Polarized Neutron Reflectometry Research Articles

Syntropic spin alignment at the interface between ferromagnetic and superconducting nitrides

Abstract The magnetic correlations at the superconductor/ferromagnet (S/F) interfaces play a crucial role in realizing dissipation-less spin-based logic and memory technologies, such as triplet-supercurrent spin-valves and “π” Josephson junctions. Here we report the observation of an induced large magnetic moment at high-quality nitride S/F interfaces. Using polarized neutron reflectometry and d.c. SQUID measurements, we quantitatively determined the magnetization profile of S/F bilayer and confirmed the induced magnetic moment in the adjacent superconductor only exists below TC. Interestingly, the direction of the induced moment in the superconductors was unexpectedly parallel to that in the ferromagnet, which contrasts with earlier findings in S/F heterostructures based on metals or oxides. First-principles calculations verified that the unusual interfacial spin texture observed in our study was caused by the Heisenberg direct exchange coupling with constant J∼4.28 meV through d-orbital overlapping and severe charge transfer across the interfaces. Our work establishes an incisive experimental probe for understanding the magnetic proximity behavior at S/F interfaces and provides a prototype epitaxial “building block” for superconducting spintronics.

Interface Effect on the Out‐of‐Plane Spin‐Orbit Torque in the Ferromagnetic CoPt Single Layers

AbstractField‐free switching of a perpendicularly magnetized heavy metal/ferromagnetic metal bilayer or single alloy layer through spin‐orbit torque (SOT) provides a potential way for next‐generation spintronic devices with fast speed and high efficiency. Here, a sizable symmetry dependence of field‐free magnetization switching via an out‐of‐plane torque in CoxPt100−x single layers is reported. It is found that the sign of in‐plane SOT in CoxPt100−x when x ≤ 25 is positive. However, it changes to negative when x > 25, while the out‐of‐plane SOT changes its sign when x > 30. The polarized neutron reflectometry measurement further suggests an interface layer with rich Pt content near the substrate, which could have a strong interface effect on the out‐of‐plane SOT. The sign of the out‐of‐plane SOT, and then the polarity of the field‐free magnetization switching, is determined by the competition between the out‐of‐plane torques arising from the bulk and interface parts in the CoxPt100−x single layers. It is expected that such interface effect of the out‐of‐plane torque is desirable to the applications in spin logic devices using symmetry dependence of field‐free magnetization switching in the ferromagnetic CoPt single layers.

Mesoscale self-organization of polydisperse magnetic nanoparticles at the water surface.

In this study, we investigated the self-ordering process in Langmuir films of polydisperse iron oxide nanoparticles on a water surface, employing in situ x-ray scattering, surface pressure-area isotherm analysis, and Brewster angle microscopy. X-ray reflectometry confirmed the formation of a monolayer, while grazing incidence small-angle x-ray scattering revealed short-range lateral correlations with a characteristic length equal to the mean particle size. Remarkably, our findings indicated that at zero surface pressure, the particles organized into submicrometer clusters, merging upon compression to form a homogeneous layer. These layers were subsequently transferred to a solid substrate using the Langmuir-Schaefer technique and further characterized via scanning electron microscopy and polarized neutron reflectometry. Notably, our measurements revealed a second characteristic length in the lateral correlations, orders of magnitude longer than the mean particle diameter, with polydisperse particles forming circular clusters densely packed in a hexagonal lattice. Furthermore, our evidence suggests that the lattice constant of this mesocrystal depends on the characteristics of the particle size distribution, specifically the mean particle size and the width of the size distribution. In addition, we observed internal size separation within these clusters, where larger particles were positioned closer to the center of the cluster. Finally, polarized neutron reflectometry measurements provided valuable insights into the magnetization profile across the layer.

Nanoscale Magnetic Arrays through Block Copolymer Templating of Polyoxometalates.

Magnetic nanoarrays promise to enable new energy-efficient computations based on spintronics or magnonics. In this work, we present a block copolymer-assisted strategy for fabricating ordered magnetic nanostructures on silicon and permalloy substrates. Block copolymer micelle-like structures were used as a template in which polyoxometalate (POM) clusters could assemble in an opal-like structure. A combination of microscopy and scattering techniques was used to confirm the structural and organizational features of the fabricated materials. The magnetic properties of these materials were investigated by polarized neutron reflectometry, nuclear magnetic resonance, and magnetometry measurements. The data show that a magnetic structural design was achieved and that a thin layer of patterned POMs strongly influenced an underlying permalloy layer. This work demonstrates that the bottom-up pathway is a potentially viable method for patterning magnetic substrates on a sub-100 nm scale, toward the magnetic nanostructures needed for spintronic or magnonic crystal devices.

