To realize the origin of efficient spin injection at organic-ferromagnetic contact in organic spintronics, we have implemented the formation of quasi-molecular magnet via surface restructuring of a strong organic acceptor, tetrafluoro-tetracyano-quinodimethane (F4-TCNQ), in contact with ferromagnetic cobalt. Our results demonstrate a spin-polarized F4-TCNQ layer and a remarkably enhanced magnetic anisotropy of the Co film. The novel magnetic properties are contributed from strong magnetic coupling caused by the molecular restructuring that displays an angular anchoring conformation of CN and upwardly protruding fluorine atoms. We conclude that the π bonds of CN, instead of the lone-pair electrons of N atoms, contribute to the hybridization-induced magnetic coupling between CN and Co and generate a superior magnetic order on the surface.
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