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Magnetite, Fe3O4, is a frequently studied magnetic oxide growing in the inverse spinel structure Fe3O4 exhibits a ferrimagnetic ground state which stems from the interplay of its three cation species due to super exchange and double exchange depending on site and oxidation state: Octahedrally coordinated Fe2+ and Fe3+ ions, and tetrahedrally coordinated Fe3+ ions. The coupling among octahedral sites is ferromagnetic, while tetrahedral and octahedral sites couple antiferromagnetically. One of the most successful ways to discriminate between the magnetic contributions of these cations are X-Ray Magnetic Circular Dichroism (XMCD) experiments across the Fe L2,3 edges, making use of a slight difference of their L edge energies and the easily resolvable antiferromagnetic coupling between the tetrahedral and the octahedral sites (c.f. Fig. 1).On the other side, X-Ray Resonant Magnetic Reflectivity(XRMR) is a technique combining the depth resolution of X-Ray Reflectivity and the site- and magnetism-sensitivity of XMCD. This enables us to determine the magnetooptical depth profiles at the energies characteristic for Fe2+oct, Fe3+tet, and Fe3+oct in the XMCD of Fe3O4/MgO(100) ultrathin films (c.f. Fig. 2). We find a ~3.9Å layer of enhanced magnetooptical absorption at the surface for both Fe3+ species but not for Fe2+ [1]. The magnetically enhanced Fe3+tet layer is additionally shifted about 3±1.5 Å into the sample compared to the Fe3+oct layer. We attribute this to the first unit cell from the surface containing an excess to Fe3+ cations.References: [1] T. Pohlmann et al., arXiv:2005.01657 [2] S. Macke and E. Goering, J. Phys.: Cond. Matter 26, 363201 (2014).

MMM 2020

Cation-Specific Magnetic Depth Profiles of Ultrathin Fe3O4 Films Obtained by X-Ray Resonant Magnetic Reflectivity (XRMR)

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High-frequency ferrite ceramics exhibiting high permeability and low magnetic loss have been recently attracting more and more attention owing to the rapid development of modern communication technologies.1-3 It is known that the magnetic performance of ferrites is strongly associated with the morphology of their polycrystalline structure.4 During the final-stage sintering, densification is typically accompanied by rapid grain growth.5 In this work, we focus on the control of grain growth and densification process for planar Co-Ti doped M-type barium hexaferrites, BaCo1.2Ti1.2Fe9.6O19, by one-step sintering (OSS) and two-step sintering (TSS) techniques. Experimental results in Fig. 1. indicate that the microstructure of the samples prepared by TSS shows visibly finer and more uniformity compared to that of the samples prepared by conventional OSS, evidence in that the grain growth during the second-step sintering of TSS is successfully suppressed while the density continues to increase. More importantly, the TSS technique shifts the resonant frequency to a higher value as shown in Fig. 2. In addition, the uniformity of the microstructure contributes to a narrower resonant peak. The reshaping of the magnetic spectra leads to a significant reduction of magnetic loss below 300 MHz. The ferrites prepared by TSS demonstrate high permeability (μ' = 18-20), low magnetic loss (tan δm = 0.1-0.3), and high Snoek's product (>25 GHz) in the frequency range of 100-400 MHz. By fitting experimental data, we have determined that low magnetic loss is derived from the small damping coefficient of spin rotation in terms of Kittel's theory. Therefore, the TSS technique provides an effective and efficient approach to prepare planar BaM hexaferrite materials for ultra-high frequency (UHF) communication devices requiring low loss and high Snoek's product.References: 1V. G. Harris, Z. Chen, Y. Chen et al., J. Appl. Phys., Vol. 99, p. 08M911 (2006). 2V. G. Harris, A. Geiler, Y. Chen et al., J. Magn. Magn. Mater., Vol. 321, p. 2035 (2009). 3V. G. Harris, IEEE Trans. Magn., Vol. 48, p. 1075 (2012). 4Q. Li, Y. Chen, and V. G. Harris, J. Magn. Magn. Mater., Vol. 453, p. 44 (2018). 5I. W. Chen and X. H. Wang, Nature, Vol. 404, p. 168 (2000).

