₂ salts, and the methodology for analysing intra‐dimer interactions, inter‐dimer interactions and MO levels

Yamamoto

Nakazawa

Tamura

et al. 2012

Physica Status Solidi (b)

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A group of [Pd(dmit) 2 ] 2 salts, whose two-dimensional structures take (pesudo-) triangular lattice, has a diversity in the ground states. In order to investigate the ground states, we have developed the methodology for analysing subtle changes in the inter-molecular interactions and MO level using the vibrational and electronic spectroscopy. This methodology is applied to several [Pd(dmit) 2 ] 2 salts. We have found some relationships between the ground states and the inter-dimer and intra-dimer interactions under HOMO-LUMO inversion.

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Spectroscopic evidence for the low-temperature charge-separated state of [Pd(dmit)2] salts

Cited by 50 publications

References 13 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

Crystal structure and band parameters of mixed crystals derived from quantum spin liquid β′‐EtMe₃Sb[Pd(dmit)₂]₂ (dmit = 1,3‐dithiol‐2‐thione‐4,5‐dithiolate)

Rich variety in the ground states of [Pd(dmit)₂]₂ salts, and the methodology for analysing intra‐dimer interactions, inter‐dimer interactions and MO levels

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Spectroscopic evidence for the low-temperature charge-separated state of [Pd(dmit)2] salts

Cited by 50 publications

References 13 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

Crystal structure and band parameters of mixed crystals derived from quantum spin liquid β′‐EtMe3Sb[Pd(dmit)2]2 (dmit = 1,3‐dithiol‐2‐thione‐4,5‐dithiolate)

Rich variety in the ground states of [Pd(dmit)2]2 salts, and the methodology for analysing intra‐dimer interactions, inter‐dimer interactions and MO levels

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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

Crystal structure and band parameters of mixed crystals derived from quantum spin liquid β′‐EtMe₃Sb[Pd(dmit)₂]₂ (dmit = 1,3‐dithiol‐2‐thione‐4,5‐dithiolate)

Rich variety in the ground states of [Pd(dmit)₂]₂ salts, and the methodology for analysing intra‐dimer interactions, inter‐dimer interactions and MO levels