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Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, Co2MnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales &lt; 10 fs. Using ultrafast high harmonic pulses to simultaneously and independently probe the magnetic state of two elements during laser excitation, we find that the magnetization of Co is enhanced, while that of Mn rapidly quenches. Density functional theory calculations show that the optical excitation directly transfers spin from one magnetic sublattice to another through preferred spin-polarized excitation pathways. This direct manipulation of spins via light provides a path toward spintronic devices that can operate on few-femtosecond or faster time scales.

MMM 2020

Direct light–induced spin transfer between different elements in a spintronic Heusler material via femtosecond laser excitation INVITED

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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Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, Co2MnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs. Using ultrafast high harmonic pulses to simultaneously and independently probe the magnetic state of two elements during laser excitation, we find that the magnetization of Co is enhanced, while that of Mn rapidly quenches. Density functional theory calculations show that the optical excitation directly transfers spin from one magnetic sublattice to another through preferred spin-polarized excitation pathways. This direct manipulation of spins via light provides a path toward spintronic devices that can operate on few-femtosecond or faster time scales.

technical paper

Mn2RuxGa (MRG) is a half-metallic compensated ferrimagnet crystallising in a cubic inverse Heusler structure (XA) with a substrate-induced biaxial strain of about 1% leading to perpendicular magnetic anisotropy of the net moment. The Mn atoms occupy two different crystallographic sites, Wyckoff positions 4a and 4c. [1] From band structure calculations we find that the states originating from the Mn4c sites dominate the transport. Anomalous Hall effect (AHE) resistance is proportional to the z-component of the magnetisation of the Mn4c sublattice. [2] The AHE measurements show loops with high remanence and only one magnetic phase, with coercivity diverging close to compensation. SQUID magnetometry measures the net moment, i.e. the sum of Mn4a and Mn4c sublattice moments. SQUID-measured magnetisation, in the same geometry as AHE, exhibits a combination of an apparent soft magnetic response in addition to a component with the coercivity observed by AHE. We infer that the net magnetic moment is canted due to non-collinearity of the sublattice moments. Our DFT calculations suggest that the non-collinearity may be due to competing exchange on the Mn4c sites as bulk antisymmetric exchange averages to zero in the -43m point group [3]. The Mn4c sublattice and net magnetisations differ by an order of magnitude, so a small canting of the Mn4c moment can result in a large canting of the net moment. X-ray magnetic circular dichroism measurements were performed to map sublattice magnetisations in the z-x plane. Both sublattices can be distinguished by L-edge absorption due to charge-transfer separation of the Mn absorption edges at the two sites by ≈ 1 eV. [2] Analysis of the mz-mx moments shows that they are indeed non-collinear (Fig.1). From balancing of torques, anisotropy fields at the Mn4a and Mn4c sublattices were found to be easy-plane -1.8 T and easy-axis 3 T, respectively (Fig.2.).References: [1] H. Kurt, K. Rode, P. Stamenov, et al., “Cubic Mn2Ga thin films: crossing the spin gap with ruthenium”, Phys. Rev. Lett., 112, p. 27201, 2014. [2] D. Betto, N. Thiyagarajah, Y.-C. Lau, et al., “Site-specific magnetism of half-metallic Mn2RuxGa thin films determined by x-ray absorption spectroscopy”, Phys. Rev. B, 91, p. 094410, 2015. [3] O. Meshcheriakova, S. Chadov, A.K. Nayak, et al. "Large Noncollinearity and Spin Reorientation in the Novel Mn2RhSn Heusler Magnet", Phys. Rev. Lett. 113, p. 087203, 2014.

Investigation of non-collinearity in Mn2RuxGa compensated ferrimagnetic half-metallic thin films

