United States

Heuser alloys present a rich phase diagram to engineer new materials and alter tunability of the desired material properties for potential technological applications in spintronic devices. We investigate the structural, static, and dynamic properties of Co1.5Ti0.5FeAl Heusler alloy thin films, with variable thickness (t = 5 nm, 10 nm, 20 nm, 35 nm, 50 nm, and 70 nm) grown by sputter beam epitaxy on cubic MgO (100), MAO (100) (Fig. 1), and hexagonal Al2O3 (110) substrates. By partial substitution of Ti for Co in parent alloy Co2FeAl i.e Co1.5Ti0.5FeAl, we demonstrate a very low total damping parameter of 0.00156 ± 0.00003 and a low linewidth term 17 ±1 Oe (Fig. 2) for 20 nm film grown on MAO (100) substrate using ferromagnetic resonance spectroscopy comparable to elemental Fe1,2. A pronounced fourfold anisotropy is consistent with the fourfold crystalline symmetry in the epitaxial thin films grown on cubic substrates. A saturation magnetization of ~ 5.0 μB/f.u. (where f.u. represents formula unit) was obtained at room temperature, nearly double the value based on the Slater-Pauling rule. Co1.5Ti0.5FeAl films simultaneously exhibit a very low damping and approximately 40 % lower moment than that of elemental Fe3. Taken together, the smaller value of damping, saturation moment, and linewidth for Co1.5Ti0.5FeAl films can significantly improve the efficiency of STT-switching and makes it a promising metallic ferromagnet to engineer low-loss spintronic devices.References: 1) B. Khodadadi, A. Rai, A. Sapkota, A. Srivastava, B. Nepal, Y. Lim, D.A. Smith, C. Mewes, S. 16 Budhathoki, A.J. Hauser, M. Gao, J.-F. Li, D.D. Viehland, Z. Jiang, J.J. Heremans, P. V Balachandran, T. Mewes, and S. Emori, Phys. Rev. Lett. 124, (2020). 2) M. Oogane, T. Wakitani, S. Yakata, R. Yilgin, Y. Ando, A. Sakuma, and T. Miyazaki, Jpn. J. Appl. Phys. 45, 3889 (2006) 3) J. M. D. Coey, Magnetism and magnetic materials. Cambridge, UK: Cambridge University Press, 2012.

MMM 2020

Structural and magnetic properties of Co1.5Ti0.5FeAl Heusler alloy epitaxial thin films

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

The nearest neighbour antiferromagnetic Ising model on the kagome lattice is well known for its high frustration and macroscopic ground state degeneracy [1,2]. Recently, new experimental realizations of Ising-like spin systems have been developed - so-called artificial spin systems - based on mesoscopic structures of chirally coupled nanomagnets [3]. On the square lattice, such systems have proven to behave as nearest neighbour Ising antiferromagnets. Because of frustration, realizations of kagome lattice Ising antiferromagnets with these mesoscopic structures (Fig.1) are much more challenging to study. From the theoretical side as well, such models still present some difficulties [4,5]. I will describe how to tackle classical frustrated spin systems using Monte Carlo techniques [5] and tensor network methods [4,6,7] (Fig.2), focusing on the kagome lattice nearest neighbour Ising antiferromagnet in an external magnetic field, and I will compare the experimental and numerical results.References: [1] K. Kanô and S. Naya, Prog. Theor. Phys., Vol. 10, p. 158 (1953) [2] A. Sütö, Z. Phys. B, Vol. 44, p. 121 (1981) [3] Z. Luo et. al., Science, Vol. 363, p. 1435 (2019) [4] B. Vanhecke, J. Colbois, L. Vanderstraeten, et. al., arXiv:2006.14341 (2020) [5] G. Rakala and K. Damle, Phys. Rev. E Vol. 96, 023304 (2017) [6] V. Zauner-Stauber, L. Vanderstraeten, et. al. Phys. Rev. B Vol. 97, 045145 (2018) [7] L. Vanderstraeten, B. Vanhecke, and F. Verstraete, Phys. Rev. E Vol. 98, 042145 (2018) 


New Approaches to the Nearest Neighbour Ising Antiferromagnet on the Kagome Lattice

