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Rafal E. Dunin-Borkowski

Publications and source records attributed to Rafal E. Dunin-Borkowski.

At least 19 recordsLinked to original sources

Compositional and Magnetic Characterisation of Oblique Co and Fe Nanowire Structures Fabricated Using Focused Electron Beam Induced Deposition

Focused electron beam induced deposition (FEBID) is an additive manufacturing technique uniquely suited for fabricating functional 3D nanostructures for a range of applications, including spintronic devices. However, the variation of growth dynamics associated with lateral movement of the electron beam results in structures with non-uniform composition when fabricating intricate 3D geometries. Herein, we measure changes in atomic composition and corresponding changes in magnetic induction in 3D ferromagnetic nanostructures with overhanging elements, e.g. bridges or arches. To investigate the effects of electron beam lateral movement, we fabricated Co and Fe nanowire (NW) structures with growth angle relative to the optic axis varying from 0° to 90°. The (scanning) transmission electron microscopy techniques of electron energy loss spectroscopy and off-axis electron holography were performed to map the NW elemental composition and magnetic induction as a function of NW growth angle. Comparison of the results reveals a reduction in metal content with increased growth angle in FEBID NWs. The magnitude of metal content reduction can be tuned by controlling electron beam parameters, and ferromagnetic NWs with approximately equal metal content at growth angles from 0° to 60° were fabricated by using the lowest viable electron beam voltage and the highest viable beam current to reduce the interaction volume and increase the metal content, respectively.

cond-mat.mes-hall↗

Inertial Dynamics of a Skymeron

Topological spin textures in antiferromagnets inherit the compensated magnetic order of the host material, resulting for skyrmions in the suppression of the skyrmion Hall effect and enabling ultrafast dynamics that make them attractive for low-power spintronic devices. In intrinsic antiferromagnets, the two sublattices are identical, but synthetic antiferromagnets offer additional control mechanisms by enabling independent tuning of the properties of two ferromagnetic layers. Analogous to a ferrimagnet, the total magnetic moment can be adjusted by compensating the two-layer moments. Here, we demonstrate that tuning the effective magnetic anisotropy difference between the two layers drives a spin-flop transition where one layer reorients and thus stabilizes an orthogonal configuration with one layer oriented along the out-of-plane direction and the other in-plane. In this transition, an antiferromagnetic skyrmion undergoes a homotopic reconfiguration into a complex spin texture comprising a skyrmion coupled to an in-plane bimeron. Element-specific X-ray microscopy resolves this texture layer by layer: one hosts an out-of-plane skyrmion coupled to an in-plane bimeron in the other. We refer to this previously unexplored three-dimensional spin texture as a skymeron. By using time-resolved pump-probe X-ray microscopy, we discover unique polarity ,dependent dynamics during current pulses: a short post-pulse inertia-like continuation of the motion, and a slower return towards the pinned initial state. Micromagnetic simulations reveal that the inertia-like propagation originates from the finite-time relaxation of reorientation of the skymeron. Our results establish layer-selective anisotropy engineering as a route to uncharted composite spin textures with internal dynamical degrees of freedom, not possible in conventional antiferromagnets with identical sublattices.

cond-mat.mes-hall↗

Formation and Magnetic Drive of 1D-Confined Topological Defect Lines in Crystals with D$_{2d}$ Symmetry

Designing and controlling topological spin textures within non-collinear magnetic backgrounds is central to the development of low-dissipation spintronic devices. Here we propose a general mechanism based on tunable magnetic anisotropy that enables the realization of one-dimensional topological defect lines embedded within intrinsic spin-spiral states of uniaxial D$_{2d}$-symmetric magnets, and is broadly applicable across diverse material platforms. Using Lorentz transmission electron microscopy and off-axis electron holography, we show that introducing in-plane magnetic anisotropy into the helical ground state stabilizes adjacent domains of conical helices with in-plane propagation vectors, sharing the same handedness but exhibit opposite net magnetization. The resulting interfacial mismatch generates confined bimeron-chains. Significantly, these defect lines are not merely induced merons; their presence is mandated by the specific D$_{2d}$ symmetry constraints inherent to the system. Applying weak magnetic fields along the conical axis drives counter-propagating motion of adjacent bimeron-chains along the helical stripes, while anisotropy-mediated confinement enables track-stable transverse drift free transport. The present work establishes a clear route to stabilize and control topological spin textures within intrinsically non-collinear magnetic states, advancing fundamental understanding and enabling low-dissipation, scalable spintronic device concepts.

