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      Highly Conductive Topologically Chiral Molecular Knots as Efficient Spin Filters

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          Abstract

          Knot-like structures were found to have interesting magnetic properties in condensed matter physics. Herein, we report on topologically chiral molecular knots as efficient spintronic chiral material. The discovery of the chiral-induced spin selectivity (CISS) effect opens the possibility of manipulating the spin orientation with soft materials at room temperature and eliminating the need for a ferromagnetic electrode. In the chiral molecular trefoil knot, there are no stereogenic carbon atoms, and chirality results from the spatial arrangements of crossings in the trefoil knot structures. The molecules show a very high spin polarization of nearly 90%, a conductivity that is higher by about 2 orders of magnitude compared with that of other chiral small molecules, and enhanced thermal stability. A plausible explanation for these special properties is provided, combined with model calculations, that supports the role of electron–electron interaction in these systems.

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          Most cited references39

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          Helicenes: synthesis and applications.

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            Chiral molecules and the electron spin

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              Chiral-induced spin selectivity enables a room-temperature spin light-emitting diode

              In traditional optoelectronic approaches, control over spin, charge, and light requires the use of both electrical and magnetic fields. In a spin-polarized light-emitting diode (spin-LED), charges are injected, and circularly polarized light is emitted from spin-polarized carrier pairs. Typically, the injection of carriers occurs with the application of an electric field, whereas spin polarization can be achieved using an applied magnetic field or polarized ferromagnetic contacts. We used chiral-induced spin selectivity (CISS) to produce spin-polarized carriers and demonstrate a spin-LED that operates at room temperature without magnetic fields or ferromagnetic contacts. The CISS layer consists of oriented, self-assembled small chiral molecules within a layered organic-inorganic metal-halide hybrid semiconductor framework. The spin-LED achieves ±2.6% circularly polarized electroluminescence at room temperature.
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                Author and article information

                Journal
                J Am Chem Soc
                J Am Chem Soc
                ja
                jacsat
                Journal of the American Chemical Society
                American Chemical Society
                0002-7863
                1520-5126
                16 November 2023
                13 December 2023
                : 145
                : 49
                : 26791-26798
                Affiliations
                []Shanghai Key Laboratory of Green Chemistry and Chemical Processes & Shanghai Frontiers Science Center of Molecule Intelligent Syntheses & Chang-Kung Chuang Institute, School of Chemistry and Molecular Engineering, East China Normal University , Shanghai 200062, China
                []Department of Chemical and Biological Physics, Weizmann Institute of Science , Rehovot 7610001, Israel
                [§ ]Key Laboratory of Polar Materials and Devices (MOE) and State Key Laboratory of Precision Spectroscopy, East China Normal University , 500 Dongchuan Rd., Shanghai 200241, China
                []Collaborative Innovation Center of Extreme Optics, Shanxi University , Taiyuan 237016 Shanxi, China
                []Institute of Eco-Chongming , Shanghai 202162, China
                [# ]Department of Physics and Astronomy, Uppsala University , Uppsala 75236, Sweden
                []State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University , Shanghai 200438, China
                Author notes
                Author information
                https://orcid.org/0000-0003-1170-7362
                https://orcid.org/0000-0001-7918-5973
                https://orcid.org/0009-0002-8549-6123
                https://orcid.org/0000-0002-9217-2218
                https://orcid.org/0000-0003-1910-366X
                https://orcid.org/0000-0003-4926-1618
                Article
                10.1021/jacs.3c08966
                10722505
                37972388
                17942960-c0b3-4c91-97ab-872ea13b7991
                © 2023 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 18 August 2023
                : 02 November 2023
                : 31 October 2023
                Funding
                Funded by: U.S. Department of Energy, doi 10.13039/100000015;
                Award ID: ER46430
                Funded by: Shanghai Frontiers Science Center of Molecule Intelligent Syntheses, East China Normal University, doi NA;
                Award ID: NA
                Funded by: Sassoon and Marjorie Peress Philanthropic Fund, doi NA;
                Award ID: NA
                Funded by: Jay and Sharon Levy, doi NA;
                Award ID: NA
                Funded by: Estate of Hermine Miller, doi NA;
                Award ID: NA
                Funded by: National Natural Science Foundation of China, doi 10.13039/501100001809;
                Award ID: 92056203
                Funded by: National Natural Science Foundation of China, doi 10.13039/501100001809;
                Award ID: 22001073
                Categories
                Article
                Custom metadata
                ja3c08966
                ja3c08966

                Chemistry
                Chemistry

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