AbstractSingle‐molecule magnetic junctions serve as an important component for the manipulation of spin‐polarized currents by chemical modifications and control of magnetic interactions in spintronic devices. We employed the nonequilibrium green function and spin‐polarized density functional theory simulations to investigate the performance of molecular junctions bearing an organic radical as spin filters. A spin‐polarized current could be generated using the junctions and, moreover, the spin‐filtering efficiency could be tuned by varying the number of magnetic units. Spin orbital and density of states analyses revealed the relationship effect of the shapes and energy levels of the dominant electron‐conducting channels in the spin‐filtering efficiency. Thus, the use of a tunable organic magnetic molecular junction system is an appealing approach for regulating spin‐polarized currents in spintronic devices.
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