Co2- based intermetallic Heusler alloys are among the most attractive half-metallic systems due to their high Curie temperatures, high spin polarization and the structural similarity to binary semiconductors [1,2]. The Co2FeGe system is one such candidate of interest for spintronic applications, but experimentally it does not form a single phase in bulk form [3,4,5]. In this work, we have introduced Cr doping to stabilize the Co2FeGe system, and examined the structural, magnetic, transport, and mechanical properties of quaternary Heusler alloys Co2-xCrxFeGe with 0 ≤ x ≤ 1, both experimentally and theoretically. Single phase microstructures are observed for Cr compositions from x = 0.25 to x = 1. The samples with Cr concentrations below x = 0.25 are multi-phase. XRD patterns at room temperature show the presence of ordered Y structure (space group F-43m, # 216) for all single-phase samples. The low-temperature saturation magnetic moments agree fairly well with our theoretical results and also obey the Slater-Pauling rule, a noted prerequisite for half metallicity. The Density functional theory calculations performed using VASP code with projector augmented wave method (PAW) and the Perdew-Burke-Enzerhof (PBE) functional predict half-metallic character in the alloys after Cr substitution. All alloys are observed to have high Curie temperatures, and show a linear dependence with the saturation magnetic moment which is expected in half metallic Co-based Heusler alloys [6]. Transport measurements were performed to explain the electronic structure of the alloys. High mechanical hardness values are also observed which makes these materials suitable for industrial applications requiring repetitive thermal cycling and resist cracking from vibrations.References: 1. I. Galanakis, P. Dederichs, and N. Papanikolaou, Physical Review B 66, 174429 (2002). 2. C. Felser, G. H. Fecher, and B. Balke, Angewandte Chemie International Edition 46, 668(2007). 3. K. R. Kumar, K. K. Bharathi, J. A. Chelvane, IEEE Transactionson Magnetics 45, 3997 (2009). 4. S. KC, R. Mahat, P. LeClair, Phys. Rev. Materials 3 (2019) 114406. 5. R. Mahat, S. KC, D. Wines, P. LeClair, Bulletin of the American Physical Society (2020). 6. G. H. Fecher, H. C. Kandpal, S. Wurmehl, C. Felser, Journal of applied Physics 99, 08J106 (2006).

Possible Half-Metallic Behavior of Co2-xCrxFeGe Heusler Alloys: Theory and Experiment

The current density required for current induced magnetization switching in magnetic devices such as Magnetoresistive Random Access Memory (MRAM) is proportional to Gilbert damping constant. The lower damping would enable more energy-efficient excitations and thus less current needed. The Gilbert damping constant of the Co2FeAl film, a half-metal material important for spintronics with its 100% spin polarization at Fermi level, has shown the lowest Gilbert damping constant among the Heusler alloys. However, the increased Gilbert damping constant in ultra-thin Co2FeAl films is undesirable for low power consumption applications such as STT-MRAM. Being able to manipulate the Gilbert damping on demand is crucial for spintronic device engineering and optimization. Here, we report that the Gilbert damping of ultra-thin Co2FeAl1+x films of nanometer thicknesses can be effectively tuned by delicately controlling the stoichiometric ratio during the growth. The Gilbert damping has been found to be the lowest of 0.065 in Co2FeAl1+0.1, which is deduced by ~50% compared to that in Co2FeAl. We have further found that the damping constant of the ultra-thin Co2FeAl1+0.1 film is restored to the value of 0.062 of the nominal stoichiometric Co2FeAl by compensating the Al composition-deficiency- as supported by the 10.37% of composition change from the scanning transmission electron microscope energy-dispersive-spectroscopy. This work offers a unique path to manipulate the Gilbert damping constant in ultra-thin Co2FeAl films by Al concentration control.

Manipulation of Gilbert damping in ultrathin half-metallic Co2FeAl1+x by composition-deficiency-compensation

While the half-metallic Heusler alloys are considered ideal materials to be used in magnetic tunnel junctions, spin-filters, and spin valves, the search for new candidate half-metal remains an active field of research [1]. One of the ways of rational material design is by doping, which is useful not only to tailor the electric and magnetic properties but also to stabilize a single-phase compound [2, 3]. In this work, we show how the introduction of Mn helps to stabilize a single-phase compound and to tune half-metallic character in the Co2FeGe alloy, which otherwise is a multi-phased normal ferromagnet. We have investigated three substitutional series viz; (Co2-αMnα)FeGe, (Co2-αFeα)MnGe, Co2(FeαMn1-α)Ge, that can be generated from the intermixing of Mn, Fe, and Co by keeping the Ge content constant in the Co2FeGe alloy. These series cover all possible site doping that can be made for a magnetic atom in a full Heusler alloy and allow us to directly compare their magnetic and electric properties. First principles calculations performed using the generalized gradient approximation (GGA) predict that a half-metal is obtained in Co2(FeαMn1-α)Ge series while the other two series generate “near half-metallic” alloys. The experimental investigation of bulk samples of the (Co2-αMnα)FeGe series shows that a single-phase compound can be achieved up to α = 1.25. For all the single-phase compounds, the magnetic moment agrees reasonably well with the Slater-Pauling moment and a very high Curie temperature (~ 1000 K) is measured for low α. The experimental investigation of other series is currently underway; however, the preliminary results show that these series also generate single-phase compounds. Hence by doping Mn, Fe, and Co for one another, many single-phase compounds can be designed from Co2FeGe, with potential half-metallic behavior that can have actual use in spintronic devicesReferences: 1. Z. Bai, L. Shen, G. Han, Spin, Vol. 02, No. 04, 1230006 (2012) 2. R. Umetsu, K. Kobayashi, A. Fujita, Phys. Rev. B, 72, 214412 (2005) 3. S. KC, R. Mahat, S. Regmi, Phys. Rev. Materials, 03, 114406 (2019)

