Recently, theoretical and experimental research predicted that ferromagnets with strong spin-orbit coupling (SOC) could serve as spin sources with dramatically enhanced spin-orbit torque (SOT) efficiency due to the combination of spin Hall effect and anomalous Hall effect (AHE), presenting potential advantages over conventional nonmagnetic heavy metals. However, materials with a strong SOC and room-temperature ferromagnetism are rare. Here, we report on a ferromagnetic (FM) interfacial phase with Curie temperature exceeding 300 K in the heavy transition-metal oxide CaRuO3, in proximity to La0.67Sr0.33MnO3. Electron energy loss and polarized neutron reflectometry spectra reveal the strong charge transfer from Ru to Mn at the interface, triggering antiferromagnetic exchange interactions between interfacial Ru/Mn ions and thus transferring magnetic order from La0.67Sr0.33MnO3 to CaRuO3. An obvious advantage of such interfacial phase is the enhanced anomalous Hall effect at temperatures from 150 to 300 K. Compared to the most promising room-temperature ferromagnetic oxide La0.67Sr0.33MnO3, the anomalous Hall conductivity σxyAHE (or anomalous Hall angle θH) of CaRuO3/La0.67Sr0.33MnO3 superlattices is increased by 30 (or 31) times at 150 K and 10 (or 3) times at 300 K. This work demonstrates a special approach for inducing ferromagnetism in heavy transition-metal oxides with strong SOC, offering promising prospects for all-oxide-based spintronic applications.

Artificial oxide heterostructures have provided promising platforms for the exploration of emergent quantum phases with extraordinary properties. Here, we demonstrate an effective approach to stabilize a distinct oxygen octahedron rotation (OOR) characterized by a - b - c + in the ultrathin LaNiO 3 sublayers of the LaNiO 3 /CaTiO 3 superlattices. Unlike the a - b - c - OOR in the LaNiO 3 bare film, the a - b - c + OOR favors high conductivity, driving the LaNiO 3 sublayer to metallic state even when the layer thickness is as thin as 2 unit cells (u.c.). Simultaneously, strongly preferred occupation of d x 2 -y 2 orbital is achieved in LaNiO 3 sublayers. The largest change of occupancy is as high as 35%, observed in the 2 u.c.-thick LaNiO 3 sublayers sandwiched between 4 u.c.-thick CaTiO 3 sublayers. X-ray absorption spectra indicate that the a - b - c + OOR pattern of LaNiO 3 achieved in the LaNiO 3 /CaTiO 3 heterostructures has significantly enhanced the Ni-3d/O-2p hybridization, stabilizing the metallic phase in ultrathin LaNiO 3 sublayers. The present work demonstrates that modulating the mode of OOR through heteroepitaxial synthesis can modify the orbital-lattice correlations in correlated perovskite oxides, revealing hidden properties of the materials.

Magnetic proximity-induced magnetism in paramagnetic LaNiO3 (LNO) has spurred intensive investigations in the past decade. However, no consensus has been reached so far regarding the magnetic order in LNO layers in relevant heterostructures. This paper reports a layered ferromagnetic structure for the (111)-oriented LNO/LaMnO3 (LMO) superlattices. It is found that each period of the superlattice consisted of an insulating LNO-interfacial phase (five unit cells in thickness, ∼1.1 nm), a metallic LNO-inner phase, a poorly conductive LMO-interfacial phase (three unit cells in thickness, ∼0.7 nm), and an insulating LMO-inner phase. All four of these phases are ferromagnetic, showing different magnetizations. The Mn-to-Ni interlayer charge transfer is responsible for the emergence of a layered magnetic structure, which may cause magnetic interaction across the LNO/LMO interface and double exchange within the LMO-interfacial layer. This work indicates that the proximity effect is an effective means of manipulating the magnetic state and associated properties of complex oxides.

The discovery of intrinsic 2D magnetic materials has opened up new opportunities for exploring magnetic properties at atomic layer thicknesses, presenting potential applications in spintronic devices. Here a new 2D ferrimagnetic crystal of nonlayered FeCr2S4 is synthesized with high phase purity using chemical vapor deposition. The obtained 2D FeCr2S4 exhibits perpendicular magnetic anisotropy, as evidenced by the out-of-plane/in-plane Hall effect and anisotropic magnetoresistance. Theoretical calculations further elucidate that the observed magnetic anisotropy can be attributed to its surface termination structure. By combining temperature-dependent magneto-transport and polarized Raman spectroscopy characterizations, it is discovered that both the measured Curie temperature and the critical temperature at which a low energy magnon peak disappeared remains constant, regardless of its thickness. Magnetic force microscopy measurements show the flipping process of magnetic domains. The exceptional air-stability of the 2D FeCr2S4 is also confirmed via Raman spectroscopy and Hall hysteresis loops. The robust anisotropic ferrimagnetism, the thickness-independent of Curie temperature, coupled with excellent air-stability, make 2D FeCr2S4 crystals highly attractive for future spintronic devices.

