Skyrmion lattice formation and destruction mechanisms probed with TR-SANS.

Magnetic skyrmions are topologically protected, nanoscale whirls of the spin configuration that tend to form hexagonally ordered arrays. As a topologically non-trivial structure, the nucleation and annihilation of the skyrmion, as well as the interaction between skyrmions, varies from conventional magnetic systems. Recent works have suggested that the ordering kinetics in these materials occur over millisecond or longer timescales, which is unusually slow for magnetic dynamics. The current work investigates the skyrmion ordering kinetics, particularly during lattice formation and destruction, using time-resolved small angle neutron scattering (TR-SANS). Evaluating the time-resolved structure and intensity of the neutron diffraction pattern reveals the evolving real-space structure of the skyrmion lattice and the timeframe of the formation. Measurements were performed on three prototypical skyrmion materials: MnSi, (Fe,Co)Si, and Cu2OSeO3. To probe lattice formation and destruction kinetics, the systems were prepared in the stable skyrmion state, and then a square-wave magnetic field modulation was applied. The measurements show that the skyrmions quickly form ordered domains, with a significant distribution in lattice parameters, which then converge to the final structure; the results confirm the slow kinetics, with formation times between 10 ms and 99 ms. Comparisons are made between the measured formation times and the fundamental material properties, suggesting the ordering temperature, saturation magnetization and magnetocrystalline anisotropy may be driving the timeframes. Micromagnetic simulations were also performed and support a scaling of the kinetics with sample volume, a behavior which is caused by the reconciling of misaligned domains.

Skyrmion-Excited Spin-Wave Fractal Networks.

Magnetic skyrmions exhibit unique, technologically relevant pseudo-particle behaviors which arise from their topological protection, including well-defined, 3D dynamic modes that occur at microwave frequencies. During dynamic excitation, spin waves are ejected into the interstitial regions between skyrmions, creating the magnetic equivalent of a turbulent sea. However, since the spin waves in these systems have a well-defined length scale, and the skyrmions are on an ordered lattice, ordered structures from spin-wave interference can precipitate from the chaos. This work uses small-angle neutron scattering (SANS) to capture the dynamics in hybrid skyrmions and investigate the spin-wave structure. Performing simultaneous ferromagnetic resonance and SANS, the diffraction pattern shows a large increase in low-angle scattering intensity, which is present only in the resonance condition. This scattering pattern is best fit using a mass fractal model, which suggests the spin waves form a long-range fractal network. The fractal structure is constructed of fundamental units with a size that encodes the spin-wave emissions and are constrained by the skyrmion lattice. These results offer critical insights into the nanoscale dynamics of skyrmions, identify a new dynamic spin-wave fractal structure, and demonstrate SANS as a unique tool to probe high-speed dynamics.

Observation of anti-damping spin-orbit torques generated by in-plane and out-of-plane spin polarizations in MnPd3.

Large spin-orbit torques (SOTs) generated by topological materials and heavy metals interfaced with ferromagnets are promising for next-generation magnetic memory and logic devices. SOTs generated from y spin originating from spin Hall and Edelstein effects can realize field-free magnetization switching only when the magnetization and spin are collinear. Here we circumvent the above limitation by utilizing unconventional spins generated in a MnPd3 thin film grown on an oxidized silicon substrate. We observe conventional SOT due to y spin, and out-of-plane and in-plane anti-damping-like torques originated from z spin and x spin, respectively, in MnPd3/CoFeB heterostructures. Notably, we have demonstrated complete field-free switching of perpendicular cobalt via out-of-plane anti-damping-like SOT. Density functional theory calculations show that the observed unconventional torques are due to the low symmetry of the (114)-oriented MnPd3 films. Altogether our results provide a path toward realization of a practical spin channel in ultrafast magnetic memory and logic devices.

Chemically Induced Magnetic Dead Shells in Superparamagnetic Ni Nanoparticles Deduced from Polarized Small-Angle Neutron Scattering.

