United States

In this work, we investigate the synthesis, along with the structural, magnetic, and surface chemical environment properties, of novel Mn-Co-NiO-based heterostructured nanocrystals (HNCs). The objective is to develop novel, well structurally ordered inverted antiferromagnetic (AFM) NiO – ferrimagnetic (FiM) spinel phase overgrowth HNCs. Inverted HNCs are particularly promising for magnetic device applications because their magnetic properties are more easily controlled by having well-ordered AFM cores, which can result in magnetic structures having large coercivities, tunable blocking temperatures, and other enhanced magnetic effects. The synthesis of the HNCs is accomplished using a two-step process: In the first step, NiO nanoparticles are synthesized using a thermal decomposition method. Subsequently, Mn-Co overgrowth phases are grown on the NiO nanoparticles via hydrothermal nanophase epitaxy, using a fixed pH level (~5.3) of the aqueous medium. This pH level was selected based on previous work in our laboratory showing that NiO/Mn3O4 HNCs of constant size have optimal coercivity and exchange bias when synthesized at a pH of 5.0.1 The crystalline structure, surface/interface chemical environment and gross morphology of the Mn-Co-NiO-based HNCs have been analyzed using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Scanning Electron Microscopy (SEM) techniques, respectively. Analysis using these techniques shows that the HNCs are composed of a NiO core and a CoMn2O4 overgrowth phase. Rietveld refinement of XRD data shows that the NiO core has the rocksalt (Fm-3m) cubic crystal structure and the CoMn2O4 overgrowth has the spinel (I41/amd) crystal structure. Moreover, an increased relative amount of the CoMn2O4 overgrowth phase is deposited with decreasing NiO core particle size during the synthesis of the HNCs. Analysis of the O 1s, Ni 2p, Co 2p, and Mn 2p regions of the XPS spectra measured from our samples is consistent with well-structured core/overgrowth phases having M-OH (M: Ni, Co, Mn) bonding at their surface regions. The results from PPMS magnetization and high-resolution transmission electron microscopy (HR-TEM) characterization of the Mn-Co-NiO-based HNCs will be discussed.&lt;br&gt;

**References:** &lt;br&gt;
(1) Shafe et al., ACS Applied Materials &amp; Interfaces, 13, 24013−24023 (2021)&lt;br&gt;


MMM 2022

Investigations of Size Dependent Properties of Mn

In this work, we investigate the synthesis, along with the structural, magnetic, and surface chemical environment properties, of novel Mn-Co-NiO-based heterostructured nanocrystals (HNCs). The objective is to develop novel, well structurally ordered inverted antiferromagnetic (AFM) NiO – ferrimagnetic (FiM) spinel phase overgrowth HNCs. Inverted HNCs are particularly promising for magnetic device applications because their magnetic properties are more easily controlled by having well-ordered AFM cores, which can result in magnetic structures having large coercivities, tunable blocking temperatures, and other enhanced magnetic effects. The synthesis of the HNCs is accomplished using a two-step process: In the first step, NiO nanoparticles are synthesized using a thermal decomposition method. Subsequently, Mn-Co overgrowth phases are grown on the NiO nanoparticles via hydrothermal nanophase epitaxy, using a fixed pH level (~5.3) of the aqueous medium. This pH level was selected based on previous work in our laboratory showing that NiO/Mn3O4 HNCs of constant size have optimal coercivity and exchange bias when synthesized at a pH of 5.0.1 The crystalline structure, surface/interface chemical environment and gross morphology of the Mn-Co-NiO-based HNCs have been analyzed using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and Scanning Electron Microscopy (SEM) techniques, respectively. Analysis using these techniques shows that the HNCs are composed of a NiO core and a CoMn2O4 overgrowth phase. Rietveld refinement of XRD data shows that the NiO core has the rocksalt (Fm-3m) cubic crystal structure and the CoMn2O4 overgrowth has the spinel (I41/amd) crystal structure. Moreover, an increased relative amount of the CoMn2O4 overgrowth phase is deposited with decreasing NiO core particle size during the synthesis of the HNCs. Analysis of the O 1s, Ni 2p, Co 2p, and Mn 2p regions of the XPS spectra measured from our samples is consistent with well-structured core/overgrowth phases having M-OH (M: Ni, Co, Mn) bonding at their surface regions. The results from PPMS magnetization and high-resolution transmission electron microscopy (HR-TEM) characterization of the Mn-Co-NiO-based HNCs will be discussed. 