Permeability Spectra of Planar M-type Barium Hexaferrites with High Snoek’s Product by Two-Step Sintering

Hexagonal ferrite materials such as BaFe12O19 and SrFe12O19 have strong anisotropic magnetic field and strong remnant magnetism. These properties enable the working frequency of devices such as phase shifter, isolator and circulator, move up to tens of GHz without a strong external bias field and even achieve self-biasing. Other features such as large saturation magnetization, large anisotropy, and low dielectric loss and most importantly, its potential of achieving self-bias, paves the way to fabrication of planar ferrite device that can play a crucial role in a next generation wireless system. The advantage of ferrite devices are their low insertion loss, high isolation, broad bandwidth and high power handling ability compared to their active counterparts. If the fabrication process of aforementioned devices can be integrated into the mature CMOS process flow as an option, it will gain great competiveness as regards the cost. In this work, thin film ferrite material was deposited by employing spin-casting method [Liu 2013] and patterned with the help of Chemical-Mechanical Polishing (CMP). The spin-casting is a low-temperature process: the nano-sized barium ferrite materials can be processed into composite and spin-casted into thin film layer. This method requires only 120°C baking under external biasing filed. In this research, we present the design, simulation, fabrication and measured results of a self-bias micro-strip line Barium hexagonal Nano-ferrite (BaM) circulator on silicon wafer as Fig. 1. This planar Y-junction circulator is 2mm by 2mm by 0.5mm in size, which is capable of future integration with the top three layers of 180nm CMOS technology. Ferrite thin film is deposited and patterned employing composite spin-casting method. Typical characterization techniques are employed together with free-space quasi-optical spectrometry to study complex permittivity and permeability of deposited film up to 120GHz. S parameters of fabricated circulators are characterized by a set of on wafer probes up to 67GHz as Fig. 2. We observed over 15dB non-reciprocal phenomenon at 55GHz.References: Liu C, Sholiyi O, Afsar M N and Williams J D (2013), “Characterization of micro-structured ferrite materials: course and fine barium, and photoresist composite,” Magnetic, IEEE Transactions on, vol. 49, pp.4319-4322, July 2013.

Hexagonal Nano-ferrites used on a V-band Self-bias On-chip Circulator for CMOS

The present work reports the synthesis of Fe3O4 nanotubes (NTs), nanorods (NRs), and nanodiscs (NDs) prepared by microwave-hydrothermal route with varying ratio of sodium phosphate/sodium sulfate ions. The Rietveld refinement analysis of the X-ray diffraction patterns divulges the presence of a metallic iron phase decreasing gradually from NTs ~16 %, NRs ~11 % to NDs ~ 0% with increasing concentration of phosphate ions as confirmed later by Mossbauer data. A sharp drop in the coercive field from NTs (~252 Oe) to NDs (~182 Oe) indicates clearly a magnetic vortex state in NDs as also reported by Lorenz microscopy and micromagnetic simulation [1]. Further, a reduction in Verwey transition temperature (NTs to NDs) is observed in zero fields cooled magnetization measurement (Figure 1(a)) related to a gradual loss of stoichiometry for Fe3O4 nanostructures. The obtained results are understood based upon a core-shell structure consist of stoichiometric Fe3O4 surrounded by a non-stoichiometric one. The magnetic vortex NDs are further analyzed for their utilization in magnetic hyperthermia applications [2,3]. The specific absorption rate (SAR) for NDs is calculated by orientation-dependent hysteresis loss through micromagnetic simulation and found to be 16 % higher at θ = 15o as compared to randomly oriented NDs, where q is the angle between magnetization (M) and applied field (H). Interestingly, the switching field (HS) of magnetic vortex NDs is responsible for a larger hysteresis loss at θ = 15o which is understood by developing a relationship with anisotropy constant (K). The theoretical SAR (~ 182 W/gNPs) of NDs is almost constant for aspect ratio β( = t/d) ≤ 0.13 whereas it is dramatically enhanced by ~5 times (~ 862 W/gNPs) at β = ~ 0.26, which is assigned due to the contribution of shape anisotropy. Our results indicate the implication of switching field (HS), orientation, anisotropy (K), and geometrical parameters (d & t) for improving the heating performance of Fe3O4 nanodiscs.References: 1. H. M. Fan, J. B. Yi, Y. Yang. ACS Nano 3:2798–2808 (2009). DOI: 10.1021/nn9006797 2 Y. Yang, X. Liu, and Y. Lv, Adv Funct Mater 25:812–820(2015) . DOI: 10.1002/adfm.201402764 3. D. H. Kim, E.A. Rozhkova, and I. V. Ulasov. Nat Mater 9:165–171(2010). DOI: 10.1038/nmat2591

