United States

We present the results of density functional calculations of the proposed low temperature charge quadrupolar ordering in Ba2MgReO6. Ba2MgReO6 is a spin-orbit-driven Mott insulator with a symmetry-lowering structural phase transition at 33 K and a canted antiferromagnetic ordering of the small (around 0.25 μB) Re magnetic moments at 18 K. The goal of our calculations is to test the existence of the quadrupolar order, and to understand its relationship to the structural and magnetic orders, which we achieve by separately isolating the ordering of the charge, spins, orbital moments, and structure. We find that the charge quadrupole ordering exists, and can be realized in the absence of magnetic ordering. In addition to shedding light on the detailed behavior of Ba2MgReO6, our work provides insight into the intriguing physics of 5d1 double perovskites in general, and illustrates a method for the analysis of magnetic ordering interactions combined with higher orders such as charge quadrupoles.

MMM 2020

Hidden Multipolar Orders in 5d1 Ba2MgReO6

The 65th Annual Conference on Magnetism and Magnetic Materials (MMM 2020) was held in a virtual form. The COVID-19 pandemic, with its associated uncertainty about international travel and the ability to gather in large groups, meant that the Steering Committee decided to cancel the face-to-face meeting that had been planned in Palm Beach, Florida November 2-6, 2020.

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technical paper

Magnetostriction plays a key role in magnetization dynamics inside soft magnetic materials, which are widely used in electronic devices for inductor cores. In general, the performance of the soft magnetic device is governed by magnetization dynamics such as domain-wall motions. Thus, it is indispensable to understand how magnetostriction affects the magnetization dynamics. We performed micromagnetic simulations in order to clarify the effects of the magnetostriction. To simulate the magnetostriction, we have to solve the elastic equations of the crystal structure.[1,2] The magnetization generates strains of the crystal structure, and deformations of the crystal are affected by the distant magnetization. We solved equations of motions for the strains, and we obtained the magnetostrictive field. We parallelized simulations using Message Passing Interface.[3] Figure 1 shows a simulation model containing two grains. Inside the grains, we consider strip-shape magnetic domains. The crystal axes are rotated -20 and 20 degrees from the x-direction in the grain A and B, respectively. We applied AC magnetic field along the x-direction. The frequency of the AC magnetic field is 100MHz. We also applied static external stress parallel to the crystal axis of the grain A. The magnetic material is Fe. Figure 2 shows energy losses as a function of the external stress using the simulation results. When the tensile strain is 20 MPa, the energy loss is 1.8 times larger than that without stress. The results of this work show that the energy loss strongly depends on the stress and the microstructure of the soft magnetic materials.References: [1] J.X. Zhang, and L.Q. Chen, Acta Materialia 53, 2845 (2005). [2] S. Bhattacharyya, T.W. Heo, K. Chang, and L.-Q. Chen, Modelling Simul. Mater. Sci. Eng. 19 035002 (2011). [3] H. Tsukahara, K. Iwano, C. Mitsumata, T. Ishikawa, K. Ono, Comput. Phys. Commun, 207, 217 (2016).

Effects of magnetostriction on domain wall dynamics inside multi-grains soft magnet revealed by micromagnetic simulations

