Tailoring the crystal structure, spin, and charge state of perovskite oxides through fluorine ion doping is an attractive and effective strategy, which could significantly modify the physical and chemical properties of base oxides. Here, BaFe1−xMnxO3−δ (x = 0, 0.1, 0.2, 0.3) and BaFe1−xMnxO2.9−δF0.1 (x = 0.1, 0.2, 0.3), belonging to 6H-type BaFeO3−δ, are prepared and investigated to evaluate the impact of F doping. The distortion of crystal structure and the reduced average valence of Mn and Fe confirm the preference for F substitution in the hexagonal layer, which are found as the key factors for the improved magnetic properties, including ferromagnetic ordering temperature, coercive force, and remanent magnetization. Moreover, the valence reduction of B-site ions and the increased resistance distinctly indicate the expense of electron hole via fluorine doping. This work describes the adjustment of crystal structure, electronic configuration, and ferromagnetic performance by simple F doping, which provides a prospect for practical magnetic materials.

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