Heteroatomic Doping Induces High‐Low Spin Isomers in Atomically Precise Au Nanoclusters

Abstract In the post‐Moore era, single‐atom magnets and metal‐fullerene clusters are gradually replacing conventional magnetic storage semiconductor devices due to their high‐density magnetic storage capability. However, the stability of these materials in room‐temperature environments remains a challenge. A solution to this problem is proposed by doping atomically precise gold nanoclusters (NCs) with heteroatoms to induce high‐ and low‐spin isomers, which are governed by the point group symmetry of metallic core using time‐dependent density functional theory (TD‐DFT) combined with the complete active space self‐consistent field (CASSCF). Based on the field‐dependent magnetic susceptibility and electron paramagnetic resonance, the high‐ and low‐spin isomers of M@Au 8 NCs (M = Fe, Cr, Mn) are formed by core–shell electron coupling to form a stable magnetism, and all of them show paramagnetic properties with the magnetic order remaining intact, and they are capable of stable information storage at room temperature. These computational results provide a novel research direction for the development of magnetic semiconductor switching devices.