The modification in magnetic films of the local magnetic properties is a fruitful strategy to achieve or optimize application required functionalities as it was shown on the development of spin waves phase shifters [1] and that of magnetic field sensors [2]. This work focuses on the use of synchrotron nanobeams to explore the possibility of modifying, at length scale of the beam size, the magnetic anisotropy of materials suitable for implementing spin waves guides. Our samples were amorphous Fe80B20 stripes (15 nm thick, 700 µm long and 15 µm wide) that were prepared using UV lithography from films grown by using pulsed laser ablation deposition. Irradiation, at the ID16B-ESRF, was performed by using a 56 nm x 56 nm spot size, an energy maximum at E = 17.5 keV and a flux of 2.21 x 1011 photons/s. Our characterization of the irradiation outcome, Figure 1, revealed that the local coercive force, measured by means of a Kerr effect device at points in between different irradiated regions (IR), in the same stripe and separated by 100 µm, increased with the IR width (varied by scanning in different areas the nanobeam). That increase can be understood by recalling that the reversal mechanisms of our stripes corresponds to the wall propagation/pinning type [3]. The wall involved in the reversal gets pinned when it finds a region at which it lowers its energy (as, for instance, a reduced anisotropy region). The depinning field (that is, the local coercivity) is related both to the local anisotropy decrease and to the domain wall width that is, approximately, 350 nm [3]. When the width of the IR is lower than that of the domain wall the local coercivity can be approximated to the local anisotropy reduction induced by the irradiation (local amorphous relaxation) multiplied by the ratio of the IR width to the wall one. Differently, when the wall is narrower than the IR the coercivity gets almost constant and measures, to a first approach, the difference in anisotropy energy between the irradiated and non-irradiated zones. We conclude about the need of implementing IR widths larger than ca. 500 nm in order to adequately stabilize a propagating wall.References: [1] R. Hertel, W. Wulfhekel, and J. Kirschner, "Domain-wall induced phase shifts in spin waves", Physical Review Letters, vol. 93, no. 25, p. 257202 (2004) [2] Isaac Koh and Lee Josephson, “Magnetic Nanoparticle Sensors”, Sensors, vol. 9, p. 8130-8145 (2009) [3] U. Urdiroz et al., "Antiphase resonance at x-ray irradiated microregions in amorphous Fe80B20 stripes," Journal of Magnetism and Magnetic Materials, https://doi.org/10.1016/j.jmmm.2020.167017

Local Coercivity at X-rays Nanobeam Irradiated Regions in Amorphous Fe80B20 stripes

The interesting magnetic behavior of chemically resistant and biologically inert glass-coated amorphous magnetic microwires has been of enduring interest since the mid-1980’s. However, their response under different mechanical loading conditions, of great interest for numerous sensor applications, has not been thoroughly explored. Here we present data connecting the magnetoelastic response of glass-coated amorphous ferromagnetic microwires with mechanical loading, revealing an exceptional magnetomechanical response. A selection of amorphous glass-coated Fe73Si11B13Nb3 microwire samples (100-110 μm outer diameter, 4 cm in length) were evenly covered with a thin layer of electrically conducting silver paint (Coating 1), electrically insulating nitrocellulose (Coating 2), or were left uncoated. The magnetomechanical response (resonant frequency and amplitude) of the wires was probed in the frequency range 30-100 kHz using a wireless pickup coil set-up of fixed 1.5 V voltage and a modulated current. It was found that the microwire resonant frequency systematically decreased on the order of ~3 kHz/mg, Fig. 1(a), independent of coating type, Fig. 1(b). These data confirm a shift in the magnetoelastic resonant frequency response of microwires that is approximately 100 times greater than that reported for Metglass amorphous magnetic ribbons (ref = Grimes et al.). These findings quantify the lower detection limits of mass loading in glass-coated amorphous magnetic microwires, where microgram differences in mass can be detected wirelessly and with no applied bias field. This exceptional responsiveness to mass loading, along with their small diameter, highlights the promise of magnetic microwires for a variety of sensor applications, including as biosensors, for civil infrastructure monitoring, and for anti-counterfeit measures. Acknowledgements – Fulbright España, I-Link A20074 (CSIC), Spanish Ministry of Science and Innovation RTI2018-095856-B-C21 and Comunidad de Madrid NANOMAGCOST S2018/NMT-4321References: [1] C.A. Grimes, S.C. Roy, S. Rani, Q. Cai, Theory, Instrumentation and Applications of Magnetoelastic Resonance Sensors: A Review, 18 (2011) 2809–2844. doi:10.3390/s110302809.

