Reduction-Induced Magnetic Behavior in LaFeO3-δ Thin Films.

The effect of oxygen reduction on the magnetic properties of LaFeO3-δ (LFO) thin films was studied to better understand the viability of LFO as a candidate for magnetoionic memory. Differences in the amount of oxygen lost by LFO and its magnetic behavior were observed in nominally identical LFO films grown on substrates prepared using different common methods. In an LFO film grown on as-received SrTiO3 (STO) substrate, the original perovskite film structure was preserved following reduction, and remnant magnetization was only seen at low temperatures. In a LFO film grown on annealed STO, the LFO lost significantly more oxygen and the microstructure decomposed into La- and Fe-rich regions with remnant magnetization that persisted up to room temperature. These results demonstrate an ability to access multiple, distinct magnetic states via oxygen reduction in the same starting material and suggest LFO may be a suitable materials platform for nonvolatile multistate memory.

Charge-Transfer-Induced Interfacial Ferromagnetism in Ferromagnet-Free Oxide Heterostructures.

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.

Emergent Ferromagnetism in CaRuO3/CaMnO3 (111)-Oriented Superlattices.

The boundary between CaRuO3 and CaMnO3 is an ideal test bed for emergent magnetic ground states stabilized through interfacial electron interactions. In this system, nominally antiferromagnetic and paramagnetic materials combine to yield interfacial ferromagnetism in CaMnO3 due to electron leakage across the interface. In this work, we show that the crystal symmetry at the surface is a critical factor determining the nature of the interfacial interactions. Specifically, by growing CaRuO3/CaMnO3 heterostructures along the (111) instead of the (001) crystallographic axis, we achieve a 3-fold enhancement of the magnetization and involve the CaRuO3 layers in the ferromagnetism, which now spans both constituent materials. The stabilization of a net magnetic moment in CaRuO3 through strain effects has been long-sought but never consistently achieved, and our observations demonstrate the importance of interface engineering in the development of new functional heterostructures.

Investigating Anisotropic Magnetoresistance in Epitaxially Strained CoFe Thin Films on a Flexible Mica.

This study investigates the crystal structure, epitaxial relation, and magnetic properties in CoFe thin films deposited on a flexible mica substrate. The epitaxial growth of CoFe thin films was successfully achieved by DC magnetron sputtering, forming three CoFe(002) domains exhibiting four-fold symmetry on the mica substrate. A notable achievement of this work was the attainment of the highest anisotropic magnetoresistance (AMR) value reported to date on a flexible substrate. Additionally, it was observed that the magnetic characteristics of the CoFe films on the flexible mica substrate display reversibility upon strain release. More importantly, the AMR effect of epitaxial CoFe films on flexible mica shows lesser dependence on the crystalline orientation and remains the same under different bending states. These findings demonstrate the potential of utilizing CoFe films on flexible substrates to develop wearable magnetoresistance sensors with diverse applications.

Current-induced Néel order switching facilitated by magnetic phase transition.

Terahertz (THz) spin dynamics and vanishing stray field make antiferromagnetic (AFM) materials the most promising candidate for the next-generation magnetic memory technology with revolutionary storage density and writing speed. However, owing to the extremely large exchange energy barriers, energy-efficient manipulation has been a fundamental challenge in AFM systems. Here, we report an electrical writing of antiferromagnetic orders through a record-low current density on the order of 106 A cm-2 facilitated by the unique AFM-ferromagnetic (FM) phase transition in FeRh. By introducing a transient FM state via current-induced Joule heating, the spin-orbit torque can switch the AFM order parameter by 90° with a reduced writing current density similar to ordinary FM materials. This mechanism is further verified by measuring the temperature and magnetic bias field dependences, where the X-ray magnetic linear dichroism (XMLD) results confirm the AFM switching besides the electrical transport measurement. Our findings demonstrate the exciting possibility of writing operations in AFM-based devices with a lower current density, opening a new pathway towards pure AFM memory applications.

