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Organic charge transfer salts based on the molecule Pd(dmit)2 display strongelectronic correlations and geometrical frustration, leading to spin liquid,valence bond solid, and superconducting states, amongst other interestingphases. The low energy electronic degrees of freedom of these materials areoften described by a single band model; a triangular lattice with a molecularorbital representing a Pd(dmit)2 dimer on each site. We use ab initioelectronic structure calculations to construct and parametrize low energyeffective 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 usingvariational Monte Carlo (VMC) simulations. Our findings suggest that theprevailing model of these systems as a t-t' triangular lattice is incomplete,and that a fully anisotropic triangular lattice (FATL) description producesimportantly different results, including a significant lowering of the criticalU of the spin-liquid phase.

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