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 FeO/MnO 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 FeO and MnO magnetic moments averaged over the unit cell are antiferromagnetically coupled, at high fields, they orient parallel to each other. This magnetic reorientation of the MnO 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 FeO 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

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

Origin of the large dispersion of magnetic properties in nanostructured oxides: FexO/Fe3O4 nanoparticles as a case study

The intimate relationship in transition-metal oxides between stoichiometry and physiochemical properties makes them appealing as tunable materials. These features become exacerbated when dealing with nanostructures. However, due to the complexity of nanoscale materials, establishing a distinct relationship between structure-morphology and functionalities is often complicated. In this regard, in the FexO/Fe3O4 system a largely unexplained broad dispersion of magnetic properties has been observed. Here we show, thanks to a comprehensive multi-technique approach, a clear correlation between magneto-structural properties in large (45 nm) and small (9 nm) FexO/Fe3O4 core/shell nanoparticles that can explain the spread of magnetic behaviors. The results reveal that while the FexO core in the large nanoparticles is antiferromagnetic and has bulk-like stoichiometry and unit-cell parameters, the FexO core in the small particles is highly non-stoichiometric and strained, displaying no significant antiferromagnetism. These results highlight the importance of ample characterization to fully understand the properties of nanostructured metal oxide

Origin of the large dispersion of magnetic properties in nanostructured oxides: FexO/Fe3O4 nanoparticles as a case study

The intimate relationship between stoichiometry and physicochemical properties in transition-metal oxides makes them appealing as tunable materials. These features become exacerbated when dealing with nanostructures. However, due to the complexity of nanoscale materials, establishing a distinct relationship between structure-morphology and functionalities is often complicated. In this regard, in the FexO/Fe3O4 system a largely unexplained broad dispersion of magnetic properties has been observed. Here we show, thanks to a comprehensive multi-technique approach, a clear correlation between the magneto-structural properties in large (45 nm) and small (9 nm) FexO/Fe3O4 core/shell nanoparticles that can explain the spread of magnetic behaviors. The results reveal that while the FexO core in the large nanoparticles is antiferromagnetic and has bulk-like stoichiometry and unit-cell parameters, the FexO core in the small particles is highly non-stoichiometric and strained, displaying no significant antiferromagnetism. These results highlight the importance of ample characterization to fully understand the properties of nanostructured metal oxides

Magnetic structures of RE PdBi half-Heusler bismuthides ( RE = Gd, Tb, Dy, Ho, Er)

We present results of neutron diffraction on single crystals of several equiatomic ternary compounds of rare-earth elements with palladium and bismuth, crystallizing with cubic MgAgAs-type structure (half-Heusler phases). Band structure calculations showed that many members of that family possess electronic band inversion, which may lead to occurrence of topological insulator or topological semimetal. But even for the compounds without intrinsic band inversion another way of topologically non-trivial state realization, through a specific antiferromagnetic order, has been theoretically proposed.Our results show that the antiferromagnetic structures of all studied bismuthides are characterized by the propagation vector, allowing for antiferromagnetic topological insulator state. Therefore, the antiferromagnetic representatives of half-Heusler family are excellent candidates for extended investigations of coexistence of superconductivity, magnetic order and non-trivial topology of electronic states