Advances in the synthesis and characterization of colloidal magnetic nanoparticles (NPs) have yielded great gains in the understanding of their complex magnetic behavior, with implications for numerous applications. Recent work using Ni NPs as a model soft ferromagnetic system, for example, achieved quantitative understanding of the superparamagnetic blocking temperature-particle diameter relationship. This hinged, however, on the critical assumption of a ferromagnetic NP volume lower than the chemical volume due to a non-ferromagnetic dead shell indirectly deduced from magnetometry. Here, we determine both the chemical and magnetic average internal structures of Ni NP ensembles via unpolarized, half-polarized, and fully polarized small-angle neutron scattering (SANS) measurements and analyses coupled with X-ray diffraction and magnetometry. The postulated nanometric magnetic dead shell is not only detected but conclusively identified as a non-ferromagnetic Ni phosphide derived from the trioctylphosphine commonly used in hot-injection colloidal NP syntheses. The phosphide shell thickness is tunable via synthesis temperature, falling to as little as 0.5 nm at 170 °C. Temperature- and magnetic field-dependent polarized SANS measurements additionally reveal essentially bulk-like ferromagnetism in the Ni core and negligible interparticle magnetic interactions, quantitatively supporting prior modeling of superparamagnetism. These findings advance the understanding of synthesis-structure-property relationships in metallic magnetic NPs, point to a simple potential route to ligand-free stabilization, and highlight the power of the currently available suite of polarized SANS measurement and analysis capabilities for magnetic NP science and technology.

Magnetic Particle Self-Assembly at Functionalized Interfaces.

We study the assembly of magnetite nanoparticles in water-based ferrofluids in wetting layers close to silicon substrates with different functionalization without and with an out-of-plane magnetic field. For particles of nominal sizes 5, 15, and 25 nm, we extract density profiles from neutron reflectivity measurements. We show that self-assembly is only promoted by a magnetic field if a seed layer is formed at the silicon substrate. Such a layer can be formed by chemisorption of activated N-hydroxysuccinimide ester-coated nanoparticles at a (3-aminopropyl)triethoxysilane functionalized surface. Less dense packing is reported for physisorption of the same particles at a piranha-treated (strongly hydrophilic) silicon wafer, and no wetting layer is found for a self-assembled monolayer of octadecyltrichlorosilane (strongly hydrophobic) at the interface. We show that once the seed layer is formed and under an out-of-plane magnetic field further wetting layers assemble. These layers become denser with time, larger magnetic fields, higher particle concentrations, and larger moment of the nanoparticles.

Layering of magnetic nanoparticles at amorphous magnetic templates with perpendicular anisotropy.

We reveal the assembly of magnetite nanoparticles of sizes 5 nm, 15 nm and 25 nm from dilute water-based ferrofluids onto an amorphous magnetic template with out-of-plane anisotropy. From neutron reflectometry experiments we extract density profiles and show that the particles self-assemble into layers at the magnetic surface. The layers are extremely stable against cleaning and rinsing of the substrate. The density of the layers is determined by and increases with the remanent magnetic moment of the particles.

Self-Assembly of Magnetic Nanoparticles in Ferrofluids on Different Templates Investigated by Neutron Reflectometry.

In this article we review the process by which magnetite nanoparticles self-assemble onto solid surfaces. The focus is on neutron reflectometry studies providing information on the density and magnetization depth profiles of buried interfaces. Specific attention is given to the near-interface "wetting" layer and to examples of magnetite nanoparticles on a hydrophilic silicon crystal, one coated with (3-Aminopropyl)triethoxysilane, and finally, one with a magnetic film with out-of-plane magnetization.

Effect of chemical substitution on the skyrmion phase in Cu2OSeO3.

Magnetic skyrmions have been the focus of intense research due to their unique qualities which result from their topological protections. Previous work on Cu2OSeO3, the only known insulating multiferroic skyrmion material, has shown that chemical substitution alters the skyrmion phase. We chemically substitute Zn, Ag, and S into powdered Cu2OSeO3 to study the effect on the magnetic phase diagram. In both the Ag and the S substitutions, we find that the skyrmion phase is stabilized over a larger temperature range, as determined via magnetometry and small-angle neutron scattering (SANS). Meanwhile, while previous magnetometry characterization suggests two high temperature skyrmion phases in the Zn-substituted sample, SANS reveals the high temperature phase to be skyrmionic while we are unable to distinguish the other from helical order. Overall, chemical substitution weakens helical and skyrmion order as inferred from neutron scattering of the q≈0.01Å-1 magnetic peak.

Interfacial-Redox-Induced Tuning of Superconductivity in YBa2Cu3O7-δ.

