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The interplay of 3d and 4f magnetism in rare\u2010earth transition metal antimonides is an ideal platform to search for such complex behavior. Here the synthesis, crystal growth, structure, and complex magnetic properties are reported of the new compound Pr<jats:sub>3<\/jats:sub>Fe<jats:sub>3<\/jats:sub>Sb<jats:sub>7<\/jats:sub> as studied by magnetization and electrical transport measurements in static and pulsed magnetic fields up to 56\u00a0T, powder neutron diffraction, and M\u00f6\u00dfbauer spectroscopy. On cooling without external magnetic field, Pr<jats:sub>3<\/jats:sub>Fe<jats:sub>3<\/jats:sub>Sb<jats:sub>7<\/jats:sub> shows spontaneous magnetization, indicating a symmetry breaking without a compensating domain structure. The Fe substructure exhibits noncollinear ferromagnetic order below the Curie temperature <jats:italic>T<\/jats:italic><jats:sub>C<\/jats:sub>\u00a0\u2248\u00a0380 K. Two spin orientations exist, which approximately align along the Fe\u2013Fe bond directions, one parallel to the <jats:italic>ab<\/jats:italic> plane and a second one with the moments canting away from the <jats:italic>c<\/jats:italic> axis. The Pr substructure orders below 40\u00a0K, leading to a spin\u2010reorientation transition (SRT) of the iron substructure. In low fields, the Fe and Pr magnetic moments order antiparallel to each other, which gives rise to a magnetization antiparallel to the external field. At 1.4\u00a0K, the magnetization approaches saturation above 40\u00a0T. The compound exhibits metallic resistivity along the <jats:italic>c<\/jats:italic> axis, with a small anomaly at the SRT.<\/jats:p>","DOI":"10.1002\/adma.202207945","type":"journal-article","created":{"date-parts":[[2022,11,30]],"date-time":"2022-11-30T03:19:51Z","timestamp":1669778391000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Unconventional Spin State Driven Spontaneous Magnetization in a Praseodymium Iron Antimonide"],"prefix":"10.1002","volume":"35","author":[{"given":"Falk","family":"Pabst","sequence":"first","affiliation":[{"name":"Fakult\u00e4t f\u00fcr Chemie und Lebensmittelchemie Technische Universit\u00e4t Dresden  01062 Dresden Germany"},{"name":"W\u00fcrzburg\u2010Dresden Cluster of Excellence ct.qmat  01062 Dresden Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Sabrina","family":"Palazzese","sequence":"additional","affiliation":[{"name":"W\u00fcrzburg\u2010Dresden 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