La0.6Sr0.4CoO3−δ Films Under Deoxygenation: Magnetic And Electronic Transitions Are Apart from The Structural Phase Transition

AbstractTopotactic phase transitions induced by changes in the oxygen vacancy concentration can largely alter the physical properties of complex oxides, including electronic and magnetic phases, while maintaining the structural integrity of the crystal lattice. An oxygen‐vacancy‐induced topotactic phase transition from perovskite (PV) to brownmillerite (BM) is achieved in epitaxial La0.6Sr0.4CoO3−δ (LSCO) thin films. Two novel intermediate states with different oxygen content are identified by X‐ray diffraction, which involves a single‐phase reduced PV state and a mixed state of co‐existing PV and BM. The combination of depth‐sensitive polarized neutron reflectometry (PNR) and Rutherford backscattering (RBS) allows a quantitative determination of magnetization and the mean oxygen content in all states, revealing a continuous transition from La0.6Sr0.4CoO2.97 to La0.6Sr0.4CoO2.5. BM formation is observed for an LSCO layer with an oxygen content of 2.67, while the magnetic and electronic transition already occurs for a layer with a higher oxygen content of 2.77 (and above) and in the absence of a BM signature. These results demonstrate that the physics of electronic metal‐to‐insulator transition (MIT), magnetic ferromagnet‐to‐non‐ferromagnet transition (FM‐to‐non‐FM), and structural PV‐to‐BM phase transition should be considered within the framework of separate but interrelated processes.

(Invited) Direct Bonding and Its Interface for High-Density Integration of Superconducting Qubits

Superconducting qubits are one of the intensive approaches to fabricate quantum computing (QC). Qubits can be manufactured by the current Si-based semiconductor manufacturing processes. However, circuits should be superconducting material such as Nb (Tc=9.29 K), Al (Tc=1.18 K), Pb (Tc=7.2 K), In (Tc=3.4 K) , etc. In current technology, qubits are arranged in planar geometry in a chip, and each qubit should wire to control and read signal lines in the same plane. When a large number of qubits are integrated, these wires would be too constrained, and several problems would be actualized, such as wiring for qubits located at the chip center, crosstalk among wiring, and so on. The signal integrity for the QC devices is much better to have qubits at short distances from the control circuitry. Therefore, 3D wiring is required for a large-scale qubit integration. 3D integration of qubits with interposer chips by flip-chip bonding is the proof-of-concept of the large-scale qubit integration. The 3D integration approaches for qubit- based devices are the same as conventional electronic devices, including the through silicon via (TSV) process for interposers and micro bump flip-chip bonding. However, they use superconducting metals instead of copper and other non-superconducting materials. Most flip-chip microbump bonding processes require thermal compression at over 170 °C. Superconducting elements are easily degraded by heat. Consequently, we apply surface activated bonding (SAB) to a superconducting metal as a low-temperature bonding process for superconducting circuits.The test element group (TEG) for the current-voltage (I-V) measurement of the bonded interface was bonded by SAB method, and at the Nb SAB interface layer is a 2- to 3-nm-thick amorphous layer and the layer consist of Si-rich interfacial layer compared to the Nb bulk area. The bonding specimens were activated on jigs made of Si during the bonding process; then the Si sputtered by FAB was redeposited on the bonding surfaces. Furthermore, the bonded specimen was wired using Al wire to a chip carrier with a stage installed into a 0.3-K cryostat. As a result, the Tc of this path is 9.3 K, which is very similar to that of Nb bulk (9.2 K). However, a small step of the Tc at 9.1-9.4 K was also observed. (Fig.1) [1]In this study, we discuss the superconducting interface of direct bonded Nb-Nb by Tc, and also the interfacial structure measured by polarized neutron reflectometry (PNR). The results show clear spin asymmetry in the superconducting state, as splitting is observed in the fringes of the parallel neutron (neutron spins parallel to the external magnetic field 0.1 T) reflection R+ and the antiparallel (neutron spins antiparallel to it) reflection R−, where the latter has become larger. This well-known effect is related to the flux penetration in the superconducting state. Therefore, unique information about the superconducting state of the buried thin film can be measured by using the polarized neutron beam. For this project the major advantage of PNR will be to characterize the superconducting state at the deeply buried Nb interfaces, sandwiched between the two substrate wafers, which would be infeasible using alternate techniques.[1] M. Fujino, et. al., J. Appl. Phys., 133, 015301, 2023 Figure 1

