Self-induced crystalline fluctuation spin-glass state in Mn7C3 binary compounds
Crystalline spin glasses are attractive compounds owing to their unique nature and applications. Here, we synthesised a bulk Pnma-type Mn7C3 spin glass by a high-temperature, high-pressure method. Experimental characterisation including X-ray diffraction and magnetic susceptibility measurements demonstrated that the compound has a triangular Ising-model-based structure, high freezing temperature of 37.4 K, and novel competition mechanism. Theoretical calculations and simulations revealed that the triangular Mn units are spontaneously frustrated and bridge neighbouring Mn units via polarised C atoms and messenger Mn atoms. Triangular C units each share one electron within a three-pronged electron cloud. This electron is the direct cause of frustration and competition in Mn7C3. The competition within the triangular Mn units suggests that the possible magnetic configurations are highly degenerate and that the Mn7C3 spin glass has high robustness. This work introduces a new family of spin glasses with ordered microgeometries that drive electronic structure disorder, and an application-friendly spin-glass material for use in fields like high-efficiency hardware and algorithm design in artificial intelligence.