Switching Field, Orientation and Shape Anisotropy Contribution on the Magnetic Heating of Fe3O4 Nanodisc

With the development of AC/DC UHV grid, large capacity transformer is widely used in power grid. After DC resistance measurement, no-load test and other operations of power transformer, mainly due to hysteresis phenomenon of ferromagnetic materials, a certain magnetic flux is left in the core, which is called residual flux. When transformer switching on without load, residual flux will lead to inrush current which is several times of the rated current. Inrush current endangers the mechanical stability and insulation strength of power transformer windings, and affects the normal operation of power system, resulting in many adverse effects. In this paper, an improved method is proposed to establish the relationship between residual flux and transient current characteristics by analyzing the transient current waveform of winding under different residual flux with different polarity DC voltage. DC voltage amplitude is determined by a criterion that the residual flux in the core should not change over 10% after the DC voltage unloaded. Based on the previous studies on positive and negative transient current, the relationship between transient characteristics and residual flux is further studied and analyzed. Combined with theory and experiment, the form of empirical formula and parameter calculation flow are determined. Compared with directly using transient current amplitude at a certain moment to calculate, using waveform characteristics to calculate residual flux is more accurate and less susceptible to measurement error and noise.References: C. Huo, Y. Wang, S. Wu, Y. Yang, and Z. Zhao, "Residual Flux Density Measurement Method for Transformer Core Considering Relative Differential Permeability," IEEE Trans. Magn., pp. 1-1, 2020. G. Wenqi, W. Youhua, Z. Zhenghan, Y. Xiaoguang, and L. Yongjian, "Residual Flux in the Closed Magnetic Core of a Power Transformer," IEEE Trans. Appl. Supercond., vol. 24, no. 3, pp. 1-4, 2014. W. Ge, J. Zhao, and Y. Wang, "Analysis of the residual flux influence on inrush current and electromagnetic force in large power transformer," The Journal of Engineering, vol. 2019, no. 16, pp. 2426-2429, 2019.

Improved Residual Flux Measurement Method based on Transient Current Characteristics used in Single-Phase Power Transformer

