Cation Dependence of the Electronic States in Molecular Triangular Lattice System β′-X[Pd(dmit)2]2: A First-Principles Study

Tsumuraya, Takao; Seo, Hitoshi; Tsuchiizu, Masahisa; Kato, Reìzo; Miyazaki, Tsuyoshi

doi:10.7566/jpsj.82.033709

Cited by 39 publications

(67 citation statements)

References 33 publications

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“…[20][21][22] Here we compare model results using the t − t approximation with a fully anisotropic triangular lattice (FATL) model, focusing our discussion on the spin-liquid candidate Sb-1. If we average the two larger t's of Sb-1, assuming t = (t a + t b )/2 and t = t c , we find that the equivalent t − t model has t /t = 0.77.…”

Section: B T − T Model Vs Fatlmentioning

confidence: 99%

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Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2

et al. 2013

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Organic charge-transfer salts based on the molecule Pd(dmit) 2 display strong electronic correlations and geometrical frustration, leading to spin-liquid, valence bond solid, and superconducting states, among other interesting phases. The low-energy electronic degrees of freedom of these materials are often described by a single band model: a triangular lattice with a molecular orbital representing a Pd(dmit) 2 dimer on each site. We use ab initio electronic structure calculations to construct and parametrize low-energy effective model Hamiltonians for a class of Me 4−n Et n X[Pd(dmit) 2 ] 2 (X = As, P, N, Sb) salts and investigate how best to model these systems by using variational Monte Carlo simulations. Our findings suggest that the prevailing model of these systems as a t − t triangular lattice is incomplete and that a fully anisotropic triangular lattice description produces importantly different results, including a significant lowering of the critical U of the spin-liquid phase.

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Section: B T − T Model Vs Fatlmentioning

confidence: 99%

“…These results are consistent with those found in past work. [20][21][22] With the t's obtained from the Wannier orbitals, we can now explore the Hubbard model for Sb-1 with VMC. We find that the spiral magnetic state |SP has optimal pitch angles θ = 7π/9,θ = 3π/9, that are commensurate to an 18 × 18 lattice size.…”

Section: A Modeling the Frontier Bandsmentioning

confidence: 99%

Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2

et al. 2013

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“…85 As for the [Pd(dmit) 2 ] salts, the first-principles calculations based on density functional theory and fitting to the tight-binding dimer model revealed a systematic variation of the interdimer transfer integrals that agrees with results obtained by the extended Hückel method. 86,87 It should be added that the firstprinciples calculations strongly support us, when structural data are difficult to obtain as is the case of the pressure effect. 88 Since the HOMO and LUMO have large anisotropy, the transfer integrals are generally sensitive to the molecular arrangement and orientation, leading to a diversity of electronic properties and enabling their fine tuning.…”

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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“…Electronic structure calculations on the anisotropic triangular lattice [22][23][24][25][26] suggest that both spin liquids κ-(BEDT-TTF) 2 Cu 2 (CN) 3 [27].…”

Section: Introductionmentioning

confidence: 99%

Spin-liquid phase due to competing classical orders in the semiclassical theory of the Heisenberg model with ring exchange on an anisotropic triangular lattice

2014

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We investigate the effect of ring exchange on the ground-state properties and magnetic excitations of the S = 1/2 Heisenberg model on the anisotropic triangular lattice with ring exchange at T = 0 using linear spin-wave theory. Classically, we find stable Néel, spiral and collinear magnetically ordered phases. Upon including quantum fluctuations to the model, linear spin-wave theory shows that ring exchange induces a large quantum disordered region in the phase diagram, completely wiping out the classically stable collinear phase. Analysis of the spin-wave spectra for each of these three models demonstrates that the large spin-liquid phase observed in the full model is a direct manifestation of competing classical orders. To understand the origin of these competing phases, we introduce models where either the four spin contributions from ring exchange, or the renormalization of the Heisenberg terms due to ring exchange are neglected. We find that these two terms favor rather different physics.

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Cation Dependence of the Electronic States in Molecular Triangular Lattice System β^′-X[Pd(dmit)₂]₂: A First-Principles Study

Cited by 39 publications

References 33 publications

Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2

Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2

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

Spin-liquid phase due to competing classical orders in the semiclassical theory of the Heisenberg model with ring exchange on an anisotropic triangular lattice

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