**References:** 
(1) Shafe et al., ACS Applied Materials & Interfaces, 13, 24013−24023 (2021)

poster

#### Welcome to the 67th Annual Conference on Magnetism and Magnetic Materials, MMM 2022!

The Conference was held from October 31 to November 4 and offers both in-person and on-demand content.

MMM 2022 is sponsored jointly by AIP Publishing and the IEEE Magnetics Society. Members of the international scientific and engineering communities interested in recent developments in fundamental and applied magnetism are invited to attend and contribute to the technical sessions. The technical program will include invited and contributed papers in oral and poster sessions, invited symposia, a tutorial, and several special sessions. This Conference provides an outstanding opportunity for worldwide participants to meet their colleagues and collaborators and discuss developments in all areas of magnetism research.

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Stoichiometric LaMnO3 has an orthorhombic crystal structure with an antiferromagnetic (TN ~ 140 K) insulating nature (1). The substitution of aliovalent cations (Sr2+ or Na1+) induce holes in the partially filled 3d shell of Mn and oxidizes the Mn3+ (t2g3eg1) to Mn4+ (t2g3eg0) and transforms the LaMnO3 to ferromagnetic metal through the double exchange coupling of Mn4+-O-Mn3+ (2). Since the Na1+ (1.39 Å) has an ionic radii closer to La3+ (1.36 Å) this would induce a twice number of holes compared to Sr2+ substitution. Drastic variations in their physical properties have also been found in different synthesis methods (3,4). Therefore, in this work, we adopted a recently emerging microwave (MW) heating to synthesise La1-xNaxMnO3 (x = 0, 0.1, 0.3) from the oxide precursors. Conduction or dielectric loss heating by MW irradiation enables the fast and homogenous reaction in few minutes. We achieved 1000 oC in 10 min and dwelled the samples for 20 min. The operating MW power alone was varied from 1000 W to 1200 W and 1400 W for x = 0.3 to examine the effect of MW power on its physical properties. Temperature-dependent magnetization and resistivity of x = 0, 0.1, 0.3 with fixed MW power (1200 W) are shown in Fig. 1 (a)&(b). A broad Curie transition is observed for undoped LaMnO3 with TC of 200 K, unlike our previous report on solid-state prepared La1-xNaxMnO3 where we observed TN = 140 K for undoped LaMnO3 (5), and the transition becomes narrow with increased TC as x increases. Insulating LaMnO3 transforms to metallic below TC upon Na doping. TC is denoted in the figure by dotted vertical lines. As the MW power increases from 1000 W to 1200 W, the resistivity of x = 0.3 decreases drastically and the metal-insulator transition also becomes sharp at a temperature very close to TC (Fig. 1(c)). The obtained microwave absorption peaks at a specific field show only a little increase with increasing the frequency of the MW signal. These findings will be correlated and discussed with the structural and morphological features acquired by microwave irradiation. 

**References:** 
(1) T. Tokura, et al., Mater. Sci. Eng. B 31(1-2), 187–191 (1995). 
(2) G.H. Rao, et al., J. Phys. Condens. Matter 11, 1523 (1999). 
(3) Y. Regaieg, et al., Materials Letters 80, 195–198 (2012). 
(4) Shuai Zhang, et al., Ceramics International 46, 584–591 (2020). 
(5) Rajasree Das, et al., Ceramics International 47, 393–399 (2021). 