Non-uniform Gd distribution and magnetization profiles within GdCoFe alloy thin films

Rare earth (RE):transition metal (TM) ferrimagnetic alloys continue to attract significant attention for spintronics. This work focuses on the elemental distribution of RE and TM elements throughout the thickness of nominally uniform films and the resulting spatial variations of the magnetization within these layers. Samples of CoFe alloyed with Gd were studied using secondary ion mass spectroscopy, polarized neutron reflectometry, and x-ray resonant magnetic reflectivity. The samples were grown by magnetron co-sputtering to control the RE:TM alloy ratio of the ferrimagnetic layer, which was combined with W and Pt layers as either under or over-layers to create sample structures such as W/Gdx(Co70Fe30)100−x/Pt, where x = 0, 8, and 23 at. %. Results show that uniformly deposited thin-films have a significant variation in the distribution of the TM and RE through the film thickness, and this leads to a spatial distribution in the net magnetization profile and a non-uniform Gd magnetization profile within the layer. These findings have implications for the application RE:TM alloys in spintronics as they may impact the perpendicular magnetic anisotropy, the ferrimagnetic compensation temperature, and interfacial spin transport.

Boron transport enhancement with different capping layers by specific annealing temperatures studied by X-ray and polarized neutron reflectometry

Boron transport enhancement with different capping layers by specific annealing temperatures studied by X-ray and polarized neutron reflectometry

Proximity‐Induced Fully Ferromagnetic Order with Eightfold Magnetic Anisotropy in Heavy Transition Metal Oxide CaRuO3

AbstractFerromagnetic 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 CaRuO3 in (001)‐(LaMnO3/CaRuO3) 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 La0.67Sr0.33MnO3. 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 CaRuO3 layers are in a fully ferromagnetic state (∼0.8 μB/Ru), in sharp contrast to the proximity‐induced canted antiferromagnetic state in 5d oxides SrIrO3 and CaIrO3 (∼0.1 μB/Ir). More than that, the magnetic anisotropy of the (001)‐(LaMnO3/CaRuO3) superlattices is eightfold symmetric, showing potential applications in the technology of multistate data storage.

The Prospects of Use of Polarized Neutron Reflectometry to Study Helimagnetism in Rare-Earth Thin Films and Nanostructures on a Compact Neutron Source DARIA

The Prospects of Use of Polarized Neutron Reflectometry to Study Helimagnetism in Rare-Earth Thin Films and Nanostructures on a Compact Neutron Source DARIA

Exchange-Biased Quantum Anomalous Hall Effect.

The quantum anomalous Hall (QAH) effect is characterized by a dissipationless chiral edge state with a quantized Hall resistance at zero magnetic field. Manipulating the QAH state is of great importance in both the understanding of topological quantum physics and the implementation of dissipationless electronics. Here, the QAH effect is realized in the magnetic topological insulator Cr-doped (Bi,Sb)2 Te3 (CBST) grown on an uncompensated antiferromagnetic insulator Al-doped Cr2 O3 . Through polarized neutron reflectometry (PNR), a strong exchange coupling is found between CBST and Al-Cr2 O3 surface spins fixing interfacial magnetic moments perpendicular to the film plane. The interfacial coupling results in an exchange-biased QAH effect. This study further demonstrates that the magnitude and sign of the exchange bias can be effectively controlled using a field training process to set the magnetization of the Al-Cr2 O3 layer. It demonstrates the use of the exchange bias effect to effectively manipulate the QAH state, opening new possibilities in QAH-based spintronics.

Tunable coupling in magnetic thin film heterostructures with a magnetic phase transition

The magnetic properties of permalloy-based trilayers of the form Py0.8Cu0.2/Py0.4Cu0.6/Py/IrMn were studied as the spacer layer undergoes a paramagnetic to ferromagnetic phase transition. We find the coupling between the free Py0.8Cu0.2 layer and the exchange bias pinned Py to be strongly temperature-dependent: there is negligible coupling above the Curie temperature of the Py0.4Cu0.6 spacer layer, strong ferromagnetic coupling below that temperature, and a tunable coupling between these extremes. Polarized neutron reflectometry was used to measure the depth profile of the magnetic order in the system, allowing us to correlate the order parameter with the coupling strength. The thickness dependence shows that these are interface effects with an inverse relationship to thickness, and that there is a magnetic proximity effect that enhances the Curie temperature of the spacer layer with characteristic length scale of about 7 nm. As a demonstration of potential functionality of such a system, the structure is shown to spontaneously flip from the antiparallel to parallel magnetic configuration once the spacer layer has developed long-range magnetic order.

