Strain gradient is a normal phenomenon around a heterostructural interface in ultrathin film, and it is important to determine its effect on magnetic interactions to understand interfacial coupling. In this work, ultrathin Pr0.67Sr0.33MnO3 (PSMO) films on different substrates are studied. For PSMO film under different in-plane strain conditions, the saturated magnetization and Curie temperature can be qualitatively explained by double-exchange interaction and the Jahn–Teller distortion. However, the difference in the saturated magnetization with zero field cooling and 5 T field cooling is proportional to the strain gradient. Strain-gradient-induced structural disorder is proposed to enhance phonon–electron antiferromagnetic interactions and the corresponding antiferromagnetic-to-ferromagnetic phase transition via a strong magnetic field during the field cooling process. A non-monotonous structural transition of the MnO6 octahedral rotation can enlarge the strain gradient in PSMO film on a SrTiO3 substrate. This work demonstrates the existence of the flexomagnetic effect in ultrathin manganite film, which should be applicable to other complex oxide systems.
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