Exceptional Magnetomechanical Response of Glass-coated Amorphous Microwires

Magnetic Tunnel Junction (MTJ) consisting of two ferromagnetic electrodes separated by thin oxide layer are used as magnetic field sensors in read-write heads as well as in spintronic logic devices. High tunnel magnetoresistance, of the order of 1000 percent is a prerequisite for such applications. Till date highest tunnel magnetoresistance is observed in MTJs consisting of CoFeB as magnetic electrode with thin MgO tunnel barrier. Post-deposition thermal annealing is an important step in which amorphous CoFeB is partially crystallized to form bcc-CoFe phase, resulting in enhancement of TMR by several orders of magnitude. In recent years buffer layers of refractory metals (W, Mo, Hf) have been used to induce perpendicular magnetic anisotropy in CoFeB films [1]. Since in a MTJ multilayer, we would like to obtain depth-resolved information about structural changes occurring in CoFeB layer with temperature. X-ray diffraction understanding wave conditions were used for this purpose. X-ray standing waves are generated using total external reflection (TER) of X-rays by the W, Mo & Hf buffer layer. We used an x-ray waveguide structure: substrate/W(30nm)/CoFeB(25nm)/ W(2nm). Various waveguide modes (TE0, TE1 etc.) can be excited in the multilayer by varying the angle of incidence of x-rays. TE0 and TE1 provide information about the center of sample and both the interfaces, respectively. In this view, GIXRD measurements were performed at PF, KEK, JAPAN, at various grazing angles to see the transformation of amorphous matrix into nano-crystalline phase. Crystallization starts from the center of film. Also, there is one additional peaks present near CoFe(110) peak at the interface. In addition, one can see that the samples have uniaxial magnetic anisotropy at its as-deposited state and show a large increase in the coercivity. Also, 250°C annealed film shows the different behavior at hard axis(figure 1).References: [1] S. Ikeda, K. Miura, H. Yamamoto, K. Mizunuma, H. D. Gan, M. Endo, S. Kanai, J. Hayakawa, F. Matsukura, and H. Ohno, Nature Mater. 9, 721 (2010).

Depth profiling study of magnetic CoFeB thin film

Exotic massless fermions have been predicted in a family of transition metal silicides and germanides, and experiments have provided evidence for these chiral fermions and their associated long Fermi-arc surface states.1,2 Additionally, a recent report has predicted that the topological properties in the electronic structure may be preserved even in the presence of complete structural disorder (e.g. amorphous materials).3 In this talk, we will discuss studies of the magnetism and transport signatures in a series of amorphous transition metal silicide and germanide thin films, MxZ1-x (M=Fe, Co; Z=Si, Ge; x=0.45-0.71). In the amorphous CoxZ1-x thin films, we will show a positive magnetoresistance at low temperature which crosses from a quadratic dependence at low field to a non-saturating linear dependence at high field (up to 14T). We will suggest these results may be an indication of Abrikosov’s quantum magnetoresistance. We will also show that not only do the amorphous thin films of FexZ1-x exhibit Stoner model-type itinerant ferromagnetism over the whole range of x studied, the equiatomic films have a larger moment per Fe than their crystalline counterparts.4,5 In contrast, the CoxZ1-x amorphous thin films only become weakly magnetic at x=0.6 and the moment per Co atom in these films scales non-linearly with Co concentration, unlike in the case of Fe. The origin of this difference between M=Fe, Co as well as the differences between Z=Si,Ge on the ferromagnetic properties will be discussed. Ultimately we show that these amorphous MxZ1-x alloys are highly tunable magnetic materials which have potential for the development of novel magnetic memory technologies. This work was supported primarily by the Department of Energy, Materials Sciences and Engineering Division Contract DE-AC02-05-CH11231 within the LBNL magnetism (NEMM) program, and in part through the Australian Research Council Centre of Excellence in Future Low Energy Electronics Technologies CE170100039 and the Australian Research Council Discovery Project DP200102477, using the Melbourne Centre for Nanofabrication of the Australian National Fabrication Facility.References: 1P. Tang et al., Phys. Rev. Lett. 119, 206402 (2017) 2D. Takane et al., Phys. Rev. Lett. 122, 076402 (2019) 3Y.B. Yang et al., Phys Rev Lett 123 076401 (2019) 4D.S. Bouma et al., Phys Rev B 101 014402 (2020) 5J. Karel et al., in preparation

