Cation Dependence of the Electronic States in Molecular Triangular Lattice System β'-X[Pd(dmit)_2]_2: A First-principles study

Abstract

The electronic structure of an isostructural series of molecular conductors, β'-X[Pd(dmit)_2]_2 is systematically studied by a first-principles method based on the density-functional theory. The calculated band structures are fitted to the tight-binding model based on Pd(dmit)_2 dimers on the triangular lattice. We find systematic variation in the anisotropy of the transfer integrals along the three directions of the triangular lattice taking different values. The transfer integral along the face-to-face stacking direction of Pd(dmit)_2 dimers is always the largest. Around the quantum spin liquid, X = EtMe_3Sb, the other two transfer integrals become comparable. We also report sensible differences in the distribution of wavefunctions near the Fermi level between the two dmit ligands of the Pd(dmit)_2 molecule.

4 pages, 5 figures

References in corpus (6)

• Two spin liquid phases in the spatially anisotropic triangular Heisenberg model
• Mott Transition in a Valence Bond Solid Insulator with a Triangular Lattice
• Ab initio two-dimensional multiband low-energy models of EtMe_3Sb[Pd(dmit)_2]_2 and κ-(BEDT-TTF)_2Cu(NCS)_2 with comparisons to single-band models
• Possibility of Gapless Spin Liquid State by One-dimensionalization
• Geometrical frustration in the spin liquid beta'-Me3EtSb[Pd(dmit)2]2 and the valence bond solid Me3EtP[Pd(dmit)2]2
• Single-Component Molecular Metals as Multiband π-d Systems

Cited by in corpus (16)

• Quantum Spin Liquid States
• Spin liquid phase in the semiclassical theory of the Heisenberg model on an anisotropic triangular lattice with ring exchange
• Spin liquid phase due to competing classical orders in the semiclassical theory of the Heisenberg model with ring exchange on an anisotropic triangular lattice
• Importance of anisotropy in the spin-liquid candidate Me3EtSb[Pd(dmit)2]2
• Electronic Correlation and Geometrical Frustration in Molecular Solids -- A Systematic ab initio Study of ${\beta }^{\prime }$-$X$[Pd(dmit)${}_2$]${}_2$
• $Ab$ $initio$ derivation and exact-diagonalization analysis of low-energy effective Hamiltonians for ${\beta }^{\prime }$-X[Pd(dmit)${}_2$]${}_2$
• First-principles study of hydrogen-bonded molecular conductor $\kappa$-H${}_3$(Cat-EDT-TTF/ST)${}_2$
• Importance of van der Waals interactions and cation-anion coupling in an organic quantum spin liquid
• Fragment Model Study of Molecular Multi-Orbital System $X$[Pd(dmit)${}_2$]${}_2$
• Frustration, ring exchange, and the absence of long-range order in EtMe${}_3$Sb[Pd(dmit)${}_2$]${}_2$: from first principles to many-body theory
• Fragmented Electronic Spins with Quantum Fluctuations in Organic Mott Insulators near Quantum Spin Liquid
• Lattice effects in the quasi-two-dimensional valence-bond-solid Mott insulator EtMe${}_3$P[Pd(dmit)${}_2$]${}_2$
• A theory of the quantum spin liquid in the hyper-honeycomb metal-organic framework [(C${}_2$H${}_5$)${}_3$NH]${}_2$Cu${}_2$(C${}_2$O${}_4$)${}_3$ from first principles
• $x$-[Pd(dmit)${}_2$]${}_2$ as a quasi-1D, scalene Heisenberg model
• Quasi-one-dimensional Spin Dynamics in a Molecular Spin Liquid System
• An ARPES Study of the Electronic Structure of the Quantum Spin Liquid EtMe3Sb[Pd(dmit)2]2