United States

Due to remarkable success in many uses today such as motors in an electric vehicle and memory devices, there have been intensive research interests centered at synthesizing a rare earth (RE)-free permanent magnetic material that has a cheap cost for mass production and various methods to improve a uniaxial magnetic anisotropy (Ku), saturation magnetization (µ0Ms) as well as thermal stability of the previously known materials. RE-free L10 ordered FeNi alloys boast with affordable cost, large µ0Ms and also notable Ku owing to their tetragonal structure but has very low stability and degree of ordering. Herein, through first-principles electronic structure calculations, we have studied possible improvements of the structural stability and magnetic properties of L10-FeNi by an interstitial doping with 2p-electron elements (B, C, and N). It is found that the additions of 12.5 at.% B and N enhance Ku up to 0.9 and 1.8 MJ/m3, respectively, which are 35% and about 3 times larger than that (0.66 MJ/m3) of FeNi. More importantly, unlike the C and N dopants, the B greatly improves the stability and reaches Ku of 2.8 MJ/m3 at 25 at.%. These results demonstrate the feasibility of possible enhancements on the magnetic anisotropy and energy product of 3d-only metals for RE-free permanent magnet applications.

MMM 2020

Improved Stability and Magnetic Anisotropy in L10 -FeNi by Interstitial Doping: A First-Principles Prediction

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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poster

The achievement of quantum error correction is a fundamental step towards the implementation of a scalable platform for quantum computation, in which logical units are made robust against errors. Here we show that magnetic molecules consisting of weakly interacting and individually addressable spins ½ centers are a very promising platform to implement repetition codes for quantum error-correction, where several spins ½ are used to encode an error protected logical qubit. In particular, we demonstrate that these challenging requirements can be fulfilled by the [Er-Ce-Er] molecular trinuclear coordination compound. We show that this complex can be exploited to efficiently implement the three-qubit quantum error correction code protecting against pure dephasing, the most important error in magnetic molecules [1]. The system is characterized by combining magnetometry, low-temperature specific heat and electron paramagnetic resonance measurements on both the trimer and the properly synthesized [LuCeLu] and [ErLaEr] analogues, which contain only one of the two types of magnetic ions. The resulting large and distinct g values, together with weak but non-negligible dipolar interactions, enable us to selectively address different transitions by a proper sequence of microwave pulses, implementing the three-qubit repetition code. The parameters obtained from the experimental characterization are finally used to perform thorough numerical simulations of the system dynamics, including the effect of pure dephasing in a Lindblad formalism. These show a remarkable gain of the quantum error correction procedure, thus proving the efficiency of the device in suppressing pure dephasing.References: [1] E. Macaluso, M. Rubin, D. Aguilà, A. Chiesa, L. Barrios, J. I. Martínez, P. J. Alonso, O. Roubeau, F. Luis, G. Aromí and S. Carretta, submitted.

A Heterometallic [LnLn’Ln] Lanthanide Complex as a Qubit with Embedded Quantum Error Correction

Low-dimensional (d=1,2) metallic systems with electron-hole symmetry are dominated at low temperatures by spin-flip fluctuations and enhanced antiferromagnetic interaction. They show, however, no long-range order at non-zero temperatures. The electronic structure is nevertheless substantially altered by the antiferromagnetic fluctuations and significantly deviates from the Fermi liquid. These changes are difficult to capture by the standard theoretical many-body techniques. We show that only many-body approaches including renormalizations of the interaction strength can successfully describe the low-temperature behavior of low-dimensional metals. We use the standard many-body perturbation expansion within which we resort to the reduced parquet equations introducing a two-particle self-consistency suppressing spurious phase transitions. They were introduced by the authors to describe quantum criticality in strongly correlated electron systems, Refs. [1-3]. We choose the one-dimensional Hubbard model and show that the solution at zero temperature and at half-filling contains an antiferromagnetic quantum critical point even if there is no long-range antiferromagnetic order at non-zero temperatures. Antiferromagnetic fluctuations open an energy gap in the spectral function that is proportional to the bare interaction strength. This behavior can be derived only if the quantum critical point and the renormalization of the interaction strength are treated consistently in both the thermodynamic response and spectral functions. That is, a balance between quantum and thermal fluctuations is maintained and consistency between one-particle and two-particle functions is accomplished.References: [1] V. Janiš, P. Zalom, V. Pokorný, and A. Klíč, Phys. Rev. B 100, 195114 (2019). [2] V. Janiš and A. Klíč, JPS Conference Proceedings 30, 011124 (2020). [3] V. Janiš, A. Klíč, and J. Yan, preprint arXiv:2006.08492 (2020).