cond-mat.mtrl-sci↗

Quantification of magnetic interactions in van der Waals heterostructures using Lorentz transmission electron microscopy and electron holography

Magnetic van der Waals (vdW) materials are promising for memory and logic applications because of their highly tunable magnetic properties and compatibility with vdW heterostructure devices. However, coupling between magnetic textures in stacked layers is difficult to resolve in conventional plan-view measurements because the magnetic signal is integrated over the sample thickness. Here, these interactions are quantified in Fe$_3$GeTe$_2$ (FGT)/graphite/FGT heterostructures using cross-sectional Lorentz transmission electron microscopy and off-axis electron holography, enabling reconstruction of the local magnetic induction within and between the layers. Domain alignment weakens with increasing FGT separation, yielding a stray-field coupling length scale of $λ= 37 \pm 7$ nm for the cross-sectional geometry studied here, corresponding to the average separation at which domain misalignment first emerges. This length scale corresponds to an approximately 23% reduction in the interlayer magnetic induction relative to bulk FGT. Surface effects result in a reduced magnetic induction compared to bulk FGT up to $\sim$100 nm from a surface. Comparisons of experimental data with model-based iterative reconstructions of the magnetization and micromagnetic simulations shows that the reduction in induction near surfaces is due to demagnetizing and stray fields. These results quantify the magnetic induction in stacked vdW magnets and guide the design of devices that require controllable coupling between magnetic textures.

cond-mat.mtrl-sci↗

Engineering altermagnetic symmetry to enable anomalous Hall response in Cr$_{1-x}$Mn$_x$Sb

Altermagnets are a promising class of materials for spintronic applications. However, compounds that simultaneously combine the symmetry required to support an anomalous Hall effect with good metallic conductivity and magnetic ordering temperatures well above room temperature have remained elusive. Here, we demonstrate that partial substitution of Cr by Mn in epitaxial CrSb(100) thin films provides a viable route to engineer the combined structural and magnetic symmetry necessary to enable an otherwise symmetry-forbidden anomalous Hall effect. We systematically explore the magnetic phase diagram of Cr(Mn)Sb thin films including neutron diffraction. This allows us to identify a magnetic symmetry that supports the anomalous Hall effect, which we demonstrate in Cr(0.75)Mn(0.25)Sb. Guided by Landau theory, we model the field-driven reorientation of the Neel vector and the resulting anomalous Hall response, achieving good qualitative agreement with the experimental observations.

cond-mat.mtrl-sci↗

Transverse quantum-state characterization of programmable electron optics

Programmable electron optics -- electronically controlled phase plates -- underpin proposals from dose-efficient phase imaging to shaped-electron X-ray sources, nearly all assuming a pure, fully coherent delivered wave whose purity has never been measured. Here we reconstruct the transverse density matrix of a microelectromechanical electrostatic spiral phase plate by mixed-state ptychography, from one four-dimensional STEM scan per state and without added hardware. The delivered beam is substantially mixed: its purity falls from approximately 0.47 to approximately 0.24 as the applied bias grows, inconsistent with a fixed lateral source-blur model, while the real-space coherence width stays near 1 nm. The same scans calibrate the device in situ, allow virtual orbital-angular-momentum sorting and, through a partial-coherence-aware transfer theory, indicate that purifying the output could improve dose efficiency roughly threefold. One acquisition thus becomes a quantum-state acceptance test for programmable electron optics, supplying the purity and coherence that emerging phase-plate and diffractive-imaging schemes assume but leave unquantified.

physics.optics↗

Quantum tomography of inelastic electron scattering \emph{via} orbital angular momentum states

