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The structure and dynamics of magnetization in a vortex spin-transfer nanooscillator, which is a three-layer spin-valve magnetic nanopillar with a small diameter, is studied during the passage of a spin-polarized current. Using micromagnetic simulation [1,2], we studied the dynamic change in the vortices structure, the formation of the C-structure vortex state and edge vortices, the trajectory of movement and the time it takes to reach different dynamic modes. The time needed for the vortices to reach different dynamic modes was found. The possibility of the dynamic generation of radial edge vortices without the presence of a Dzyaloshinsky field or an external inhomogeneous magnetic field is shown. We demonstrate that a vortex in a thick magnetic layer can be a generator of spin waves in a thin magnetic layer with an adjustable oscillation frequency. We consider also multilayer magnetic structures, which are periodically alternating layers of two materials with different physical properties. In such systems it is possible to generate localized magnetization waves (LMW) of the magnetic solitons and breathers type [3]. Special interest in magnetic solitons and breathers is currently associated with the appearance of new experimental techniques that allow to study formation and propagation of localized magnetization waves of nanometer dimensions and their interaction with domain walls (DW). The possibility of controlling the structure and dynamic parameters of magnetic solitons and breathers using an external magnetic field is shown [4]. Dependences of the center of the DW and amplitudes of the LMW on time are constructed and analyzed in the presence of three, five and seven layers. It is shown that the LMW vibrations for the case of five layers can be described by two harmonic oscillators, for the case of seven layers, three harmonic oscillators. This work was supported by RFBR, project No19-02-00316\19 and No20-31-90048.References: 1. A.E.Ekomasov et al., Journal of Magnetism and Magnetic Materials, 471, 2019, 513-520; 2. E.G. Ekomasov et al., Chelyabinsk Physical and Mathematical Journal. 2020. Vol. 5, iss. 2. P. 161–173; 3. A.M. Gumerov et al., Journal of Physics: Conference Series. VII Euro-Asian Symposium “Trends in Magnetism”. 2019. V. 1389. p. 012004: 1–6; 4. E.G. Ekomasov et al., Letters on Materials 10 (2), 2020 pp. 141-146.

MMM 2020

The structure and dynamics of magnetic vortices and solitons in multilayer ferromagnetic nanostructures.

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Recently, additive manufacturing (AM) of functional materials started integrating an additional physical property available besides the mechanical stability in printed parts. This additional property can be an increased electrical conductivity or as addressed here a specific magnetic stray field. AM allows near-net-shape manufacturing of complex magnet shapes, avoiding significant machining waste during conventional manufacture of the final shape from sintered magnet blocks. However, the development of the AM process in general requires a qualified starting material for each process such as powder bed fusion [1], binder jetting or material extrusion. Since the supply of metal powders for AM is limited in general, and there is no Nd-Fe-B based powder designed for use in AM, the development of a Nd-Fe-B-based starting material for commercial production is the goal of the EIT Raw Materials funded project 3DREMAG [2]. Commercial powders designed for injection molding are already used for different AM techniques in combination with different polymers and binders [3 and references therein]. E.g. self-produced Mn-Al powders were used in electron beam melting to produce polymer (and rare-earth element) free hard magnetic fully dense bodies [4]. The printing process was followed by a heat treatment to achieve 90% of the hard ferromagnetic tau-phase in the samples. It is very challenging to obtain fully dense Nd-Fe-B magnets by AM due to the specific microstructure of uniform micrometer sized Nd2Fe14B grains separated by a rare-earth rich grain boundary phase that has to be established to achieve high remanence and coercivity. To obtain sufficient amounts of powders that can be processed by powder bed fusion, Nd-Fe-B strip cast flakes are milled and further plasma spheroidized. First results of lab scale production of the powders and first AM tests will be presented and discussed.References: [1] Mateusz Skalon, Michael Görtler, Benjamin Meier, Siegfried Arneitz, Nikolaus Urban, Stefan Mitsche, Christian Huber, Joerg Franke and Christof Sommitsch, Influence of Melt-Pool Stability in 3D Printing of NdFeB Magnets on Density and Magnetic Properties, Materials 13 (2020), 139. [2] http://3dremag.eu [3] Christian Huber, Gerald Mitteralmskogler, Michael Goertler, Iulian Teliban, Martin Groenefeld, Dieter Suess, Additive manufactured isotropic NdFeB magnets by stereolithography, fused filament fabrication, and selective laser sintering, arXiv:1911.02881 [4] I. Radulov, V. Popov Jr, A. Koptyug, F. Maccari, A. Kovalevsky, S. Essel, J. Gassmann, K. Skokov, M. Bamberger, Production of net-shape Mn-Al permanent magnets by electron beam melting, Additive Manufacturing 30 (2019) 100787.

