Insights into Magnetic Interactions in a Monodisperse Gd12Fe14 Metal Cluster

The largest Ln–Fe metal cluster [Gd12Fe14(μ3‐OH)12(μ4‐OH)6(μ4‐O)12(TEOA)6(CH3COO)16(H2O)8]⋅(CH3COO)2(CH3CN)2⋅(H2O)20 (1) and the core–shell monodisperse metal cluster of 1 a@SiO2 (1 a=[Gd12Fe14(μ3‐OH)12(μ4‐OH)6(μ4‐O)12(TEOA)6(CH3COO)16 (H2O)8]2+) were prepared. Experimental and theoretical studies on the magnetic properties of 1 and 1 a@SiO2 reveal that encapsulation of one cluster into one silica nanosphere not only effectively decreases intermolecular magnetic interactions but also significantly increases the zero‐field splitting effect of the outer layer Fe3+ ions. Sphere of influence: The magnetic properties of Gd12Fe14 and Gd12Fe14@SiO2 were investigated. The encapsulation of a single‐molecule cluster into one silica nanosphere influences not only the intermolecular magnetic interaction but also the zero‐field splitting effects of the Fe3+ ions.