Magnetically active atomic distances may impact the magnetic ordering in a given system both directly and indirectly. We synthesize three novel quasi one-dimensional organic-inorganic hybrid cobalt chloride chain compounds (CH3NH3CoCl3, CH(NH2)2CoCl3, and C(NH2)3CoCl3) and characterize their magnetic and thermodynamic properties. These materials crystallize in a hexagonal perovskite-type structure consisting of chains of face-sharing Co-Cl octahedra separated by the respective organic cation. Temperature and field-dependent magnetic susceptibility analyses reveal that each compound possesses antiferromagnetic intrachain coupling, and that the strength of the correlations is comparable across the three materials. Moreover, the interchain Co-Co distance, which depends on the size of the organic cation, is directly related to the temperature at which long-range magnetic ordering occurs.
The SI includes atomic coordinates, Wyckoff positions, and occupancies for each material, a comparison of experimental and calculated PXRD patterns, and a detailed analysis of the temperature-dependent susceptibility for MACoCl3.