A Group-Theoretic Approach to the Origin of Chirality-Induced Spin-Selectivity in Nonmagnetic Molecular Junctions
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Título: | A Group-Theoretic Approach to the Origin of Chirality-Induced Spin-Selectivity in Nonmagnetic Molecular Junctions |
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Autor/es: | Dednam, Wynand | García-Blázquez, Manuel Antonio | Zotti, Linda A. | Lombardi, Enrico B. | Sabater, Carlos | Pakdel, Sahar | Palacios Burgos, Juan José |
Grupo/s de investigación o GITE: | Grupo de Nanofísica |
Centro, Departamento o Servicio: | Universidad de Alicante. Departamento de Física Aplicada |
Palabras clave: | Spin-polarization | Quantum transport | Chirality | Symmetry | DFT calculations | Enantiomers |
Fecha de publicación: | 22-mar-2023 |
Editor: | American Chemical Society |
Cita bibliográfica: | ACS Nano. 2023, 17(7): 6452-6465. https://doi.org/10.1021/acsnano.2c11410 |
Resumen: | 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. |
Patrocinador/es: | J.J.P. and M.A.G.B acknowledge financial support from Spanish MICIN through Grant No. PID2019-109539GB-C43/AEI/10.13039/501100011033, the María de Maeztu Program for Units of Excellence in R&D (Grant No. CEX2018-000805-M), the Comunidad Autónoma de Madrid through the Nanomag COST-CM Program (Grant No. S2018/NMT-4321), the Generalitat Valenciana through Programa Prometeo/2021/017, the Centro de Computación Científica of the Universidad Autónoma de Madrid, and the computer resources of the Red Española de Supercomputación. L.A.Z. thanks financial support from MCIN/AEI/10.13039/501100011033 (grant PID2021-125604NB-I00) and from the Universidad Autónoma de Madrid/Comunidad de Madrid (Grant No. SI3/PJI/2021-00191). C.S. thanks the financial support from the Generalitat Valenciana through CIDEXG/2022/45, CDEIGENT/2018/028 and PROMETEO/2021/017. S.P. acknowledges the grant from Erasmus+ 2018 programme (Collaboration between University of Tehran, Iran and Autonomous University of Madrid, Spain). |
URI: | http://hdl.handle.net/10045/133135 |
ISSN: | 1936-0851 (Print) | 1936-086X (Online) |
DOI: | 10.1021/acsnano.2c11410 |
Idioma: | eng |
Tipo: | info:eu-repo/semantics/article |
Derechos: | © 2023 The Authors. Published by American Chemical Society. Creative Commons Attribution 4.0 International License (CC BY 4.0) |
Revisión científica: | si |
Versión del editor: | https://doi.org/10.1021/acsnano.2c11410 |
Aparece en las colecciones: | INV - Grupo de Nanofísica - Artículos de Revistas |
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