Excitation by light pulses enables the manipulation of phases of quantum condensed matter. Here, we photoexcite high-energy holon-doublon pairs as a way to alter the magnetic free energy landscape of the Kitaev-Heisenberg magnet α-RuCl3,[1,2] with the aim to dynamically stabilize a proximate spin liquid phase. The holon-doublon pair recombination through multimagnon emission [3] is tracked through the time-evolution of the magnetic linear dichroism originating from the competing zigzag spin ordered ground state. A small holon-doublon density suffices to reach a spin disordered state. The phase transition is described within a dynamic Ginzburg-Landau framework, corroborating the quasistationary nature of the transient spin disordered phase. Our work provides insight into the coupling between the electronic and magnetic degrees of freedom in α-RuCl3 and suggests a new route to reach a proximate spin liquid phase in Kitaev-Heisenberg magnets.[4]References: [1] A. Banerjee et al., Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet, Nat. Mater. 15, 733-740 (2016). [2] H. Takagi et al.,Concept and realization of Kitaev quantum spin liquids, Nat. Rev. Phys. 1, 264-280 (2019). [3] Z. Lenarcic et al., Ultrafast charge recombination in a photoexcited Mott-Hubbard insulator, Phys. Rev. Lett. 111, 016401 (2013). [4] R.B. Versteeg et al. Nonequilibrium quasistationary spin disordered state in the Kitaev-Heisenberg magnet α-RuCl3, arXiv:2005.14189 [cond-mat.str-el] (2020) 


Nonequilibrium quasistationary spin disordered state in the Kitaev-Heisenberg magnet α-RuCl3

One dimensional spin S = 1/2 chain systems provide a perfect platform to explore many of the quantum phenomena and the related excitations. We report here the discovery of a stimulating magnetic ground state in a tetragonal compound Ti4MnBi2 that contains perfectly linear chains of Mn-ions with dMn-Mn = 2.49 Å running along the crystallographic c-axis and which are separated from each other by a large interchain distance dchain ≈7.4 Å. Our electrical transport measurements and electronic structure calculations establish that compound is metallic. Curie-Weiss fit to the susceptibility data suggests that Mn moments are in low-spin S = 1/2 configuration. The results show that despite the presence of a sizable antiferromagnetic (AFM) interaction [Jc = 18(6) K], the full-moment long range magnetic ordering is not achieved down to 50 mK. Neutron diffraction measurement performed on an assembly of aligned single crystals detect a weak AFM order within the Mn chains, with a further evidence of the reduced-moment ordering coming from heat capacity data. Apparently, strong quantum fluctuations overcome the magnetic order and the material enters into a state at low temperatures which can be best described as a ``quantum admixture" of a quantum spin liquid and a long-range magnetically ordered states, resulting into a highly reduced value of the ordered moment μ << 1 μB.References: A. Pandey, P. Miao, M. Klemm, H. He, H. Wang, X. Qian, J. W. Lynn, and M. C. Aronson, Phys. Rev. B in press (2020). 

Incipient antiferromagnetic order in metallic Ti4MnBi2 containing linear Mn chains of spin S = 1/2

The realization of energy efficient spin-current based electronics relies on the existence of low-loss magnetic insulator thin films capable of generating spin currents without an accompanying charge current. Currently, the number of such materials is extremely limited, with the only candidates being the garnets Y3Fe5O12 (YIG) [1] and Lu3Fe5O12 (LuIG) [2] along with the recently discovered spinels Ni0.65Zn0.35Al0.8Fe1.2O4 (NZAFO) [3] and MgAl0.5Fe1.5O4 (MAFO) [4,5]. Bulk phase Li0.5Fe2.5O4 (LFO) is well known to have the lowest Gilbert damping parameter (α ≈ 0.002) among the spinel ferrites, but thus far LFO thin films have not lived up to these expectations. In this talk, we demonstrate the realization of epitaxial ultra-thin (~3 nm) LFO thin films on MgAl2O4 substrates with an ultra-low damping parameter of α ≈ 0.0013 and an FMR linewidth of 1.17 mT at 20.6 GHz. Such a damping value rivals those of YIG and is comparable to the lowest damping previously reported in sub-10-nm magnetic films [2]. LFO also offers distinct advantages over YIG such as smaller external field requirements and thinner interfacial magnetic dead layers due to the low growth temperature, making it ideal for magnetic switching applications. Our results show the promise of LFO as a new candidate for spin-current based spintronics. This work was supported by the U.S. Department of Energy, Director, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Contract No. DESC0008505.References: [1] B. M. Howe, S. Emori, H. Jeon, IEEE Magnetics Letters., Vol. 6, p. 1-4 (2015) [2] C. L. Jermain, H. Paik, S. V. Aradhya, Applied Physics Letters., Vol. 109, p. 192408 (2016) [3] M. T. Gray, S. Emori, B. A. Gray, Physics Review Applied., Vol. 9, p. 064039 (2018) [4] S. Emori, D. Yi, S. Crossley, Nano Letters., Vol. 18, p. 4273-4278 (2018) [5] J. J. Wisser, S. Emori. L. Riddiford, Applied Physics Letters., Vol. 115, p. 132404 (2019) 


