Knot-Driven Spin Selectivity: Topological Chirality-Induced Robust Spin Polarization in Molecular Knots

Compared to traditional structural chiral materials (e.g., DNA, helicene), topological chirality in trefoil knot molecules has demonstrated multiple remarkable advantages in chirality-induced spin selectivity (CISS), including ultra-high spin polarization of nearly 90%, conductivity increased by two orders of magnitude, and high-temperature stability (up to 350$^{\circ}$C). However, the underlying physical mechanism remains elusive. This work establishes, for the first time, a fundamental theoretical framework for topological chirality-induced spin selectivity (TCISS) in trefoil knot molecules and identifies the necessary conditions for knot-driven spin selectivity. Our calculation results reveal that a trefoil knot molecule can exhibit spin polarization exceeding 60% along with significant conductivity. Notably, neither reducing the lattice number nor applying strain regulation significantly diminishes this ultra-high spin polarization, highlighting its robustness. Importantly, when the topological knot degenerates into a trivial structure, accompanied by the transition from topological chirality to structural chirality, the spin polarization sharply declines, demonstrating a strong correlation between the ultrahigh spin polarization and the knot topology. Our theory not only successfully elucidates the physical mechanism of TCISS, but also uncovers a new spin-polarized transport phenomenon termed knot-driven spin selectivity, offering new guiding principles for designing nonmagnetic materials for spintronics device applications.