Antiferromagnetic Fluctuations in One-Dimensional Hubbard Model

For nearly 100 years the localized-exchange-interaction, as represented by the Heisenberg Hamiltonian H = Σ J(r) Si. Sj, has been viewed as the primary underlying cause of magnetism in magnetic materials. An inescapable consequence of the Heisenberg Hamiltonian is that the magnetic dispersion relation at small k must go as ω∝k2 (for sufficiently short-range J(r)). Empirical evidence over the past 60 years has persistently given indications, however, that the measured dispersion-relation exponents in various ferromagnetic systems were invariably smaller than 2. The empirical evidence thus appears to be in direct conflict with the applicability of the Heisenberg Hamiltonian to explain spin ordering in real ferromagnets. The very first attempt to determine ω(k) at small k, using Spin Wave Resonance (SWR) showed near linear dependence,1 but the belief in the validity of theory was so strong that a way was always found to force agreement (e.g., by renumbering1,2 the resonances so as to obtain the expected ω∝k2 dependence). Such ad hoc renumbering, as well as postulation of magnetization and anisotropy variations within the films, etc., have been used to this day to insist that ω must be ∝k2. Neutron scattering (NS) has not been precise enough until recently to measure ω∝kd at small k. But a recent measurement3 on CrSiTe3 showed that d is indeed <2, despite the authors' attempt to fit the data to ω∝k2. Indirect evidence from precision NMR measurements had previously shown that empirically4 only ω∝ k; k1.5; and k1.75 for 3D ferromagnets, and ∝ k and k1.5 for 2D ferromagnets, appear to characterize simple ferromagnets. These behaviors may be understood as resulting from the exchange interaction being a collective-exchange effect, instead of an interatomic-exchange effect. If d<2, then 2D magnets can order spontaneously (the Mermin-Wagner theorem no longer applies).. This is consonant with the existence of high Tc magnetic monolayers and quasi-2D magnets, no matter the strength of the anisotropy fields. A full replacement model Hamiltonian is yet to be discovered. However, a simple spin-wave scheme can already be formulated from just the small-k approximations and is in excellent agreement with experimental evidence.References: 1. M.H. Seavey and P.E.Tannenwald, Phys Rev Lett 1, 168 (1958); J Appl Phys, 30, S227 (1959) - SWR in permalloy 2. P.K. Schwob and G.E. Everett, J Phys Colloque C1, 1066 (1971). Also, P.K. Schwob et al, PR B 10, 165 (1974) - SWR in EuS - 3. T.J. Williams et al, PR B 92, 144404 (2015) - NS in CrSiTe3 - 4. N. Bykovetz, J Appl Phys 55, 2062 (1984). Please note the obvious typographical error in the abstract, where n=0 should be replaced by n=∞

Is it Time to Sideline the Renowned Heisenberg Hamiltonian?