Termination switching of antiferromagnetic proximity effect in topological insulator.

This work reports the ferromagnetism of topological insulator, (Bi,Sb)2Te3 (BST), with a Curie temperature of approximately 120 K induced by magnetic proximity effect (MPE) of an antiferromagnetic CrSe. The MPE was shown to be highly dependent on the stacking order of the heterostructure, as well as the interface symmetry: Growing CrSe on top of BST results in induced ferromagnetism, while growing BST on CrSe yielded no evidence of an MPE. Cr-termination in the former case leads to double-exchange interactions between Cr3+ surface states and Cr2+ bulk states. This Cr3+-Cr2+ exchange stabilizes the ferromagnetic order localized at the interface and magnetically polarizes the BST Sb band. In contrast, Se-termination at the CrSe/BST interface yields no detectable MPE. These results directly confirm the MPE in BST films and provide critical insights into the sensitivity of the surface state.

Probing the low-temperature limit of the quantum anomalous Hall effect.

Quantum anomalous Hall effect has been observed in magnetically doped topological insulators. However, full quantization, up until now, is limited within the sub-1 K temperature regime, although the material's magnetic ordering temperature can go beyond 100 K. Here, we study the temperature limiting factors of the effect in Cr-doped (BiSb)2Te3 systems using both transport and magneto-optical methods. By deliberate control of the thin-film thickness and doping profile, we revealed that the low occurring temperature of quantum anomalous Hall effect in current material system is a combined result of weak ferromagnetism and trivial band involvement. Our findings may provide important insights into the search for high-temperature quantum anomalous Hall insulator and other topologically related phenomena.

Evidence of Spin Frustration in a Vanadium Diselenide Monolayer Magnet.

Monolayer VSe2 , featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic 2D transition-metal dichalcogenides (2D-TMDs). Herein, by means of in situ microscopy and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, direct spectroscopic signatures are established, that identify the metallic 1T-phase and vanadium 3d1 electronic configuration in monolayer VSe2 grown on graphite by molecular-beam epitaxy. Element-specific X-ray magnetic circular dichroism, complemented with magnetic susceptibility measurements, further reveals monolayer VSe2 as a frustrated magnet, with its spins exhibiting subtle correlations, albeit in the absence of a long-range magnetic order down to 2 K and up to a 7 T magnetic field. This observation is attributed to the relative stability of the ferromagnetic and antiferromagnetic ground states, arising from its atomic-scale structural features, such as rotational disorders and edges. The results of this study extend the current understanding of metallic 2D-TMDs in the search for exotic low-dimensional quantum phenomena, and stimulate further theoretical and experimental studies on van der Waals monolayer magnets.

Phase-driven magneto-electrical characteristics of single-layer MoS2.

Magnetism of the MoS2 semiconducting atomic layer was highlighted for its great potential in the applications of spintronics and valleytronics. In this study, we demonstrate an evolution of magneto-electrical properties of single layer MoS2 with the modulation of defect configurations and formation of a partial 1T phase. With Ar treatment, sulfur was depleted within the MoS2 flake leading to a 2H (low-spin) → partial 1T (high-spin) phase transition. The phase transition was accompanied by the development of a ferromagnetic phase. Alternatively, the phase transition could be driven by the desorption of S atoms at the edge of MoS2via O2 treatment while with a different ordering magnitude in magnetism. The edge-sensitive magnetism of the single-layer MoS2 was monitored by magnetic force microscopy and validated by a first-principle calculation with graded-Vs (sulfur vacancy) terminals set at the edge, where band-splitting appeared more prominent with increasing Vs. Treatment with Ar and O2 enabled a dual electrical characteristic of the field effect transistor (FET) that featured linear and saturated responses of different magnitudes in the Ids-Vds curves, whereas the pristine MoS2 FET displayed only a linear electrical dependency. The correlation and tuning of the Vs-1T phase transition would provide a playground for tailoring the phase-driven properties of MoS2 semiconducting atomic layers in spintronic applications.