The physical properties of a quantum system, whether pure or mixed, are described fully by its density matrix. Recovery of the density matrix through projective measurements -- referred to as quantum state tomography -- is a cornerstone of quantum optics and metrology. The implementation of this approach in transmission electron microscopy, in particular for the characterisation of an electron beam after inelastic scattering, has remained a longstanding challenge as a result of the complexity of scanning high-dimensional phase spaces, with the number of required measurements growing quadratically with space dimensionality. Here, we introduce a simplified approach by restricting tomography to the electron orbital angular momentum (OAM) subspace. By using an electron optical device known as an OAM sorter, we discretise the phase space into a finite set of measurable states, thus significantly reducing the experimental and computational burden. The resulting measurements suffice to probe essential features of inelastic scattering. We demonstrate the technique by studying the inelastic scattering of a structured electron probe exciting volume plasmons in a carbon film. The combined use of a structured beams and OAM-resolved quantum tomography reveals symmetry-breaking effects and offers insight into the coherence and evolution of the scattered quantum states. Analysis of the diagonalised density matrices further reveals the nature of the induced state transitions, demonstrating the power of the approach for quantum tomography of electron scattering.

quant-ph↗

Polarization of photoluminescence by optically driven orbital reconstruction in magnetically ordered CrCl3

Control of magnetic order through optical manipulation of orbital states can be realized in a wide range of materials, including insulators. In the latter case, electrons are excited into different electronic states, whose character may be a complex result of spin-orbit-lattice coupling. Here, we use a combination of polarization-resolved photoluminescence spectroscopy and density functional theory calculations to study excited Cr3+ ions in bulk, insulating antiferromagnetic CrCl3. Our results demonstrate a temperature-dependent preferential polarization direction below ~17 K, which reorients in the presence of an applied in-plane magnetic field. Density functional theory calculations reveal a local distortion of the ligand field and the generation of out-of-plane spin and orbital moments, following Cr3+ ion excitation. These changes link the photoluminescence polarization to the magnetic state of CrCl3. Our findings provide insight into the excited-state electronic structure of Cr3+ ions and suggest that CrCl3 is a promising candidate for opto-orbitronic applications.

cond-mat.mtrl-sci↗

Towards reliable electrical measurements of superconducting devices inside a transmission electron microscope

Correlating structure with electronic functionality is central to the engineering of quantum materials and devices whose properties depend sensitively on disorder. Transmission electron microscopy (TEM) offers high spatial resolution together with access to structural, electronic, and magnetic degrees of freedom. However, operando electrical transport measurements on functional quantum devices remain rare, particularly at liquid helium temperature. Here, we demonstrate electrical transport measurements of niobium nitride (NbN) devices inside a TEM using a continuous-flow liquid-helium-cooled sample holder. By optimizing a thermal radiation shield to limit radiation from the nearby pole pieces of the objective lens, we achieve an estimated base sample temperature of 8-9 K, as inferred from the superconducting transition temperatures of our devices. We find that both electron beam illumination and objective lens excitation perturb the superconducting state. In addition, we evaluate the imaging capabilities and stability of the sample holder at low temperature by imaging the magnetic domain structure of the van der Waals ferromagnet CrBr$_3$. Finally, we perform calculations that underscore the importance of cryo-shielding for minimizing thermal radiation onto the device. This capability enables correlative low-temperature TEM studies, in which structural, spectroscopic, and electrical transport data can be obtained from the same device, thereby providing a platform for probing the microscopic origins of quantum phenomena.

cond-mat.supr-con↗

Physics-informed Bayesian Optimization for Quantitative High-Resolution Transmission Electron Microscopy

Quantitative high-resolution transmission electron microscopy (HRTEM) provides an indispensable means to understand the structure-property relationships of a material in atomic dimensions. Successful quantification requires reliable retrieval of essential atomic structural information despite artifacts arising from unwanted but practically unavoidable imaging imperfections. Experimental observation carried out in tandem with model-based iterative image simulation shows vast applications in quantitative structural and chemical determination of objects spanning zero to three dimensions [Prog. Mater. Sci. 133, 101037, 2023]. However, the large number of parameters involved in the simulations make the current multi-step, user-guided iterative approach highly time consuming, thereby restricting its application primarily to small sample areas and to experienced users. In this work, we implement and apply a physics-informed Bayesian optimization (BO) framework to advance HRTEM quantification towards full automation and large-field-of-view analysis. Unlike conventional optimization approaches, our method adopts a stepwise strategy that fully leverages the strength of BO in handling high-dimensional parameters, while its probabilistic engine rigorously and efficiently refines the parameter space to enable rapid quantification. Using a BaTiO3 single crystal that contains heavy, medium and light elements as a model system, we demonstrate that the three-dimensional crystal structure can be determined from a single HRTEM image with a three to four order-of-magnitude improvement in time efficiency. This approach thus opens new avenues for fast and automated image quantification over larger sample volumes and, potentially, in the time domain.