Solid-state ionic approaches for modifying ion distributions in getter/oxide heterostructures offer exciting potentials to control material properties. Here, we report a simple, scalable approach allowing for manipulation of the superconducting transition in optimally doped YBa2Cu3O7-δ (YBCO) films via a chemically driven ionic migration mechanism. Using a thin Gd capping layer of up to 20 nm deposited onto 100 nm thick epitaxial YBCO films, oxygen is found to leach from deep within the YBCO. Progressive reduction of the superconducting transition is observed, with complete suppression possible for a sufficiently thick Gd layer. These effects arise from the combined impact of redox-driven electron doping and modification of the YBCO microstructure due to oxygen migration and depletion. This work demonstrates an effective step toward total ionic tuning of superconductivity in oxides, an interface-induced effect that goes well into the quasi-bulk regime, opening-up possibilities for electric field manipulation.

Nanoparticle architecture preserves magnetic properties during coating to enable robust multi-modal functionality.

Magnetic iron oxide nanoparticles (MIONs) have established a niche as a nanomedicine platform for diagnosis and therapy, but they present a challenging surface for ligand functionalization which limits their applications. On the other hand, coating MIONs with another material such as gold to enhance these attachments introduces other complications. Incomplete coating may expose portions of the iron oxide core, or the coating process may alter their magnetic properties. We describe synthesis and characterization of iron oxide/silica/gold core-shell nanoparticles to elucidate the effects of a silica-gold coating process and its impact on the resulting performance. In particular, small angle neutron scattering reveals silica intercalates between iron oxide crystallites that form the dense core, likely preserving the magnetic properties while enabling formation of a continuous gold shell. The synthesized silica-gold-coated MIONs demonstrate magnetic heating properties consistent with the original iron oxide core, with added x-ray contrast for imaging and laser heating.

Spin canting across core/shell Fe3O4/MnxFe3-xO4 nanoparticles.

Magnetic nanoparticles (MNPs) have become increasingly important in biomedical applications like magnetic imaging and hyperthermia based cancer treatment. Understanding their magnetic spin configurations is important for optimizing these applications. The measured magnetization of MNPs can be significantly lower than bulk counterparts, often due to canted spins. This has previously been presumed to be a surface effect, where reduced exchange allows spins closest to the nanoparticle surface to deviate locally from collinear structures. We demonstrate that intraparticle effects can induce spin canting throughout a MNP via the Dzyaloshinskii-Moriya interaction (DMI). We study ~7.4 nm diameter, core/shell Fe3O4/MnxFe3-xO4 MNPs with a 0.5 nm Mn-ferrite shell. Mössbauer spectroscopy, x-ray absorption spectroscopy and x-ray magnetic circular dichroism are used to determine chemical structure of core and shell. Polarized small angle neutron scattering shows parallel and perpendicular magnetic correlations, suggesting multiparticle coherent spin canting in an applied field. Atomistic simulations reveal the underlying mechanism of the observed spin canting. These show that strong DMI can lead to magnetic frustration within the shell and cause canting of the net particle moment. These results illuminate how core/shell nanoparticle systems can be engineered for spin canting across the whole of the particle, rather than solely at the surface.

Self-Assembled Layering of Magnetic Nanoparticles in a Ferrofluid on Silicon Surfaces.

This article describes the three-dimensional self-assembly of monodisperse colloidal magnetite nanoparticles (NPs) from a dilute water-based ferrofluid onto a silicon surface and the dependence of the resultant magnetic structure on the applied field. The NPs assemble into close-packed layers on the surface followed by more loosely packed ones. The magnetic field-dependent magnetization of the individual NP layers depends on both the rotational freedom of the layer and the magnetization of the adjacent layers. For layers in which the NPs are more free to rotate, the easy axis of the NP can readily orient along the field direction. In more dense packing, free rotation of the NPs is hampered, and the NP ensembles likely build up quasi-domain states to minimize energy, which leads to lower magnetization in those layers. Detailed analysis of polarized neutron reflectometry data together with model calculations of the arrangement of the NPs within the layers and input from small-angle scattering measurements provide full characterization of the core/shell NP dimensions, degree of chaining, arrangement of the NPs within the different layers, and magnetization depth profile.

Complex Three-Dimensional Magnetic Ordering in Segmented Nanowire Arrays.