Spintronic with garnets materials is an emerging field that promises the use of pure spin currents to realize low power electronics thanks to the insulating character and low Gilbert dampings of this family of materials. The recent demonstration of the possibility to control the magnetization dynamics with a DC current through spin-orbit-torques (SOT) provides some great perspectives in tunable spin wave devices for magnonic applications. An example illustrating these opportunities is the auto-oscillations that can be induced in YIG/Pt bilayers using SOT [1] or compensate the damping of propagating spin-waves [2]. In Bi doped YIG/Pt that shows a perpendicular anisotropy, coherent spin-waves emission can be generated by SOT [3]. However, SOT induced irreversible switching of magnetization has only been observed so far in Tm3Fe5O12 (TmIG) thin films covered with Pt, with the disadvantage that TmIG has a much larger Gilbert damping than YIG and BiYIG [4], which limits the scope of applications. In this study, we grew some series of epitaxial TmIG with different thicknesses (from 6 to 50nm) by pulsed laser deposition (PLD) on sGGG(111)-oriented substrate. Their structural characterization demonstrated the high epitaxial strain of the films up to a thickness of 25nm. Epitaxial strain could be maintained up to films thickness of 50 nm as shown in the XRD pattern in Figure 1. Kerr microscopy was used to image the magnetics domains of the samples and their hysteresis loops. The results attest the strong perpendicular magnetic anisotropy of these TmIG samples as depicted in Figure 2. Magnetic dynamical properties were probed by broadband ferromagnetic resonance with a coplanar waveguide. We hence found that the Gilbert damping of TmIG can still be improved for very thin films by tailoring the growth parameter to achieve a ferromagnetic linewidth of 72 Oe at 12 GHz, narrower than recent results in literature [5,6]. This work has been funded by the European Union’s Horizon 2020 research and innovation program within the FET-OPEN project CHIRON under grant agreement No. 801055.References: [1] V. E. Demidov, S. Urazhdin, G. De Loubens, et al., Physics Reports, 673, 1-31 (2017) [2] V. E. Demidov, S. Urazhdin, A. Anane, et al., Journal of Applied Physics, 127, 170901 (2020) [3] M. Evelt, L. Soumah, A. B. Rinkevich, et al., Physical Review Applied, 10 (4), 041002 (2018) [4] L. Soumah, N. Beaulieu, L. Qassym, et al., Nature Communications, 9, 3355 (2018) [5] C. Tang, P. Sellappan, Y. Liu et al., Physical Review B, 94, 140403(R) (2016) [6] O. Ciubotariu, A. Semisalova, K. Lenz et al., Scientific Reports, 9, 17474 (2019)

Narrow Ferromagnetic Resonance Linewidth in Perpendicularly Magnetized Tm3Fe5O12 Thin Films Grown by Pulsed Laser Deposition