Ferromagnetic materials have played a significant role in magnetic memory devices. However, due to inherent limitations associated with stray field generation and vulnerability to external stimulation, antiferromagnetic materials are increasingly investigated as alternatives. Specifically, metallic tetragonal antiferromagnets with easy-plane magnetism are appealing because of the degenerate domains with 90° difference of Néel vector for binary information storage and the possibility of electrical switching. To understand the switching process, the magnetocrystalline anisotropy is essential, acting as an energy barrier between two degenerate states. In this study, we used density functional theory (DFT) to unravel the origin of the magnetocrystalline anisotropy in Fe2As, one of the metallic tetragonal antiferromagnets with easy-plane magnetism. The tetragonal structure allows two possible anisotropies out-of-plane and in-plane. Here, we calculate the spin-orbit interaction (SOI) in a DFT framework and the magnetic dipole-dipole interaction (MDD) based on the DFT ground state structure using a classical model. The computed out-of-plane |K1| anisotropy coefficient is 830 kJ/m3, composed to one-third of MDD and two-thirds of SOI, both of which exhibit the same two-fold symmetry. Conversely, the MDD contribution for in-plane anisotropy is almost imperceptible, leading to an in-plane |K22| anisotropy coefficient of 280 J/m3 with four-fold symmetry, due to SOI. The lowest frequency of a spin-wave is calculated using our anisotropy result, and it is predicted as 0.64 THz. Based on the frequency and anisotropy, the fast dynamics and high speed of switching are anticipated. However, low thermal stability might be observed due to the small in-plane anisotropy barrier. ** The Illinois Materials Research Science and Engineering Center is supported by the National Science Foundation MRSEC program under NSF Award Number DMR-1720633.

Ab initio Study of Magnetocrystalline Anisotropy in Antiferromagnetic Fe2As

The physics of the chiral magnet MnSi touches onto several fundamental questions in condensed-matter physics, from the stabilisation of exotic states like chiral skyrmions [1] to the interplay between localised and itinerant magnetism. Under mechanical pressure, or chemical pressure in the form of Fe doping in Mn1-xFexSi, a non-Fermi liquid behaviour sets-in which has been attributed to a chiral spin liquid and quantum fluctuations [2]. The origin and nature of these phenomena are still an open question, which we address by combining small angle neutron scattering and neutron spin echo spectroscopy [3-5]. Our results show that the destabilisation of the long range helical periodicity, close to the quantum critical points, is driven by the modification of the electronic state but with different microscopic mechanisms for mechanical and chemical pressure. Mechanical pressure enhances the itinerant electron character of MnSi leading to a softening of the magnetic moment. On the other hand, chemical doping increases the weight of achiral RKKY interactions. The resulting frustration explains both the destabilisation of long range helical periodicity and the enhancement of the precursor region with increasing doping.References: 1. S. Mühlbauer et al., Science 323, 915 (2009). 2. C. Pfleiderer, et al., Nature 414, 427 (2001) 3. L. J. Bannenberg et al., Phys. Rev B 100, 054447 (2019). 4. L. J. Bannenberg, et al., Phys. Rev. B 98, 184431 (2018). 5. C. Pappas, et al., in preparation

Helimagnetic correlations close to the Quantum Critical Points of MnSi under mechanical and chemical pressure. INVITED

Magnetic navigation systems (MNSs) capable of generating various types of magnetic fields have been widely studied for the effective manipulation of biomedical magnetic robots [1-4]. Previous researchers proposed a geometrically and electrically efficient MNS comprised of a simple triad of electromagnetic coils (TEC) that can generate two-dimensional (2D) magnetic robot motions [3]. However, the TEC suffered from the restricted working area of the magnetic robot due to the nonlinearly distributed magnetic field throughout the system. In this research, we propose a method to precisely generate 2D magnetic torque and force of a magnetic robot regarding the robot's current position inside the TEC. Since the TEC is composed of three identical circular coils located at the vertices of an equilateral triangle, the magnetic field at a certain position inside the TEC can be expressed in terms of the three coils' currents and a position vector by using Jacobian and transformation matrices [4]. From this expression, we established several constraint equations to optimally manipulate the magnetic robot’s 2D motions at any position within the TEC. Fig. 1 shows several simulated magnetic fields of the TEC to propel a magnetic robot (red dots) in the direction of the x-axis. It shows that the TEC can generate a relatively uniform magnetic force within the nearby area of a magnetic robot, making it possible to move the magnetic robot in the desired direction (Fig. 2). We then constructed the TEC and a closed-loop visual tracking system to demonstrate that the TEC can manipulate a magnetic robot inside the TEC in a closed-loop manner. The results showed that the proposed method and system can improve the magnetic robot’s admissible working area in the TEC effectively and precisely.References: [1] M. Kummer, J. Abbott, and B. E. Kratochvil et al., IEEE Transactions on Robotics, Vol. 26, pp. 1006-1017, 2010. [2] Q. Cao, X. Han, B. Zhang, and L. Li et al., IEEE Transactions on Applied Superconductivity, Vol. 22, 2012. [3] H. Lee and S. Jeon, AIP Advances. Vol. 10, 2020. [4] G. Go, H. Choi, and S. Jeong et al., Sensors and Actuators, Vol. 205, P. 215-223, 2014.