Nd-Fe-B based permanent magnetic materials design for additive manufacturing: 3DREMAG

The coercivity of RE2Fe14B-type permanent magnet is strongly influenced by the microstructural features such as grain boundary phases as well as grain size. Micromagnetic simulations are powerful tools for revealing the correlation between microstructure and the evolution of hard magnetic properties, including the effects of grain size and grain boundary phases. We have combined micromagnetic simulations and experiments to elucidate the role of excess RE (Nd/Pr) in determining the resulting hard magnetic properties of Nd-Pr-Fe-B melt-spun ribbons. Also, the effect of non-magnetic grain refining refractory carbide (TiC) on both the microstructure and magnetic hardening was studied. For the simulated polycrystalline microstructure of Nd-Pr-Fe-B magnets (Fig. 1(a)) with a mean grain size of 40 nm, the coercivity increases with decreasing inter-grain magnetic exchange interaction Fig. 1(b). The increasing trend in magnetic coercivity of measured melt-spun (Nd, Pr)–Fe–B alloys is ascribed to weak inter-grain exchange coupling due to non-magnetic RE-rich grain boundary phase (Fig. 1(c)) and/or TiC at grain boundary (Fig. 1(d)). This work provides useful information on the role of non-magnetic grain boundary phase to improve the coercivity in Nd-Pr-Fe-B magnets. Combined with experimental and modeling results, we will discuss the mechanism responsible for the enhancements in coercivity and the suitability of the alloys for high performance permanent magnet development. This research was supported by the Critical Materials Institute, an Energy Innovation Hub funded by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Manufacturing Office.

Understanding the Enhancement in Hard Magnetic Properties of Rapidly Solidified (Nd, Pr)-Fe-B Melt-spun Ribbons

Sintered R2Fe14B (R: rare earth element) magnets with 50 at substitution of Nd by Y and Ce were studied in order to reduce the amount of precious rare earth elements used and to make effective use of the surplus rare earth elements. Nd was substituted with Y for larger magnetization and Ce for higher coercivity. By substituting 50 at% of Nd by Y and Ce with an equiatomic composition, a maximum energy density of 355 kJ/m3 was achieved with the residual flux density of 1.38 T and the coercivity of 533 kA/m as shown in Fig. 1. In order to increase the coercivity, the introduction of R6Fe13Ga grain boundary phase to lead the magnetic separation between grains, which is commonly used for Nd2Fe14B, was studied, however the coercivity was not improved due to a large magnetization of R6Fe13Ga, 0.3 to 0.5 T. By introducing the RFe2 grain boundary phase, the coercivity of 1063 kA/m with the residual flux density of 1.22 T was achieved at the composition of Ce of 40% in the total rare earth elements in R2Fe14B sintered magnet. The magnetization of the RFe2 phase was estimated to be about 0.3 T and was not sufficiently low. Since the RFe2 boundary phase improved the covering of the grains, the magnetic separation was enhanced to increase the coercivity.

Magnetic Properties of R2Fe14B Sintered Magnets Substituted 50 at Substitution of Nd with Y and Ce

Pr2Fe14B-based thin films are the useful nano-material for the high-tech performance of the magnetic devices. With its studied outstanding magnetic property such as high uniaxial magnetocrystalline anisotropy (Ku), high coercivity (Hc), high saturation magnetization (Ms), large energy products (BHmax), excellent anisotropic behavior, and super low spin-reorientation at temperature about 4.2 K, Pr2Fe14B magnetic thin films become an alternative candidate for the Nd2Fe14B-based magnetic thin films. In this study, the perpendicular magnetic anisotropy (PMA) Pr-Fe-B films were deposited on corning glass substrate at 600 °C with Si3N4 cover layer and underlayer from Pr25Fe65B10 alloy target by RF magnetron sputtering technique. VSM, XRD, SEM, TEM, and EDS measurements were applied to investigate the relationship between thickness and the microscopic magnetization structures of the PrFeB layer which initiated and propagated crystallization of PMA Pr2Fe14B phase. The magnetic properties of sputtered Pr-Fe-B film was also investigated in terms of the micro-texture evolution. The structure with thickness 50 nm showed the initial point of crystalline characteristic. The initial appearance signal of c-axis orientation of Pr2Fe14B phase and the perpendicular coercive force in the film were comparable at 50 nm, and were alternatively evolved on glass substrates. SEM, TEM, and EDS results revealed that localized grains occurred at the initial stages of growth, and developed non-uniform grain networks across the substrate. The highly c-axis oriented films have a special microstructure which Pr2Fe14B phase showed blossom surface morphology. The exchange coupling was mainly explained for the two-phase nanostructure formed from hard magnetic phase and soft magnetic phase. The texture with the c-axis perpendicular to the film plane had finely signal of development after in-situ annealing at 600 °C. The magnetization irregularity of the thin film was strongly affected by the underlayer and the substrate. The magnetic analysis assuming that the value of film was composed of the correlation between microstructures and magnetic properties on underlayer and substrates.

