Continuous Tuning of Yafet–Kittel Spin Canting in Spinel Co _x Mn _{3− x}

The Yafet–Kittel (Y–K) ferrimagnetic phase represents a prototypical noncollinear magnetic structure in spinel oxides, yet its continuous tuning remains a significant challenge. Herein, Co _x Mn _{3− x} O ₄ (0.00 ≤  x  ≤ 1.00) compounds were synthesized via solid‐state reaction, enabling the successful realization of a continuously modulated Y–K phase. Structural analyses reveal that the Co ²⁺ ions predominantly occupy tetrahedral sites at low Co concentrations, but begin to populate octahedral sites once x exceeds 0.50. As the Co content x increases from 0.00 to 1.00, the magnetic ordering temperature of the Y–K phase rises monotonically from 41 to 80 K, reflecting the substantially stronger Co–Mn superexchange interactions compared to Mn–Mn coupling. Concurrently, the saturation magnetic moments decrease dramatically from 1.81 to 0.21 μ _B /f.u., accompanied by a progressive increase in the canting angle of the B‐site cation spins—from 31.7° to 66.3°.