Competing Anisotropy-Tunneling Correlation of the CoFeB/MgO Perpendicular Magnetic Tunnel Junction: An Electronic Approach.

We intensively investigate the physical principles regulating the tunneling magneto-resistance (TMR) and perpendicular magnetic anisotropy (PMA) of the CoFeB/MgO magnetic tunnel junction (MTJ) by means of angle-resolved x-ray magnetic spectroscopy. The angle-resolved capability was easily achieved, and it provided greater sensitivity to symmetry-related d-band occupation compared to traditional x-ray spectroscopy. This added degree of freedom successfully solved the unclear mechanism of this MTJ system renowned for controllable PMA and excellent TMR. As a surprising discovery, these two physical characteristics interact in a competing manner because of opposite band-filling preference in space-correlated symmetry of the 3d-orbital. An overlooked but harmful superparamagnetic phase resulting from magnetic inhomogeneity was also observed. This important finding reveals that simultaneously achieving fast switching and a high tunneling efficiency at an ultimate level is improbable for this MTJ system owing to its fundamental limit in physics. We suggest that the development of independent TMR and PMA mechanisms is critical towards a complementary relationship between the two physical characteristics, as well as the realization of superior performance, of this perpendicular MTJ. Furthermore, this study provides an easy approach to evaluate the futurity of any emerging spintronic candidates by electronically examining the relationship between their magnetic anisotropy and transport.

A facile green antisolvent approach to Cu2+-doped ZnO nanocrystals with visible-light-responsive photoactivities.

An environmentally benign antisolvent method has been developed to prepare Cu(2+)-doped ZnO nanocrystals with controllable dopant concentrations. A room temperature ionic liquid, known as a deep eutectic solvent (DES), was used as the solvent to dissolve ZnO powders. Upon the introduction of the ZnO-containing DES into a bad solvent which shows no solvation to ZnO, ZnO was precipitated and grown due to the dramatic decrease of solubility. By adding Cu(2+) ions to the bad solvent, the growth of ZnO from the antisolvent process was accompanied by Cu(2+) introduction, resulting in the formation of Cu(2+)-doped ZnO nanocrystals. The as-prepared Cu(2+)-doped ZnO showed an additional absorption band in the visible range (400-800 nm), which conduced to an improvement in the overall photon harvesting efficiency. Time-resolved photoluminescence spectra, together with the photovoltage information, suggested that the doped Cu(2+) may otherwise trap photoexcited electrons during the charge transfer process, inevitably depressing the photoconversion efficiency. The photoactivity of Cu(2+)-doped ZnO nanocrystals for photoelectrochemical water oxidation was effectively enhanced in the visible region, which achieved the highest at 2.0 at% of Cu(2+). A further increase in the Cu(2+) concentration however led to a decrease in the photocatalytic performance, which was ascribed to the significant carrier trapping caused by the increased states given by excessive Cu(2+). The photocurrent action spectra illustrated that the enhanced photoactivity of the Cu(2+)-doped ZnO nanocrystals was mainly due to the improved visible photon harvesting achieved by Cu(2+) doping. These results may facilitate the use of transition metal ion-doped ZnO in other photoconversion applications, such as ZnO based dye-sensitized solar cells and magnetism-assisted photocatalytic systems.

Instrument for x-ray absorption spectroscopy with in situ electrical control characterizations.

We report a synchrotron-based setup capable of performing x-ray absorption spectroscopy and x-ray magnetic circular dichroism with simultaneous electrical control characterizations. The setup can enable research concerning electrical transport, element- and orbital-selective magnetization with an in situ fashion. It is a unique approach to the real-time change of spin-polarized electronic state of a material/device exhibiting magneto-electric responses. The performance of the setup was tested by probing the spin-polarized states of cobalt and oxygen of Zn(1-x)Co(x)O dilute magnetic semiconductor under applied voltages, both at low (~20 K) and room temperatures, and signal variations upon the change of applied voltage were clearly detected.