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DOE OSTI2019

Room–Temperature Insulating Ferromagnetic (Ni,Co) 1+2 x Ti 1– x O 3 Thin Films

Insulating uniaxial room–temperature ferromagnets are a prerequisite for commonplace spin wave–based devices, the obstacle in contemporary ferromagnets being the coupling of ferromagnetism with large conductivity. It is shown that the uniaxial A 1 + 2x Ti 4+ 1 – x O 3 (ATO), A = Ni 2+ ,Co 2+ , and 0.6 < x ≤ 1, thin films are electrically insulating ferromagnets already at room temperature. Here, the octahedra network of the ATO and the corundum and ilmenite structures are the same yet different octahedra–filling proved to be a route to switch from the antiferromagnetic to ferromagnetic regime. Octahedra can continuously be filled up to x = 1, or vacated (–0.24 < x < 0) in the ATO structure. TiO–layers, which separate the ferromagnetic (Ni,Co)O–layers and intermediate the antiferromagnetic coupling between the ferromagnetic layers in the NiTiO 3 and CoTiO 3 ilmenites, can continuously be replaced by (Ni,Co)O–layers to convert the ATO–films to ferromagnetic insulator with abundant direct cation interactions.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Electro-optic switching in iron oxide nanoparticle embedded paramagnetic chiral liquid crystal via magneto-electric coupling

The variation in optical texture, electro-optic, and dielectric properties of iron oxide nanoparticles (NPs) embedded ferroelectric liquid crystal (FLC) with respect to change in temperature and electrical bias conditions are demonstrated in the current investigations. Improvement in spontaneous polarization and response time in nanocomposites has been attributed to magneto-electric (ME) coupling resulting from the strong interaction among the ferromagnetic nanoparticle's exchange field (due to unpaired e{sup −}) and the field of liquid crystal molecular director. Electron paramagnetic resonance spectrum of FLC material gives a broad resonance signal with superimposed components indicating the presence of a source of spin. This paramagnetic behavior of host FLC material had been a major factor in strengthening the guest host interaction by giving an additional possibility of (a) spin-spin interaction and (b) interactions between magnetic-dipole and electric-dipole moments (ME effects) in the composite materials. Furthermore, the phenomenon of dielectric and static memory effect in these composites are also observed which yet again confirms the coupling of magnetic NP's field with FLC's director orientation. We therefore believe that such advanced soft materials holding the optical and electrical properties of conventional LCs with the magnetic and electronic properties of ferromagnetic nanoparticles are going to play a key role in the development of futuristic multifunctional optical devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2013

Effects of ruthenium seed layer on the microstructure and spin dynamics of thin permalloy films

The spin dynamics and microstructure properties of a sputtered 12 nm Ni{sub 81}Fe{sub 19} thin film have been enhanced by the use of a ruthenium seed layer. Both the ferromagnetic resonance field and linewidth are enhanced dramatically as the thickness of ruthenium seed layer is increased. The surface anisotropy energy constant can also be largely tailored from 0.06 to 0.96 erg/cm{sup -2} by changing the seed layer thickness. The changes to the dynamics magnetization properties are caused by both ruthenium seed layer induced changes in the Ni{sub 81}Fe{sub 19} structure properties and surface topography properties. Roughness induced inhomogeneous linewidth broadening is also seen. The damping constant is highly tunable via the ruthenium thickness. This approach can be used to tailor both the structure and spin dynamic properties of thin Ni{sub 81}Fe{sub 19} films over a wide range. And it may benefit the applications of spin dynamics and spin current based devices.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Structural and magnetic properties of CoTeMo⁢O 6

