Tuning the Ferrotoroidic Coupling and Magnetic Hysteresis in Double‐Triangle Complexes {Dy 3 M III Dy 3 } via the M III ‐linker

We present the syntheses, structures, magnetic data and theoretical analyses for two families of heptanuclear clusters, wherein two staggered dysprosium(III) triangles are linked by various M(III) d‐/p‐block ions. The families differ in the counter‐anion and are of formulae [Dy III 6 M III (OH) 8 ( o ‐tol) 12 (MeOH) 5 (NO 3 )] ⋅ 4MeOH and [Dy III 6 M III (OH) 8 ( o ‐tol) 12 (MeOH) 6 ]Cl ⋅ 6MeOH (M=Cr, Mn, Fe, Co, Al; o ‐tol= o ‐toluate). We find that variation of the central metal ion M is crucial in tuning the toroidal moments on the triangular units, with diamagnetic M linking ions enhancing the ferrotoroidic coupling. By detailed simulation and analysis of various magnetic measurements, including sub‐kelvin microSquid hysteresis loops, we identified the specific signature of the M linking ions’ modulation of toroidal properties, including the mechanism whereby anisotropic, paramagnetic M ions lead to hysteresis profiles with larger remnant magnetisations and broader coercive fields.