Elucidating individual magnetic contributions in bi-magnetic Fe3O4/Mn3O4 Core/Shell nanoparticles by polarized powder neutron diffraction

Heterogeneous bi-magnetic nanostructured systems have had a sustained interest during the last decades owing to their unique magnetic properties and the wide range of derived potential applications. However, elucidating the details of their magnetic properties can be rather complex. Here, a comprehensive study of Fe3O4/Mn3O4 core/shell nanoparticles using polarized neutron powder diffraction, which allows disentangling the magnetic contributions of each of the components, is presented. The results show that while at low fields the Fe3O4 and Mn3O4 magnetic moments averaged over the unit cell are antiferromagnetically coupled, at high fields, they orient parallel to each other. This magnetic reorientation of the Mn3O4 shell moments is associated with a gradual evolution with the applied field of the local magnetic susceptibility from anisotropic to isotropic. Additionally, the magnetic coherence length of the Fe3O4 cores shows some unusual field dependence due to the competition between the antiferromagnetic interface interaction and the Zeeman energies. The results demonstrate the great potential of the quantitative analysis of polarized neutron powder diffraction for the study of complex multiphase magnetic materials.I.V.G. acknowledges financial support from the Russian Foundation for Basic Research under Grant No 20-02-00109. A.G.R. and J.N. acknowledge financial support from the grants PID2019-106229RB-I0 funded by MCIN/AEI/10.13039/50110001103 and 2021-SGR-00651 from Generalitat de Catalunya. I.K. and A.G. acknowledge the European Union's H2020 reserach and innovation program, Grant agreement No 871072. A.G.R. acknowledges financial support from RYC2019-027449-I funded by MCIN/AEI/10.13039/501100011033. ICN2 is funded by the CERCA programme/Generalitat de Catalunya. The ICN2 is supported by the CEX2021–001214–S grant funded by MCIN/AEI/10.13039/501100011033. M.E. acknowledges the grants RYC2018-024396-I and PID2019-106165GB-C22 funded by MCIN/AEI/ 10.13039/501100011033 and by “ESF Investing in your future.” A.L.O. acknowledges financial support from the grants PID2021-122613OB-I00 funded by MCIN/AEI/ 10.13039/501100011033 and PJUPNA2020 from Universidad Pública de Navarra