High Magnetic Field Study on Giant Negative Magnetoresistance in the Molecular Conductor TPP[Cr(Pc)(CN)2]2

Abstract

We investigated the magnetic and transport properties of the phthalocyanine molecular conductor TPP[Cr(Pc)(CN)2]2 in magnetic fields of up to 54 T. We observed giant negative magnetoresistance which hardly depends on the magnetic field direction owing to the isotropic nature confirmed by electron spin resonance measurements. The magnitude of magnetoresistance [|ρ(μ0H)/ρ(0 T) − 1|] is proportional to the square of magnetization as observed in the case of the spin scattering process, while the proportionality coefficient increases with decreasing the temperature. The magnetization does not saturate even at 53 T, indicating the existence of the large antiferromagnetic exchange interactions between the localized spins. In spite of this antiferromagnetic exchange interaction and low dimensionality, a convex magnetization curve was observed in the low temperature and high magnetic field range. To reproduce this magnetization curve, we proposed a model taking into account the antiferromagnetic exchange interaction between the neighboring π-electron spins.