physics.comp-ph↗

Designing electrostatic MEMS-based electron optics: the case of the spiral phase plate

A new generation of microfabricated MEMS for electron optics is changing electron microscopy for the better. These devices allow operations on the electron beam that are impossible with conventional electron optics. Unprecedented phase landscapes like tunable spiral phase plates and localized strong phase gradients are just some examples of what can be achieved. This work establishes the methodological foundation to design and control MEMS based phase plates. The design strategy is rooted on a novel analytical and numerical modeling of thin electrodes with accurate account of the fringing fields having a major role in the thin-MEMS geometry. We designed, fabricated and characterized experimentally a spiral phase plate, and assessed the quality of the generated vortex beam while discussing the most relevant control parameters and design approaches.

physics.ins-det↗

Magnetic skyrmion lattice disclinations in pentagon- and heptagon-shaped FeGe crystals

Magnetic skyrmions in chiral magnets typically arrange into hexagonal lattices, with their structural order influenced by factors such as temperature, external magnetic fields and geometric constraints. While translational defects in skyrmion lattices such as dislocations have been extensively studied, individual angular defects, or disclinations, remain largely unexplored. Here, we report on the stabilization of five-fold and seven-fold disclinations in pentagon- and heptagon-shaped FeGe nanocrystals created using focused ion beam milling. The magnetic and elastic structures of the disclinated lattices are investigated using Fresnel imaging and off-axis electron holography in a transmission electron microscope. The results are supported by micromagnetic simulations and analytical models based on linear elasticity theory.

cond-mat.mtrl-sci↗

Residual neural-field ptychography for dose-efficient electron, X-ray, and optical nanoscopy

Ptychography spans from sub-angstrom to meter scales yet suffers from convergence instability and excessive data redundancy. Here we introduce self-correcting residual neural fields as a dose-efficient framework for electron, X-ray, and optical ptychography. Unlike approaches that split complex fields, our complex-valued architecture employs holomorphic phasor activation e^iωz to preserve intrinsic phase-amplitude coupling. We reformulate reconstruction as residual learning, where the network learns only corrections to physical priors rather than complete wavefields. By embedding the physical model as a differentiable layer within the network, we enable end-to-end automatic differentiation where experimental parameters are jointly corrected alongside the neural fields. We validate our scheme across conventional, near-field, coded, and Fourier ptychography and achieve record-breaking lensless resolution of 244-nm linewidth with visible light. Extending to electron wavelengths, we reveal synaptic connectivity in brain sections with superior performance over conventional approaches. Our framework provides a solution for high-throughput, dose-efficient nanoscopy across the electromagnetic spectrum.

physics.optics↗

Identifying grain boundary and intragranular pinning centres in Sm2(Co,Fe,Cu,Zr)17 permanent magnets to guide performance optimisation

Permanent magnets draw their properties from a complex interplay of chemical composition and phase, each with their associated intrinsic magnetic properties. Gaining an understanding of these interactions is the key to deciphering the origins of a permanent magnets' magnetic performance and facilitate the engineering of much improved-performing magnets. Here, we use advanced multiscale microscopy and microanalysis on a bulk Sm2(Co,Fe,Cu,Zr)17 pinning-type high-performance magnet with outstanding thermal and chemical stability. Comparison of the microstructure in regions of different composition, we demonstrate that the pinning of magnetic domains, imaged by nanoscale magnetic induction mapping, is controlled by the composition and atomic arrangement of copper. This is confirmed by micromagnetic simulations. Contrary to the belief that grain boundaries are "weak links" in magnetic materials, we demonstrate grain boundaries undergo magnetization reversal at relatively low fields (0.1-0.3 T), but this remains confined to these regions and does not significantly impact the magnet's coercivity. Our results showcase that it is the optimal microstructure within the grain itself that is crucial for achieving the desired magnetic properties.

cond-mat.mtrl-sci↗

Direct observation of nanoscale pinning centers in Ce(Co0.8Cu0.2)5.4 permanent magnets

