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Creating and protecting magnetic nanomaterials

Coated nanofibers and methods for forming the same. A magnetic nanofiber is formed and a barrier coating is deposited on the magnetic nanofiber by atomic layer deposition (“ALD”) process. The coated nanofiber may include a reduced magnetic nanostructure and a barrier coating comprising a first oxide coating on the nanofiber, the coating being non-reactive with the magnetic polymer nanofiber, the barrier coating have a thickness of 2 nm to 12 nm.

Mane, Anil U.↗

Spin Textures at Conformal Surfaces and Interfaces: CRADA Final Report

The scientific and technological exploration of artificially designed three-dimensional magnetic nanostructures opens the path to exciting novel physical phenomena, originating from the increased complexity in spin textures, topology, and frustration in three dimensions. Theory predicts that the equilibrium magnetic ground state of two-dimensional systems which reflects the competition between symmetric (Heisenberg) and antisymmetric (Dzyaloshinskii-Moriya interaction (DMI)) exchange interaction is significantly modified on curved surfaces when the radius of local curvature becomes comparable to fundamental magnetic length scales. In this CRADA we performed collaboratively an experimental study of the spin texture in an 8 nm thin magnetic multilayer with growth-induced in-plane anisotropy and DMI deposited onto the curved surface of a 1.8µm long non-magnetic carbon nanowire with a 67 nm radius. The sample was fabricated in Juelich and with collaborators at BESSY in Berlin. Using magnetic soft x-ray tomography at the ALBA synchrotron in Spain, the three-dimensional spin configuration in this nanotube was retrieved with about 30nm spatial resolution. The transition between two vortex configurations on the two ends of the nanotube with opposite circulation occurs through a domain wall that is aligned at an inclined angle relative to the wire axis. Three-dimensional micromagnetic simulations support the experimental observations and represent a visualization of the curvature-mediated DMI. They also allow a quantitative estimate of the DMI value for the magnetic multilayered nanotube.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Curvature-mediated spin textures in magnetic multi-layered nanotubes

The scientific and technological exploration of artificially designed three-dimensional magnetic nanostructures opens the path to exciting novel physical phenomena, originating from the increased complexity in spin textures, topology, and frustration in three dimensions. Theory predicts that the equilibrium magnetic ground state of two-dimensional systems which reflects the competition between symmetric (Heisenberg) and antisymmetric (Dzyaloshinskii-Moriya interaction (DMI)) exchange interaction is significantly modified on curved surfaces when the radius of local curvature becomes comparable to fundamental magnetic length scales. Here, we present an experimental study of the spin texture in an 8 nm thin magnetic multilayer with growth-induced in-plane anisotropy and DMI deposited onto the curved surface of a 1.8 {\mu}m long non-magnetic carbon nanowire with a 67 nm radius. Using magnetic soft x-ray tomography the three-dimensional spin configuration in this nanotube was retrieved with about 30nm spatial resolution. The transition between two vortex configurations on the two ends of the nanotube with opposite circulation occurs through a domain wall that is aligned at an inclined angle relative to the wire axis. Three-dimensional micromagnetic simulations support the experimental observations and represent a visualization of the curvature-mediated DMI. They also allow a quantitative estimate of the DMI value for the magnetic multilayered nanotube.

Josten, Elisabeth↗

Ultrathin, High-Aspect Ratio, and Free-Standing Magnetic Nanowires by Exfoliation of Ferromagnetic Quasi-One-Dimensional van der Waals Lattices

Driven by numerous discoveries of novel physical properties and integration into functional devices, interest in one-dimensional (1D) magnetic nanostructures has grown tremendously. Traditionally, such structures are accessed with bottom-up techniques, but these require increasing sophistication to allow precise control over crystallinity, branching, aspect ratio, and surface termination, especially when approaching the subnanometer regime in magnetic phases. In this work, we show that mechanical exfoliation of bulk quasi-one-dimensional crystals, a method similar to those popularized for two-dimensional van der Waals (vdW) lattices, serves as an efficient top-down method to produce ultrathin freestanding nanowires that are both magnetic and semiconducting. We use CrSbSe 3 as a representative quasi-1D vdW crystal with strong magnetocrystalline anisotropy and show that it can be exfoliated into nanowires with an average cross-section of 10 ± 2.8 nm. The CrSbSe 3 nanowires display reduced Curie–Weiss temperature but higher coercivity and remanence than the bulk phase. The methodology developed here for CrSbSe 3 , a representative for a vast class of 1D vdW lattices, serves as a blueprint for investigating confinement effects for 1D materials and accessing functional nanowires that are difficult to produce via traditional bottom-up methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chemical Design of Spin Frustration to Realize Topological Spin Glasses