With the unprecedented surge in wireless communication systems, microwave (MW) absorbers are becoming increasingly important for civil as well as military applications. When a MW signal is incident on a surface, the signal energy is divided into three parts: (i) reflected, (ii) transmitted and (iii) absorbed energies. For the usual metal-backed MW absorbing coating, transmitted energy=0; thus, minimizing reflection is the key for good absorbers. The reflection of EM energy can be curtailed by two methods: (i) an increase in absorption, and (ii) the quarter wavelength cancellation [1,2]. The loss of EM energy may originate from a number of processes within the absorber such as conduction, resonances, and relaxations etc. MW signal, on passing through an absorber dissipates its energy in the form of heat through interactions with the dielectric and magnetic structures of a material. Hence, in terms of two characteristic material parameters: relative permeability (μ*) and relative permittivity (ε*) in the absorbing medium are to be tailored for attaining a strong and broadband MW absorption. For MW absorbing applications, U-type hexaferrite phase with chemical formula Ba4Me2Fe36O60 (Me2U, Me: divalent transition-metal cation) has most complicated crystal structure and is least studied [3-11]. In present work, we investigate the preparation and MW absorbing properties of the nanoscale U-type hexaferrites (NANO-U) for development of a broadband MW absorber. The nano-powders are prepared using two different methods: (1) mechanical jet-milling of bulk U-type hexaferrite prepared by the standard solid-state reaction route at ∼1250 °C, designated here as (NANO-U)JM and (2) a novel one-pot chemical route, designated here as (NANO-U)C. In the first method, average particle size ∼20–50 nm powders were achieved; whereas, the (NANO-U)C powders of controlled particle sizes (∼65 to ∼170 nm) were prepared by changing the holding time (4, 6, 8 and 10 h) at a constant optimized working temperature of ∼900 °C. Four samples of (NANO-U)C were prepared that are designated as per their holding time as- (NANO-U)C4, (NANO-U)C6, (NANO-U)C8, (NANO-U)C10. A blend of all powders in equi-proportion, is designated as (NANO-U)CMIX, The advantage of one-pot chemical method is attainability of comparable particles sizes of a few tens of nm, at much lower working temperatures. We compare the EM parameters and MW absorbing properties of (NANO-U)JM , (NANO-U)C and bulk U-type hexaferrite powders. It is interesting to note that the (NANO-U)JM demonstrates excellent reflection loss (RL) of ∼ -43.8 dB (99.99% MW absorption) at ∼11.3 GHz frequency with a broad bandwidth of 8.6 GHz (8.9 ≤ f ≤ 17.5 GHz) for 90% or more MW absorption. The values for (NANO-U)C too are comparable, with RL of -44.2 dB (99.99% MW absorption) at 11.6 GHz frequency for (NANO-U)C8 and a broadband MW absorption with an excellent bandwidth of 8.4 GHz (9.3 ≤ f ≤ 17.7 GHz) for (NANO-U)CMIX. Significantly improved MW absorption performance are demonstrated in NANO-U hexaferrites, in comparison to the previously reported nanoscale spinel ferrites (-38.9 dB or 99.8% MW absorption along with a bandwidth of ∼3.7 GHz only). We believe that nanoscale particle sizes in U-type hexaferrites result in synergistic enhancements of the dielectric and magnetic losses. A self-explanatory schematic representation of the various possible loss mechanisms in NANO-U absorbers is shown in Fig. 1. Easy tunability, large magnetic anisotropy, presence of disordered surface spin states, defect polarization centres, greater magnetic and dielectric losses and large hopping conduction are responsible for large and broad-band MW absorption in NANO-U hexaferrites. These economical and easily processed U-type hexaferrite ultrafine particles can be used in the paints and sheets for wide-band and strong MW absorbing coating applications.References: (1) Y. Huang, H. Zhang, G. Zeng, Z. Li, D. Zhang, H. Zhu, R. Xie, L. Zheng, J. Zhu, J. Alloys Compd., 682 (2016) 138-143. (2) L. Wan, J. Zhang, Y. Chen, H. Wang, W. Hu, L. Liu, Y. Deng, J. Phys. D: Appl. Phys., 48 (2015) 355302-355310. (3) D. Lisjak, M. Drofenik, J. Appl. Phys., 93 (2003) 8011-8013. (4) M.N. Afsar, D. Lisjak, A. Bahadoor, Y. Wang, IEEE Trans. Magn., 41 (2005) 3472–3474. (5) D. Lisjak, V.B. Bregar, M. Drofenik, J. Magn. Magn. Mater., 310 (2007) 2558-2560. (6) R.S. Meena, S. Bhattacharya, R. Chatterjee, J. Magn. Magn. Mater., 322 (2010) 2908-2914. (7) R.S. Meena, S. Bhattacharya, R. Chatterjee, Mater. Sci. Eng., B, 171 (2010) 133-138. (8) R.S. Meena, S. Bhattacharya, R. Chatterjee, J. Magn. Magn. Mater., 322 (2010) 1923-1928. (9) R.S. Meena, S. Bhattacharya, R. Chatterjee, Mater. Des., 31 (2010) 3220–3226. (10) S. Padhy, S. Sanyal, R.S. Meena, R. Chatterjee, A. Bose, Journal of Electromagnetic Waves and Applications, 27 (2013) 191-204. (11) S. Padhy, S. Sanyal, R.S. Meena, R. Chatterjee, A. Bose, IET Microw. Antennas Propag., 8 (2014) 165–170.



