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We report a highly asymmetric magnetoresistance (MR) bias dependence, with the inverse MR peaking at a negative bias and a sign reversal occurring at a positive bias in prototypical La0.7Sr0.3MnO3 (LSMO)/Alq3/Co organic spin valve (OSV) with a tunnel barrier between LSMO and Alq3. This behavior is in strong contrast with the commonly found inverse MR in entire bias range for LSMO/Alq3/Co OSVs. The MR bias voltage dependence is independent on the type of the tunnel barrier, either SrTiO3 or Al2O3. Together with first-principle calculations, we demonstrate that the strongly hybridized Co d-states with Alq3 molecules at the interface are responsible for the efficient d-states spin injection and the observed MR bias dependence is originated from the energy dependent density of states of Co d-states. These findings open up new possibilities to engineer interfacial bonding between ferromagnetic materials and a wide variety of molecule selections for the desired spin transport properties. ? 2014 IOP Publishing and Deutsche Physikalische Gesellschaft.

Strong asymmetrical bias dependence of magnetoresistance in organic spin valves: the role of ferromagnetic/organic interfaces