Magnetism and Transport Signatures in Amorphous Transition Metal Silicide and Transitional Metal Germanide Thin Films

Magnetic core has been widely used in integrated inductor as it can provide a high inductance and reduce the device size due to its high permeability [1]. At the same time, the relatively high loss tangent and saturation current will diminish the performance enhancement in the high frequency and high current applications, respectively [2]. The dilemma has resulted in the investigation of magnetic core materials, among which CoZrTaB demonstrated a low Hk, high resistivity and low loss tangent below 500 MHz, which is compatible with most of the integrated voltage regulators’ working frequency [3]. Here we fabricated CoZrTaB thin films with sputtering on different substrates and characterized them comprehensively. The CoZrTaB thin films have been fabricated in single layer and multi-layer structures (Fig. 1(a)), of which the VSM results, shown in Fig. 2, suggest that the Hk change of the multi-layer structure can be neglected while it can suppress the eddy current at high working frequency. Compared with the continuously sputtered 400nm CoZrTaB thin film, the multi-layer thin film shows a more desirable hysteresis loop with a single domain. The surface roughness of the Si and two kinds polyimide was extracted with the AFM, followed by the VSM characterization to verify the performance degradation. In addition, the material characterization such as XRD and RBS have been conducted to acquire the information of phase and element ratio of the CoZrTaB thin film, as shown in Fig.1 (b)(c). A comparison is made with the previous reported results from Gardner [4] and Koh [5] to see the successful implantation of the CoZrTaB thin film on different substrates.References: [1] Xu, Wei, et al. "Performance enhancement of on-chip inductors with permalloy magnetic rings." IEEE Electron Device Letters 32.1 (2010): 69-71. [2] Bechir, M. H., et al. "Magnetic inductor model which take into account permeability and loss tangent of the magnetic material." 2015 Symposium on Design, Test, Integration and Packaging of MEMS/MOEMS (DTIP). IEEE, 2015. [3] Burton, Edward A., et al. "FIVR—Fully integrated voltage regulators on 4th generation Intel® Core™ SoCs." 2014 IEEE Applied Power Electronics Conference and Exposition-APEC 2014. IEEE, 2014. [4] Gardner, Donald S., et al. "Integrated on-chip inductors with magnetic films." 2006 International Electron Devices Meeting. IEEE, 2006. [5] Koh, Kisik, et al. "High frequency microwave on-chip inductors using increased ferromagnetic resonance frequency of magnetic films." 2015 28th IEEE International Conference on Micro Electro Mechanical Systems (MEMS). IEEE, 2015.

The Improvement of the CoZrTaB Thin Films on Different Substrates for Flexible Device Applications

It is well known that both the anisotropy K and the exchange stiffness A in magnetic materials decrease as the temperature increases [1]. The temperature dependence of these parameters is often expressed as a power law in the reduced magnetization (m), e.g. calculations for Co indicate that the Callen-Callen law K(m)∼ m3 is a very good approximation for the anisotropy, while for the exchange stiffness, A(m) ∼ m1.8 [1]. Since the domain wall width is proportional to the square root of A/K, it increases with temperature, as does the domain wall energy. However, in thin films with an interfacial Dzyaloshinskii-Moriya interaction (DMI), the DMI constant (D) also enters in the expression for the domain wall energy. As the DMI leads to chiral domain walls and skyrmions, determining the temperature dependence of D and hence the domain wall energy is important from both fundamental and applied points of view. We report on our study of multilayers of Pt/ Co68Fe22B10/Ir and Pt/Co68B32/Ir multilayers, deposited by dc magnetron sputtering onto a silicon oxide substrate. Wide-field Kerr microscopy was used to image the domains in the demagnetised state. We measured the domain period in the temperature range from -264 to 17 °C [Fig.1], enabling a calculation of D following the approach of Woo et al [2] as shown in [Fig.2]. In a second study, we deposited the same multilayers onto BaTiO3 (BTO) (100), which undergoes structural phase transitions close to 0 and -100 °C and thus exerts a strain on the multilayers. Images of domains in a [Pt/CoB/Ir]x10 superlattice were obtained using X-ray magnetic circular dichroism - photoemission electron microscopy (XMCD-PEEM). It was found that the domain period increases as the temperature increases as shown in [Fig.1]. However the DMI for all the samples decreases when the temperature increases as shown in [Fig.1].References: [1] Moreno et al., Phys. Rev. B 94, 104433 (2016) [2] Woo et al., Nat. Mater. 15, 501 (2016) [3]Bennett, et al., Scientific reports, 6, p.22708 (2016).

