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Experimental investigations are combined with density functional theory to explore site\u2010selective Eu\n 3+<\/jats:sup>\n substitution as a strategy to enhance the magnetic properties of Fe\n 3<\/jats:sub>\n O\n 4<\/jats:sub>\n thin films. The substitution location of Eu\n 3+<\/jats:sup>\n , that is, octahedral versus tetrahedral, is confirmed by electrical resistivities and valence band photoemission measurements. Tetrahedrally Eu\u2010substituted Fe\n 3<\/jats:sub>\n O\n 4<\/jats:sub>\n exhibited an exceptionally enhanced saturation magnetization\n M<\/jats:italic>\n S<\/jats:sub>\n of up to 4.4 \u03bc\n B<\/jats:sub>\n \/f.u. because of noncollinearity, whereas octahedrally Eu\u2010substituted Fe\n 3<\/jats:sub>\n O\n 4<\/jats:sub>\n showed significantly reduced\n M<\/jats:italic>\n S<\/jats:sub>\n . X\u2010ray absorption spectroscopy and X\u2010ray magnetic circular dichroism measurements clearly revealed that in the tetrahedrally Eu\u2010substituted Fe\n 3<\/jats:sub>\n O\n 4<\/jats:sub>\n , the Eu\n 3+<\/jats:sup>\n magnetic moment positively contributed to the orbital magnetic moment that exhibited strong magnetic anisotropy. The deviation of the observed\n M<\/jats:italic>\n S<\/jats:sub>\n from the lower value predicted by N\u00e9el's theory of collinear ferrimagnetism further supported the role of noncollinearity. These results provide empirical evidence for the spin configuration of tetrahedrally Eu\u2010substituted Fe\n 3<\/jats:sub>\n O\n 4<\/jats:sub>\n and a new perspective for designing practical ferrimagnetic 4\n f<\/jats:italic>\n compounds with exceptional\n M<\/jats:italic>\n S<\/jats:sub>\n .\n <\/jats:p>","DOI":"10.1002\/smll.202411133","type":"journal-article","created":{"date-parts":[[2025,2,25]],"date-time":"2025-02-25T23:37:43Z","timestamp":1740526663000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Noncollinear Magnetism in Fe\n 3<\/sub>\n O\n 4<\/sub>\n Induced via Site\u2010Selective Rare\u2010Earth Substitution Boosting Its Saturation Magnetization"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5849-5638","authenticated-orcid":false,"given":"Haining","family":"Li","sequence":"first","affiliation":[{"name":"Department of Electrical Engineering and Information 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