Development of a Position-Based Precise Magnetic Torque and Force Generation Method Using a Triad of Electromagnetic Coils for Biomedical Magnetic Robot Applications

The structural and magnetic properties Fe1-xPtx nanoparticles are highly dependent on the composition x, which can be tailored to suit potential applications such as ultrahigh density storage media, biomedicine and catalysis.[1, 2] Most of the studies so far have been focused on equiatomic Fe-Pt with the highly anisotropic L10 structure. In bulk, FePt3 in the L12 structure is paramagnetic at room temperature and shows two coexisting antiferromagnetic transitions at TN1~160 K and TN2~120 K. [3] Recently, L10 FePt nanoparticles have been chemically synthesized through a halide mediated route without requiring any post annealing. [4, 5]. In this work, we studied the effect of elemental iodine as our halide intermediary in the synthesis of FePt nanoparticles using a co-reduction of Fe(acac)3 and (NH4)2PtCl2 with 1,2-hexadecanediol in trioctylamine and oleylamine. Our study showed that the elemental iodine facilitated primarily the formation of FePt3. When iodine was not used, the as-made nanoparticles had mostly the disordered fcc in structure (Figure 1). Annealing all of the as-made nanoparticles led to an increased particle size and transformation to the L12 ordered structure. The longer the annealing time, the greater the atomic ordering (Figure 1). Thermomagnetic data showed that the magnetic properties depend strongly on the degree of atomic ordering. The as-made particles with the disordered fcc structure are ferromagnetic with an ordering temperature of 380 K. The samples annealed at 700°C for 30 minutes showed a lower ordering temperature of ~250 K and another magnetic transition at 135 K possibly due to an antiferromagnetic structure. Room temperature hysteresis loops showed that the coercivity of our samples increased with annealing at 700°C up to 0.23 kOe. Future work is focused on finding the optimum conditions to obtain a highly ordered and monodispersed L12 FePt3 nanoparticles without the need for any additional heat treatment. This work was supported by DOE Grant FG02-90ER45413.References: [1] Sun, S., Adv. Mater., 18, 393 (2006) [2] Zhu, K., Ju, Y., Yang, Z., Acc. Chem. Res., 51, 404-413 (2018) [3] A.T. Heitsch, D.C. Lee, B.A. Korgel, J. Phys. Chem. C 114, 2512–2518 (2010) [4] W. Lei et al., Nano Lett., 18, 7839-7844 (2018) [5] W. Lei et al., Nanoscale, 9, 12855 (2017)

Structural and Magnetic Properties of Iodide-Mediated Chemically Synthesized FePt3 Nanoparticles

The magnetic properties of hexaferrite nanoparticles critically depend on the intrinsic anisotropy induced by its size as well as the morphology. This study demonstrates the controllable growth of barium hexaferrite (BaFe12O19) platelets using a salt-assisted sol-gel method. We employed salts like KBr, KCl, KI, and K2CO3 as a matrix to assist the formation of BaFe12O19 nanoplatelets from its precursor mixture gamma-Fe2O3 and BaCO3. Within the detection limit of the x-ray diffraction technique, pure barium hexaferrite phases are obtained through the salt-assisted sol-gel process. The reaction of pre-calcined precursors in the presence of potassium-based salts favors a template mechanism, resulting in platelet-shaped barium hexaferrite (fig 1). The salt matrix acts as a barrier, preventing possible particle coarsening at high-temperature treatments and promotes the evolution of the hard magnetic phase. The width and thickness of the plates decrease with the addition of high melting point potassium halide salts. The magnetization and coercivity at 300 K of the barium hexaferrite particles were also systematically analyzed as a function of the dimension of platelets. Barium hexaferrite platelets of 0.20 μm width and 0.07 μm thickness yielded coercivity of the order of 4.6 kOe and saturation magnetization, close to 71 emu/g. Plate-shaped hexaferrite particles could be stacked and aligned by applying an external magnetic field and pressure, which could result in high-performance bulk hexaferrite magnets.References: [1] W. Yongfei, L. Qiaoling, Z. Cunrui, and J. Hongxia, J. Alloys Compd. Vol.467, p.284 (2009). [2] A. Z. Eikeland, M. Stingaciu, A. H. Mamakhel, M. Saura-Múzquiz, and M. Christensen, Sci. Rep. Vol.8, p.7325 (2018).