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Effect of microwave instant heating on magnetic, electric, thermoelectric and microwave absorption properties of La0.7Na0.3MnO3

The inverse Faraday effect (IFE) [1,2,3] phenomenologically describes the static magnetization induced by the circularly polarized light. In experiments, the IFE is able to reverse the magnetization of magnets with strong laser pulse, providing an optical method of ultrafast magnetization manipulation. Recently, sensitive detection of the effective magnetic field induced by a continuous laser can be carried out electrically through the inverse spin Hall effect [4]. Here, we study inverse Faraday effect in Dirac Hamiltonian with random impurities using Keldysh formalism and diagrammatic perturbation theory in low frequency regime [5]. The mass term in Dirac Hamiltonian is essential for the IFE, where the spin magnetic moment induced by circularly polarized light is proportional to frequency of the incident light within THz regime. For massive Dirac electrons, the corrections due to the short-range impurities on spin magnetic moment vertex exhibits mixing of spin magnetic moment vertex and spin angular momentum vertex. The spin magnetic density response is divergently enhanced by the vertex corrections near the band edge. 
**References** [1] P. Pershan, Physical Review 130, 919 (1963).
[2] K. Taguchi, and G. Tatara, Physical Review B 84, 174433 (2011).
[3] K. Taguchi, T. Imaeda, M. Sato, and Y. Tanaka, Phys. Rev. B 93, 201202(R) (2016).
[4] M. Kawaguchi, H. Hirose, Z. Chi, Y.-C. Lau, F. Freimuth, and M. Hayashi, arXiv preprint arXiv:2009.01388 (2020).
[5] G. Qu, and G. Tatara. arXiv preprint arXiv:2201.10155(2022).

Theory of Inverse Faraday effect in massive Dirac electrons

The rare-earth nitrides are the only known series of intrinsic ferromagnetic semiconductors, with a range of magnetic behaviours stemming from the contribution of both spin and orbital 4f moments. The similar chemistry of the rare-earths and the common structure of the nitrides simplifies their combination in superlattices and solid solutions. Recent studies of rare-earth nitride superlattices have shown enhanced superconductivity [1] and magnetic exchange spring behaviour that results from the competition between the Zeeman and Exchange interactions [2]. Yet, little has been published to date exploring the combination of these nitrides in solid-solutions.

We show (with reference to magnetometry, XMCD and anomalous Hall effect measurements) that the same Exchange/Zeeman competition that leads to a complex twisted magnetic phase in superlattices manifests quite differently in solid solutions. Leading, where an orbital-dominant ferromagnet (SmN) is paired with a spin-only ferromagnet (GdN), to a composition exhibiting a net zero magnetic moment (A compensation point). 
**References** [1] E.-M. Anton, S. Granville, A. Engel et. al. , Phys. Rev. B, Vol. 94, 024106 (2016)
[2] E.-M. Anton, W. Holmes-Hewett, J. McNulty et. al. , AIP Advances, Vol. 1, 015348 (2021)

Exchange/Zeeman Competition in the Rare Earth Nitrides and the Resulting Magnetic Compensation

