Abstract

Direct evidence of an organic-based magnet with a finite electron spin polarization at the Fermi edge is shown from spin-resolved photoemission of the $[{\text{Fe}}^{\text{II}}(\text{TCNE}){(\text{NCMe})}_{2}][{\text{Fe}}^{\text{III}}{\text{Cl}}_{4}]$ organic-based magnet. The 23% majority-based spin polarization at the Fermi edge is observed at 80 K in zero applied field. Ab initio calculations at the density functional level (0 K) are in accord with a semiconductor with 100% majority-based electron spin polarization at the band edges, commensurate with our experimental results and model prediction for a half-semiconductor. Organic-based magnets may prove to be important for realizing polarized electron injection into semiconductors for magnetoelectronic applications.

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