Manifestation of initial crystallization and c-axis texture in Pr-Fe-B thin films grown on glass substrates

Nd–Fe–B permanent magnets are indispensable materials for high-technology commercial products such as motors, electronic devices, etc., because of their high coercive force. However, the mechanism of the coercive force has not been well understood [1]. For the understanding of the microscopic mechanisms, atomistic modeling, which is a new trend of permanent-magnet modeling, is important. We have studied dynamical and static properties of the Nd magnet, Nd2Fe14B, by applying the stochastic LLG equation [2] and Monte Carlo methods to an atomistic model, in which microscopic parameters were introduced by first-principles calculations [2-7]. We have shown the temperature dependencies of the magnetization, domain-wall profiles, dipolar-interaction effect, ferromagnetic resonance, inhomogeneity effect, surface Nd anisotropy effect, etc. [2-7] In this presentation, we mainly show dynamical aspects of the magnet, focusing on the effect of the interface between grains and grain boundaries. There exist difficulties to estimate long relaxation times of barrier-crossing magnetization reversal quantitatively due to the limitation of simulation time and the dependence on the damping factor. Here we propose a statistical method to estimate precisely long relaxation times in the stochastic region, by which one can identify an initial transient process and a long-time regularly relaxation process. We show an estimation of the coercive force of a single grain using this method [6]. Local environments around rare-earth ions at the interfaces of rare-earth magnets may be different from those in the bulk. First-principles studies have suggested that the magnetocrystalline anisotropies of the Nd atoms at the (001) surface of grains in the Nd magnet have in-plane (c-plane) anisotropy, while those in the bulk have out-of-plane anisotropy. Thus, we investigated the effect of the surface magnetic anisotropy of the Nd atoms on the coercivity in the Nd magnet (Fig. 1). We analyzed the coercive force in three cases, in which the Nd atoms in surface layers have (I) no anisotropy, (II) in-plane anisotropy, and (III) doubly reinforced anisotropy for not only the (001) surface but also (100) surface, with the layer-depth dependence [6]. We find that at zero temperature the modification of the anisotropy of the Nd atoms at the first-surface layer reduces the coercive force in cases I and II and enhances the force in case III, but at room temperature, this modification does not affect the coercive force, and the modification at several surface layers is necessary to reduce or enhance the coercivity at room temperature. We also present the nucleation and pinning fields of the Nd magnet as a function of the strength of the anisotropy energy of the soft magnet and also as a function of the thickness of the soft magnet (Fig. 2) [7]. In the Nd magnet, reflecting the lattice structure, the properties of domain walls (DWs) depend on their moving directions. Bloch and Néel DWs move along the a (or b) and c axes, respectively. We show the difference in the nucleation and pinning fields between the Bloch and Néel DWs. We find that the thermal fluctuation effect affects the threshold fields in the Nd magnet significantly. We also find that the strength of the anisotropy energies of the soft magnet phase is not so important for the pinning field, while it is essential for the nucleation field, etc.References: [1] S. Hirosawa et al., Adv. Nat. Sci.: Nanosci. Nanotechnol. 8, 013002 (2017). [2] M. Nishino and S. Miyashita, Phys. Rev. B 91, 134411 (2015); 100, 020403(R) (2019). [3] M. Nishino et al., Phys. Rev. B 95, 094429 (2017). [4] S. Miyashita et al., Scr. Mater. 154, 259 (2018). [5] T. Hinokihara et al., Phys. Rev. B. 97, 104427 (2018). [6] M. Nishino et al., submitted. [7] I. E. Uysal et al., Phys. Rev. B 101, 094421 (2020).

