Extreme Domain Wall Speeds under Ultrafast Optical Excitation.

Time-resolved ultrafast EUV magnetic scattering was used to test a recent prediction of >10 km/s domain wall speeds by optically exciting a magnetic sample with a nanoscale labyrinthine domain pattern. Ultrafast distortion of the diffraction pattern was observed at markedly different timescales compared to the magnetization quenching. The diffraction pattern distortion shows a threshold dependence with laser fluence, not seen for magnetization quenching, consistent with a picture of domain wall motion with pinning sites. Supported by simulations, we show that a speed of ≈66 km/s for highly curved domain walls can explain the experimental data. While our data agree with the prediction of extreme, nonequilibrium wall speeds locally, it differs from the details of the theory, suggesting that additional mechanisms are required to fully understand these effects.

Quantifying Spin-Mixed States in Ferromagnets.

We quantify the presence of spin-mixed states in ferromagnetic 3D transition metals by precise measurement of the orbital moment. While central to phenomena such as Elliot-Yafet scattering, quantification of the spin-mixing parameter has hitherto been confined to theoretical calculations. We demonstrate that this information is also available by experimental means. Comparison of ferromagnetic resonance spectroscopy with x-ray magnetic circular dichroism results show that Kittel's original derivation of the spectroscopic g factor requires modification, to include spin mixing of valence band states. Our results are supported by ab initio relativistic electronic structure theory.

Near- and Extended-Edge X-Ray-Absorption Fine-Structure Spectroscopy Using Ultrafast Coherent High-Order Harmonic Supercontinua.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9} photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26} photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

Nondestructive Measurement of the Evolution of Layer-Specific Mechanical Properties in Sub-10 nm Bilayer Films.

We use short wavelength extreme ultraviolet light to independently measure the mechanical properties of disparate layers within a bilayer film for the first time, with single-monolayer sensitivity. We show that in Ni/Ta nanostructured systems, while their density ratio is not meaningfully changed from that expected in bulk, their elastic properties are significantly modified, where nickel softens while tantalum stiffens, relative to their bulk counterparts. In particular, the presence or absence of the Ta capping layer influences the mechanical properties of the Ni film. This nondestructive nanomechanical measurement technique represents the first approach to date able to distinguish the properties of composite materials well below 100 nm in thickness. This capability is critical for understanding and optimizing the strength, flexibility and reliability of materials in a host of nanostructured electronic, photovoltaic, and thermoelectric devices.

Probing the timescale of the exchange interaction in a ferromagnetic alloy.

The underlying physics of all ferromagnetic behavior is the cooperative interaction between individual atomic magnetic moments that results in a macroscopic magnetization. In this work, we use extreme ultraviolet pulses from high-harmonic generation as an element-specific probe of ultrafast, optically driven, demagnetization in a ferromagnetic Fe-Ni alloy (permalloy). We show that for times shorter than the characteristic timescale for exchange coupling, the magnetization of Fe quenches more strongly than that of Ni. Then as the Fe moments start to randomize, the strong ferromagnetic exchange interaction induces further demagnetization in Ni, with a characteristic delay determined by the strength of the exchange interaction. We can further enhance this delay by lowering the exchange energy by diluting the permalloy with Cu. This measurement probes how the fundamental quantum mechanical exchange coupling between Fe and Ni in magnetic materials influences magnetic switching dynamics in ferromagnetic materials relevant to next-generation data storage technologies.

Phase-sensitive detection of spin pumping via the ac inverse spin Hall effect.

We use a phase-sensitive, quantitative technique to separate inductive and ac inverse spin Hall effect (ISHE) voltages observed in Ni(81)Fe(19)/normal metal multilayers under the condition of ferromagnetic resonance. For Ni(81)Fe(19)/Pt thin film bilayers and at microwave frequencies from 7 to 20 GHz, we observe an ac ISHE magnitude that is much larger than that expected from the dc spin Hall angle Θ(SH)(Pt) = 0.1. Furthermore, at these frequencies, we find an unexpected, ≈ 110° phase of the ac ISHE signal relative to the in-plane component of the resonant magnetization precession. We attribute our findings to a dominant intrinsic ac ISHE in Pt.

Full field tabletop EUV coherent diffractive imaging in a transmission geometry.

