Percolation-induced ferrimagnetism from vacancy order in [Gua]Mn1–xFe2x/3(HCOO)3 hybrid perovskites

We report the magnetic behaviour of the hybrid perovskites [Gua]Mn1–xFe2x/3(HCOO)3 (0 < x < 0.88), showing that vacancy ordering drives bulk ferrimagnetism for x > 0.6. The behaviour is rationalised 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 magnetisation. Our results open up a new avenue for the design of multiferroic hybrid perovskites.