Here, we have conducted a comprehensive investigation into the magnetic properties of the chiral multiferroic material CoTeMo⁢O 6 . In contrast with the previous claim of canted antiferromagnetic order with ferromagnetic components [Y. Doi et al., J. Solid State Chem. 182, 3232 (2009)], our investigation reveals an antiferromagnetic ground state with compensated moments, providing an interesting platform for exploring exotic material properties. Through careful measurements of magnetization under a series of applied fields, we demonstrate that there exist two sequential field-induced magnetic transitions in CoTeMo⁢O 6 , with one occurring at 𝐻 𝑐⁢1 =460 Oe along the 𝑎 axis, and the other at 𝐻 𝑐⁢2 =1.16 T with the field along the 𝑏 axis. The values of 𝐻 𝑐⁢1 and 𝐻 𝑐⁢2 exhibit strong angular dependence and diverge with different rates as the applied field is rotated 90 ° within the 𝑎⁢𝑏 plane. This reflects the distinct nature of these transitions, which is further supported by the different critical behavior of 𝐻 𝑐⁢1 and 𝐻 𝑐⁢2 , characterized by the values of 𝛾, in the function of 𝐻 𝑐 =𝐻 0 ⁡(1−𝑇/𝑇 𝑐 ) 𝛾 . Furthermore, we have demonstrated that there exist structural and magnetic twin domains in CoTeMo⁢O 6 that strongly affect the experimental measurement of their macroscopic properties. Intriguingly, these twin domains can be related to the orthorhombicity/chirality of the crystal structure with the space group 𝑃⁢2 1 ⁢2 1⁢ 2. We further explored the magnetic and structural domains with uniaxial pressure and polarized light microscopy. Our results suggest that CoTeMo⁢O 6 could be used as a unique platform for investigating the intriguing physics involving intertwined degrees of freedom. The tunability of the underlying domain distribution and its strong anisotropy could also be useful for developing functional devices and applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Synchrotron X-ray spectroscopic study of the antiferromagnetic-ferromagnetic transition in Ni-doped FeRh epitaxial thin films

Here we investigate the change of magnetism and electronic structure across the antiferromagnetic (AFM)-ferromagnetic (FM) transition of Ni-doped FeRh epitaxial thin films by x-ray magnetic circular dichroism (XMCD) and hard x-ray photoemission spectroscopy (HAXPES). The Rh L edge XMCD results indicate that the remnant FM phase at low temperature possesses smaller Rh moment than the normal FM phase which can undergo AFM-FM transition. The HAXPES results confirm an increase of Rh 4d density of state at the Fermi level and a possible "well-screened" state at the Ni 2p photoemission in the FM phase. FM fluctuation of the inter-site Fe-Fe exchange coupling within the AFM phase can be interpreted from the temperature dependence of the Fe 2p HAXPES results.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Annealing influence on the Gilbert damping parameter and the exchange constant of CoFeB thin films

We present a study of the influence of the annealing temperature T{sub a} on the magnetic properties of Co{sub 40}Fe{sub 40}B{sub 20} thin films. Using a vector network analyzer ferromagnetic resonance (VNA-FMR) setup and the magneto-optical Kerr effect, the dependence of the Gilbert damping parameter α, the exchange constant A, the saturation magnetization as well as the coercive field and the Kerr signal on T{sub a} is reported. Additionally, the correlation with the crystalline properties of the films studied by X-ray diffractometry is discussed. We found that while the damping parameter α and the coercive field show sharp changes starting at a certain T{sub a} value, the exchange constant A and the Kerr signal show a steady evolution. A differential modification of the film surface compared to the bulk is discussed as a possible reason. In any case, we found that the low damping values are preserved at the first onset of crystallization.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Optical and magneto-optical properties of Co-doped CeO{sub 2−δ} films in the 0.5 to 4 eV range

Magnetically doped Ce{sub 1−x}Co{sub x}O{sub 2−δ} (nominal x = 0.05 and 0.10) films were systematically studied by spectroscopic ellipsometry and magneto-optical spectroscopy. The samples were prepared by pulsed laser deposition on MgO(100) substrates and grew as textured polycrystalline films with thickness between 200 and 750 nm. They exhibited room temperature ferromagnetism and an out-of-plane easy axis attributed to magnetoelastic effects from the in-plane compressive strain. The dispersion of dielectric function of Ce{sub 1−x}Co{sub x}O{sub 2−δ} films was parametrized by the sum of Tauc-Lorentz and damped Lorentz oscillators and adjusted numerically. Deduced optical band gaps were similar to those of pure CeO{sub 2}, but the Co doping increased the optical absorption. The magneto-optical spectroscopy was carried out in both Faraday and Kerr configurations in the photon energy range from 0.5 to 4 eV, showing a strong dependence of the magneto-optical effect on the Co content near the optical band edge.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

Topological Magnetic-Spin Textures in Two-Dimensional van der Waals Cr 2 Ge 2 Te 6

