Spin Selectivity in Chiral Hybrid Cobalt Halide Films with Ultrasmooth Surface

Introducing chirality into low-dimensional hybrid organic-inorganic halides (HOIHs) creates brand-new opportunities for HOIHs in spintronics and spin-related optoelectronics owing to chirality-induced spin selectivity (CISS). However, preparing smooth films of low-dimensional HOIHs with small roughness is still a great challenge due to the hybrid and complex crystal structure, which severely inhibits their applications in spintronic devices. Exploring new lead-free chiral HOIHs with both efficient spin selectivity and excellent film quality is urgently desired. Here, cobalt-based chiral metal halide crystals (R/S-NEA)2 CoCl4 constructed by 0D [CoCl4 ] tetrahedrons and 1-(1-naphtyl)ethylamine (NEA) are synthesized. The orderly configuration of NEA molecules stabilized by noncovalent CH···π interaction endows (NEA)2 CoCl4 with good film-forming ability. (NEA)2 CoCl4 films exhibit strong chiroptical activity (gCD ≈ 0.05) and significant spin-polarized transport (CISS efficiency up to 90%). Furthermore, ultrasmooth films (roughness ∼ 0.3 nm) with enhanced crystallinity can be achieved by incorporating tiny amount tris(8-oxoquinoline)aluminum that has analogous conjugated structure to NEA. The realization of highly efficient spin selectivity and sub-nanometer roughness in lead-free chiral halides can boost the practical process of low-dimensional HOIHs in spintronics and other fields.