Chiral Van Der Waals Superlattices for Enhanced Spin‐Selective Transport and Spin‐Dependent Electrocatalytic Performance

Abstract The emergence of the chiral‐induced spin‐selectivity (CISS) effect offers a new avenue for chiral organic molecules to autonomously manipulate spin configurations, thereby opening up possibilities in spintronics and spin‐dependent electrochemical applications. Despite extensive exploration of various chiral systems as spin filters, one often encounters challenges in achieving simultaneously high conductivity and high spin polarization ( SP ). In this study, a promising chiral van der Waals superlattice, specifically the chiral TiS 2 crystal, is synthesized via electrochemical intercalation of chiral molecules into a metallic TiS 2 single crystal. Multiple tunneling processes within the highly ordered chiral layered structure of chiral TiS 2 superlattices result in an exceptionally high SP exceeding 90%. This remarkable observation of significantly high SP within the linear transport regime is unprecedented. Furthermore, the chiral TiS 2 electrode exhibits enhanced catalytic activity for oxygen evolution reaction (OER) due to its remarkable spin‐selectivity for triplet oxygen evolution. The OER performance of chiral TiS 2 superlattice crystals presented here exhibits superior characteristics to previously reported chiral MoS 2 catalysts, with an approximately tenfold increase in current density. The combination of metallic conductivity and high SP sets the stage for the development of a new generation of CISS materials, enabling a wide range of electron spin‐based applications.