Two-dimensional (2D) van der Waals (vdW) materials show a range of profound physical properties that can be tailored through their incorporation in heterostructures and manipulated with external forces. The recent discovery of long-range ferromagnetic order down to atomic layers provides an additional degree of freedom in engineering 2D materials and their heterostructure devices for spintronics, valleytronics, and magnetic tunnel junction switches. In this work, using direct imaging by cryo-Lorentz transmission electron microscopy we show that topologically nontrivial magnetic-spin states, skyrmionic bubbles, can be realized in exfoliated insulating 2D vdW Cr 2 Ge 2 Te 6 . Due to the competition between dipolar interactions and uniaxial magnetic anisotropy, hexagonally packed nanoscale bubble lattices emerge by field cooling with magnetic field applied along the out-of-plane direction. Despite a range of topological spin textures in stripe domains arising due to pair formation and annihilation of Bloch lines, bubble lattices with single chirality are prevalent. In conclusion, our observation of topologically nontrivial homochiral skyrmionic bubbles in exfoliated vdW materials provides a new avenue for novel quantum states in atomically thin insulators for magneto-electronic and quantum devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Analysis of ultrafast magnetization switching dynamics in exchange-coupled ferromagnet–ferrimagnet heterostructures

Magnetization switching in ferromagnets has so far been limited to the current-induced spin–orbit–torque effects. Recent observation of helicity-independent all-optical magnetization switching (HI-AOS) in an exchange-coupled ferromagnet–ferrimagnet (FM-FEM) heterostructures expanded the range and applicability of such ultrafast heat-driven magnetization switching. Here we report the element-resolved HI-AOS dynamics of such an exchange-coupled system, using a modified microscopic three-temperature model. We have studied the effect of (i) the Curie temperature of the FM, (ii) FEM composition, (iii) the long-range Ruderman–Kittel–Kasuya–Yosida (RKKY) exchange-coupling strength, and (iv) the absorbed optical energy on the element-specific time-resolved magnetization dynamics. The phase-space of magnetization illustrates how the RKKY coupling strength and the absorbed optical energy influence the switching time. Our analysis demonstrates that the threshold switching energy depends on the composition of the FEM and the switching time depends on the Curie temperature of the FM as well as RKKY coupling strength. Importantly, this simulation anticipates new insights into developing faster and more energy-efficient spintronics devices.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Enhancing ferromagnetic resonance absorption for very thin insulating magnetic films with spin plasmonics

We consider enhancing the ferromagnetic resonance (FMR) absorption of very thin insulating magnetic films by placing it on top of a dielectric. We find that the signal is enhanced by at least an order of magnitude due to a new nonreciprocal interface resonance that is a mixture of the magnetic surface plasmon mode and a wave guide mode. This resonance occurs over a wide range of thicknesses of the dielectric that is still much less than the wavelength and is made possible by the negative magnetic susceptibility of the magnetic layer. The line width of absorption is reduced by an order of magnitude less than the Gilbert damping parameter. At some frequency, the group velocity of this resonance is negative. Experimentally, very thin yttrium iron garnet (YIG) films are grown on a Gadolinium Gallium Garnet (GGG) substrate which can be considered the dielectric. Our model applies to experiments performed in the YIG/GGG system. Indeed, our picture resolves the disagreement on the magnitude of the spin diffusion lengths obtained with the FMR and the Brillouin scattering techniques. It also provides for a way to make new adaptive thin film miniaturized photonic nonreciprocal devices with low loss.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

RKKY Exchange Bias Mediated Ultrafast All-Optical Switching of a Ferromagnet

The discovery of ultrafast helicity-independent all-optical switching (HI-AOS), as well as picosecond all-electrical switching of a ferrimagnet, has inspired the ultrafast spintronics community to explore ultrafast switching of a ferromagnet to achieve practical ultrafast storage and memory devices. Two explored mechanisms of HI-AOS of a ferromagnet in ferromagnet-ferrimagnet heterostructure are: a) exploiting the indirect exchange coupling with and b) injection of non-local spin current originated from a switching ferrimagnet. Here, in this manuscript, exchange mediated HI-AOS of a Ruderman–Kittel–Kasuya–Yosida (RKKY) exchange coupled “[Co/Pt]-multilayers/Pt spacer/CoGd” heterostructure is demonstrated. The authors have measured layer-resolved static magnetic properties, single-shot HI-AOS, and magnetization dynamics of the ferromagnetic Co/Pt multilayers (MLs), that are ferromagnetically or antiferromagnetically coupled with ferrimagnetic CoGd layers. Time-resolved magnetization dynamics reveal a 3.5 ps switching time of the Co/Pt MLs, which is the fastest switching of a ferromagnet reported to date. Employing an extended microscopic three-temperature model, the temporal dynamics of the exchange coupled ferromagnet–ferrimagnet heterostructure are simulated, qualitatively and quantitatively explaining the experimental switching phenomena. This work experimentally as well as theoretically establishes the mechanism of exchange mediated all-optical switching of ferromagnet-ferrimagnet heterostructures, which can be integrated with a magnetic tunnel junction for efficient reading after ultrafast energy-efficient switching.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Ferromagnetism of Fe 3 Sn and alloys