A comprehensive three-dimensional picture of magnetic ordering in high-density arrays of segmented FeGa/Cu nanowires is experimentally realized through the application of polarized small-angle neutron scattering. The competing energetics of dipolar interactions, shape anisotropy, and Zeeman energy in concert stabilize a highly tunable spin structure that depends heavily on the applied field and sample geometry. Consequently, we observe ferromagnetic and antiferromagnetic interactions both among wires and between segments within individual wires. The resulting magnetic structure for our nanowire sample in a low field is a fan with magnetization perpendicular to the wire axis that aligns nearly antiparallel from one segment to the next along the wire axis. Additionally, while the low-field interwire coupling is ferromagnetic, application of a field tips the moments toward the nanowire axis, resulting in highly frustrated antiferromagnetic stripe patterns in the hexagonal nanowire lattice. Theoretical calculations confirm these observations, providing insight into the competing interactions and resulting stability windows for a variety of ordered magnetic structures. These results provide a roadmap for designing high-density magnetic nanowire arrays for spintronic device applications.

Tailoring exchange couplings in magnetic topological-insulator/antiferromagnet heterostructures.

Magnetic topological insulators such as Cr-doped (Bi,Sb)2Te3 provide a platform for the realization of versatile time-reversal symmetry-breaking physics. By constructing heterostructures exhibiting Néel order in an antiferromagnetic CrSb and ferromagnetic order in Cr-doped (Bi,Sb)2Te3, we realize emergent interfacial magnetic phenomena which can be tailored through artificial structural engineering. Through deliberate geometrical design of heterostructures and superlattices, we demonstrate the use of antiferromagnetic exchange coupling in manipulating the magnetic properties of magnetic topological insulators. Proximity effects are shown to induce an interfacial spin texture modulation and establish an effective long-range exchange coupling mediated by antiferromagnetism, which significantly enhances the magnetic ordering temperature in the superlattice. This work provides a new framework on integrating topological insulators with antiferromagnetic materials and unveils new avenues towards dissipationless topological antiferromagnetic spintronics.

Atomically engineered ferroic layers yield a room-temperature magnetoelectric multiferroic.

Materials that exhibit simultaneous order in their electric and magnetic ground states hold promise for use in next-generation memory devices in which electric fields control magnetism. Such materials are exceedingly rare, however, owing to competing requirements for displacive ferroelectricity and magnetism. Despite the recent identification of several new multiferroic materials and magnetoelectric coupling mechanisms, known single-phase multiferroics remain limited by antiferromagnetic or weak ferromagnetic alignments, by a lack of coupling between the order parameters, or by having properties that emerge only well below room temperature, precluding device applications. Here we present a methodology for constructing single-phase multiferroic materials in which ferroelectricity and strong magnetic ordering are coupled near room temperature. Starting with hexagonal LuFeO3-the geometric ferroelectric with the greatest known planar rumpling-we introduce individual monolayers of FeO during growth to construct formula-unit-thick syntactic layers of ferrimagnetic LuFe2O4 (refs 17, 18) within the LuFeO3 matrix, that is, (LuFeO3)m/(LuFe2O4)1 superlattices. The severe rumpling imposed by the neighbouring LuFeO3 drives the ferrimagnetic LuFe2O4 into a simultaneously ferroelectric state, while also reducing the LuFe2O4 spin frustration. This increases the magnetic transition temperature substantially-from 240 kelvin for LuFe2O4 (ref. 18) to 281 kelvin for (LuFeO3)9/(LuFe2O4)1. Moreover, the ferroelectric order couples to the ferrimagnetism, enabling direct electric-field control of magnetism at 200 kelvin. Our results demonstrate a design methodology for creating higher-temperature magnetoelectric multiferroics by exploiting a combination of geometric frustration, lattice distortions and epitaxial engineering.

Structural and magnetic depth profiles of magneto-ionic heterostructures beyond the interface limit.

