Spintronics holds great potential for next-generation high-speed and low-power consumption information technology. Recently, lead halide perovskites (LHPs), which have gained great success in optoelectronics, also show interesting magnetic properties. However, the spin-related properties in LHPs originate from the spin-orbit coupling of Pb, limiting further development of these materials in spintronics. Here, we demonstrate a new generation of halide perovskites, by alloying magnetic elements into optoelectronic double perovskites, which provide rich chemical and structural diversities to host different magnetic elements. In our iron-alloyed double perovskite, Cs2Ag(Bi:Fe)Br6, Fe3+ replaces Bi3+ and forms FeBr6 clusters that homogenously distribute throughout the double perovskite crystals. We observe a strong temperature-dependent magnetic response at temperatures below 30 K, which is tentatively attributed to a weak ferromagnetic or antiferromagnetic response from localized regions. We anticipate that this work will stimulate future efforts in exploring this simple yet efficient approach to develop new spintronic materials based on lead-free double perovskites.

Center of Artificial Photosynthesis for Solar Fuels School of Science Westlake University Hangzhou 310024 China

Department of Chemistry KTH Royal Institute of Technology SE 10044 Stockholm Sweden

Department of Chemistry Northwestern University Evanston IL 60208 USA

Department of Materials Science and Engineering National Defense Academy Yokosuka Kanagawa 239 8686 Japan

Department of Physical Science Osaka Prefecture University Sakai Osaka 599 8531 Japan

Department of Physics Chemistry and Biology Linköping University Linköping SE 581 83 Sweden

Faculty of Science Health Education and Engineering University of the Sunshine Coast 90 Sippy Downs Drive Sippy Downs QLD 4556 Australia

Institute of Macromolecular Chemistry of the Czech Academy of Sciences Heyrovskeho nam 2 162 06 Prague 6 Czech Republic

Japan Synchrotron Radiation Research Institute SPring 8 Sayo Hyogo 679 5198 Japan

Materials Science Division Argonne National Laboratory Argonne IL 60439 USA

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