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Thermal ammonolysis of quasi-two-dimensional (quasi-2D) CoTa2O6 yields theO2-/N3- and anionic vacancy ordered Co2+Ta5+2O6-xN2x/3$\Box$x/3 (x $\leq$ 0.15)that exhibits a transition from antiferromagnetism to defect engineered aboveroom-temperature ferromagnetism as evidenced by diffraction, spectroscopic andmagnetic characterizations. First-principles calculations reveal the origin offerromagnetism is a particular CoON configuration with N located at Wyckoffposition 8j, which breaks mirror symmetry about ab plane. A pressure-inducedelectronic phase transition is also predicted at around 24.5 GPa, accompaniedby insulator-to-metal transition and magnetic moment vanishing.

Defect Engineered Room-Temperature Ferromagnetism in Quasi-Two-Dimensional Nitrided CoTa2O6