Interfacial symmetry breaking leading to the preferential orbital occupation in complex oxide heterostructures offer effective routes to tailor magnetic anisotropy. We demonstrate the modulation of magnetic anisotropy in ${\mathrm{La}}_{0.7}{\mathrm{Sr}}_{0.3}{\mathrm{MnO}}_3$ (LSMO) thin films interfaced with the infinite-layer cuprate ${\mathrm{SrCuO}}_2$ (SCO). Static magnetization measurements show a pronounced in-plane magnetic anisotropy in LSMO/SCO bilayers compared to bare LSMO films, consistent with shifts in the resonance field as a function of the angle in ferromagnetic resonance measurements. In addition, a more than two-fold increase in the Gilbert damping is observed across all LSMO/SCO bilayers relative to the bare LSMO films, further supporting the interfacial modification of magnetic anisotropy and magnetization dynamics. However, inserting a thin ${\mathrm{SrTiO}}_3$ (STO) spacer in the control LSMO/STO/SCO sample exhibits the magnetic response similar to that of bare LSMO. This underscores the key role of the LSMO/SCO interface in the observed enhanced magnetic anisotropy. First-principles density functional theory calculations reveal a relatively larger occupation of the $3d_{x^2-y^2}$ orbital near the Fermi level in LSMO/SCO, accounting for the enhanced in-plane magnetic anisotropy, while ruling out the possibility of Rashba field-induced change in magnetic anisotropy. This work provides a comprehensive understanding of enhanced in-plane magnetic anisotropy and magnetization dynamics in the nonisostructural LSMO/SCO heterostructure.

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• Magnetism
• Cuprates
• Interfaces
• Magnetic thin films
• Manganites
• Density functional theory
• Ferromagnetic resonance
• Magnetization measurements