Chiral-induced spin selectivity (CISS), whereby helical molecules polarize the spin of electrical current, is an intriguing effect with potential applications in nanospintronics. In this nascent field, the study of paramagnetic chiral molecules, which could introduce another degree of freedom in the control of the spin transport, remains so far unexplored. To address this challenge, herein, we propose the use of self-assembled monolayers of helical lanthanide-binding peptides. In order to elucidate the effect of the paramagnetic nuclei, monolayers of the peptide coordinating paramagnetic or diamagnetic ions are prepared. By means of spin-dependent electrochemistry, CISS effect is demonstrated by cyclic voltammetry and impedance measurements for both samples. Additionally, an implementation of the standard liquid-metal drop electron transport setup has been carried out, demonstrating their suitability for solid-state devices. Remarkably, the inclusion of a paramagnetic center in the peptide increases the spin polarization as independently proved by different techniques. These findings permit the inclusion of magnetic biomolecules in the CISS field, paving the way to their implementation in a new generation of spintronic nanodevices.

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