Malatong Ruttapol, Sato Takuro, Kumsampao Jakkapan, Minato Taketoshi, Suda Masayuki, Promarak Vinich, Yamamoto Hiroshi M
Institute for Molecular Science, Myodaiji, Okazaki, 444-8585, Japan.
The Graduate University for Advanced Studies, Myodaiji, Okazaki, 444-8585, Japan.
Small. 2023 Aug;19(32):e2302714. doi: 10.1002/smll.202302714. Epub 2023 May 8.
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.
手性分子最近作为一种高效的自旋选择性电荷发射源——即手性诱导自旋选择性(CISS),重新引起了人们的关注,这可能为新型固态自旋电子器件中有机手性材料的迷人应用提供了可能。然而,CISS的实际应用仍远未完成,迄今为止,诸如(i)自旋的外部可控性、(ii)功能耐久性以及(iii)自旋极化效率的提高等相当基本的障碍尚未克服。在本研究中,通过开发一种基于过度拥挤烯烃(OCA)的分子马达的自组装单层(SAM)来解决这些问题。利用该系统,成功证明了通过切换分子手性,可以以极其稳定的方式对自旋极化方向进行外部且重复的操纵,这是通过分子与电极之间形成共价键来实现的。此外,还发现通过将OCA与简单链烷硫醇混合来定制的OCA自组装单层的更高立体有序结构,可显著提高单个OCA分子的自旋极化效率。所有这些发现为大力推动基于CISS的自旋电子器件的发展提供了可靠的可行性研究,这些器件能够同时实现可控性、耐久性和高自旋极化效率。