Patterning spins to generate collective behavior is at the core of condensed matter physics. Physicists develop techniques, including the fabrication of magnetic nanostructures and precision layering of materials specifically to engender frustrated lattices. As chemists, we can access such exotic materials through targeted chemical synthesis and create new lattice types by chemical design. Here, in this study, we introduce a new approach to induce magnetic frustration on a modified honeycomb lattice through a competition of alternating antiferromagnetic (AFM) and ferromagnetic (FM) nearest-neighbor interactions. By subtly modulating these two types of interactions through facile synthetic modifications, we created two systems: (1) a topological spin glass and (2) a frustrated spin-canted magnet with low-temperature exchange bias. To design this unconventional magnetic lattice, we used a metal–organic framework (MOF) platform, Ni 3 (pymca) 3 X 3 (NipymcaX where pymca = pyrimidine-2-carboxylato and X = Cl, Br). We isolated two MOFs, NipymcaCl and NipymcaBr, featuring canted Ni 2+ -based moments. Despite this similarity, differences in the single-ion anisotropies of the Ni 2+ spins result in distinct magnetic properties for each material. NipymcaCl is a topological spin glass, while NipymcaBr is a rare frustrated magnet with low-temperature exchange bias. Density functional theory calculations and Monte Carlo simulations on the NipymcaX lattice support the presence of magnetic frustration as a result of alternating AFM and FM interactions. Our calculations enabled us to determine the ground-state spin configuration and the distribution of spin–spin correlations relative to paradigmatic kagomé and triangular lattices. This modified honeycomb lattice is similar to the electronic Kekulé-O phase in graphene and provides a highly tunable platform to realize unconventional spin physics.

Exchange bias↗

Electronic Structure and Quantum Spin Correlations in Novel Magnetic Compounds

This project has studied the development of new magnetic materials with high magnetocrystalline anisotropy, magnetization, and high Curie temperatures, novel magnetic nanostructures that show skyrmions in the length scale of the range of 10 nm, and Heusler compounds with noncoplanar and noncollinear spin structures with topological Hall effect. The materials investigated towards this project are promising for next-generation energy and information devices. Most importantly, this project has provided fundamental understanding of science and technology behind the above-mentioned materials and insights for future strategies to satisfy the rapidly growing demands of magnetic materials in many applications.

36 MATERIALS SCIENCE↗

Eigenvalue-Based Micromagnetic Analysis of Switching in Spin-Torque-Driven Structures

We present an eigenvalue-based approach for studying the magnetization dynamics in magnetic nanostructures driven by spintronic excitations, such as spin-transfer torque and spin-orbit torque. The approach represents the system dynamics in terms of normal oscillation modes (eigenstates) with corresponding complex eigenfrequencies. The dynamics is driven by a small number of active eigenstates and often considering just a single eigenstate is sufficient. We develop a perturbation theory that provides semianalytical dynamic solutions by using eigenstates for the case in the absence of damping and spintronic excitations as a basis. The approach provides useful insights into dynamics in such systems and allows solving several difficulties in their modeling, such as extracting the switching current in magnetic random-access memories and understanding switching mechanisms. We show that the presented approach directly predicts the critical switching current, i.e., switching current for an infinite time. The approach also provides solutions for the switching dynamics allowing the switching current to be obtained for a finite switching time, provided that the system symmetry is broken, e.g., by tilting the polarizer, so that switching by a finite pulse is possible.

42 ENGINEERING↗

Fe-carbide/Fe-oxide-based nanocomposites synthesized as magnetic nanomaterials via laser ablation synthesis in solution (LASiS)

Magnetic nanostructured materials (MNMs) have gained prominence in materials technology developments owing to their potential biomedical applications for hyperthermia cancer treatment, and transplant organ cryopreservation. Herein, we report the facile and cost-effective synthesis of Fe-based composite MNMs, comprising both Fe@Fe 2 O 3 and Fe 3 C@C core-shell nanoparticles (NPs), via Laser Ablation Synthesis in Solution (LASiS) using Fe targets ablated under acetone and toluene. Detailed materials characterizations using electron microscopy-based imaging, diffraction studies, and spectroscopic analyses - including Raman and Mössbauer spectroscopy - relate the structure-composition properties for different Fe-oxide/carbide phases in the aforesaid MNMs to their respective magnetic responses. Specifically, we confirm the presence of ultra-small (2–10 nm) amorphous Fe-oxide NPs, as well as Fe@Fe 2 O 3 core-shell NPs (20–40 nm) in the samples synthesized by ablating Fe under acetone. In contrast, samples synthesized under toluene indicate a higher concentration of Fe 3 C@C core-shell NPs (20–40 nm) with a relatively low concentration of Fe 2 O 3 NPs (2–10 nm). Furthermore, the crystallinity of the metallic phases and carbonaceous shell coatings are systematically increased by carrying out LASiS under heated toluene (up to ~95 °C). Importantly, mössbauer spectroscopy results indicate that the elevation in toluene temperature leads to an increase in the concentrations of Fe 3 C@C NPs from ~40 % to ~53 % (at.).