Nanoscale U-Type Hexaferrites as Microwave Absorbers INVITED

During the past few years, the Mo3O8 quantum magnets with kagome layers formed by Mo atoms have attracted a great deal of attention as a new candidate to realise quantum spin liquid states. The magnetic susceptibility of LiZn2Mo3O8 has been experimentally shown to follow a Curie-Weiss law with the low- and high-temperature regimes whose Curie constants are related as CL~1/3CH. Originally, the disappearance of 2/3 of the paramagnetic spins at low temperatures in LiZn2Mo3O8 was attributed to valence bond condensation on the trimerized lattice of the Mo3O13 clusters [1], and several possible scenarios have been proposed to describe this unusual behaviour [2,3]. However, their adequacy was questioned by recently synthesized Li2InMo3O8, that shows a conventional Neel 120° magnetic order, and its counterpart Li2ScMo3O8, where no magnetic order has been observed down to 0.5 K [4]. Motivated by these studies, we combine rigorous first-principles calculations and effective low-energy models to study the microscopic origin of magnetism in LiZn2Mo3O8, Li2InMo3O8, and Li2ScMo3O8. Considering the extended Hubbard model constructed in the basis of Wannier functions for the Mo d states on the anisotropic kagome lattice, we argue that the magnetic properties of these systems can be described by two different regimes of electron localization defined by the competition of kinetic energy and intersite Coulomb interactions. Being in the strong interaction limit, LiZn2Mo3O8 will be proposed to reveal a plaquette charge order due to the correlated collective motion of electrons, where the partial spin pairing decoupling 2/3 of the spin originates from the asymmetry of tunneling processes. On the other hand, Li2InMo3O8 and Li2ScMo3O8 will be shown to fall into a cluster Mott insulator regime with the electrons localized at the Mo3O13 clusters, where the former exhibits long-range antiferromagnetic order and the latter is more likely to reveal short-range order with quantum spin liquid-like excitations.References: [1] J. P. Sheckelton, J. R. Neilson, D. G. Soltan, T. M. McQueen, Nat. Mater., Vol. 11, p. 493 (2012). [2] Rebecca Flint and Patric A. Lee, Phys. Rev. Lett., Vol. 111, p. 217201 (2013). [3] Gang Chen, Hae-Young Kee, and Yong Baek Kim, Phys. Rev. B, Vol. 93, p. 245134 (2016). [4] Yuya Haraguchi, Chishiro Michioka, Masaki Imai et. al, Phys. Rev. B, Vol. 92, p. 014409 (2015). 

First-principles studies of quantum magnetism in Mo3O8 cluster systems

Perovskite manganites La1−xSrxMnO3 (LSMO) (0.30 ≤x ≤0.40) exhibits interesting physical properties such as; colossal magnetoresistance, high spin-polarized current (~90%), Curie temperature (~370K) due to coupling between the charge, spin and orbital degrees of freedom, making it potential candidate for research for decades and application [1-3]. Additionally, a material with high magneto-crystalline anisotropy (MCA), which also depends on temperature, is largely influenced by crystal structure and spin-orbital coupling. In this abstract, we present structural, transport, magnetic and magneto-crystalline anisotropy in La1−xSrxMnO3 (x=0.30, 0.33, 0.36, 0.40) synthesized using solid-state reaction method. X-ray diffraction patterns of all the samples were well indexed by a rhombohedral structure with R3c space group. It is observed that lattice parameters and unit cell volume decrease monotonically upon increasing Sr concentration. X-ray photoelectron spectroscopy confirms the presence of Mn4+ and Mn3+, the ratio which from 1.37-1.54 % as increasing Sr2+ concentration. From the ρ(T) and M(T) data analysis we observe that TMI and MS is larger for x=0.33 composition, which suggest weakening of the double-exchange interaction and Jahn-Teller distortion in x=0.30, 0.36 and 0.40 [4]. We have calculated MCA constant (K1) fitting the law of approach [5-6] to saturation magnetisation data at higher magnetic field, well fitted with the equation, M=MS[1-a/H-b/H2]-χ with K12= (105/8)×b . The obtained K1 in order of ~105 erg/cm3 , slightly decreased as Sr2+ increases which is understood due to reduction of crystal volume. In all samples, the value of K1 at 100 K is higher than that at 300 K, suggesting that the samples at 100 K are more magnetically ordered than at 300 K. This work is supported by SERB-DST, New Delhi (EMR/2016/005424), Ames Lab and MRF (MITM)References: 1. J.B. Goodenough, Phys. Rev. 100 564-573 (1955) 2. C.N.R. Rao, J. Phys. Chem. B. 104 (2000) 5877-5889. 3.Ganesha Channagoudra, Ajay Kumar Saw and Vijaylakshmi Dayal, Thin Solid Films, 709, 138132 (2020) 4. A. Urushibara, Y. Moritomo, Y. Tokura, Phys. Rev. B. 51 (1995) 14103-14109. 5. A. D. Souza, P.D. Babu, Mamatha Daivajna, J. Alloys Compd. 797 (2019) 874-882 6. M. Suliga, K. Chwastek, Acta Phys. Pol. A. 135 (2019) 243–245.