VCMA effect describes the fact that in a capacitor, in which one of electrodes is made of a thin ferromagnetic metal, the magnetic properties of the ferromagnetic metal changes, when a voltage is applied to the capacitor[1]. Inside a metal the electrical field is screened by free electrons and cannot penetrate deep inside the metal. As a result, the voltage, which is applied to the capacitor dielectric (gate), may penetrate into and affect only the few uppermost atomic layers of the metal near the gate. However, the change of magnetic properties of the uppermost layer by the gate voltage affects the magnetic properties of the whole film. This can be only the case if the interfacial perpendicular magnetic anisotropy (PMA) is affected by the gate voltage [2]. The strength of PMA is characterized by the anisotropy field Hani and proportional to the strength of spin-orbit interaction, demagnetization field and magnetization of nanomagnet.
Fig.1 shows the measured Hani and coefficient of spin-orbit interaction kso in FeCoB nanomagnet under a different gate voltage. kso defies the strength of the spin-orbit interaction[3]. Hani decreases and kso increases under an increase of gate voltage. It is unexpected because Hani is linearly proportional to kso [3] and should increase when kso increases. It means that even though the strength of the spin-orbit interaction is affected by the gate voltage, but additionally to kso there is another voltage- dependent parameter, which defines the voltage dependence of Hani. The intrinsic field in nanomagnet or demagnetization field might be such a parameter.
Fig.2 shows measured Hani and kso of different nanomagnet of different wafers. The same tendency exists in all measured nanomagnets. 
**References** [1] Y. Shiota, T. Nozaki, F. Bonell, S. Murakami, T. Shinjo, Y. Suzuki, Nat. Mater. 11 (2012) 39–43.
[2] V. Zayets, T. Nozaki, H.Saito, A. Fukushima, S.Yuasa, arXiv:1812.07077 ( 2018).
[3] V.Zayets, IOA-07, MMM 2021. 

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Unexpected opposite dependencies of anisotropy field and strength of spin orbit interaction on gate voltage measured in FeCoB nanomagnet

This study aims to fabricate a voltage-tuneable magneto resistive sensor with the ability to measure small magnetic field signals in three dimensions. Sensing direction in magneto resistive sensors is linked to the magnetization of reference layer. Materials like CoFe1, CoFeB2 and Heusler alloys3 are good choices as reference layers due to their adjustable magnetic anisotropies. Here, using ionic liquid gating (ILG), we observed that magnetic anisotropy of reference layer CoFeB is switchable in MgO(1.5nm)/CoFeB(1.6nm)/W(0.5nm) stack. We used ionic liquid N, N-diethyl-N-methyl N-(2-methoxyethyl) ammonium bis (trifluoromethylsulfonyl) imide (DEME TFSI) (IoLiTec) for applying the gate voltage (VG) ranging between ±3.5V. Using the magneto-optical Kerr effect, we have investigated the change of anisotropy using different gate voltages. We found that magnetic anisotropy switches from out-of-plane (virgin state) to in-plane upon the application of +3.5V, whereas removal of applied voltage +3.5V or application of -3.5V, switches magnetic anisotropy back to out-of-plane, demonstrating the switching behaviour of the stack is reversible and repeatable. Moreover, we observed that out-of-plane to in-plane anisotropy switching time is higher (~45 sec) compared to in-plane to out-of-plane switching time (~25 sec). Hence, a stack having stronger out-of-plane and switchable anisotropy is ideal to use in voltage tuneable magneto resistive sensors. 
**References** 1. Parkin, S. S. P. et al., Nat. Mater., 2004, 3, 862–867.
2. Yuasa, S. & Djayaprawira, D. D., J. Phys. D. Appl. Phys., 2007, 40, 337-354.
3. Palmstrøm, C. J., Prog. Cryst. Growth Charact. Mater., 2016, 62, 371–397. 

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Switching of Magnetic Anisotropy in MgO/CoFeB/W stack by Ionic Liquid Gating for Voltage Tuneable Magneto Resistive Sensor

Reservoir computing (RC) has been considered as one of the key computational principles beyond von-Neumann computing. Magnetic skyrmions, topological particle-like spin textures in magnetic thin films, are particularly promising for implementing RC [1] since they respond strongly nonlinear to external stimuli and feature inherent multiscale dynamics. We propose and demonstrate experimentally a conceptually new approach to skyrmion RC that exploits the thermally activated diffusive motion of skyrmions [2]. By confining the thermal and low-energy, electrically gated skyrmion motion, together with employing spatially resolved input and readout, we find that already a single skyrmion in a confined, triangular geometry (Fig. 1) suffices to realize non-linearly separable functions, which we demonstrate for the XOR gate along with all other Boolean logic gate operations [3] (Fig. 2). Our proposed concept can be readily extended by linking multiple confined geometries and/or by including more skyrmions in the reservoir, suggesting high potential for scalable and low-energy reservoir computing.

