Restoring Symmetry and Enhancing Exchange via Chiral Molecular-Magnetic Hexagons

Modified behaviors of molecules, designed for device or energy applications, can occur due to lattice-molecule incompatibilities in point-group symmetries (PGS), long-range interactions between neighboring molecules, or lattice-molecule charge transfer. Such sensitivities are a prerequisite for the use of quantum molecules as devices, but removing certain broken symmetries is desirable from the standpoint of simplifying their behaviors. Here, we demonstrate symmetry restoration to molecular-magnetic lattices and show that it leads to strengthened exchange coupling due to dipolar electrostatic interactions between neighboring molecules and due to manifestations of an earlier identification of a spin-sensitive slightly mobile electron by et al. [Hooshmand, Z. <i>Phys. Rev. B</i> 2021, 104, 134411]. Starting with a broken symmetry molecular magnet of current interest, we demonstrate a more robust structure composed of six molecular magnets on an <i>h-</i>BN-like surface. The broken point-group symmetry is healed by constructing interpenetrating equilateral triangular structures that are appropriately ratcheted to preserve 3-fold rotational symmetry and inversion symmetry.