We demonstrate the first general tabletop EUV coherent microscope that can image extended, non-isolated, non-periodic, objects. By implementing keyhole coherent diffractive imaging with curved mirrors and a tabletop high harmonic source, we achieve improved efficiency of the imaging system as well as more uniform illumination at the sample, when compared with what is possible using Fresnel zone plates. Moreover, we show that the unscattered light from a semi-transparent sample can be used as a holographic reference wave, allowing quantitative information about the thickness of the sample to be extracted from the retrieved image. Finally, we show that excellent tabletop image fidelity is achieved by comparing the retrieved images with scanning electron and atomic force microscopy images, and show superior capabilities in some cases.

Mode- and size-dependent Landau-Lifshitz damping in magnetic nanostructures: evidence for nonlocal damping.

We demonstrate a strong dependence of the effective damping on the nanomagnet size and the particular spin-wave mode that can be explained by the theory of intralayer transverse-spin pumping. The effective Landau-Lifshitz damping is measured optically in individual, isolated nanomagnets as small as 100 nm. The measurements are accomplished by use of a novel heterodyne magneto-optical microwave microscope with unprecedented sensitivity. Experimental data reveal multiple standing spin-wave modes that we identify by use of micromagnetic modeling as having either localized or delocalized character, described generically as end and center modes. The damping parameter of the two modes depends on both the size of the nanomagnet as well as the particular spin-wave mode that is excited, with values that are enhanced by as much as 40% relative to that measured for an extended film. Contrary to expectations based on the ad hoc consideration of lithography-induced edge damage, the damping for the end mode decreases as the size of the nanomagnet decreases. The data agree with the theory for damping caused by the flow of intralayer transverse spin currents driven by the magnetization curvature. These results have serious implications for the performance of nanoscale spintronic devices such as spin-torque-transfer magnetic random access memory.

Controlling the competition between optically induced ultrafast spin-flip scattering and spin transport in magnetic multilayers.

The study of ultrafast dynamics in magnetic materials provides rich opportunities for greater fundamental understanding of correlated phenomena in solid-state matter, because many of the basic microscopic mechanisms involved are as-yet unclear and are still being uncovered. Recently, two different possible mechanisms have been proposed to explain ultrafast laser induced magnetization dynamics: spin currents and spin-flip scattering. In this work, we use multilayers of Fe and Ni with different metals and insulators as the spacer material to conclusively show that spin currents can have a significant contribution to optically induced magnetization dynamics, in addition to spin-flip scattering processes. Moreover, we can control the competition between these two processes, and in some cases completely suppress interlayer spin currents as a sample undergoes rapid demagnetization. Finally, by reversing the order of the Fe/Ni layers, we experimentally show that spin currents are directional in our samples, predominantly flowing from the top to the bottom layer.

Tabletop extreme ultraviolet reflectometer for quantitative nanoscale reflectometry, scatterometry, and imaging.

Imaging using coherent extreme-ultraviolet (EUV) light provides exceptional capabilities for the characterization of the composition and geometry of nanostructures by probing with high spatial resolution and elemental specificity. We present a multi-modal tabletop EUV imaging reflectometer for high-fidelity metrology of nanostructures. The reflectometer is capable of measurements in three distinct modes: intensity reflectometry, scatterometry, and imaging reflectometry, where each mode addresses different nanostructure characterization challenges. We demonstrate the system's unique ability to quantitatively and non-destructively measure the geometry and composition of nanostructures with tens of square microns field of view and sub-nanometer precision. Parameters such as surface and line edge roughness, density, nanostructure linewidth, and profile, as well as depth-resolved composition, can be quantitatively determined. The results highlight the applicability of EUV metrology to address a wide range of semiconductor and materials science challenges.

Kinetics of zero valent iron nanoparticle oxidation in oxygenated water.

Zero valent iron (ZVI) nanoparticles are versatile in their ability to remove a wide variety of water contaminants, and ZVI-based bimetallic nanoparticles show increased reactivity above that of ZVI alone. ZVI nanoparticles degrade contaminants through the reactive species (e.g., OH*, H(2(g)), H(2)O(2)) that are produced during iron oxidation. Measurement and modeling of aqueous ZVI nanoparticle oxidation kinetics are therefore necessary to optimize nanoparticle design. Stabilized ZVI and iron-nickel nanoparticles of approximately 150 nm in diameter were synthesized through solution chemistry, and nanoparticle oxidation kinetics were determined via measured mass change using a quartz crystal microbalance (QCM). Under flowing aerated water, ZVI nanoparticles had an initial exponential growth behavior indicating surface-dominated oxidation controlled by migration of species (H(2)O and O(2)) to the surface. A region of logarithmic growth followed the exponential growth which, based on the Mott-Cabrera model of thin oxide film growth, suggests a reaction dominated by movement of species (e.g., iron cations and oxygen anions) through the oxide layer. The presence of ethanol or a nickel shell on the ZVI nanoparticles delayed the onset of iron oxidation and reduced the extent of oxidation. In oxygenated water, ZVI nanoparticles oxidized primarily to the iron oxide-hydroxide lepidocrocite.

