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The understanding of orbital hybridization and spin-polarization at theorganic-ferromagnetic interface is essential in the search for efficient hybridspintronic devices. Here, using first-principles calculations, we report asystematic study of spin-split hybrid states of C$_{60}$ deposited on variousferromagnetic surfaces: bcc-Cr(001), bcc-Fe(001), bcc-Co(001), fcc-Co(001) andhcp-Co(0001). We show that the adsorption geometry of the molecule with respectto the surface crystallographic orientation of the magnetic substrate as wellas the strength of the interaction play an intricate role in thespin-polarization of the hybrid orbitals. We find that a largespin-polarization in vacuum above the buckyball can only be achieved if themolecule is adsorbed upon a bcc-(001) surface by its pentagonal ring. Thereforebcc-Cr(001), bcc-Fe(001) and bcc-Co(001) are the optimal candidates.Spin-polarized scanning tunneling spectroscopy measurements on single C$_{60}$adsorbed on Cr(001) and Co/Pt(111) also confirm that both the symmetry of thesubstrate and of the molecular conformation have a strong influence on theinduced spin polarization. Our finding may give valuable insights for furtherengineering of spin filtering devices through single molecular orbitals.

Symmetry-selected spin-split hybrid states in C$_{60}$/ferromagnetic interfaces