36 MATERIALS SCIENCE↗

Cherenkov-type three-dimensional breakdown behavior of the Bloch-point domain wall motion in the cylindrical nanowire

A three-dimensional breakdown behavior of the magnetic Bloch-point domain wall (BP-DW) propagation was investigated in a ferromagnetic nanowire with the variation of the external magnetic field by means of micromagnetic simulation. As magnetic field strength increases up to a threshold value, the BP-DW velocity approaches a critical phase velocity of the spontaneously emitting spin wave (SW), where a Cherenkov-type DW breakdown phenomenon is observed originating from an interaction between the spontaneously emitting SW and the BP-DW. It is found that the velocity of the BP-DW approaches a maximum value (~2000 m/s) due to the intrinsic reversal time of a BP spin texture. This suggests that although cylindrical ferromagnetic nanowires might be free from the two-dimensional Walker breakdown phenomenon, there exists a Cherenkov-type three-dimensional breakdown behavior.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Ultrafast laser-induced spin–lattice dynamics in the van der Waals antiferromagnet CoPS 3

CoPS 3 stands out in the family of the van der Waals antiferromagnets XPS 3 (X = Mn, Ni, Fe, and Co) due to the unquenched orbital momentum of the magnetic Co 2+ ions, which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump–probe technique, we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and, thus, results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4 T 1g → 4 T 2g electronic transition in Co 2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent B g phonon mode at the frequency of about 4.7 THz.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Modulating above-room-temperature magnetism in Ga-implanted Fe 5 GeTe 2 van der Waals magnets

The creation of van der Waals (vdW) ferromagnets with tunable Curie temperature (T C ) and magnetic anisotropy is essential in developing vdW magnet-based devices. Here, we report an effective and reliable method for modulating the magnetic properties of vdW Fe 5 GeTe 2 by site-specific Ga + implantation. In this study, we report an easy axis in the ab-plane for bulk Fe 5 GeTe 2 (T C = 310 K) and an axis out of the plane for thin Fe 5 GeTe 2 flakes (T C = 290 K). Combining element-resolved photoemission electron microscopy and spatially resolved magneto-optic Kerr microscopy, we find that the implantation of a tiny amount of 10 –3 Ga + ·Å –3 in Fe 5 GeTe 2 greatly enhances the T C from 290 to 360 K and switches the magnetic easy axis from the out-of-plane c axis to the ab-plane. The room-temperature x-ray magnetic circular dichroism signal is enhanced from 0% to 9% at an implantation level of 10 –2 Ga + ·Å –3 . These results provide new opportunities for tailoring the magnetic properties of vdW materials beyond room temperature.

36 MATERIALS SCIENCE↗

Spin dynamics in permalloy nano-ellipses for honeycomb and square lattices

We report experimental and theoretical studies of spin dynamics in lattice structures of permalloy (Ni 80 Fe 20 ) nano-ellipses, with four different types of networks including honeycomb and square lattices. The lattices are patterned at the center line of the co-planar wave guide and consist of non-contacting or contacting ellipses. Micromagnetic simulations show excellent agreement with the broadband ferromagnetic resonance (FMR) experimental results. We find the existence of a spin-wave mode localized in the vertex region of the contacting nano-ellipse network. Our finding has important implications when designing an artificial spin ice (ASI) network for functional magnonics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Exsolution Synthesis of Nanocomposite Perovskites with Tunable Electrical and Magnetic Properties