Due to the strong interlayer coupling between multiple degrees of freedom, oxide heterostructures have demonstrated exotic properties that are not shown by their bulk counterparts. One of the most interesting properties is ferromagnetism at the interface formed between "nonferromagnetic" compounds. Here we report on the interfacial ferromagnetic phase induced in the superlattices consisting of the two paramagnetic oxides CaRuO3 (CRO) and LaNiO3 (LNO). By varying the sublayer thickness in the superlattice period, we demonstrate that the ferromagnetic order has been established in both CaRuO3 and LaNiO3 sublayers, exhibiting an identical Curie temperature of ∼75 K. The X-ray absorption spectra suggest a strong charge transfer from Ru to Ni at the interface, triggering superexchange interactions between Ru/Ni ions and giving rise to the emergent ferromagnetic phase. Moreover, the X-ray linear dichroism spectra reveal the preferential occupancy of the d3z2-r2 orbital for the Ru ions and the dx2-y2 orbital for the Ni ions in the heterostructure. This leads to different magnetic anisotropy of the superlattices when they are dominated by CRO or LNO sublayers. This work clearly demonstrates a charge-transfer-induced interfacial ferromagnetic phase in the whole ferromagnet-free oxide heterostructures, offering a feasible way to tailor oxide materials for desired functionalities.

Due to the strong interactions from multiple degrees of freedom at the interfaces, electron-correlated oxide heterostructures have provided a promising platform for creating exotic quantum states. Understanding and controlling the coupling effects at the oxide interface are prerequisites for designing emergent interfacial phases with desired functionalities. Here, we report the dimensional control of the interface coupling-induced ferromagnetic (FM) phase in perovskite-CaRuO 3 /infinite-layered-SrCuO 2 superlattices. Structural analysis reveals the occurrence of chain-type to planar-type structural transitions for the SrCuO 2 layer as the layer thickness increases. The Hall and magnetoresistance measurements indicate the appearance of an interfacial FM state in the originally paramagnetic CaRuO 3 layers when the CaRuO 3 layer is in proximity to the chain-type SrCuO 2 layers; this superlattice has the highest Curie temperature of ~75 K and perpendicular magnetic anisotropy. Along with the thickness-driven structural transition of the SrCuO 2 layers, the interfacial FM order gradually deteriorates and finally disappears. As shown by the X-ray absorption results, the charge transfer at the CaRuO 3 /chain-SrCuO 2 and CaRuO 3 /plane-SrCuO 2 interfaces are different, resulting in dimensional control of the interfacial magnetic state. The results from our study can be used to facilitate a new method to manipulate interface coupling and create emergent interfacial phases in oxide heterostructures.

Due to the strong interlayer coupling between multiple degrees of freedom, oxide heterostructures usually produce distinct interfacial phases with unexpected functionalities. Here, we report on the realization of quasi-two-dimensional ferromagnetic state in ultrathin La0.7Sr0.3MnO3 (LSMO) layer down to two unit cells (u.c.), being sandwiched by the planar infinite-layer structured SrCuO2 layers (P-SCO). We find the LSMO/P-SCO interface coupling has greatly suppressed the magnetic dead layer of LSMO, resulting in an emergent interfacial ferromagnetic phase. Thus, robust ferromagnetic order can be maintained in the 2 u.c.-thick LSMO layer (∼7.7 Å), showing a Curie temperature of ∼260 K and remarkable perpendicular magnetic anisotropy. X-ray absorption spectra reveal notable charge transfer from Mn to Cu at the interface, and thus, resulted preferential d3z2−r2 orbital occupation for interfacial Mn ions plays an important role in the inducing of perpendicular magnetic anisotropy in quasi-two-dimensional LSMO layer. Our work demonstrates a unique approach for tuning the properties of oxides via an interface engineering of oxygen coordination in perovskite/infinite-layer heterostructures.

