Chiral Nanohoops as an Efficient Spin Polarization System

A central challenge in molecular spintronics is to achieve a high spin polarization at low operating voltages and ambient conditions while maintaining good electrical conductivity. Chiral conjugated nanohoops, characterized by their curved and strained π ‐systems, as well as their ability to be functionalized with anchoring groups, represent promising scaffolds for organic spintronics. Here, the synthesis and spin‐selective properties of axially chiral nanohoops incorporating an antiaromatic dibenzo[ a , e ]pentalene (DBP) unit are reported. DBP enables good charge transport and can be functionalized with a thiomethyl anchoring group. Using magnetic‐conductive atomic force microscopy (mc‐AFM) and magnetoresistance (MR) measurements, asymmetry in spin transport is shown, with temperature‐dependent MR indicating vibrational contributions to spin selectivity. Despite the formation of a supramolecular structure and non‐selective adsorption on the surface, the nanohoops exhibit high spin polarization at ambient temperature and low voltage operation, along with a high conductivity, a rare combination in organic spintronics.