Finite-Temperature Dynamical and Static Properties of the Nd Magnet Studied by an Atomistic Modeling INVITED

High-Frequency Signal injection (HFSW)method is a technology to obtain the rotor position information from the high-frequency response of the injected voltage or current signal. While this method is quite sensitive to the motor parameters, the correct parameter decides the rotor position estimation accuracy. In traditional scheme, the d-q axis inductance is set as a constant value under the rated conditions in the high-frequency mathematical models, while the d-q axis inductance varies in different operating conditions exactly. Even in the same operating conditions, the d-q axis inductance also changes due to the magnetic field saturation caused by phase current. JMAG simulation verifies the assumption, as shown in Fig.1. However, very little about that has been discussed in the published papers corresponding to HFSW method. Inspired by current linkage harmonics and torque ripple [1], a modified motor model considering non-linear change of inductance is proposed in this paper, where motor parameter is changing with magnetic field saturation. With the adoption of new model, the traditional HFSW injection equation is also modified in the paper. Compared with the traditional scheme, the modified model takes the dynamic change of d-q axis inductance into consideration and reduced the influence of the induction variation. Simulation in matlab Simulink shows a good performance in rotor error suppression and steady state error depression. The proposed method has also been employed in a 4p-24s permanent magnet synchronous motor. Fig.2 exhibits the high frequency incremental current in α-β axis while Fig.2 shows the incremental current with the modified high frequency square wave injection equation. (The variation of inductance is reflected as 5th and 7th current harmonics in α-β axis). It can be verified that the proposed method can not only compensate the HFI current harmonics caused by non-linear changes in d-q axis inductance but also maintain the good steady-state and dynamic performance of traditional systems.References: [1] Ponomarev, P. , Petrov, I. , & Pyrhonen, J. . (2014). Influence of travelling current linkage harmonics on inductance variation, torque ripple and sensorless capability of tooth-coil permanent-magnet synchronous machines. IEEE Transactions on Magnetics, 50(1), 1-8.

Sensorless Control Scheme for PMSM Based on High-Frequency Square-Wave Voltage Injection considering Non-linear Change of Inductance in D-Q Axis

The presence in wastewater of complex organic compounds, pharmaceuticals, etc, is a problem due to the difficulty of removing these compounds in traditional water treatment plants. The current available processes, like reverse osmosis, are costly and complicated, so new materials and processes for the removal of these compounds are necessary. Iron-based magnetic particles are one of the materials most studied recently for the elimination of contaminants, both through physical and chemical processes. The manufacture of these particles is cheap and simple, and their magnetic properties make their recovery for reuse one of their main advantages. The Fenton reaction is an oxidation process capable of degrading organic compounds through hydroxyl radicals. Iron-based magnetic particles can be a catalyst for heterogeneous Fenton processes, but they present the problem of electronic depletion, as the iron ions of the surface become oxidized, reducing the efficiency of catalysis, and adsorption of the particles reducing the available surface further. In our study, we developed Fenton process to degrade colorant content of waters, achieving a very good efficiency. We have also studied the kinetics of the process. To solve the problem of spent particles by regenerating the magnetic particles used we have used reducing agents, so that the efficiency of the particles for catalysing the Fenton reaction is maintained or increased after repeated uses. Efficiency is obtained by measuring the relative degradation of methylene blue, an organic dye. We have tested two different agents and compared with non-regenerated particles. The relative degradation of non-regenerated particles has reduced to less than 20% after the 2nd use, while particles regenerated one of the reducing agents had the degradation reduced to less than 20% after 8 re-uses, and particles regenerated with another reducing agent maintained relative degradation above 70% for all 10 re-uses that were tested.References: Paulo A. Augusto, Teresa Castelo-Grande, Diana Vargas, Lorenzo Hernández, Leticia Merchán, Angel M. Estevez, Juan Gómez, José M. Compaña, Domingos Barbosa, 2020. Water Decontamination with Magnetic Particles by Adsorption and Chemical Degradation. Influence of the Manufacturing Parameters. Materials, Volume 13, Issue 10 (2020)

Regeneration and Reuse of Magnetic Particles for Wastewater Treatment

The magnetic tunnel junction(MTJ) based molecular spintronics device (MTJMSD) approach provides solutions to decades-old fabrication difficulties in mass-producing molecular spintronics-based computer devices. To producing MTJMSD, molecular channels are bridged across the insulator of an MTJ with exposed side edges. In an MTJMSD, two ferromagnets (FMs) are simultaneously connected by an insulator film and the molecular channels along the exposed sides. In our prior experimental studies, we observed that paramagnetic molecules connected to ferromagnet produced unprecedented antiferromagnetic coupling when the competing coupling via insulator was minimized[1]. In this paper, our Monte Carlo Simulation (MCS) study the effect of varying coupling via insulator (Ji) on the magnetic properties of an MTJMSD. To complement our prior work[1], we assumed molecules produced strong antiferromagnetic coupling. The nature (ferromagnetic or antiferromagnetic) and magnitude of Ji determined the resultant effect. Antiferromagnetic Ji enhanced the pre-existing antiferromagnetic molecular coupling effect. Ferromagnetic Ji competed with molecular coupling. Ferromagnetic Ji/kT~0.4 coupling made two FM electrodes parallel by overcoming the molecular coupling effect (Fig.1). We also studied the impact of thermal energy on the Ji ability to impact the MTJMSD properties. The Ji variation critically impacted the temporal evolution of the equilibrium MTJMSD magnetic moment. For the Ji's intermediate values, ferromagnetic electrodes exhibited different phases around the junction area (Fig 2). Our MCS intends to consider the impact of defects and even intentional insemination of nanostructure within insulator thickness to producing direct coupling that competes with molecular coupling.References: [1] P. Tyagi, C. Baker, C. D'Angelo, Nanotechnology 2015, 26, 305602.