Ultra-low Magnetic Damping in Epitaxial Li0.5Fe2.5O4 Thin Films

High magnetostriction and low damping are two crucial properties for voltage tunable high frequency devices using magnetostrictive ferromagnet-piezoelectric hybrid structures to achieve low microwave loss [1, 2]. FeGa is a promising candidate for such devices as it is free of rare earth elements and has a large magnetostriction [3]. We grew epitaxial FeGa films on MgO (100) substrates using off-axis sputtering technique. Broadband ferromagnetic resonance (FMR) is used to investigate the magnetization dynamics of the epitaxial FeGa thin films. The resonance field Hres versus frequency f data is fitted using the Kittel equation to extract the reduced gyromagnetic ratio γ′, the effective magnetization Meff, and the four-fold magnetic anisotropy H4. The frequency dependence of the linewidth data is used to extract the effective damping αeff and residual linewidth ΔH0 due to inhomogeneities in the film. We report ultra-low residual linewidth, ΔH0 = 13±1 [Oe] – indicative of the high quality of the epitaxial films- significantly lower than reported previously [4]. The effective damping parameter αeff is found to be as low as 0.0065(+0.0005 -0.0001), as shown in figure 1, which is one order magnitude lower than previously reported values [5, 6]. In-plane angular dependence of resonance field Hres clearly demonstrates a four-fold in-plane anisotropy arising from the crystal symmetry. The four-fold anisotropy extracted from the Kittel plot H4 = -786±15 [Oe] is in good agreement with the value determined from fitting of in-plane rotation data H4 = -795±1 [Oe] as shown in figure 2.References: 1) V. Novosad et al., Journal of applied physics 87, 6400 (2000). 2) J. Lou et al., Applied Physics Letters 92, 262502 (2008). 3) A. E. Clark et al., Materials transactions 43, 881 (2002). 4) B. K. Kuanr et al., Journal of Applied Physics 115, 17C112 (2014). 5) D. Parkes et al., Scientific reports 3, 2220 (2013). 6) D. B. Gopman et al., IEEE transactions on magnetics 53, 1 (2017). 


Low damping and linewidth in magnetostrictive epitaxial FeGa thin films using ferromagnetic resonance

Identifying the origins of ferromagnetic resonance (FMR) linewidth broadening is essential for the fundamental understanding of magnetic relaxation, often discussed in terms of “damping”. It is not yet well understood how inhomogeneity and structural disorder contribute to magnetic relaxation in polycrystalline thin films, even though they are widely used in device applications. In this presentation, we systematically examine the impact of inhomogeneity and disorder on the FMR linewidth of sputter-grown polycrystalline Fe and Fe80V20 films with thickness 2-25 nm and different seed layers. A highly nonlinear frequency dependence of FMR linewidth is observed for Fe films on Cu/Ti seed layers. As shown in Fig. 1, all linewidth vs frequency data are quantitatively reproduced with a two-magnon scattering model [1, 2, 3] that accounts for a random distribution of the effective anisotropy field among grains in the polycrystalline film. The fit results indicate that a larger grain size is correlated with stronger two-magnon scattering, which – somewhat counterintuitively – may be accompanied by a lower Gilbert damping parameter. Films with the strongest two-magnon scattering contribution (cf. 10-nm-thick Fe/Cu/Ti, Fig. 1) exhibit the highest coercivity, pointing to a connection between magnetic inhomogeneity and the observed non-Gilbert relaxation. In addition, it is found that two-magnon scattering is reduced by changing the seed layer or alloying Fe with V (Fig. 2). We will discuss the possible mechanisms that lead to narrower FMR linewidths in polycrystalline Fe(V) films. The fundamental understanding gained from our study enables a coherent approach to develop low-loss polycrystalline magnetic media for power-efficient spintronic devices.References: [1] R. McMichael and P. Krivosik, IEEE Trans. Mag., Vol. 40, p.2 (2004) [2] S. Kalarickal, P. Krivosik and J. Das, Phys. Rev. B, Vol. 77, p.054427 (2008) [3] W. Peria, T. Peterson and A. McFadden, Phys. Rev. B, Vol. 101, p.134430 (2020) 


