Prediction of half-metallic conductivity in Prussian Blue derivatives

Half-metallicity and spin-crossover behavior are predicted for two well-defined Prussian Blue (PB) analogues using periodic density functional calculations with GGA + U and hybrid exhange-correlation potentials. Fully oxidized PB possesses a narrow spin-polarized band through which it should be possible to control the spin conduction by oxidative/reductive doping. Fully reduced PB is also a half-metal in its high-spin phase and exhibits an Fe2+ spin-crossover. A simple model is used to rationalize the electronic properties of these systems which may have potential applications in spintronics.