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

Abstract

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, amongst 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) EtnX[Pd(dmit)2]2 (X=As,P,N,Sb) salts and investigate how best to model these systems by using variational Monte Carlo (VMC) 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 (FATL) description produces importantly different results, including a significant lowering of the critical U of the spin-liquid phase.

5 pages, 6 figures,final version

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• Quantum domain walls induce incommensurate supersolid phase on the anisotropic triangular lattice
• Unconventional dual 1D-2D quantum spin liquid revealed by $ab$ $initio$ studies on organic solids family
• Emergence of quasi-one-dimensional physics in Mo${}_3$S${}_7$(dmit)${}_3$, a nearly-isotropic three-dimensional molecular crystal
• 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)${}_2$
• Spin-orbit coupling in {Mo${}_3$S${}_7$(dmit)${}_3$}
• 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
• $x$-[Pd(dmit)${}_2$]${}_2$ as a quasi-1D, scalene Heisenberg model