Percolation-Induced Ferrimagnetism from Vacancy Order in [Gua]Mn1- xFe2 x/3(HCOO)3 Hybrid Perovskites

Johnathan M Bulled; Alexandra Willis; Zoé Faure Beaulieu; Simon J Cassidy; Jonas Bruckmoser; Hanna L B Boström; Andrew L Goodwin

doi:10.1021/jacs.4c03407

Percolation-Induced Ferrimagnetism from Vacancy Order in [Gua]Mn_{1- x}Fe_{2 x/3}(HCOO)₃ Hybrid Perovskites

J Am Chem Soc. 2024 May 22;146(20):13714-13718. doi: 10.1021/jacs.4c03407. Epub 2024 May 9.

Authors

Johnathan M Bulled¹, Alexandra Willis¹, Zoé Faure Beaulieu¹, Simon J Cassidy¹, Jonas Bruckmoser², Hanna L B Boström^{1

3

4}, Andrew L Goodwin¹

Affiliations

¹ Department of Chemistry, University of Oxford, Inorganic Chemistry Laboratory, Oxford OX1 3QR, United Kingdom.
² Department of Chemistry, Technical University of Munich, Lichtenbergstraße 4, 85748 Garching, Germany.
³ Wallenberg Initiative Materials Science for Sustainability, Department of Materials and Environmental Chemistry, Stockholm University, SE-114 18 Stockholm, Sweden.
⁴ Department of Materials and Environmental Chemistry, Stockholm University, SE-114 18 Stockholm, Sweden.

PMID: 38723156
DOI: 10.1021/jacs.4c03407

Abstract

We report the magnetic behavior of the hybrid perovskites [Gua]Mn_1-xFe_2x/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.