Study of Structural, Transport and Magneto-Crystalline Anisotropic Properties in La1-xSrxMnO3 (0.30 ≤ x ≤ 0.40) Perovskite Manganite

The interaction between the 3d-host ferromagnetism and antiferromagnetism and Ce Kondo-type spin fluctuation and are heavy-fermion behavior in 1:2:2 type of Ce compounds is a very interesting topic and currently still unclear. The clarification of this interaction is very valuable for understanding the physics for such class of magnetic materials. In this presentation, experimental results of x-ray diffraction, x-ray absorption, magnetic susceptibility, and electrical resistivity measurements on a re-entrant ferronmagnetic material system, the Sm1-x-yGdxCey Mn2Ge2 (0 ≤ x + y ≤ 1) series, are reported and discussed for the first time. The Ce valence is found to be nearly trivalent in these materials by Ce-L3 edge measurement. The magnetic susceptibility results show that the substitution of Ce for either Sm or Gd atoms in the rare-earth sublattice expands temperature range of the antiferromagnetic phase and shift this range entirely to low temperature side. It is found such effect is stronger in the Ce for Sm substitution process than in the Ce for Gd substitution process. The temperature dependent resistivity results indicate that Ce spin-fluctuation is strongly quenched by the 3d-host magnetic field in these materials and this quenching effect is analyzed in depth.

Effects of Rare-earth Sublattice on 3d Transition-metal-host Magnetism in the Re-entrant Ferromagnetic Sm1-x-yGdxCey Mn2Ge2 Series with 0 ≤ x + y ≤ 1