Ferromagnetic materials with a strong spin‐orbit coupling (SOC) have attracted much attention in recent years because of their exotic properties and potential applications in energy‐efficient spintronics. However, such materials are scarce in nature. Here, a proximity‐induced paramagnetic to ferromagnetic transition for the heavy transition metal oxide CaRuO 3 in (001)‐(LaMnO 3 /CaRuO 3 ) superlattices is reported. Anomalous Hall effect is observed in the temperature range up to 180 K. Maximal anomalous Hall conductivity and anomalous Hall angle are as large as ∼15 Ω −1 cm −1 and ∼0.93%, respectively, by one to two orders of magnitude larger than those of the typical 3d ferromagnetic oxides such as La 0.67 Sr 0.33 MnO 3 . Density functional theory calculations indicate the existence of avoid band crossings in the electronic band structure of the ferromagnetic CRO layer, which enhances Berry curvature thus strong anomalous Hall effects. Further evidences from polarized neutron reflectometry show that the CaRuO 3 layers are in a fully ferromagnetic state (∼0.8 μ B /Ru), in sharp contrast to the proximity‐induced canted antiferromagnetic state in 5d oxides SrIrO 3 and CaIrO 3 (∼0.1 μ B /Ir). More than that, the magnetic anisotropy of the (001)‐(LaMnO 3 /CaRuO 3 ) superlattices is eightfold symmetric, showing potential applications in the technology of multistate data storage.

By modifying the entangled multi‐degrees of freedom of transition‐metal oxides, interlayer coupling usually produces interfacial phases with unusual functionalities. Herein, a symmetry‐mismatch‐driven interfacial phase transition from paramagnetic to ferromagnetic state is reported. By constructing superlattices using CaRuO3 and SrTiO3, two oxides with different oxygen octahedron networks, the tilting/rotation of oxygen octahedra near interface is tuned dramatically, causing an angle increase from ≈150° to ≈165° for the RuORu bond. This in turn drives the interfacial layer of CaRuO3, ≈3 unit cells in thickness, from paramagnetic into ferromagnetic state. The ferromagnetic order is robust, showing the highest Curie temperature of ≈120 K and the largest saturation magnetization of ≈0.7 µB per formula unit. Density functional theory calculations show that the reduced tilting/rotation of RuO6 octahedra favors an itinerant ferromagnetic ground state. This work demonstrates an effective phase tuning by coupled octahedral rotations, offering a new approach to explore emergent materials with desired functionalities.

Magnetic skyrmions are scarcely investigated for single-crystal quality films, for which skyrmions may have a remarkable performance. Even in the limited studies in this aspect, the skyrmions are usually probed by the topological Hall effect, missing important information on dynamic properties. Here, we present a comprehensive investigation on the generation/manipulation of magnetic skyrmions in La0.67Ba0.33MnO3 single-crystal films. Using the technique of magnetic force microscopy, the current-driven skyrmion dynamics are directly observed. Unlike isolated skyrmions produced by magnetic field alone, closely packed skyrmions can be generated by electric pulses in a magnetic background, with a high density (∼60/μm2) and a small size (dozens of nanometers). The threshold current moving skyrmions is ∼2.3 × 104 A/cm2, 2-3 orders of magnitude lower than that required by metallic multilayers or van der Waals ferromagnetic heterostructures. Our work demonstrates the great potential of single-crystal oxide films in developing skyrmion-based devices.

Artificial oxide heterostructures have provided promising platforms for the exploration of emergent quantum phases with extraordinary properties. One of the most interesting phenomena is the interfacial magnetism formed between two non-magnetic compounds. Here, a robust ferromagnetic phase emerged at the (111)-oriented heterointerface between paramagnetic CaRuO3 and diamagnetic SrTiO3 is reported. The Curie temperature is as high as ≈155 K and the saturation magnetization is as large as ≈1.3 µB per formula unit for the (111)-CaRuO3/SrTiO3 superlattices, which are obviously superior to those of the (001)-oriented counterparts and are comparable to the typical itinerant ferromagnet SrRuO3. A strong in-plane magnetic anisotropy with six-fold symmetry is further revealed by the anisotropic magnetoresistance measurements, presenting a large in-plane anisotropic field of 3.0-3.6 T. More importantly, the magnetic easy axis of the (111)-oriented superlattices can be effectively tuned from 〈 11 2 ¯ $11\overline{2}$ 1〉 to 〈 1 1 ¯ 0 $1 \bar{1}0$ 〉 directions by increasing the layer thickness of SrTiO3. The findings demonstrate a feasible approach to enhance the interface coupling effect by varying the stacking orientation of oxide heterostructures. The tunable magnetic anisotropy also shows potential applications in low-power-consumption or exchange spring devices.