Two-magnon Scattering in Polycrystalline Fe and FeV Alloy Thin Films

Magnetic materials showing perpendicular magnetic anisotropy (PMA) and low damping are of great importance in spintronics. Co/Ni multilayers have been known to exhibit large tunable PMA [1], high spin polarization [2] and relatively low intrinsic damping [3]. In this study we investigated a series of Pt/[Co/Ni]N/Ir multilayers grown on Si/SiO2 with a Ta/Pt seed adhesion layer and the multilayer stack was capped with an Ir/Pt/Ta capping layer. Broadband ferromagnetic resonance (FMR) and polar angle dependent FMR measurements reveal the presence of a strong fourth-order contribution to the perpendicular anisotropy. Polar angle dependent data are fitted using the Smit-Beljers relation [4] to extract both the second and fourth-order anisotropy constants (shown in Fig.1). This model explains the data qualitatively and we observe systematic deviations for samples near or in the easy cone state of the phase diagram. We find that the effective Gilbert damping scales with the inverse multilayer thickness, indicating a significant interfacial contribution to the damping process.References: 1. G. Daalderop, P. Kelly and F. D. Broeder, Physical Review Letters., vol 68, p:682-685 (1992) 2. S. Mangin, D. Ravelsona, J. A. Katine, et.al., Nature Materials., vol 5, p:210-215 (2006) 3. J. M. Shaw, H. T. Nembach and T. J. Silva, Journal of Applied Physics., vol 108, p: 093922 (2010) 4. J. Smith and H. Beljers, Philips Research Reports., vol 10, p:113 (1955) 



Higher-order contribution to perpendicular anisotropy and interfacial damping of Co/Ni multilayers

Insulator / 3d ferromagnet / 5d metal trilayers with broken inversion symmetry along the film normal direction is of great interest, since the broken symmetry is known to contribute to the perpendicular magnetic anisotropy (PMA) and the conversion of in-plane charge current to perpendicular spin current through the Rashba spin-orbit coupling [1, 2]. Here, we report on the PMA and magnetization dynamics of the MgO/Fe/Au trilayer with the Fe layer thickness from 0.4 nm to 1.2 nm, and compare the results with the Au/Fe/Au system with a symmetric structure along the film normal. These trilayers were grown on MgO(001) substrate by molecular beam epitaxy method. The PMA and dynamics were investigated by the time-resolved magneto-optical Kerr effect (TRMOKE) measurements. Figure 1 shows Fe thickness dependence of (a) effective anisotropy field Hkeff, (b) g-factor, (c) anisotropy distribution ΔHkeff, and (d) damping constant α of MgO/Fe/Au and Au/Fe/Au trilayers. Both MgO/Fe/Au and Au/Fe/Au showed an increase of Hkeff with decreasing the Fe thickness, and MgO/Fe/Au was confirmed to exhibit slightly larger Hkeff than Au/Fe/Au due to the Rashba effect. The g-factor of both trilayers decreased from the bulk value with decreasing the Fe thickness. ΔHkeff increased at Fe thickness of 0.8 nm for both trilayers which is considered to be due to the relaxation of lattice mismatch around the Fe thickness of 1 nm. The damping constant α of both trilayers increased with decreasing the Fe thickness from 0.8 nm to 0.4 nm due to the effect of spin pumping. The reduction of α at Fe thickness of 0.8 nm is explained by the effect of two-magnon scattering which is enhanced by the increase of ΔHkeff. Interestingly, MgO/Fe/Au trilayers show larger damping constant than Au/Fe/Au with the same Fe thickness, which may reflect the Rashba spin-orbit coupling and/or the variation in the density of states at the Fermi level.References: [1] S. E. Barnes et. al., Sci. Rep. 4, 4105 (2014). [2] I. M. Miron et al., Nat. Mater. 9, 230 (2010).

