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, Reìzo; Fukunaga, Tomohiro; Yamamoto, Hiroshi; Ueda, Kunihiro; Cui, Hongchang

doi:10.1002/pssb.201100645

Cited by 12 publications

(19 citation statements)

References 21 publications

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“…Consequently, in a unified phase diagram the three materials are arranged in the order EtMe -AgCN -CuCN on the descending horizontal U/W scale ( Fig. 2h), consistent with ab initio density functional theory (DFT) and extended Hückel calculations (Supplementary information S1, Table S1) [22,23,24,25,11,8].…”

Section: Optical Studiessupporting

confidence: 72%

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Quantum spin liquids unveil the genuine Mott state

et al. 2018

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The localization of charge carriers by electronic repulsion was suggested by Mott in the 1930s to explain the insulating state observed in supposedly metallic NiO. The Mott metal-insulator transition has been subject of intense investigations ever since-not least for its relation to high-temperature superconductivity. A detailed comparison to real materials, however, is lacking because the pristine Mott state is commonly obscured by antiferromagnetism and a complicated band structure. Here we study organic quantum spin liquids, prototype realizations of the single-band Hubbard model in the absence of magnetic order. Mapping the Hubbard bands by optical spectroscopy provides an absolute measure of the interaction strength and bandwidth-the crucial parameters that enter calculations. In this way, we advance beyond conventional temperature-pressure plots and quantitatively compose a generic phase diagram for all genuine Mott insulators based on the absolute strength of the electronic correlations. We also identify metallic quantum fluctuations as a precursor of the Mott insulator-metal transition, previously predicted but never observed. Our results suggest that all relevant phenomena in the phase diagram scale with the Coulomb repulsion U, which provides a direct link to unconventional superconductivity in cuprates and other strongly correlated materials.

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Section: Optical Studiessupporting

confidence: 72%

“…Plate-like organic single crystals were grown during several months by air oxidation in acetone (EtMe) [23,44] and electrochemical oxidation (AgCN and CuCN) [45,25] in RIKEN, Nagoya, Stuttgart and Argonne. The samples reach typical dimensions of 3 and -(BEDT-TTF) 2 Cu 2 (CN) 3 , respectively.…”

Section: Methodsmentioning

confidence: 99%

Quantum spin liquids unveil the genuine Mott state

et al. 2018

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“…Single crystals of P-salt 1, P-salt 2, Sb-salt 1 and Sb-salt 2 were synthesised by aerial oxidation from the acetone solution of [(CH 3 ) 4 P] 2 [Pd(dmit) 2 ], [(C 2 H 5 ) 2 (CH 3 ) 2 P] 2 [Pd(dmit) 2 ], [(CH 3 ) 4 Sb] 2 [Pd(dmit) 2 ] and [(C 2 H 5 )(CH 3 ) 3 Sb] 2 [Pd(dmit) 2 ], respectively 17 . The thickness of the single-crystal of Sb-salt 2 was ca .…”

Section: Methodsmentioning

confidence: 99%

“…The 2D layers of κ -type compounds always consist of isosceles or equilateral triangular lattices 18 , while the 2D layers in X[Pd(dmit) 2 ] 2 can be equilateral, isosceles or scalene lattices, depending on X 17,25 . Therefore, there is a variety of 2D layers that X[Pd(dmit) 2 ] 2 can have, whereas the 2D layers of κ -type compounds are specific.…”

Section: Introductionmentioning

confidence: 99%

Charge and Lattice Fluctuations in Molecule-Based Spin Liquids

Yamamoto

Fujimoto

Naito

et al. 2017

Sci Rep

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Spin liquid (SL) systems have been the subject of much attention recently, as they have been theoretically predicted to not freeze, even at 0 K. Despite extensive searches being made for such a system, only a few candidates have been found. All of these candidates share geometrical frustrations that are based on triangular lattices. We applied vibrational spectroscopy to one of the candidates of a molecule-based SL system, and we compared its results against three antiferromagnetic compounds and four charge-ordered compounds. All of their structural motifs belong to triangular lattices. The C=C stretching modes in the SL state indicated that there were charge and lattice fluctuations. These fluctuations were suppressed but non-negligible in the AF compounds. This finding is potentially significant, as it indicates that a hidden lattice and charge fluctuation are the driving force of a geometrical frustration, which eventually leads to a SL state.

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“…The following two types of mixed crystals have been examined; Me 4 SbEtMe 3 Sb (AFLOQSL), and EtMe 3 SbEt 2 Me 2 Sb (QSLCO) salts. 89 Mass spectrometric analysis revealed that the molar ratios of different crystals vary very little and the mixed crystals are homogeneous. All the mixed crystals retain the space group of C2/c.…”

Section: Award Accountsmentioning

confidence: 99%

Development of π-Electron Systems Based on [M(dmit)2] (M = Ni and Pd; dmit: 1,3-dithiole-2-thione-4,5-dithiolate) Anion Radicals

Kato¹

2014

Bulletin of the Chemical Society of Japan

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Molecular conductors based on [M(dmit)2] (M = Ni and Pd) present a variety of π electron systems that pave the way for a higher stage of solid-state science. Supramolecular interactions between [Ni(dmit) 2 ] anion and halogen-containing cations provide bilayer systems that are characterized by coexistence of two crystallographically independent anion layers with different molecular arrangements and contrasting (for example, metal/insulator and ferromagnetic/antiferromagnetic) properties. In [Pd(dmit) 2 ] salts in the Mott insulating state, a small energy difference between HOMO and LUMO coupled with strong dimerization affords HOMOLUMO band inversion. The dimer units [Pd(dmit) 2 ] 2 ¹ form a triangular lattice, and interplay of strong electron correlation and spin frustration generates a wide variety of magnetic/charge states including antiferromagnetic long-range order, quantum spin liquid, charge order, and valence bond order, depending on counter cations. The cation dependence is attributed to a systematic arch-shaped molecular distortion that tunes the anisotropy of interdimer transfer integrals. This means that the [Pd(dmit) 2 ] molecular skeleton is sufficiently flexible within the crystal field, and molecular degrees of freedom play an important role in fine tuning of the electronic state.

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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)

Cited by 12 publications

References 21 publications

Quantum spin liquids unveil the genuine Mott state

Quantum spin liquids unveil the genuine Mott state

Charge and Lattice Fluctuations in Molecule-Based Spin Liquids

Development of π-Electron Systems Based on [M(dmit)2] (M = Ni and Pd; dmit: 1,3-dithiole-2-thione-4,5-dithiolate) Anion Radicals

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