Effect of gas composition during Pt sputtering on structural and magnetic properties of CoFeB thin films.

Ultrathin Ta/CoFeB/Pt trilayer structures are relevant to a wide range of spintronic applications, from magnetic tunnel junctions to skyrmionics devices. Controlling the perpendicular magnetic anisotropy, Gilbert damping and Dzyaloshinskii-Moriya interaction in the CoFeB layer is key for these applications. We examine the role of sputter gas composition during the Pt overlayer deposition of a Ta/CoFeB/Pt trilayer in Ar, Kr and Xe working gas environments during direct current magnetron sputtering. Decreasing density of the Pt layer (from 21 g/cm3 to 15 g/cm3) was apparent in specular x-ray reflectivity measurements of the trilayer films when increasing the molecular weight of the sputtering gas from Ar to Kr to Xe. Significant effects on the Gilbert damping and the interfacial Dzyaloshinskii-Moriya interaction (DMI) energy were observed, with increases in the damping from 0.037(1) to 0.042(1) to 0.048(1), and reductions in the interfacial DMI from 0.47(4) mJ/m2 to 0.45(5) mJ/m2 to 0.39(4) mJ/m2. The ability to control the perpendicular magnetization and DMI strength of these materials through judicious interfacial control is a means toward magnetic devices with better stability at smaller lateral dimension, key to device scaling for spintronic device arrays.

Skyrmions in synthetic antiferromagnets and their nucleation via electrical current and ultra-fast laser illumination.

Magnetic skyrmions are topological spin textures that hold great promise as nanoscale information carriers in non-volatile memory and logic devices. While room-temperature magnetic skyrmions and their current-induced motion were recently demonstrated, the stray field resulting from their finite magnetisation and their topological charge limit their minimum size and reliable motion. Antiferromagnetic skyrmions allow to lift these limitations owing to their vanishing magnetisation and net zero topological charge, promising ultra-small and ultra-fast skyrmions. Here, we report on the observation of isolated skyrmions in compensated synthetic antiferromagnets at zero field and room temperature using X-ray magnetic microscopy. Micromagnetic simulations and an analytical model confirm the chiral antiferromagnetic nature of these skyrmions and allow the identification of the physical mechanisms controlling their size and stability. Finally, we demonstrate the nucleation of synthetic antiferromagnetic skyrmions via local current injection and ultra-fast laser excitation.

Correlation between Dzyaloshinskii-Moriya interaction and orbital angular momentum at an oxide-ferromagnet interface.

We report on the Dzyaloshinskii-Moriya (DMI) interaction at the interface between a ferromagnet and an oxide. We demonstrate experimentally that oxides can give rise to DMI. By comparison of systems comprised of Pt/Co90Fe10/oxide and Cu/Co90Fe10/oxide, we also show how oxidation of one interface can enhance and add to the total DMI of that generated by the Pt interface. This is due to the fact that the DMI on both interfaces promotes left-handed chirality. Finally, by use of ferromagnetic resonance spectroscopy, we show that the DMI and the spectroscopic splitting factor, which is a measure of the orbital momentum, are correlated. This indicates the importance of hybridization and charge transfer at the oxide interface for the DMI.

Nonlinear losses in magnon transport due to four-magnon scattering.

We report on the impact of nonlinear four-magnon scattering on magnon transport in microstructured Co25Fe75 waveguides with low magnetic damping. We determine the magnon propagation length with microfocused Brillouin light scattering over a broad range of excitation powers and detect a decrease of the attenuation length at high powers. This is consistent with the onset of nonlinear four-magnon scattering. Hence, it is critical to stay in the linear regime, when deriving damping parameters from the magnon propagation length. Otherwise, the intrinsic nonlinearity of magnetization dynamics may lead to a misinterpretation of magnon propagation lengths and, thus, to incorrect values of the magnetic damping of the system.

Ultrafast demagnetization dynamics at the M edges of magnetic elements observed using a tabletop high-harmonic soft x-ray source.