Size-Dependent Magnetic Properties of Barium Hexaferrite Platelets Synthesized Using a Salt Assisted Sol-Gel Technique

GdMn2 is a member of a series of Laves phase containing a rare-earth element and a magnetic 3d-transition metal with very peculiar magnetic properties[1]. Doping with a non-magnetic element such as indium affects these properties[2,3]. GdMnIn is reported to crystalize in the hexagonal MgNi2-type structure presenting a spin-glass behavior with no magnetic order attributed to the triangular spin frustration of magnetic ions[3]. The observed absence of long-range interactions by magnetization measurements along with the almost impossible measurements with neutron diffraction due to the presence of Gd with very high neutron absorption cross section makes the investigation of local exchange interactions in this compound very difficult. In the present work, measurements of hyperfine interactions at In sites using 111In(111Cd) probe nuclei were carried out by perturbed angular correlations (PAC) technique to investigate the local magnetic exchange in GdMnIn compound. Results displayed in Fig. 1 for the behavior of the major component (Vzz) of the electric field gradient (efg) tensor and the distribution of electric quadrupole frequency (δ) show a strong instability of the electronic environment of In sites when temperature decreases indicating a Mn-In disorder. The weak magnetic hyperfine field at In sites also shown in Fig.1 with an anomalous temperature dependence below around 140 K along with the increase in the angle between Bhf and Vzz directions suggest a weak long-range exchange interaction.References: [1] K. Krop, Physica B 319, 9–16 (2002). [2] S.K. Dhar, C. Mitra, P. Manfrinetti, R. Palenzona, and A. Palenzona, J. Phase Equilibria 23, 79-82 (2002). [3] S. De Negri, D. Kaczorowski, A. Grytsiv, E. Alleno, M. Giovannini, R. Gorzelniak, P. Rogl, C. Godart, A. Saccone, and R. Ferro, J. Alloys Compounds 365, 58–67 (2004).

Local inspection of magnetic properties in GdMnIn by measuring hyperfine interactions

Herein, employing first-principles prediction and rigid-band analysis, we have demonstrated an extremely large uniaxial magnetic anisotropy (Ku) up to 3 MJ m−3 in rare-earth (RE) free magnet α''-phase Fe16N2 by replacing Fe with more valence electron elements, Co to Zn in the periodic table, which is more than 60% of Ku (4.9 MJ m−3) attained for RE-included permanent magnet Nd2Fe14B, while improving thermal stability. Such a supreme Ku can be attributed to the mutual mechanisms of the Jahn-Teller orbital splitting and excess electron-induced energy level changes in the rigid-band selection rule. Moreover, we reveal that the replacement by Ti in addition to the above replacements can improve the thermal stability further by an order of magnitude in terms of the formation enthalpy without much suppressing Ku. These results provide an instructive guideline for simultaneous improvements of the thermal stability and energy product in 3d-only permanent magnets without RE or heavy-metal elements. Keywords: Rare-earth free permanent magnets, First-principle calculations, Uniaxial magnetic anisotropy E-mail: ochirkhuyag.t@inu.ac.kr , *schong@ulsan.ac.kr , †odkhuu@inu.ac.kr This work is supported by Future Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2016M3D1A1027835) and by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korean government (MOTIE) (20192010106850, development of magnetic materials for IE4 class motor).

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