The paired-electron crystal in the two-dimensional frustrated quarter-filled band

The competition between antiferromagnetic and spin-singlet ground states within quantum spin models and the ½-filled band Hubbard model has received intense scrutiny. Here we demonstrate a frustration-induced transition from Néel antiferromagnetism to a spin-singlet state in the interacting ¼-filled band on an anisotropic triangular lattice. While the antiferromagnetic state has equal charge densities, 0.5, on all sites, the spin-singlet state is a paired-electron crystal, with pairs of charge-rich sites separated by pairs of charge-poor sites. The paired-electron crystal provides a natural description of the spin-gapped state proximate to superconductivity in many organic charge transfer solids. Pressure-induced superconductivity in these correlated-electron systems is likely a result of a transition from the ¼-filled band valence bond solid to a valence bond liquid.