Hexagonal Fe 3 Sn has many of the desirable properties for a new permanent magnet phase with a Curie temperature of 725 K, a saturation moment of 1.18 MA/m. and anisotropy energy, K 1 of 1.8 MJ/m 3 . However, contrary to earlier experimental reports, we found both experimentally and theoretically that the easy magnetic axis lies in the hexagonal plane, which is undesirable for a permanent magnet material. One possibility for changing the easy axis direction is through alloying. We used first principles calculations to investigate the effect of elemental substitutions. The calculations showed that substitution on the Sn site has the potential to switch the easy axis direction. Transition metal substitutions with Co or Mn do not have this effect. We attempted synthesis of a number of these alloys and found results in accord with the theoretical predictions for those that were formed. However, the alloys that could be readily made all showed an in-plane easy axis. The electronic structure of Fe 3 Sn is reported, as are some are magnetic and structural properties for the Fe 3 Sn 2 , and Fe 5 Sn 3 compounds, which could be prepared as mm-sized single crystals.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Study of structural and ferromagnetic resonance properties of spinel lithium ferrite (LiFe{sub 5}O{sub 8}) single crystals

The effect of B-site cation ordering on the room temperature structural and ferromagnetic resonance (FMR) properties of single crystal spinel lithium ferrite (LiFe{sub 5}O{sub 8}, LFO) have been investigated. A detailed microstructural analysis is done through X-ray diffraction, polarized Raman spectroscopy, and transmission electron microscopy (TEM) to examine the effect of post-annealing on the B-site cation ordering. The X-ray diffraction pattern of the as-grown crystal indicates a disordered state of the crystal. However, the annealed sample shows additional superlattice reflections corresponding to the ordered phase. This ordering is further confirmed by Raman spectra and TEM images, which reveal ordering of Li and Fe ions at the octahedral sites contrasting with the relatively high degree of octahedral site disorder in the as-grown crystal. To study the effect of B-site ordering on the magnetic properties and FMR linewidth, vibrating sample magnetometry and broadband FMR measurements have been performed for both the ordered and disordered phases of lithium ferrite. The value of saturation magnetization for both phases is ∼290 emu/cm{sup 3}. A single mode FMR profile is observed for both phases with little distortion. The linewidth characteristics of the ordered and disordered phases of lithium ferrite phases are compared, and it is observed that the linewidth is independent of the cation ordering. Both the phases exhibit a low linewidth (∼26 Oe at 30 GHz) and the effective damping parameter for the as-grown and annealed samples is determined to be 0.0021 ± 0.0001.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Exchange bias effect in Ti doped nanocrystalline SrFeO{sub 3-δ}

Materials of Ti doped nanocrystalline SrFeO{sub 3-δ} were synthesized through solid state reaction. Detailed magnetization measurements were carried out in zero field cooled (ZFC) and field cooled (FC) conditions. Compounds of SrFe{sub 1-x}Ti{sub x}O{sub 3-δ} (x = 0.1 to 0.3) are found to be spin glass and parent compound is a helical antiferromagnet. Non magnetic Ti{sup 4+} reduces the strength of exchange interactions and the curvature of hysteresis is changed towards concave nature. Exchange bias is observed below the peak temperature (irreversibility in magnetization (T{sub Irr})) in ZFC-FC of SrFe{sub 1-x}Ti{sub x}O{sub 3-δ} (x = 0 to 0.3). The coercivity and exchange bias field values are found to be decreases with increase in temperature. Observed exchange bias effect is attributed to competition between antiferromagnetic superexchange and ferromagnetic double exchange interactions.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Absence of a Dirac gap in ferromagnetic Cr x (Bi 0.1 Sb 0.9 ) 2-x Te 3

