Highly Durable Spin Filter Switching Based on Self‐Assembled Chiral Molecular Motor

Abstract Chiral molecules have recently received renewed interest as highly efficient sources of spin‐selective charge emission known as chiral‐induced spin selectivity (CISS), which potentially offers a fascinating utilization of organic chiral materials in novel solid‐state spintronic devices. However, a practical use of CISS remains far from completion, and rather fundamental obstacles such as (i) external controllability of spin, (ii) function durability, and (iii) improvement of spin‐polarization efficiency have not been surmounted to date. In this study, these issues are addressed by developing a self‐assembled monolayer (SAM) of overcrowded alkene (OCA)‐based molecular motor. With this system, it is successfully demonstrated that the direction of spin polarization can be externally and repeatedly manipulated in an extremely stable manner by switching the molecular chirality, which is achieved by a formation of the covalent bonds between the molecules and electrode. In addition, it is found that a higher stereo‐ordering architecture of the SAM of OCAs tailored by mixing them with simple alkanethiols considerably enhances the efficiency of spin polarization per a single OCA molecule. All these findings provide the creditable feasibility study for strongly boosting development of CISS‐based spintronic devices that can simultaneously fulfill the controllability, durability, and high spin‐polarization efficiency.