Perpendicular anisotropy and damping of MgO/Fe/Au trilayers with broken inversion symmetry

Recently, antiferromagnetic spintronics have attracted great attention, with extensive research devoted to spin transport between ferromagnetic (FM) and antiferromagnetic (AFM) materials in FM/AFM heterostructures [1-6]. In order to enable a deeper understanding of the mechanisms behind this effect, it would be invaluable to perform time resolved studies of GHz spin dynamics in systems with antiferromagnetic order with sensitivity to each absorber site individually, however, to date experimental techniques that offer these capabilities are lacking. Here, we present the first experimental observation of dynamic X-ray magnetic linear dichroism (XMLD) from GHz spin precessions driven by ferromagnetic resonance (FMR). We explore the capabilities of this new technique in two model systems, a ferromagnetic metal, i.e., Ni80Fe20 (Py), and a ferrimagnetic insulator, i.e., Ni0.65Zn0.35Al0.8Fe1.2O4 (NZAFO). Both systems yield dynamic XMLD signals consistent with our models. Under experimental geometries with oblique x-ray polarization (i.e., when the angle between static magnetization and x-ray polarization is near 45°) the dynamic XMLD response occurs primarily at the fundamental frequency of the driving RF excitation (see Fig. 1). This effect is well suited for in-plane magnetic anisotropy studies conducted in normal incidence geometry. For studies that require complementary geometries (e.g., vertical or horizontal polarization), the dynamic signal can be extracted from the 2nd harmonic response. This also works for grazing incidence measurements that are sensitive to in- vs. out-of-plane magnetic anisotropy. The presented results are a breakthrough achievement in detecting dynamic manifestations of the XMLD effect at technologically relevant, GHz frequencies. By utilizing the sensitivity of XMLD to the spin axis rather than the spin direction, one can expand conventional x-ray detected FMR towards the direct dynamic study of antiferromagnetic order.References: [1] C. Hahn et al., EPL 108, 57005 (2014) [2] H. Wang et al., Phys. Rev. Lett. 113, 097202 (2014) [3] W. Lin et al., Phys. Rev. Lett. 116, 186601 (2016) [4] Z. Qiu et al., Nat. Commun. 7, 12670 (2016) [5] Q. Li et al., Nat. Commun. 10, 5265 (2019) [6] M. Dabrowski et al., Phys. Rev. Lett. 124, 217201 (2020)

Experimental realization of linearly polarized x-ray detected ferromagnetic resonance

Confirming the origin of Gilbert damping by experiment has remained a challenge for many decades. This is the case even for some of the simplest and most technologically relevant ferromagnetic metals, such as pure Fe. Here, we experimentally identify intrinsic Gilbert damping that increases with decreasing electronic scattering in thin films of BCC Fe [1]. We directly compare the temperature dependence of Gilbert damping and electronic transport in pristine epitaxial films (Figure 1). Our observation of “conductivity-like” damping, which cannot be accounted for by classical eddy current loss, is in excellent quantitative agreement with theoretical predictions of Gilbert damping due to intraband scattering (often understood in terms of the “breathing Fermi surface” model) [2,3], as shown in Figure 2. While this fundamental damping mechanism was originally proposed more than 40 years ago [4], our study is the first to confirm it unambiguously for thin films of a pure ferromagnetic metal. Our results also reveal – somewhat counterintuitively – that disorder can reduce intrinsic damping in ferromagnetic metals particularly at low temperatures. This suggest that optimally disordered films may exhibit enhanced spin coherence required for cryogenic and quantum information devices.References: [1] B. Khodadadi, A. Rai, A. Sapkota, et al. Phys. Rev. Lett., Vol. 124, 157201 (2020). [2] K. Gilmore, Y. U. Idzerda, and M.D. Stiles, Phys. Rev. Lett., Vol. 99, 27204 (2007). [3] S. Mankovsky, D. Kodderitzsch, G. Woltersdorf, and H. Ebert, Phys. Rev. B, Vol. 87, 14430 (2013). [3] V. Kamberský and Czechoslov. J. Phys., Vol. 26, 1366 (1976).

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Structural and magnetic properties of Co1.5Ti0.5FeAl Heusler alloy epitaxial thin films

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