Interplay Between Mn, Fe, and Co in the Co2FeGe Alloy to Design Novel Singe-Phase Compounds with Potential Spintronic Application

The ferromagnetic Heusler compound Co2MnGa is a promising Weyl semimetal with the Fermi energy in the vicinity of the Weyl nodes. Bulk Co2MnGa recently attracted attention because of an exceptionally large anomalous Nernst effect [1,2] and exotic surface states [3]. Simultaneously, Co2MnGa thin films were successfully prepared and showed interesting transport properties [4]. Beside others, the non-trivial topology of the band structure of Weyl semimetals leads to unexpected magneto-thermoelectic transport phenomena which will be discussed in this talk. We report on our observation of a record large anomalous Nernst coefficient in Co2MnGa thin films - up to -3µV/K [5, 6], and discuss the procedure for the quantitative determination of the anomalous Nernst coefficient. Several samples with comparable saturated magnetization were studied, yielding significantly different anomalous Nernst responses. We conclude that the microscopic origin of the anomalous Nernst effect in Co2MnGa is complex and contains contributions from the intrinsic Berry phase and surface states. We further employ a series of Co2MnGa thin films to study the validity of the Mott relation by measuring all four transport coefficients - the longitudinal resistivity, anomalous Hall, Seebeck and anomalous Nernst coefficients [6]. We show that the measured anomalous Nernst signal can be connected to the remaining three magneto-thermal transport coefficients in the whole sample series. This is strong evidence that the Mott relation holds also in Weyl semimetals, where the intrinsic Berry curvature dominates the transport. In the last part of the talk we focus on another magneto-transport phenomena and its thermal counterpart – anisotropic magnetoresistance and anisotropic magneto-thermopower. We show that due to high epitaxial quality of the Co2MnGa films both non-crystalline and crystalline contributions to the anisotropic magnetoresistance can be measured. Interestingly, we do not observe the same crystalline contributions in the magneto-thermopower measurements [7].References: [1] S. N. Guin et al., NPG Asia Materials 11, 16 (2019) [2] A. Sakai et al., Nat. Phys. 13, 1119-1124 (2018) [3] I. Belopolski et al., Science 365, 1278-1281 (2019) [4] A. Markou et al., PRB 100, 054422 (2019) [5] H. Reichlova et al., APL 113, 212405 (2018) [6] G. H. Park, H.R. et al. PRB 101, 060406(R) (2020) [7] P. Ritzinger, H.R. et al., in preparation

Magneto-Thermal Transport in Weyl Semimetal Co2MnGa Thin Films INVITED

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).

First-Principles Prediction of the Enhanced Uniaxial Magnetic Anisotropy and Thermal Stability in α''-Fe16N2

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.

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

Glass-ceramic (GC) materials have formability advantages of glasses controlled crystallization of functional ceramic phases. Here, we obtain GCs containing the hard magnetic phases Ba- or Sr-hexaferrite from a borate glass. Twelve compositions were explored, varying B2O3 and Ba/Fe or Sr/Fe ratio. Selected compositions were heat treated from 30○C to 700-900○C. Resulting phases were identified using X-ray diffraction (XRD) as α-Fe2O3 plus SrB2O4 and SrFe12O19 or their Ba equivalents. Vibrating sample magnetometry (VSM) also identified Fe3O4. The best compositions for hexaferrite GCs contained 40-42 mol% B2O3 and Fe/(Sr,Ba) ratios of 0.5-1. Heat treatments for one Sr glass were performed at 625○C or 675○C to assess phase development at the peak crystallization temperatures determined by thermal analysis, but both treatments yielded only SrB2O4 by XRD; however, coercivity increased from the quenched glass (395 Oe) to 625○C (460 Oe) to 675○C treatment (520 Oe). Selected glasses were studied with in-situ crystallization, measuring magnetic properties during heating to 800○C in the VSM. Hysteresis measurements on initial heating showed predominantly paramagnetism. After cooling and reheating, wasp-waisted loops were observed with Hc > 650 Oe, dropping to 0 at 650○C, with changes occurring 290○C, 490○C (TC of SrFe12O19) and 550○C (TC of Fe3O4 suggesting oxidation despite Ar heating gas). First order reversal curve (FORC) measurements confirmed low and high coercivity phases. These results suggest that crystallization of magnetic phases is most significant on cooling, and that this glass might allow alignment of the anisotropic hexaferrite crystals while heating and cooling with an applied field.

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Direct light–induced spin transfer between different elements in a spintronic Heusler material via femtosecond laser excitation INVITED

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Investigation of non-collinearity in Mn2RuxGa compensated ferrimagnetic half-metallic thin films

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