We use few-femtosecond soft x-ray pulses from high-harmonic generation to extract element-specific demagnetization dynamics and hysteresis loops of a compound material for the first time. Using a geometry where high-harmonic beams are reflected from a magnetized Permalloy grating, large changes in the reflected intensity of up to 6% at the M absorption edges of Fe and Ni are observed when the magnetization is reversed. A short pump pulse is used to destroy the magnetic alignment, which allows us to measure the fastest, elementally specific demagnetization dynamics, with 55 fs time resolution. The use of high harmonics for probing magnetic materials promises to combine nanometer spatial resolution, elemental specificity, and femtosecond-to-attosecond time resolution, making it possible to address important fundamental questions in magnetism.

Near-unity spin Hall ratio in Ni x Cu1-x alloys.

We report a large spin Hall effect in the 3d transition metal alloy Ni x Cu1-x for x ∈ {0.3, 0.75}, detected via the ferromagnetic resonance of a permalloy (Py = Ni80Fe20) film deposited in a bilayer with the alloy. A thickness series at x = 0.6, for which the alloy is paramagnetic at room temperature, allows us to determine the spin Hall ratio θ SH ≈ 1, spin diffusion length λs, spin mixing conductance G ⇅, and damping due to spin memory loss αSML. We compare our results with similar experiments on Py/Pt bilayers measured using the same method. Ab initio band structure calculations with disorder and spin-orbit coupling suggest an intrinsic spin Hall effect in Ni x Cu1-x alloys, although the experiments here cannot distinguish between extrinsic and intrinsic mechanisms.

Domain-wall motion and interfacial Dzyaloshinskii-Moriya interactions in Pt/Co/Ir(t Ir)/Ta multilayers.

The interfacial Dzyaloshinskii-Moriya interaction (DMI) is important for chiral domain walls (DWs) and for stabilizing magnetic skyrmions. We study the effects of introducing increasing thicknesses of Ir, from zero to 2 nm, into a Pt/Co/Ta multilayer between the Co and Ta layers. There is a marked increase in magnetic moment, due to the suppression of the dead layer at the interface with Ta, but the perpendicular anisotropy is hardly affected. All samples show a universal scaling of the field-driven DW velocity across the creep and depinning regimes. Asymmetric bubble expansion shows that DWs in all of the samples have the left-handed Néel form. The value of in-plane magnetic field at which the creep velocity shows a minimum drops markedly on the introduction of Ir, as does the frequency shift of the Stokes and anti-Stokes peaks in Brillouin light scattering (BLS) measurements. Despite this qualitative similarity, there are quantitative differences in the DMI strength given by the two measurements, with BLS often returning higher values. Many features in bubble expansion velocity curves do not fit simple models commonly used, namely a lack of symmetry about the velocity minimum and no difference in velocities at high in-plane fields. These features are explained by the use of a new model in which the depinning field is allowed to vary with in-plane field in a way determined from micromagnetic simulations. This theory shows that the velocity minimum underestimates the DMI field, consistent with BLS giving higher values. Our results suggest that the DMI at an Ir/Co interface has the same sign as the DMI at a Pt/Co interface.

Magnetoelasticity of Co25Fe75 thin films.

We investigate the magnetoelastic properties of Co25Fe75 and Co10Fe90 thin films by measuring the mechanical properties of a doubly clamped string resonator covered with multilayer stacks containing these films. For the magnetostrictive constants, we find λ Co25 Fe75 = (-20.68 ± 0.25) × 10-6 and λ Co10 Fe90 = (-9.80 ± 0.12) × 10-6 at room temperature, in contrast to the positive magnetostriction previously found in bulk CoFe crystals. Co25Fe75 thin films unite low damping and sizable magnetostriction and are thus a prime candidate for micromechanical magnonic applications, such as sensors and hybrid phonon-magnon systems.

High spin-wave propagation length consistent with low damping in a metallic ferromagnet.

We report ultralow intrinsic magnetic damping in Co25Fe75 heterostructures, reaching the low 10-4 regime at room temperature. By using a broadband ferromagnetic resonance technique in out-of-plane geometry, we extracted the dynamic magnetic properties of several Co25Fe75-based heterostructures with varying ferromagnetic layer thicknesses. By measuring radiative damping and spin pumping effects, we found the intrinsic damping of a 26 nm thick sample to be α 0 ≲ 3.18 × 10-4. Furthermore, using Brillouin light scattering microscopy, we measured spin-wave propagation lengths of up to (21 ± 1) µm in a 26 nm thick Co25Fe75 heterostructure at room temperature, which is in excellent agreement with the measured damping.