Brownian Reservoir Computing Realized Using Geometrically Confined Skyrmions

Spiking neural networks have attracted a lot of interest in the past decade as they meet the need of energy efficiency in deep neural network computing (1). Using spikes instead of continuous signals enables low power operation, event-based computations and fast response time, which is better adapted to spatial-temporal data. Combined with unsupervised and local learning rules such as the spike-timing-dependant plasticity rule (2), SNN with magnetic tunnel junction (MTJ) based neurons provide interesting solutions for embedded technologies with better back-end-of-line compatibility (3) compared to other technologies.
For the spike generation, we propose an MTJ-based neuron composed of two magnetized layers (M1 and M2), with low thermal stabilities, separated by an oxide tunnel barrier. Under applied current, the spin-transfer torque (STT) enables an alternating switching of both magnetic layers leading to a so-called “windmill motion” (see Fig1.a-c) previously predicted by simulation for in-plane and out-of-plane magnetized MTJs (4,5). Here we designed, fabricated and characterized such type of structure and were able to achieve steady alternating magnetization reversal of both layers generating a characteristic spike-like resistive response.
MTJ stacks of FeCoB/MgO/FeCoB, with varying FeCoB thicknesses, were deposited by magnetron sputtering and patterned into nano-pillars with diameters ranging from 50 to 200 nm. The electrical characterization of the nano-pillars reveals essential changes of the magnetization dynamics depending on the pillar diameters, layer thicknesses, voltage, applied magnetic field and temperature of the junction. As predicted by the simulation, the frequency of the oscillations and the width of the spikes evolve with the voltage amplitude and the applied field. Important similarities confirm the parameter dependence with temperature and bias voltage. Controlling the spiking rates at low voltages is a critical requirement to build an efficient spiking neural network.
References Acknowledgements:
This work was supported by ANR via grant SpinSpike Projet-ANR-20-CE24-0002. 

**References:** 
(1) A. Tavanaei, M. Ghodrati and S.R. Kheradpisheh, Neural networks, 111, 47-63 (2019). 
(2) T. Iakymchuk, A. Rosado-Muñoz and J.F. Guerrero-Martínez, EURASIP Journal on Image and Video Processing 2015, 1-11 (2015). 
(3) D. Shum, D. Houssameddine and S.T. Woo, 2017 Symposium on VLSI Technology. IEEE pp. T208-T209 (2017). 
(4) R. Matsumoto, S. Lequeux, and J. Grollier, Physical Review Applied, 11(4), 044093 (2019) 
(5) G. Gupta, Z. Zhu and G. Liang, arXiv preprint arXiv, 1611.05169 (2016). 

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Spiking dynamics with dual free layer MTJ

Magnetic random access memory (MRAM) is a promising candidate for beyond-CMOS memory and logic technologies and has been developed for commercial purposes in recent years (1). The key building block of commercial MRAM is magnetic tunnel junction (MTJ), which is operated through either spin transfer torque (STT) or spin-orbit torque (SOT). STT-based MRAM benefits from higher cell density but suffers from reliability and energy-efficiency due to the current flow through the MTJ whereas SOT-based MRAM has superior reliability, endurance, and faster switching times (2). For realizing the ultralow switching current density and ultrafast switching MRAM cell, two or more driving forces are normally employed to switch MTJs. One acts as the principal switching mechanism and the other serves to assist in switching. For example, ultrafast switching speed of ~ 0.27 ns has been reported in SOT switching of perpendicular MTJs (p-MTJs) assisted with STT and voltage-controlled magnetic anisotropy (VCMA), however, the key challenge is still large switching current densities (Jc) ~ 2.0×108 A/cm2 for SOT and ~ 2.3×106 A/cm2 for STT (3).
Voltage controlled exchange coupling (VCEC) occurs in perpendicular MTJs (p-MTJs) with synthetic antiferromagnetic (SAF) free layers and can realize bidirectional switching at switching current densities as low as 1 x 105 A/cm2 (4). In this work, we designed and fabricated the p-MTJ stacks with SAF free layers on bi-layered spin Hall channels (Ta/Pd). The p-MTJ stacks were patterned into 150-nm pillars, and MTJ devices are switched through combination of SOT and VCEC effects, as illustrated in Fig. 1(a). Bidirectional switching of p-MTJs were obtained with current densities as low as 3×103 A/cm2 for VCEC and 6.8×107 A/cm2 for SOT, as shown in Fig. 1(b), where the VCEC switching current density is two orders of magnitude lower than the reported value for VCEC-only switching [4]. Furthermore, by studying the contribution of SOT and VCEC for MTJ switching, it is found that SOT plays a crucial role for ultralow-energy VCEC bidirectional magnetization switching. 

