Percolation-Induced Ferrimagnetism from Vacancy Order in [Gua]Mn1–x Fe2x/3(HCOO)3 Hybrid Perovskites

We report the magnetic behavior of the hybrid perovskites [Gua]­Mn1–x Fe2x/3□ x/3(HCOO)3 (0 ≤ x ≤ 0.88), showing that vacancy ordering drives bulk ferrimagnetism for x > 0.6. The behavior is rationalized in terms of a simple microscopic model of percolation-induced ferrimagnetism. Monte Carlo simulations driven by this model reproduce the experimental dependence of magnetic susceptibility on x and show that, at intermediate compositions, domains of short-range vacancy order lead to the emergence of local magnetization. Our results open up a new avenue for the design of multiferroic hybrid perovskites.