Sophie A. Morley

Scanning transmission X-ray microscopy and ptychography have become mature tools for high-resolution, element-specific imaging of nanoscale structures. However, transmission geometries impose stringent constraints on sample thickness and preparation, thereby limiting investigations of extended or bulk specimens, especially in the soft X-ray region. Here, we demonstrate reflection-geometry soft X-ray ptychography as a robust imaging mode. Instrumental feasibility and spatial resolution are established using a lithographically defined Siemens star and barcode test pattern on a multilayer substrate. We empirically demonstrate a full-pitch spatial resolution of ca. 45 nm from Fourier ring correlation analysis of the reconstructed object. The results highlight the potential of the reflection geometry for nondestructive X-ray studies of materials without the need for transmissive samples.

Magnetic skyrmions are topologically protected spin textures that can act as reconfigurable nanoscale information carriers. In synthetic antiferromagnets, interlayer exchange coupling provides a control parameter beyond the interfacial Dzyaloshinskii-Moriya interaction and magnetic anisotropy. Here we engineer a synthetic antiferromagnet of two chemically distinct ferromagnets, CoB and CoFeB, in which the external field and interlayer exchange act asymmetrically on the sublattices. Their competition, acting as an effective field, gives rise to two skyrmion families in different field regimes: conventional-polarity skyrmions at large fields, and inverse-polarity skyrmions at smaller fields, where the effective field reverses sign. Using element-resolved X-ray magnetometry, correlative magnetic force and Lorentz transmission electron microscopies, and micromagnetic modelling, we show that all textures reside solely in the CoFeB layers, driven by a Ruderman-Kittel-Kasuya-Yosida exchange field from the CoB layers. This effective-field route enables programmable three-dimensional spin textures with layer-selected polarity for skyrmion-based computing.

We demonstrate an experimental approach to determine magneto-optical effects that combines x-ray magnetic circular dichroism (XMCD) with x-ray interferometry, based on the concepts of Young's canonical double slit. By covering one of two slits with a magnetic thin film and employing XMCD, we show that it is possible to determine both the real and the imaginary parts of the complex refractive index by measuring the fringe shifts that occur due to a change in the sample magnetization. Our hybrid spectroscopic-interferometric methodology provides a means to probe changes in the magnetic refractive index in terms of the electron spin moment.

Scanning transmission X-ray microscopy and ptychography have become mature tools for high-resolution, element-specific imaging of nanoscale structures. However, transmission geometries impose stringent constraints on sample thickness and preparation, thereby limiting investigations of extended or bulk specimens, especially in the soft X-ray region. Here, we demonstrate reflection geometry soft X-ray ptychography as a robust imaging mode. Instrumental feasibility and spatial resolution are established using a lithographically defined Siemens star and barcode test pattern on a multilayer substrate. We empirically demonstrate a full-pitch spatial resolution of ca. 45 nm from Fourier ring correlation analysis of the reconstructed object. The results highlight the potential of the reflection geometry for nondestructive X-ray studies of materials without the need for transmissive samples.

A nematic phase lacks translation order but has orientational order. Nematic phases have been discovered in a variety of systems, including liquid crystals, correlated materials, and superconductors. Here, we report on a magnetic nematic phase, where the basis components are composed of magnetic helices. We directly probed the order parameters associated with the magnetic helices using resonant soft x-ray scattering and find two distinct nematic phases with complex spatiotemporal signatures. Using x-ray correlation spectroscopy, we find that near the phase boundary between the two nematic phases, fluctuations coexist on multiple disparate timescales. Our micromagnetic simulations and density functional theory calculations show that the fluctuations occur concomitantly with a reorientation of the magnetic helices, indicating spontaneous symmetry breaking and the emergence of additional degrees of freedom. Our results provide a framework for characterizing exotic phases that can be extended to a broad class of physical systems.