Temperature dependence of the Dzyaloshinskii-Moriya constant in ultrathin Pt/Co(Fe)B/Ir films

A- and B-site ordered quadruple perovskites with the chemical formula AA'3B2B'2O12 can form with a 1:3 ratio at the A site. A unique feature for this specially ordered perovskite is that three different atomic sites (A', B, and B' sites) can all accommodate magnetic transition metals. As a consequence, multiple magnetic interactions can occur at A', B and/or B' sites, giving rise to a series of intriguing physical phenomena. CaCu3Fe2Re2O12 is a good example, which shows the half-metallic electronic structure, large magnetization, and very high Curie temperature [1]. Here we have investigated a series of ferrimagnetic compounds ACu3Fe2Re2O12(A=Ca, Sr, Ba, Pb, Sc, Y, La) by using density functional theory and Monte Carlo simulations. We found that all compounds with A2+ ions exhibit high Curie temperatures (above 405 K), and the compounds with A3+substitution yield even higher Tc (above 502 K). By examining interatomic exchange parameters, we found that the antiferromagnetic exchange couplings between Re and Cu as well as Re and Fe are responsible for this very high Curie temperature. For the compounds with A3+ substitution, an electron doping at the band around the Fermi level dominated by the Re ions strengthen the Re-Cu, Re-Fe and Re-Re exchange interactions, which cause an increase in the critical temperatures. In summary, this work demonstrates a design strategy of enhancing spin ordering temperatures by replacing A-site non-magnetic ions.References: 1. Chen, Wei-tin, Masaichiro Mizumaki, Hayato Seki, Mark S. Senn, Takashi Saito, Daisuke Kan, J. Paul Attfield, and Yuichi Shimakawa. "A half-metallic A-and B-site-ordered quadruple perovskite oxide CaCu3Fe2Re2O12 with large magnetization and a high transition temperature." Nature Communications 5, no. 1 (2014): 1-7.

Electronic structure and magnetism of half-metallic quadruple perovskite ACu3Fe2Re2O12(A=Ca, Sr, Ba, Pb, Sc, Y, La) by first principles theory