Nanostructured functional oxides play an important role in enabling clean energy technologies and novel memory and processor devices. Using thin-film La 0.6 Sr 0.4 FeO 3 (LSF) as a model system, the novel utility of exsolution in fabricating self-assembled metal oxide nanocomposites with tunable functionalities is shown. Exsolution triggers the formation of metallic iron (Fe 0 ) nanoparticles, Ruddlesden–Popper domains, and nm-scale percolated Fe-deficient channels in LSF. Combining multimodal characterization with numerical modeling, the chemical, magnetic, and electrical properties of the exsolution-synthesized nanocomposite at different stages of Fe 0 exsolution as well as during redox cycling are assessed. After exsolution, the electronic conductivity of the nanocomposite LSF increased by more than two orders of magnitude. Based on numerical analysis representing all the constituents, it is expected that this increase in conductivity originates mainly from the Fe-deficient percolating channels formed during exsolution. Moreover, the exsolved nanocomposite is redox-active even at moderate temperatures. Such redox capabilities can enable dynamic control of the nanocomposite functionality by tailoring the oxygen non-stoichiometry. This concept is demonstrated with a continuous modulation of magnetization between 0 and 110 emu cm -3 . These findings point out that exsolution may serve as a platform for scalable fabrication of complex metal oxide nanocomposites for electrochemical and electronic applications.

36 MATERIALS SCIENCE↗

Unusual Magnetic Hysteresis and Transition between Vortex and Double Pole States Arising from Interlayer Coupling in Diamond-Shaped Nanostructures

Controlling the magnetic ground states at the nanoscale is a long-standing basic research problem and an important issue in magnetic storage technologies. Here, we designed a nanostructured material that exhibits very unusual hysteresis loops due to a transition between vortex and double pole states. Arrays of 700 nm diamond-shaped nanodots consisting of Py(30 nm)/Ru(t Ru )/Py(30 nm) (Py, permalloy (Ni 80 Fe 20 )) trilayers were fabricated by interference lithography and e-beam evaporation. We show that varying the Ru interlayer spacer thickness (t Ru ) governs the interaction between the Py layers. We found this interaction mainly mediated by two mechanisms: magnetostatic interaction that favors antiparallel (antiferromagnetic, AFM) alignment of the Py layers and exchange interaction that oscillates between ferromagnetic (FM) and AFM couplings. For a certain range of Ru thicknesses, FM coupling dominates and forms magnetic vortices in the upper and lower Py layers. For Ru thicknesses at which AFM coupling dominates, the magnetic state in remanence is a double pole structure. Our results showed that the interlayer exchange coupling interaction remains finite even at 4 nm Ru thickness. Furthermore, the magnetic states in remanence, observed by magnetic force microscopy (MFM), are in good agreement with corresponding hysteresis loops obtained by the magneto-optic Kerr effect (MOKE) and micromagnetic simulations.

interlayer exchange interaction↗

Intervening Oxygen Enabled Magnetic Moment Modulation in Spinel Nanostructures

Oxygen vacancies and lattice oxygen on the surface of nanoparticles play crucial roles in the magnetism of transition metal oxides. A fundamental understanding of the interactions between the 2p orbitals of oxygen anions and the 3d orbitals of metal cations is of immense interest for applications due to specific electronic, magnetic, and chemical properties. The spinel nanostructures Co 3 O 4 ,Fe 3 O 4 , and CoFe 2 O 4 present a unique model to alter coordination and bonding due to d electrons and oxygen 2p states. We performed complementary experimental techniques and corresponding model calculations to show that the overall net magnetism differs significantly between the O 2 -rich and -deficient environments. It was found that in monometallic spinel oxides (e.g., Co 3 O 4 and Fe 3 O 4 ), the changes in the spin moment are relatively small (~0.08μ B per formula unit) compared to those in the bimetallic spinel oxide CoFe 2 O 4 (~0.40 μ B per formula unit). Finally, our study illustrates that the O 2 -rich/deficient conditions alter the exchange of O h sites and adjust the metal ion moments so as to impact the overall magnetism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unipolar arc plasmas on nanostructured tungsten surfaces under perpendicular magnetic field

Abstract Unipolar arcing is an important phenomenon in terms of wall erosion and the subsequent plasma contamination in nuclear fusion devices. In this study, unipolar arc plasmas are experimentally explored under the presence of the external magnetic field perpendicular to a tungsten (W) sample on which a ‘fuzz’ nanostructure surface is formed. It is found that the fuzz layer thickness, d fuzz , plays a dominant role in determining the motion of arc spots, the arc ignition probability, and arc plasma parameters. High-speed imaging reveals that the motion of arc spots becomes more collective, as d fuzz increases. Interestingly, arc spots make a circle while moving outward. With increasing d fuzz , the amount of eroded W atoms increases, as indicated from an observed increase in the total visible emission intensity, while the arc ignition probability is found to drop. The physical mechanisms are discussed, in detail, based on spectroscopic measurements of the electron temperature, obtained from Boltzmann plots of both W I and W II, and the electron density, determined from Stark broadening of W I lines.

Physics↗