The discovery of chiral-induced spin selectivity (CISS) opens up the possibility to manipulate spin orientation without external magnetic fields and enables new spintronic device designs1-4. Although many approaches have been explored for introducing CISS into solid-state materials and devices, the resulting systems so far are often plagued by high inhomogeneity, low spin selectivity or limited stability, and have difficulties in forming robust spintronic devices5-8. Here we report a new class of chiral molecular intercalation superlattices (CMIS) as a robust solid-state chiral material platform for exploring CISS. The CMIS were prepared by intercalating layered two-dimensional atomic crystals (2DACs) (such as TaS2 and TiS2) with selected chiral molecules (such as R-α-methylbenzylamine and S-α-methylbenzylamine). The X-ray diffraction and transmission electron microscopy studies demonstrate highly ordered superlattice structures with alternating crystalline atomic layers and self-assembled chiral molecular layers. Circular dichroism studies show clear chirality-dependent signals between right-handed (R-) and left-handed (S-) CMIS. Furthermore, by using the resulting CMIS as the spin-filtering layer, we create spin-selective tunnelling junctions with a distinct chirality-dependent tunnelling current, achieving a tunnelling magnetoresistance ratio of more than 300 per cent and a spin polarization ratio of more than 60 per cent. With a large family of 2DACs of widely tunable electronic properties and a vast selection of chiral molecules of designable structural motifs, the CMIS define a rich family of artificial chiral materials for investigating the CISS effect and capturing its potential for new spintronic devices.

California NanoSystems Institute University of California Los Angeles Los Angeles CA USA

Department of Chemistry and Biochemistry University of California Los Angeles Los Angeles CA USA

Department of Inorganic Chemistry University of Chemistry and Technology Prague Prague Czech Republic

Department of Materials Science and Engineering University of California Irvine Irvine CA USA

Department of Materials Science and Engineering University of California Los Angeles Los Angeles CA USA

Department of Physics and Astronomy University of California Irvine Irvine CA USA

Hunan Key Laboratory of Two Dimensional Materials State Key Laboratory for Chemo Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University Changsha China

Irvine Materials Research Institute University of California Irvine Irvine CA USA

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Nature. 2022 Jun;606(7916):865-866. doi: 10.1038/d41586-022-01732-w. PubMed

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Roadmap for Photonics with 2D Materials

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