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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. [ABSTRACT FROM AUTHOR]

2D magnets have recently drawn enormous interest. As an air‐stable A‐type van der Waals antiferromagnet (AFM), CrSBr has attracted great attention but has also led to controversies about its large‐span ordering temperatures. Herein, a systematic study of the magnetic phase transition in single‐crystalline CrSBr with ultrahigh‐quality through surface‐sensitive X‐ray magnetic linear dichroism and X‐ray magnetic circular dichroism measurements combined with vibrating sample magnetometry for characterization of bulk magnetization is reported. The interlayer AFM order of both surface and bulk CrSBr is revealed to maintain a similar Néel temperature within the range of 132–142 K. However, the intralayer ferromagnetic (FM) order of surface CrSBr is found to sustain up to ≈238 K, 70 K higher than the value obtained from the bulk CrSBr, demonstrating a dramatically different surface and bulk Curie temperature in CrSBr. Moreover, a half‐filled t2g electronic state for Cr3+ ions with magnetic moment of ≈3 µB/Cr in CrSBr is clearly identified. These results enrich the understanding of the electronic structure and magnetism in CrSBr, providing this material as a promising building block for future spintronic devices. [ABSTRACT FROM AUTHOR]

The advent of van der Waals (vdW) ferromagnetic (FM) and antiferromagnetic (AFM) materials offers unprecedented opportunities for spintronics and magneto‐optic devices. Combining magnetic Kerr microscopy and density functional theory calculations, the AFM‐FM transition is investigated and a surprising abnormal magneto‐optic anisotropy in vdW CrSBr associated with different magnetic phases (FM, AFM, or paramagnetic state) is discovered. This unique magneto‐optic property leads to different anisotropic optical reflectivity from different magnetic states, permitting direct imaging of the AFM Néel vector orientation and the dynamic process of the AFM‐FM transition within a magnetic field. Using Kerr microscopy, not only the domain nucleation and propagation process is imaged but also the intermediate spin‐flop state in the AFM‐FM transition is identified. The unique magneto‐optic property and clear identification of the dynamics process of the AFM‐FM phase transition in CrSBr demonstrate the promise of vdW magnetic materials for future spintronic technology. [ABSTRACT FROM AUTHOR]

Hafnium‐based binary oxides have attracted considerable attention due to their robust ferroelectricity at the nanoscale and compatibility with silicon‐based electronic technologies. To further promote the potential of Hafnium oxides for practical device applications, it is essential to effectively harness the interplay between structural symmetry, domain configuration, and ferroelectricity. Here, using Hf0.5Zr0.5O2/La0.67Sr0.33MnO3 (HZO/LSMO) heterostructures as a model system, the anisotropic strain‐mediated symmetry engineering and ferroelectricity enhancement are systematically investigated. By growing the heterostructures on (110)‐oriented perovskite substrates, considerable anisotropic strain is imposed on the LSMO bottom electrodes. Such an anisotropically‐strained LSMO layer acts as a structural template and effectively tune the structural symmetry, polar/non‐polar phase ratio, and ferroelectricity of the HZO top layer. Specifically, the anisotropic tensile strain stabilizes the ferroelectric rhombohedral and orthorhombic phases, thus enhancing the remnant polarization (Pr) up to 22 µC cm−2. In contrast, the anisotropic compressive strain facilitates the formation of non‐ferroelectric tetragonal phases, leading to a suppressed Pr down to 8 µC cm−2. These findings provide a guideline for understanding and modulating the intrinsic structure‐ferroelectricity relationship of HZO through anisotropic strain‐mediated symmetry engineering, which may shed light on the development of hafnium‐oxide‐based electronic devices. [ABSTRACT FROM AUTHOR]

Oxide heterostructures have great potential for spintronics applications due to their well‐defined heterointerfaces and vast functionalities. To integrate such compelling features into practical spintronics devices, effective control of the magnetic switching behavior is key. Here, continuous control of the magnetic coercive field in SrTiO3/SrRuO3 ultrathin heterostructures is achieved by oxygen vacancy (VO) engineering. Pulsed laser deposition of an oxygen‐deficient SrTiO3 capping layer can trigger VO migration into the SrRuO3 layer while avoiding the formation of Ru vacancies. Moreover, by varying the thickness and growth conditions of the SrTiO3 capping layer, the value of the coercive field (HC) in the ferromagnetic SrRuO3 layer can be continuously tuned. The maximum enhancement of HC at 5 K is 3.2 T. Such a wide‐range tunability of HC may originate from a VO‐induced enhancement of perpendicular magnetic anisotropy and domain wall pinning. This study offers effective approaches for controlling physical properties of oxide heterostructures via VO engineering, which may facilitate the development of oxide‐based functional devices. [ABSTRACT FROM AUTHOR]

Ferroelectric materials owning a polymorphic nanodomain structure usually exhibit colossal susceptibilities to external mechanical, electrical, and thermal stimuli, thus holding huge potential for relevant applications. Despite the success of traditional strategies by means of complex composition design, alternative simple methods such as strain engineering have been intensively sought to achieve a polymorphic nanodomain state in lead‐free, simple‐composition ferroelectric oxides in recent years. Here, a nanodomain configuration with morphed structural phases is realized in an epitaxial BaTiO3 film grown on a (111)‐oriented SrTiO3 substrate. Using a combination of experimental and theoretical approaches, it is revealed that a threefold rotational symmetry element enforced by the epitaxial constraint along the [111] direction of BaTiO3 introduces considerable instability among intrinsic tetragonal, orthorhombic, and rhombohedral phases. Such phase degeneracy induces ultrafine ferroelectric nanodomains (1–10 nm) with low‐angle domain walls, which exhibit significantly enhanced dielectric and piezoelectric responses compared to the (001)‐oriented BaTiO3 film with uniaxial ferroelectricity. Therefore, the finding highlights the important role of epitaxial symmetry in domain engineering of oxide ferroelectrics and facilitates the development of dielectric capacitors and piezoelectric devices. [ABSTRACT FROM AUTHOR]