Emergence of quasi-one-dimensional physics in a nearly-isotropic three-dimensional molecular crystal: Ab initio modeling of Mo3S7(dmit)3

We report density functional theory calculations forMo(3)S(7) (dmit)(3). We derive an ab initio tight-binding model from overlaps of Wannier orbitals; finding a layered model with interlayer hopping terms similar to 3/4 the size of the in-plane terms. The in-plane Hamiltonian interpolates the kagome and honeycomb lattices. It supports states localized to dodecahedral rings within the plane, which populate one-dimensional (1D) bands and lead to a quasi-1D spin-one model on a layered honeycomb lattice once interactions are included. Two lines of Dirac cones also cross the Fermi energy.