Hamiltonian of the V15 spin system from first-principles density-functional calculations.

ABSTRACT

We report first-principles all-electron density-functional-based studies of the electronic structure, magnetic ordering, and anisotropy for the V15 molecular magnet. From these calculations, we determine a Heisenberg Hamiltonian with five antiferromagnetic and one ferromagnetic exchange couplings. We perform direct diagonalization to determine the temperature dependence of the susceptibility. This Hamiltonian reproduces the experimentally observed spin S = 1/2 ground state and low-lying S = 3/2 excited state. A small anisotropy term is necessary to account for the temperature independent part of the magnetization curve.