Electrical, optical, and magnetic properties of amorphous yttrium iron oxide thin films and consequences for non-local resistance measurements

We present magnetic characterization, charge resistivity, and optical photoluminescence measurements on amorphous yttrium iron oxide thin films (a-Y–Fe–O), with supporting comparisons to amorphous germanium (a-Ge) films. We measured magnetic properties with both SQUID magnetometry and polarized neutron reflectometry. These results not only confirm that a-Y–Fe–O is a disordered magnetic material with strong predominantly antiferromagnetic exchange interactions and a high degree of frustration, but also that it is best understood electrically as a disordered semiconductor. As with amorphous germanium, a-Y–Fe–O obeys expectations for variable-range hopping through localized electron states over a wide range of temperature. We also clarify the consequences of charge transport through such a semiconducting medium for non-local voltage measurements intended to probe spin transport in nominally insulating magnetic materials. We further compare non-local resistance measurements made with “quasi-dc” automated current reversal to ac measurements made with a lock-in amplifier. These show that the “quasi-dc” measurement has an effective ac current excitation with frequency up to approximately 22 Hz, and that this effective ac excitation can cause artifacts in these measurements including incorrect sign of the non-local resistance. This comprehensive investigation of non-local resistance measurements in a-Y–Fe–O shows no evidence of spin transport on micrometer length scales, which is contrary to our original work, and in line with more recent investigations by other groups.

Strain-tunable Berry curvature in quasi-two-dimensional chromium telluride

Magnetic transition metal chalcogenides form an emerging platform for exploring spin-orbit driven Berry phase phenomena owing to the nontrivial interplay between topology and magnetism. Here we show that the anomalous Hall effect in pristine Cr2Te3 thin films manifests a unique temperature-dependent sign reversal at nonzero magnetization, resulting from the momentum-space Berry curvature as established by first-principles simulations. The sign change is strain tunable, enabled by the sharp and well-defined substrate/film interface in the quasi-two-dimensional Cr2Te3 epitaxial films, revealed by scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. This Berry phase effect further introduces hump-shaped Hall peaks in pristine Cr2Te3 near the coercive field during the magnetization switching process, owing to the presence of strain-modulated magnetic layers/domains. The versatile interface tunability of Berry curvature in Cr2Te3 thin films offers new opportunities for topological electronics.

Three-dimensional structure of hybrid magnetic skyrmions determined by neutron scattering

Magnetic skyrmions are topologically protected chiral spin textures which present opportunities for next-generation magnetic data storage and logic information technologies. The topology of these structures originates in the geometric configuration of the magnetic spins - more generally described as the structure. While the skyrmion structure is most often depicted using a 2D projection of the three-dimensional structure, recent works have emphasized the role of all three dimensions in determining the topology and their response to external stimuli. In this work, grazing-incidence small-angle neutron scattering and polarized neutron reflectometry are used to determine the three-dimensional structure of hybrid skyrmions. The structure of the hybrid skyrmions, which includes a combination of N\'eel-like and Bloch-like components along their length, is expected to significantly contribute to their notable stability, which includes ambient conditions. To interpret the neutron scattering data, micromagnetic simulations of the hybrid skyrmions were performed, and the corresponding diffraction patterns were determined using a Born approximation transformation. The converged magnetic profile reveals the magnetic structure along with the skyrmion depth profile, including the thickness of the Bloch and N\'eel segments and the diameter of the core.

Nitrogen-Based Magneto-ionic Manipulation of Exchange Bias in CoFe/MnN Heterostructures.

Electric field control of the exchange bias effect across ferromagnet/antiferromagnet (FM/AF) interfaces has offered exciting potentials for low-energy-dissipation spintronics. In particular, the solid-state magneto-ionic means is highly appealing as it may allow reconfigurable electronics by transforming the all-important FM/AF interfaces through ionic migration. In this work, we demonstrate an approach that combines the chemically induced magneto-ionic effect with the electric field driving of nitrogen in the Ta/Co0.7Fe0.3/MnN/Ta structure to electrically manipulate exchange bias. Upon field-cooling the heterostructure, ionic diffusion of nitrogen from MnN into the Ta layers occurs. A significant exchange bias of 618 Oe at 300 K and 1484 Oe at 10 K is observed, which can be further enhanced after a voltage conditioning by 5 and 19%, respectively. This enhancement can be reversed by voltage conditioning with an opposite polarity. Nitrogen migration within the MnN layer and into the Ta capping layer cause the enhancement in exchange bias, which is observed in polarized neutron reflectometry studies. These results demonstrate an effective nitrogen-ion based magneto-ionic manipulation of exchange bias in solid-state devices.

