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

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@Au₈ 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.