The ability to manipulate electron spin in organic molecular materials offers a new and extremely tantalizing route towards spin electronics, both from fundamental and technological points of view. This is mainly due to the unquestionable advantage of weak spin–orbit and hyperfine interactions in organic molecules, which leads to the possibility of preserving spin-coherence over times and distances much longer than in conventional metals or semiconductors. Here we demonstrate theoretically that organic spin valves, obtained by sandwiching an organic molecule between magnetic contacts, can show a large bias-dependent magnetoresistance and that this can be engineered by an appropriate choice of molecules and anchoring groups. Our results, obtained through a combination of state-of-the-art non-equilibrium transport methods and density functional theory, show that although the magnitude of the effect varies with the details of the molecule, large magnetoresistance can be found both in the tunnelling and the metallic limit.
Building on Lambert's expertise in spin-polarised transport, this paper (56 citations) predicts giant magnetoresistance in single-molecule metallic spin valves. It has stimulated the formation of two UK and EU multi-disciplinary research consortia in molecular spintronics. Bailey, Garcia-Suarez and Sanvito are past or present members of Lambert's group. RAE_import_type : Journal article RAE_uoa_type : Physics