Absence of magnetic interactions in Ni–Nb ferromagnet–superconductor bilayers

Studies of ferromagnet-superconductor hybrid systems have uncovered magnetic interactions between the competing electronic orderings. The electromagnetic (EM) proximity effect predicts the formation of a spontaneous vector potential inside a superconductor placed in proximity to a ferromagnet. In this work, we use a Nb superconducting layer and Ni ferromagnetic layer to test for such magnetic interactions. We use the complementary, but independent, techniques of polarized neutron reflectometry and detection Josephson junctions to probe the magnetic response inside the superconducting layer at close to zero applied field. In this condition, Meissner screening is negligible, so our measurements examine only additional magnetic and screening contributions from proximity effects. We report the absence of any signals originating from EM proximity effect in zero applied field. Our observations indicate that either EM proximity effect is below the detection resolution of both of our experiments or may indicate a new phenomenon that requires extension of current theory. From our measurements, we estimate a limit of the size of the zero field EM proximity effect in our Ni–Nb samples to be ±0.27 mT.

Unraveling the sign reversal of the anomalous Hall effect in ferromagnet/heavy-metal ultrathin films

The sign reversal in the anomalous Hall effect (AHE) that occurs for material offers great prospects for AHE-based spintronic devices design. However, the mechanisms are still controversial in ultrathin ferromagnetic/heavy metal thin film systems due to the complicatedly interfacial effects. Here, we investigate the AHE sign reversal in ultrathin ferromagnetic ${\mathrm{Mn}}_{2}\mathrm{CoAl}/\mathrm{Pd}$ films, a system which has shown unusual AHE, significant spin-orbit coupling, and magnetic texturing. Element-sensitive cross-sectional STEM imaging and the depth-resolved magnetization profile from polarized neutron reflectometry identifies the presence of a second ferromagnetic layer from intermixed Co-Pd. To quantitatively explain the sign reversal of the AHE, we build a model based on two contributions, ferromagnetic ${\mathrm{Mn}}_{2}\mathrm{CoAl}$ and the intermixed CoPd layer. We also clarify that contributions to the AHE from magnetic proximity and spin Hall effect are negligible. Our work demonstrates that interfacial alloying can be a critical factor and provides insightful methods to determine the origins of the AHE in ferromagnet/heavy-metal thin film systems.

Significantly Enhanced Room-Temperature Ferromagnetism in Multiferroic EuFeO3-δ Thin Films.

Regulating the magnetic properties of multiferroics lays the foundation for their prospective application in spintronic devices. Single-phase multiferroics, such as rare-earth ferrites, are promising candidates; however, they typically exhibit weak magnetism at room temperature (RT). Here, we significantly boosted the RT ferromagnetism of a representative ferrite, EuFeO3, by oxygen defect engineering. Polarized neutron reflectometry and magnetometry measurements reveal that saturation magnetization reaches 0.04 μB/Fe, which is approximately 5 times higher than its bulk phase. Combining the annular bright-field images with theoretical assessment, we unravel the underlying mechanism for magnetic enhancement, in which the decrease in Fe-O-Fe bond angles caused by oxygen vacancies (VO) strengthens magnetic interactions and tilts Fe spins. Furthermore, the internal relationship between magnetism and VO was established by illustrating how the magnetic structure and magnitude change with VO configuration and concentration. Our strategy for regulating magnetic properties can be applied to numerous functional oxide materials.

Topical Review of Quantum Materials and Heterostructures Studied by Polarized Neutron Reflectometry

A review of the applications of polarized neutron reflectometry (PNR) for the investigation of quantum materials is provided. Recent studies of superconductors, strongly correlated oxides, hydrogen‐induced modifications, topological insulators and chiral magnets are highlighted. The PNR technique uses a quantum beam of spin‐polarized neutrons to measure the nanomagnetic structure of thin films and heterostructures, with a sensitivity to magnetization at the scale of 10–2000 emu cm−3 and a vertical spatial resolution of 1–500 nm. From simple beginnings studying the magnetic flux penetration at superconducting surfaces, today the PNR technique is widely used for investigating many different types of thin film structures, surfaces, interfaces, and 2D materials. PNR measurements can reveal a number of details about magnetic, electronic, and superconducting properties, in tandem with chemical information including the stoichiometry of light elements such as oxygen and hydrogen.