**References:** 
(1) J.-P. Wang et al, DAC '17: Proceedings of the 54th Annual Design Automation Conference 16, pp. 1-6 (2017). 
(2) Y. C. Liao et al, IEEE J. Explor. Solid-State Computat. 6, pp. 9-17 (2020). 
(3) E. Grimaldi et al, Nat. Nanotechnol. 15, pp. 111-117 (2020). 
(4) D. Zhang et al, Nano Lett., 22, pp. 622-629 (2022). 

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Ultra low current density switching via voltage

Racetrack memory is expected to be a memory device that supports the information society because of its high speed and low power consumption. Although many studies have been conducted to improve the speed of magnetic domain wall movement, few studies have been conducted from the viewpoint of Joule heat. Therefore, we have investigated the relationship between Joule heat and domain wall motion in the 2022 Joint MMM-INTERMAG.(1) 
In elucidating the mechanism of this current-driven domain wall motion, although the domain wall width is an essential parameter for improving the domain wall moving speed and the critical current density, the details of the domain wall width are still unknown. Generally, MFM is used for magnetic domain observation. In MFM, as shown in FIG. 1, it is possible to observe the magnetic domain shape by vibrating a thin magnetic needle up and down, but it is challenging to investigate the accurate magnetic flux density distribution. However, suppose the TMR head can be contacted with the sample and scanned. In that case, the distance between the sample and the TMR head can be kept constant to measure the accurate magnetic flux density distribution created by the magnetic recording domain. FIG. 2 shows a TMR head scan image of a magnetic domain recorded in a racetrack memory having a width of 10 μm and a length of 100 μm. The result of line scanning by enlarging this domain wall is also shown in the figure. The recording material is TbCo ferrimagnetic material, the domain wall movement is fast, and the critical current density is small (2). Despite the small saturation magnetization due to ferrimagnetism and thin film (10 nm), the TMR head could measure a clear change in magnetic flux density within a range of ± 20 mT. 

**References:** 
(1) Sota, K. et al. Relationship between pulse width and domain wall velocity in current induced domain wall motion in GdFeCo wire and the effect of joule heat on the racetrack memory, Joint MMM-Intermag Conference, 3628926 (2022) 
(2) Sina, R. et al. Fast Current Induced Domain Wall Motion in Compensated GdFeCo Nanowire, Joint MMM-Intermag Conference, 3786257 (2022) 

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Evaluation of magnetic flux density distribution of magnetic domains recorded in racetrack memory by TMR head

Unidirectional spin Hall magnetoresistance (USMR) is a magnetoresistance effect with potential applications to read two-terminal spin-orbit-torque (SOT) devices directly. In this work, we observed a large USMR value (up to 0.710-11 per A/cm2, 50% larger than reported values from heavy metals) in sputtered amorphous PtSn4/CoFeB bilayers. Ta/CoFeB bilayers with interfacial MgO insertion layers are deposited as control samples. The control experiments show that increasing the interfacial resistance can increase the USMR value, which is the case in PtSn4/CoFeB bilayers. The observation of a large USMR value in an amorphous spin-orbit-torque material has provided an alternative pathway for USMR application in two-terminal SOT devices. 

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