Enhancement of Perpendicular Magnetic Anisotropy in Tm3Fe5O12(111) Epitaxial Films via Synergistic Stoichiometry and Strain Engineering

Abstract Establishing a reliable control of perpendicular magnetic anisotropy (PMA) is challenging but essential for the full utilization of rare‐earth iron garnets in spintronic devices. In this study, a feasible approach to enhance the PMA of ferrimagnetic thulium iron garnet (TmIG) films is presented. This approach involves precise adjustments in cation stoichiometry and epitaxial strain state. By fine‐tuning the pre‐ablation process and oxygen partial pressure during pulsed laser deposition, a series of high‐quality TmIG films can grow with variable cation stoichiometry, i.e., the Tm/Fe molar ratio. The finding reveals that cation stoichiometry plays a crucial role in determining the magnetic properties of the TmIG films. Particularly, the stoichiometric TmIG film has the strongest PMA due to the maximized magnetostriction coefficient. Combining this stoichiometry optimization and strain engineering, an unprecedented PMA strength of ≈30 kJ m −3 for TmIG is achieved. This achievement demonstrates a simple and effective method for harnessing the magnetic properties of rare‐earth iron garnet films, paving the way for their advanced applications in next‐generation spintronic devices.