Magnetism breaks the time-reversal symmetry expected to open a Dirac gap in 3D topological insulators that consequently leads to the quantum anomalous Hall effect. The most common approach of inducing a ferromagnetic state is by doping magnetic 3d elements into the bulk of 3D topological insulators. In Cr 0.15 (Bi 0.1 Sb 0.9 ) 1.85 Te 3 , the material where the quantum anomalous Hall effect was initially discovered at temperatures much lower than the ferromagnetic transition, T C , the scanning tunneling microscopy studies have reported a large Dirac gap of ~20–100 meV. The discrepancy between the low temperature of quantum anomalous Hall effect (< C ) and large spectroscopic Dirac gaps (>>T C ) found in magnetic topological insulators remains puzzling. Here, we used angle-resolved photoemission spectroscopy to study the surface electronic structure of the pristine and potassium doped surface of Cr 0.15 (Bi 0.1 Sb 0.9 ) 1.85 Te 3 . Upon potassium deposition, the p-type surface state of the pristine sample was turned into an n-type, allowing the spectroscopic observation of Dirac point. Finally, we find a gapless surface state, with no evidence of a large Dirac gap reported in tunneling studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Ultrafast optically induced spin transfer in ferromagnetic alloys

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Identifying the sources of ferromagnetism in sol-gel synthesized Zn{sub 1−x}Co{sub x}O (0≤x≤0.10) nanoparticles

We have carefully investigated the structural, optical and electronic properties and related them with changes in the magnetism of sol-gel synthesized Zn{sub 1−x}Co{sub x}O (0≤x≤0.10) nanoparticles. Samples with x≤0.05 were free of spurious phases. Samples with x≤0.03 were found to be with only high spin Co{sup 2+} ions into ZnO structure, whereas sample with x=0.05, exhibited the presence of high spin Co{sup 2+} and low spin Co{sup 3+}. We found that the intensity of the main EPR peak associated with Co{sup 2+} varies with the nominal Co content in a similar manner as the saturation magnetization and coercive field do. These results point out that the ferromagnetism in these samples should directly be correlated with the presence of divalent cobalt ions. Bound magnetic polaron (BMP) model and the charge transfer model are insufficient to explain the ferromagnetic properties of Zn{sub 1−x}Co{sub x}O nanoparticles. The room temperature ferromagnetism (RTFM) may be originated from a combination of several factors such as the interaction of high spin Co{sup 2+} ions, perturbation/alteration and/or changes in the electronic structure of ZnO close to the valence band edge and grain boundary effects. - Graphical abstract: The intensity of the main EPR peak associated with Co{sup 2+} varies with the nominal Co content in a similar manner as the saturation magnetization and coercive field do. These results point out that the ferromagnetism in these samples should directly be correlated with the presence of Co{sup 2+} ions. Display Omitted - Highlights: • Systematic and carefully study of physical-chemical properties of Zn{sub 1−x}Co{sub x}O nanoparticles. • Samples with x=0.01 and 0.03 were found to be with only high spin Co{sup 2+}. • Sample with x=0.05, exhibited the presence of high spin Co{sup 2+} and low spin Co{sup 3+}. • The BMP and charge transfer models seem not explain the ferromagnetic properties. • RTFM: high spin Co{sup 2+} ions, defects close to the valence band and grain boundary effects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2013

[Bmim][TfO] ionic liquid-assisted oriented growth of Co{sub 3}O{sub 4} nanoworms

Graphical abstract: Display Omitted Highlights: ► First time, we have used [Bmim][TfO]IL for the synthesis of Co{sub 3}O{sub 4} nanoworms. ► IL assists to form oriented growth of cubic Co{sub 3}O{sub 4} nanoworms without intermediate. ► Cubic Co{sub 3}O{sub 4} nanoworms are in the range of 20 nm width and 100–200 nm length. ► IL and oxidizing agent have not altered the Co{sub 3}O{sub 4} structural characteristics. ► Co{sub 3}O{sub 4} nanoworms exhibit crystalline domain dependent weak ferromagnetism. -- Abstract: Monodispersed worm-like structure of Co{sub 3}O{sub 4} nanocrystals of 20 nm width and 100–200 nm length are prepared directly without any intermediate product by 1-n-butyl-3-methylimidazolium trifluoromethane sulfonate ionic liquid ([Bmim][TfO] IL) assisted precipitation method. The higher concentration of [Bmim][TfO] IL in the reaction medium leads to the formation of homogeneous nanoworms. The effect of synthesis temperature and the oxidizing agent (H{sub 2}O{sub 2}) on the Co{sub 3}O{sub 4} particle's morphology and their magnetic properties are discussed. Thermogravimetric analysis (TGA), powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), field emission scanning electron microscopy (FE-SEM) and transmission electron microscopy (TEM) analysis were used to characterize the Co{sub 3}O{sub 4} monodispersed nanoworms. The magnetic property of the spinel Co{sub 3}O{sub 4} nanoworms is highly dependent on crystalline domains and exhibits weak ferromagnetic behavior with a narrow hysteresis loop opening.

36 MATERIALS SCIENCE↗