Programmable Helicity and Spin Polarization in Pt6L4 Coordination Capsules through Guest-Mediated Chiral Control

Programmable regulation of spin polarization enables molecular-scale spin filtering, yet reversible control of its sign in supramolecular systems remains challenging. Herein, a chiral-directing strategy modulates multiple helical states of octahedral capsules, enabling programmable and reversible control of chirality-induced spin selectivity (CISS). The strategy transfers (R)-1,1'-bi-2-naphthol chirality to induce capsule helicity, followed by controlled helicity inversion upon introduction of (R)-1,1'-binaphthyl-2,2'-diylhydrogen phosphate via host-guest interactions. Magnetic circular dichroism (MCD) reveals chirality-dependent changes in electronic states, while magnetic conductive atomic force microscopy (mc-AFM) independently demonstrates spin-selective charge transport. Systematic modulation of host-guest electronic coupling enables reversible switching of spin polarization. These results demonstrate that dynamic, chirality-matched host-guest interactions emulate enzymatic stereochemical control, offering molecular-level insight and a general design principle for chiral coordination architectures with programmable spin functions.