Fluctuations of the order parameter near the phase transition boundary in complex oxides could be key to designing probabilistic bits and stochastic synapses. Direct probes of fluctuations how- ever are non-trivial due to the requirement of coherent spatio-temporal probes. Here, we report magnetic and lattice fluctuation dynamics in prototypical perovskite nickelate systems of NdNiO3 and SmNiO3 using X-ray photon correlation spectroscopy. For NdNiO3, our studies show strong coupling of structural and magnetic order parameters with slowdown of fluctuation timescales by one order of magnitude near Néel temperature irrespective of the epitaxial strain of the film. For SmNiO3, no such slowdown is observed emphasizing the distinct nature of structural fluctuations. Our measurements of diffraction wavevector dependence, indicate that short range structural fluctuations are surprisingly slow (3-5x slower) compared to long range fluctuations. Our results reveal novel insights into fluctuations enabled by coherent x-rays, expanding the unique capability of spatio-temporal probes to investigate quantum materials.

The Fe/Gd multilayer system hosts a number of magnetic phases, such as stripe, mixed stripe and skyrmion, skyrmion lattice, and isolated skyrmions for a wide range of temperature and magnetic field. We report different Hall transport signals in a Fe/Gd system through multimodal correlative resonant soft x-ray scattering (RSXS), Hall effect, magneto-optic Kerr effect, and transmission x-ray microscopy measurements. The simultaneous nature of the RSXS and Hall transport measurements allowed us to accurately connect various features in the transport data with the specific magnetic phases. We found that the topological Hall effect (THE) shows peaks with opposite signs, which we attribute to two different mechanisms. Our multimodal correlative study indicates that the sign reversal in THE occurs when the system transforms to and from a skyrmion lattice and low density isolated skyrmion phases. We propose that the skyrmion lattice contributes to the THE through a Berry phase induced emergent magnetic field mechanism in one case, and a skew scattering mechanism corresponding to the isolated low density skyrmion state.

Van der Waals (vdW) magnetic materials are comprised of layers of atomically thin sheets, making them ideal platforms for studying magnetism at the two-dimensional (2D) limit. These materials are at the center of a host of novel types of experiments, however, there are notably few pathways to directly probe their magnetic structure. We confirm the magnetic order within a single crystal of NiPS₃ and show it can be accessed with resonant elastic X-ray diffraction along the edge of the vdW planes in a carefully grown crystal by detecting structurally forbidden resonant magnetic X-ray scattering. We find the magnetic order parameter has a critical exponent of β ~ 0.36, indicating that the magnetism of these vdW crystals is more adequately characterized by the three-dimensional (3D) Heisenberg universality class. We verify these findings with first-principles density functional theory, Monte-Carlo simulations, and density matrix renormalization group calculations.

The presence of multiple competing periodicities may result in a system to go through states with modulated periodicities, an example of which is the self-similar staircase-like structure called the Devil’s Staircase. Herein we report on a novel staircase structure of domain periodicity in an amorphous and centrosymmetric Fe/Gd magnetic thin film system wherein the reciprocal space wavevector Q due to the ordered stripe domains does not evolve continuously, rather exhibits a staircase structure. Resonant X-ray scattering experiments show jumps in the periodicity of the stripe domains as a function of an external magnetic field. When resolved in components, the length-scale step change along Q_x was found to be an integral multiple of a minimum step height of 7 nm, which resembles closely to the exchange length of the system. Modeling the magnetic texture in the Fe/Gd system as an achiral spin arrangement, we have been able to reproduce the steps in the magnetization using a Landau-Lifshitz spin dynamics calculation. Our results indicate that anisotropy and not the dipolar interaction is the dominant cause for the staircase pattern, thereby revealing the effect of achiral magnetism.

X-ray beams with orbital angular momentum (OAM) are a promising tool for x-ray characterization techniques. Beams with OAM have a helicity—an azimuthally varying phase—which leads to a gradient of the light field. New material properties can be probed by utilizing the helicity of an OAM beam. Here, we demonstrate a dichroic effect in resonant diffraction from an artificial antiferromagnet with a topological defect. We found that the scattered OAM beam has circular dichroism at the antiferromagnetic Bragg peak whose sign is coupled to its helicity, which reveals the real-space configuration of the antiferromagnetic ground state. Thermal cycling of the artificial antiferromagnet can change the ground state, as indicated by reversal of the sign of circular dichroism. This result is one of the first demonstrations of a soft x-ray spectroscopy characterization technique utilizing the OAM of x rays. This helicity-dependent circular dichroism exemplifies the potential to utilize OAM beams to probe matter in a way that is inaccessible using currently available x-ray techniques.