Rare-earth orthochromites (RCrO3) with orthorhombically distorted perovskite (ABO3) structure exhibit a wealth of magnetic phenomena such as temperature-induced magnetization reversal (TMR), spin-reorientation (SR), spin-flipping (SF), and exchange-bias (EB). These occur as a result of magnetic interactions among the cations such as Cr3+–Cr3+, Cr3+–R3+ and R3+–R3+, where R is the rare earth element, such as Gd, Sm, Tm [1]. Rare-earth orthochromites also form a class of magnetoelectric multiferroics which exhibit the coexistence of ferroelectric and magnetic orders [1]. Single crystalline GdCrO3, exhibit a giant magnetic entropy change (ΔSm) at a reasonable magnetic field, making it a potential candidate for the application in magnetic refrigeration [2]. TMR and EB have been reported in several RCrO3 compounds due to the competition between the R3+ moment and the canted weak ferromagnetic (FM) component of Cr3+ ions [3]. In the present work, GdCrO4 samples were obtained using sol-gel technique [4]. X-ray diffraction and Raman techniques were used to identify the phase of the samples. Calcination of the samples at 600 °C led to GdCrO4 phase formation [5]. Further calcination of the samples at 1000 °C led to the decomposition of GdCrO4 into GdCrO3. Upon heat treatment, the Cr5+ oxidation state in the GdCrO4-zircon phase reduces to the relatively stable Cr3+ together with oxygen loss to stabilize the GdCrO3 perovskite-structure [5]. The role of thermal decomposition of GdCrO4 to GdCrO3 on crystal structure and magnetic transitions, studied using XRD and vibrating sample magnetometer (VSM), will be discussed. Magnetization measurements as a function of temperature (M-T) with different probing magnetic fields were carried out to locate the various magnetic transitions in the samples under different measurement protocols such as zero field cooled (ZFC), field cool cooling (FCC) and field cool warming (FCW). Anomalies in the M-T curves observed at T ≈ 10 K and T ≈ 170 K correspond to spin - flip and Néel transitions, respectively. This is in agreement with previously reported values [1]. The hysteresis loops measured across the transition temperatures validate the magnetic transitions as observed in the M-T curves.References: [1] S. Mahana, U. Manju and D. Topwal, J. Phys. D: Appl. Phys. 51 (2018) 305002. [2] L. Yin, J. Yang, X. Kan, W. Song, J. Dai and Y. Sun, J. Appl. Phys. 117 (2015)133901. [3] B.B. Dash and S. Ravi, Solid State Sciences 83 (2018) 192. [4] P. Mohanty, A.R.E. Prinsloo, B.P. Doyle, E. Carleschi, C.J. Sheppard, AIP Advances 8 (2018) 056424. [5] A.J. Dossantos-Garcia, E. Climent-Pascual, J.M. Gallardo-Amores, M.G. Rabie, Y. Doi, J. Romero de Paz, B. Beuneu, R. Saez-Puche, Journal of Solid State Chemistry 194 (2012) 119.

Thermal Decomposition of GdCrO4 to GdCrO3: Structure and Magnetism

Magnetization reversal in 1D structures attracts increasing interest due to its connection with the development of novel spintronics, logic devices, actuators and manipulators for nano-sized objects. Amorphous micro-scale objects (stripes, films, rods) are attractive as materials with an extremely high magnetic softness, but difficult to be studied because of amorphous state and macro scale. Magnetic domain structure and magnetization reversal mechanism in amorphous fibers are defined by magnetoelastic energy, which leads to (i) very sensitive tunability of magnetic anisotropy and (ii) unusually fast domain wall propagation when reversing the magnetization. The role of relaxation processes under current annealing and conventional annealing in initially stressed amorphous materials is considered as a part of the complex process involving both magnetostriction constant change and stress components redistribution [1, 2]: a sign of the magnetostriction can be changed through annealing, which leads to the change of a type of magnetic domain structure. Moreover, the relationships between anisotropy constant and characteristics of domain wall dynamics are established: anisotropy value at the fiber axis enters the expressions for domain wall width, length, slope, velocity and mobility, whereas rate of anisotropy radial variation influences only on the length of domain wall [3]. Configuration of the head-to-head domain wall is visualized as a particular solution of Landau-Lifshitz-Gilbert equation. 1D amorphous fibers are considered as prospective magnetic materials suitable for multiferroic applications especially when they are incorporated into piezo-polymer matrices [4]. Due to the sensitivity of soft magnetic materials to low magnetic field, this approach can be used for the design of new self-biased magnetoelectric composites that provide large ME coupling under an external AC magnetic field in the absence of a DC magnetic field.References: 1. K. Chichay, V. Rodionova et al., Journal of Alloys and Compounds 835 (2020) 154843; 2. G. Nematov, I. Baraban et al., Journal of Alloys and Compounds 837 (2020) 155584; 3. M. Vereshchagin, I. Baraban et al., Journal of Magnetism and Magnetic Materials 504 (2020) 166646; 4. A. Amirov, V. Rodionova et al., Materials, 13, 916 (2020).

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Effects of magnetostriction on domain wall dynamics inside multi-grains soft magnet revealed by micromagnetic simulations

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Quantum Spin Nematic Liquid in the S=1 Antiferromagnetic Chain with the Biquadratic Interaction

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