We report on the effect of varying the Y element on the structural, electronic and magnetic properties of Co2YIn (Y=Nb, Ti) Heusler compounds using Density Functional Theory (DFT). The effect of the lattice parameter and total number of valence electrons on spin polarization and the magnetic properties of the Heusler compounds is revealed by comparing with Co2VIn Heusler compound, which has the same number of valence electrons as Co2NbIn, Nb and V being from the same group in the periodic table, whereas it has almost the same lattice constant as Co2TiIn, but differing in the total number of valence electrons by one, Ti and V being next neighbors in the same period of the periodic table. The optimized lattice parameters for Co2NbIn and Co2TiIn are found to be 6.20 Å and 6.05 Å respectively, while that of Co2VIn has been reported to be 6.00 Å. Co2NbIn is half metallic with an energy band gap of 0.1 eV in the minority states and has total magnetic moments of 2.02 µB/f.u. very close to the 2.00 µB/f.u. predicted by the Slater-Pauling rule, while Co2TiIn is not half metallic but has a highly spin polarized electronic structure having a spin polarization of 89.59% and total magnetic moments of 1.04µB/f.u. While reducing the number of the valence electrons by one in Co2TIIn has a significant effect on the magnetic moments and spin polarization, an increase in the lattice parameter while maintaining the same number of valence electrons in Co2NbIn does not result in the destruction of the half metallic gap.References: [1] T. Graf, C. Felser, and S. S. P. Parkin, “Heusler Compounds: Applications in Spintronics,” in Handbook of Spintronics, Y. Xu, D. D. Awschalom, and J. Nitta, Eds. Springer Netherlands, 2016, pp. 335–364. [2] A. Birsan and P. Palade, “Band structure calculations of Ti2FeSn: A new half-metallic compound,” Intermetallics, vol. 36, pp. 86–89, May 2013. [3] C. Felser, L. Wollmann, S. Chadov, G. H. Fecher, and S. S. P. Parkin, “Basics and prospective of magnetic Heusler compounds,” APL Mater., vol. 3, no. 4, p. 41518, Apr. 2015. [4] J. Ma et al., “Computational investigation of half-Heusler compounds for spintronics applications,” Phys. Rev. B, vol. 95, no. 2, p. 24411, Jan. 2017. [5] S. Mizukami and A. A. Serga, “Advancement in Heusler compounds and other spintronics material designs and applications,” J. Phys. Appl. Phys., vol. 48, no. 16, p. 160301, 2015. [6] X. Xu et al., “Electronic structures of Heusler alloy Co2FeAl1−xSix surface,” Rare Met., vol. 31, no. 2, pp. 107–111, Apr. 2012. [7] T. Graf, C. Felser, and S. S. P. Parkin, “Simple rules for the understanding of Heusler compounds,” Prog. Solid State Chem., vol. 39, no. 1, pp. 1–50, May 2011. [8] T. Graf, S. S. P. Parkin, and C. Felser, “Heusler Compounds—A Material Class With Exceptional Properties,” IEEE Trans. Magn., vol. 47, no. 2, pp. 367–373, Feb. 2011. [9] E. Sasioglu, L. M. Sandratskii, and P. Bruno, “Role of conduction electrons in mediating exchange interactions in Mn-based Heusler alloys,” Quanten-Theorie der Materialien, PreJuSER-754, 2008. [10] I. Galanakis and P. Mavropoulos, “Spin-polarization and electronic properties of half-metallic Heusler alloys calculated from first principles,” J. Phys. Condens. Matter, vol. 19, no. 31, p. 315213, 2007. [11] H. Luo et al., “Prediction of half-metallic properties for the Heusler alloys Mn2CrZ (Z=Al, Ga, Si, Ge, Sb): A first-principles study,” J. Magn. Magn. Mater., vol. 320, no. 3, pp. 421–428, Feb. 2008. [12] I. Galanakis, “Orbital magnetism in the half-metallic Heusler alloys,” Phys Rev B, vol. 71, no. 1, p. 12413, Jan. 2005. [13] I. Galanakis, P. H. Dederichs, and N. Papanikolaou, “Origin and properties of the gap in the half-ferromagnetic Heusler alloys,” Phys. Rev. B, vol. 66, no. 13, p. 134428, Oct. 2002. [14] M. Zipporah, R. Pathak, M. Robinson, J. Mwabora, R. Skomski, and A. Kashyap, “First-principle investigation of structural, electronic and magnetic properties of Co2VIn and CoVIn Heusler compounds,” AIP Adv., vol. 7, no. 5, p. 55705, Jan. 2017. [15] S. Khenchoul, A. Guibadj, B. Lagoun, A. Chadli, and S. Maabed, “First-Principles Prediction of Structural, Magnetic, Electronic, and Elastic Properties of Full-Heusler Compounds Co2YIn (Y = Ti, V),” J. Supercond. Nov. Magn., vol. 29, no. 9, pp. 2225–2233, Sep. 2016. [16] Enamullah et al., “Electronic structure, magnetism, and antisite disorder in CoFeCrGe and CoMnCrAl quaternary Heusler alloys,” Phys Rev B, vol. 92, no. 22, p. 224413, Dec. 2015. [17] I. Galanakis, P. H. Dederichs, and N. Papanikolaou, “Slater-Pauling behavior and origin of the half-metallicity of the full-Heusler alloys,” Phys Rev B, vol. 66, no. 17, p. 174429, Nov. 2002. [18] L. Wollmann, S. Chadov, J. Kübler, and C. Felser, “Magnetism in cubic manganese-rich Heusler compounds,” Phys. Rev. B, vol. 90, no. 214420, Dec. 2014.

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