Electric field control of magnetism provides a promising route towards ultralow power information storage and sensor technologies. The effects of magneto-ionic motion have been prominently featured in the modification of interface characteristics. Here, we demonstrate magnetoelectric coupling moderated by voltage-driven oxygen migration beyond the interface in relatively thick AlOx/GdOx/Co(15 nm) films. Oxygen migration and Co magnetization are quantitatively mapped with polarized neutron reflectometry under electro-thermal conditioning. The depth-resolved profiles uniquely identify interfacial and bulk behaviours and a semi-reversible control of the magnetization. Magnetometry measurements suggest changes in the microstructure which disrupt long-range ferromagnetic ordering, resulting in an additional magnetically soft phase. X-ray spectroscopy confirms changes in the Co oxidation state, but not in the Gd, suggesting that the GdOx transmits oxygen but does not source or sink it. These results together provide crucial insight into controlling magnetism via magneto-ionic motion, both at interfaces and throughout the bulk of the films.

Controllable positive exchange bias via redox-driven oxygen migration.

Ionic transport in metal/oxide heterostructures offers a highly effective means to tailor material properties via modification of the interfacial characteristics. However, direct observation of ionic motion under buried interfaces and demonstration of its correlation with physical properties has been challenging. Using the strong oxygen affinity of gadolinium, we design a model system of GdxFe1-x/NiCoO bilayer films, where the oxygen migration is observed and manifested in a controlled positive exchange bias over a relatively small cooling field range. The exchange bias characteristics are shown to be the result of an interfacial layer of elemental nickel and cobalt, a few nanometres in thickness, whose moments are larger than expected from uncompensated NiCoO moments. This interface layer is attributed to a redox-driven oxygen migration from NiCoO to the gadolinium, during growth or soon after. These results demonstrate an effective path to tailoring the interfacial characteristics and interlayer exchange coupling in metal/oxide heterostructures.

Realization of ground-state artificial skyrmion lattices at room temperature.

The topological nature of magnetic skyrmions leads to extraordinary properties that provide new insights into fundamental problems of magnetism and exciting potentials for novel magnetic technologies. Prerequisite are systems exhibiting skyrmion lattices at ambient conditions, which have been elusive so far. Here, we demonstrate the realization of artificial Bloch skyrmion lattices over extended areas in their ground state at room temperature by patterning asymmetric magnetic nanodots with controlled circularity on an underlayer with perpendicular magnetic anisotropy (PMA). Polarity is controlled by a tailored magnetic field sequence and demonstrated in magnetometry measurements. The vortex structure is imprinted from the dots into the interfacial region of the underlayer via suppression of the PMA by a critical ion-irradiation step. The imprinted skyrmion lattices are identified directly with polarized neutron reflectometry and confirmed by magnetoresistance measurements. Our results demonstrate an exciting platform to explore room-temperature ground-state skyrmion lattices.

Magnetic structure and ordering of multiferroic hexagonal LuFeO_{3}.

We report on the magnetic structure and ordering of hexagonal LuFeO_{3} films of variable thickness grown by molecular-beam epitaxy on YSZ (111) and Al_{2}O_{3} (0001) substrates. These crystalline films exhibit long-range structural uniformity dominated by the polar P6_{3}cm phase, which is responsible for the paraelectric to ferroelectric transition that occurs above 1000 K. Using bulk magnetometry and neutron diffraction, we find that the system orders into a ferromagnetically canted antiferromagnetic state via a single transition below 155 K regardless of film thickness, which is substantially lower than that previously reported in hexagonal LuFeO_{3} films. The symmetry of the magnetic structure in the ferroelectric state implies that this material is a strong candidate for linear magnetoelectric coupling and control of the ferromagnetic moment directly by an electric field.

Self assembly of magnetic nanoparticles at silicon surfaces.

Neutron reflectometry was used to study the assembly of magnetite nanoparticles in a water-based ferrofluid close to a silicon surface. Under three conditions, static, under shear and with a magnetic field, the depth profile is extracted. The particles have an average diameter of 11 nm and a volume density of 5% in a D2O-H2O mixture. They are surrounded by a 4 nm thick bilayer of carboxylic acid for steric repulsion. The reflectivity data were fitted to a model using a least square routine based on the Parratt formalism. From the scattering length density depth profiles the following behavior is concluded: the fits indicate that excess carboxylic acid covers the silicon surface and almost eliminates the water in the densely packed wetting layer that forms close to the silicon surface. Under constant shear the wetting layer persists but a depletion layer forms between the wetting layer and the moving ferrofluid. Once the flow is stopped, the wetting layer becomes more pronounced with dense packing and is accompanied by a looser packed second layer. In the case of an applied magnetic field the prolate particles experience a torque and align with their long axes along the silicon surface which leads to a higher particle density.