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1. Bulk-like dielectric and magnetic properties of sub 100 nm thick single crystal Cr2O3 films on an epitaxial oxide electrode

   https://doi.org/10.1038/s41598-020-71619-1  

   Vu, N. M.; Luo, X.; Novakov, S.; Jin, W.; Nordlander, J.; Meisenheimer, P. B.; Trassin, M.; Zhao, L.; Heron, J. T. (December 2020, Scientific Reports)

   null (Ed.)

   Abstract The manipulation of antiferromagnetic order in magnetoelectric Cr 2 O 3 using electric field has been of great interest due to its potential in low-power electronics. The substantial leakage and low dielectric breakdown observed in twinned Cr 2 O 3 thin films, however, hinders its development in energy efficient spintronics. To compensate, large film thicknesses (250 nm or greater) have been employed at the expense of device scalability. Recently, epitaxial V 2 O 3 thin film electrodes have been used to eliminate twin boundaries and significantly reduce the leakage of 300 nm thick single crystal films. Here we report the electrical endurance and magnetic properties of thin (less than 100 nm) single crystal Cr 2 O 3 films on epitaxial V 2 O 3 buffered Al 2 O 3 (0001) single crystal substrates. The growth of Cr 2 O 3 on isostructural V 2 O 3 thin film electrodes helps eliminate the existence of twin domains in Cr 2 O 3 films, therefore significantly reducing leakage current and increasing dielectric breakdown. 60 nm thick Cr 2 O 3 films show bulk-like resistivity (~ 10 12 Ω cm) with a breakdown voltage in the range of 150–300 MV/m. Exchange bias measurements of 30 nm thick Cr 2 O 3 display a blocking temperature of ~ 285 K while room temperature optical second harmonic generation measurements possess the symmetry consistent with bulk magnetic order. 

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2. Microstructural Underpinnings of Giant Intrinsic Exchange Bias in Epitaxial NiCo ₂ O ₄ Thin Films

   https://doi.org/10.1002/aelm.202400149  

   Yang, Detian; Subedi, Arjun; Liu, Chao; Ambaye, Haile; Lauter, Valeria; Dowben, Peter_A; Liu, Yaohua; Xu, Xiaoshan (November 2024, Advanced Electronic Materials)

   Abstract Understanding intrinsic exchange bias in nominally single‐component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo₂O₄, the origin of intrinsic exchange bias in NiCo₂O₄(111) films deposited on Al₂O₃(0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X‐ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo₂O₄(111)/Al₂O₃(0001) arises from a reconstructed antiferromagnetic rock‐salt Ni_xCo_1‐xO layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo₂O₄, an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties. 

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3. Anomalous Hall effect and perpendicular magnetic anisotropy in ultrathin ferrimagnetic NiCo ₂ O ₄ films

   https://doi.org/10.1063/5.0097869  

   Chen, Xuegang; Wu, Qiuchen; Zhang, Le; Hao, Yifei; Han, Myung-Geun; Zhu, Yimei; Hong, Xia (June 2022, Applied Physics Letters)

   The inverse spinel ferrimagnetic NiCo₂O₄possesses high magnetic Curie temperature T_C, high spin polarization, and strain-tunable magnetic anisotropy. Understanding the thickness scaling limit of these intriguing magnetic properties in NiCo₂O₄thin films is critical for their implementation in nanoscale spintronic applications. In this work, we report the unconventional magnetotransport properties of epitaxial (001) NiCo₂O₄films on MgAl₂O₄substrates in the ultrathin limit. Anomalous Hall effect measurements reveal strong perpendicular magnetic anisotropy for films down to 1.5 unit cell (1.2 nm), while T_Cfor 3 unit cell and thicker films remains above 300 K. The sign change in the anomalous Hall conductivity [Formula: see text] and its scaling relation with the longitudinal conductivity ([Formula: see text]) can be attributed to the competing effects between impurity scattering and band intrinsic Berry curvature, with the latter vanishing upon the thickness driven metal–insulator transition. Our study reveals the critical role of film thickness in tuning the relative strength of charge correlation, Berry phase effect, spin–orbit interaction, and impurity scattering, providing important material information for designing scalable epitaxial magnetic tunnel junctions and sensing devices using NiCo₂O₄. 

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4. Intrinsic exchange bias from interfacial reconstruction in an epitaxial Ni _x Co _y Fe _{3− x −y} O ₄ (111)/ $\alpha$ -Al ₂ O ₃ (0001) thin film family

   https://doi.org/10.1088/1361-648X/ad789d  

   Yang, Detian; Liu, Yaohua; Xu, Xiaoshan (September 2024, Journal of Physics: Condensed Matter)

   Abstract Intrinsic exchange bias is known as the unidirectional exchange anisotropy that emerges in a nominally single-component ferro-(ferri-)magnetic system. In this work, with magnetic and structural characterizations, we demonstrate that intrinsic exchange bias is a general phenomenon in (Ni, Co, Fe)-based spinel oxide films deposited on $\alpha$-Al₂O₃(0001) substrates, due to the emergence of a rock-salt interfacial layer consisting of antiferromagnetic CoO from interfacial reconstruction. We show that in Ni_xCo_yFe_3−x−yO₄(111)/ $\alpha$-Al₂O₃(0001) films, intrinsic exchange bias and interfacial reconstruction have consistent dependences on Co concentrationy, while the Ni and Fe concentration appears to be less important. This work establishes a family of intrinsic exchange bias materials with great tunability by stoichiometry and highlights the strategy of interface engineering in controlling material functionalities. 

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5. Imaging Local Effects of Voltage and Boron Doping on Spin Reversal in Antiferromagnetic Magnetoelectric Cr ₂ O ₃ Thin Films and Devices

   https://doi.org/10.1002/adfm.202408542  

   Erickson, Adam; Shah, Syed_Qamar_Abbas; Mahmood, Ather; Buragohain, Pratyush; Fescenko, Ilja; Gruverman, Alexei; Binek, Christian; Laraoui, Abdelghani (August 2024, Advanced Functional Materials)

   Abstract Chromia (Cr₂O₃) is a magnetoelectric oxide that permits voltage‐control of the antiferromagnetic (AFM) order, but it suffers technological constraints due to its low Néel Temperature (T_N≈307 K) and the need of a symmetry‐breaking applied magnetic field to achieve reversal of the Néel vector. Recently, boron (B) doping of Cr₂O₃films led to an increaseT_N>400 K and allowed the realization of voltage magnetic‐field free controlled Néel vector rotation. Here, the impact of B doping is directly imaged on the formation of AFM domains in Cr₂O₃thin films and elucidates the mechanism of voltage‐controlled manipulation of the spin structure using nitrogen‐vacancy (NV) scanning probe magnetometry. A stark reduction and thickness dependence of domain size in B‐doped Cr₂O₃(B:Cr₂O₃) films is found, explained by the increased germ density, likely associated with the B doping. By reconstructing the surface magnetization from the NV stray‐field maps, a qualitative distinction between the undoped and B‐doped Cr₂O₃films is found, manifested by the histogram distribution of the AFM ordering, that is, 180°domains for pure films, and 90°domains for B:Cr₂O₃films. Additionally, NV imaging of voltage‐controlled B‐doped Cr₂O₃devices corroborates the 90°rotation of the AFM domains observed in magnetotransport measurement. 

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