Based on ab initio theory, the interracial spin polarization of a benzene-dithiolate molecule vertically adsorbed on a nickel surface is investigated by adopting different microscopic con- tact configurations. The results demonstrate a strong dependence of the interfacial spin polarization on the contact configuration, where the sign of spin polarization may vary from positive to negative with the change of contact configuration. By analyzing the projected density of states, an interracial orbital hybridization between the 3d orbital of the nickel atom and the sp3 hybridized orbital of the sulfur atom is observed. We also simulated the interracial adsorption in mechanically controllable break junction experiments. The magne- toresistance obtained from Julliere model is about 27% based on the calculated interracial spin polarization, which is consistent with experimental measurement.
