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Dednam, W.; García-Blázquez, M. A.; Zotti, Linda A.; Lombardi, E. B.; Sabater, C.; Pakdel, S.; Palacios, J. J.
ACS nano, 04/2023, Letnik: 17, Številka: 7Journal Article
Spin–orbit coupling gives rise to a range of spin-charge interconversion phenomena in nonmagnetic systems where certain spatial symmetries are reduced or absent. Chirality-induced spin-selectivity (CISS), a term that generically refers to a spin-dependent electron transfer in nonmagnetic chiral systems, is one such case, appearing in a variety of seemingly unrelated situations ranging from inorganic materials to molecular devices. In particular, the origin of CISS in molecular junctions is a matter of an intense current debate. Here, we derive a set of geometrical conditions for this effect to appear, hinting at the fundamental role of symmetries beyond otherwise relevant quantitative issues. Our approach, which draws on the use of point-group symmetries within the scattering formalism for transport, shows that electrode symmetries are as important as those of the molecule when it comes to the emergence of a spin-polarization and, by extension, to the possible appearance of CISS. It turns out that standalone metallic nanocontacts can exhibit spin-polarization when relative rotations which reduce the symmetry are introduced. As a corollary, molecular junctions with achiral molecules can also exhibit spin-polarization along the direction of transport, provided that the whole junction is chiral in a specific way. This formalism also allows the prediction of qualitative changes of the spin-polarization upon substitution of a chiral molecule in the junction with its enantiomeric partner. Quantum transport calculations based on density functional theory corroborate all of our predictions and provide further quantitative insight within the single-particle framework.
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