LAUSR

Significance In contrast to conventional electronics, spintronics devices exploit the electron spin as an additional degree of freedom. The chirality-induced spin selectivity (CISS) effect, in which chiral molecules act as spin filters in electron transport, provides a pathway to control spins in molecules. We describe an approach that integrates both spin-polarizing and spin-propagating functionality into organic structures that feature low charge transport resistances. Binding chiral ligands to molecular wires controls polarized spin handedness, regulates spin currents, generates large NIR rotational strengths, and provides a mechanism to flip the favored spin orientation for spin transmission through chiral organic molecules. This work points the way to materials that provide both high spin selectivity and large-magnitude spin currents via the CISS mechanism. A critical spintronics challenge is to develop molecular wires that render efficiently spin-polarized currents. Interplanar torsional twisting, driven by chiral binucleating ligands in highly conjugated molecular wires, gives rise to large near-infrared rotational strengths. The large scalar product of the electric and magnetic dipole transition moments (μ→ij⋅m→ij), which are evident in the low-energy absorptive manifolds of these wires, makes possible enhanced chirality-induced spin selectivity–derived spin polarization. Magnetic-conductive atomic force microscopy experiments and spin-Hall devices demonstrate that these designs point the way to achieve high spin selectivity and large-magnitude spin currents in chiral materials.