We show that the electronic structures of the title compounds predicted by
density functional theory (DFT) are well described by tight binding models. We
determine the frustration ratio, J'/J, of the Heisenberg model on the
anisotropic triangular lattice, which describes the spin degrees of freedom in
the Mott insulating phase for a range of Pd(dmit)2 salts. All of the
antiferromagnetic materials studied have J'/J 0.9, consistent
with predictions for the Heisenberg model. All salts with 0.5 < J'/J < 0.9,
where many-body theories find a number of competing ground states, are known,
experimentally, to be charge ordered, valence bond solids or spin liquids.Comment: Accepted for publication in Phys. Rev. Lett. 4+11 pages, 3+15
figures, major rewrite, added calculations of Hubbard