Heterostructures composed of dissimilar oxides with different properties offer opportunities to develop emergent devices with desired functionalities. A key feature of oxide heterostructures is interface electronics and orbital reconstructions. Here, we combined infinite-layered SrCuO2 and perovskite SrRuO3 into heterostructures. A rare high spin state as large as 3.0 μB f.u-1 and an increase in Curie temperature by 12 K are achieved in an ultrathin SrRuO3 film capped by a SrCuO2 layer. Atomic-scale lattice imaging shows the uniform CuO2-plane-to-RuO5-pyramid connection at the interface, where the regularly arranged RuO5 pyramids were elongated along the out-of-plane direction. As revealed by theoretical calculations and spectral analysis, these features finally result in an abnormally high spin state of the interfacial Ru ions with highly polarized eg orbitals. The present work demonstrates that oxygen coordination engineering at the infinite-layer/perovskite oxide interface is a promising approach towards advanced oxide electronics.

Two-dimensional electron gases (2DEGs) formed at the interface between two oxide insulators present a promising platform for the exploration of emergent phenomena. While most of the previous works focused on SrTiO3-based 2DEGs, here we took the amorphous-ABO3/KTaO3 system as the research object to study the relationship between the interface conductivity and the redox property of B-site metal in the amorphous film. The criterion of oxide–oxide interface redox reactions for the B-site metals, Zr, Al, Ti, Ta, and Nb in conductive interfaces was revealed: the formation heat of metal oxide, Δ H f o , is lower than –350 kJ/(mol O) and the work function of the metal Φ is in the range of 3.75 eV < Φ < 4.4 eV. Furthermore, we found that the smaller absolute value of Δ H f o and the larger value of Φ of the B-site metal would result in higher mobility of the two-dimensional electron gas that formed at the corresponding amorphous-ABO3/KTaO3 interface. This finding paves the way for the design of high-mobility all-oxide electronic devices.

Heterostructures composed of dissimilar perovskite oxides with different properties provide an opportunity to observe emergent phenomena, and have promising applications. A key feature of oxide heterostructures is interfacial electronic and orbital reconstruction. In this paper, we demonstrate a dramatic variation in magnetic anisotropy caused by electric tuning of the charge-transfer process in a La0.8Sr0.2CoO3/La0.67Sr0.33MnO3 bilayer structure. By repeatedly changing the valence state of Co ions in the La0.8Sr0.2CoO3 top layer using ionic-liquid gating, reversible switching of the magnetic easy axis of the bottom La0.67Sr0.33MnO3 layer between the out-of-plane and the in-plane direction is achieved, accompanying a modulation of the interfacial exchange coupling. Mn-to-Co charge transfer and its effect on the interfacial orbital occupancy are further confirmed by x-ray absorption spectroscopy and x-ray-linear-dichroism analysis. The considerable interfacial charge transfer causes an overlap of the Mn and Co 3d orbitals, resulting in orbital reconstruction in the La0.67Sr0.33MnO3 layer and thus magnetic anisotropy. This work demonstrates a promising method for tuning the orbital occupancy and related properties of perovskite heterostructures.

Two-dimensional electron gases (2DEGs) formed at the interface between two oxide insulators present a promising platform for the exploration of emergent phenomena. While most of the previous works focused on SrTiO3-based 2DEGs, here we report on a systematic investigation of the 2DEGs at amorphous-LaAlO3/KTaO3 (a-LAO/KTO) interfaces, focusing on the effect of fabrication conditions on 2DEGs. We found that 2DEGs can be formed in a wide temperature range from room temperature to 750 degrees under the oxygen pressure 1 x 10(-4) Pa. Unexpectedly, its performance shows a unusual strong dependence on fabrication temperature: the Hall mobility increases rapidly with the decrease of substrate temperature. The highest extracted mobility of charge carriers coming from d(xz)/d(yz) subband is similar to 6.6 x 10 (3) cm(2) V(-1)s(-1), achieved under the condition of T-s = 100 degrees C and P-O2 = 3 x 10(-5) Pa. This value is higher than that of the 2DEGs of a-LAO/SrTiO3 by a factor of 30, which reveals the unique character of the 2DEGs formed by 5d electrons. Two-band model is applied for the analysis of the transport behavior, from which information on carrier density and Hall mobility and their dependence on fabrication conditions are determined.