Effect of Direct Exchange Coupling Via the Insulator On the Magnetic Tunnel Junction Based Molecular Spintronics Devices with Pre-existing Strong Molecule Induced Antiferromagnetic Coupling

Paramagnetic molecules, with a net spin state, can tailor magnetic exchange coupling strength between two ferromagnetic electrodes in a magnetic tunnel junction based molecular spintronics devices (MTJMSD). The MTJMSD approach provides solutions to fabrication difficulties in the mass production of molecular-based computer devices. MTJMSD is produced by bridging the molecular channels across the insulator of an MTJ with exposed side edges. Our prior experimental and Monte Carlo Simulations(MCS) studies showed that paramagnetic molecules produced unprecedented strong antiferromagnetic coupling between two ferromagnets[1]. The overall antiferromagnetic coupling occurred when a paramagnetic molecule made antiferromagnetic coupling to the first electrode and ferromagnetic coupling to the second electrode. In this paper, we report the study on the effect of coupling among molecules (Jm) on the MTJMSD. This study is critical because prior work in the MTJMSD area focused on the coupling between molecules and ferromagnets. For the first time, we studied the effect of Jm (coupling between molecules) using the Ising Model of MTJMSD. MTJMSD used in this study was 11x 10 x 50 size, with 11 being the thickness of the MTJMSD, and 5x10x50 being the size of each electrode. In this study, while other parameters were kept constant, we varied Jm between -1 to 1, using a step size of 0.2, at simulation counts varying from 10,000 to 500M. It was observed at the various simulation counts that the molecules were settling in the same spin direction for Jm=-1, 0, 1. The only anomaly occurred at 200M simulation counts, where the two ferromagnetic electrodes had spins in opposite directions, which gives room for more investigations for the future. A general observation of the spin states shows that at lower simulation counts, that is at 10million, 1million, and 100,000, the spin states become more random without a clear spin direction. Investigating the effect of coupling on the magnetic properties of the MTJMSD, with smaller step sizes of about 0.1, using the MCS could produce more revealing results, as we couple the Jm with both ferromagnetic electrodes.References: Tyagi, P.; Baker, C.; D'Angelo, C., Nanotechnology 2015, 26, 305602.

Monte Carlo Simulation Study Of The Effect Of Inter-Molecular Coupling On The Magnetic Properties Of Magnetic Tunnel Junction Based Molecular Spintronics Devices

We discuss our latest efforts toward using a single, optically active nitrogen-vacancy (NV) spin sensor (implanted in a single-crystal diamond substrate) to measure magnetic thermal noise modified by spin Hall torques [1] in a Py/Pt nanowire [2]. In this poster, we first present our subtractive method for fabricating magnetic nanocircuits on diamond, and initial characterization of working Py(5 nm)/Pt(5 nm) nanowires. We reliably achieve contacts with few-ohms of resistance and 200 nm of overlap at each end of the 2-μm-long, 400-nm-wide wire, and we observe an anisotropic magnetoresistance of 0.4%. Importantly, we observe that the subtractive patterning process (masked ion milling) used to define the devices reduces the NV spin resonance contrast by a factor of ∼5, but that subsequent exposure to an oxygen plasma returned the contrast to its nominal level without affecting the nanowire behavior. Finally, we present progress toward using transport measurements to estimate thermal time scales in these systems (while calibrating the RF current in the nanowire), as well as preliminary NV readout of spin-transfer-controlled magnetic thermal noise.References: [1] C. Du, T. van der Sar, et al., Science, 357, 195-198 (2017) [2] A. Solyom, Z. Flansberry, et al., Nano Lett., 18, 6494-6499 (2018)

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Nd-Fe-B based permanent magnetic materials design for additive manufacturing: 3DREMAG

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