Permanent magnets containing rare earth elements are essential components for the electrification of society. Ce(Co1-xCux)5 permanent magnets are a model system known for their substantial coercivity, yet the underlying mechanism remains unclear. Here, we investigate Ce(Co0.8Cu0.2)5.4 magnets with a coercivity of ~1 T. Using transmission electron microscopy (TEM) and atom probe tomography (APT), we identify a nanoscale cellular structure formed by spinodal decomposition. Cu-poor cylindrical cells (~5-10 nm in diameter, ~20 nm long) have a disordered CeCo5-type structure and a composition Ce(Co0.9Cu0.1)5.3. Cu-rich cell boundaries are ~ 5 nm thick and exhibit a modified CeCo5 structure, with Cu ordered on the Co sites and a composition Ce(Co0.7Cu0.3)5.0. Micromagnetic simulations demonstrate that the intrinsic Cu concentration gradients up to 12 at.% Cu/nm lead to a spatial variation in magnetocrystalline anisotropy and domain wall energy, resulting in effective pinning and high coercivity. Compared to Sm2Co17-type magnets, Ce(Co0.8Cu0.2)5.4 displays a finer-scale variation of conventional pinning with lower structural and chemical contrast in its underlying nanostructure. The identification of nanoscale chemical segregation in nearly single-phase Ce(Co0.8Cu0.2)5.4 magnets provides a microstructural basis for the long-standing phenomenon of "giant intrinsic magnetic hardness" in systems such as SmCo5-xMx, highlighting avenues for designing rare-earth-lean permanent magnets via controlled nanoscale segregation.

cond-mat.mtrl-sci↗

Topotactic phase transition in epitaxial La0.7Sr0.3MnO3-δ films induced by oxygen getter assisted thermal annealing

Oxygen vacancies play a crucial role in controlling the physical properties of complex oxides. In La0.7Sr0.3MnO3-δ, the topotactic phase transition from Perovskite (PV) to Brownmillerite (BM) can be triggered e.g. via oxygen removal during thermal annealing. Here we report on a very efficient thermal vacuum annealing method using aluminum as an oxygen getter material. The topotactic phase transition is characterized by X-ray Diffraction which confirms a successful transition from PV to BM in La0.7Sr0.3MnO3-δ thin films grown via physical vapor deposition. The efficiency of this method is confirmed using La0.7Sr0.3MnO3-δ micron-sized bulk powder. The accompanying transition from the original Ferromagnetic (FM) to an Antiferromagnetic (AF) state and the simultaneous transition from a metallic to an insulating state is characterized using Superconducting Quantum Interference Device (SQUID)-magnetometry and Alternating Current (AC) resistivity measurements, respectively. The near surface manganese oxidation states are probed by synchrotron X-ray Absorption Spectroscopy. Moreover, X-ray Reflectivity, Atomic Force Microscopy and Scanning Transmission Electron Microscopy reveal surface segregation and cation redistribution during the oxygen getter assisted annealing process.

cond-mat.mtrl-sci↗

Switchable Exchange Bias Resulting from Correlated Domain Structures in Orthogonally Coupled Antiferromagnet/Ferromagnet van der Waals Heterostructures

Van der Waals (vdW) magnetic heterostructures offer a versatile platform for engineering interfacial spin interactions with atomic precision, enabling nontrivial spin textures and dynamic behaviors. In this work, we report robust asymmetric magnetization reversal and exchange bias in Fe3GeTe2 (FGT), driven by interlayer exchange coupling with the A-type antiferromagnet CrSBr. Despite the orthogonal magnetic anisotropies out-of-plane easy axis in FGT and in-plane in CrSBr, we observe a strong interfacial exchange interaction that gives rise to pronounced and switchable exchange bias and asymmetric switching in FGT, persisting up to the Néel temperature of CrSBr (132 K) as revealed by anomalous Hall effect measurements. We uncover the microscopic origin of this behavior through cross-sectional magnetic imaging of the domain structure using off-axis electron holography. The results reveal that the asymmetric switching and exchange bias arise from the influence of CrSBr on the domain configuration of FGT, where the in-plane antiferromagnetic state of CrSBr promotes the formation of stripe-like domain structures in FGT with circular rotation of magnetization in the cross-sectional bc plane defined by the easy axes of both FGT and CrSBr. These findings elucidate the mechanism of exchange bias in orthogonally coupled van der Waals systems and demonstrate a pathway for stabilizing three-dimensional domain structures in ferromagnets through interfacial exchange interactions.

cond-mat.mtrl-sci↗

Identifying the Origin of Thermal Modulation of Exchange Bias in MnPS3/Fe3GeTe2 van der Waals Heterostructures

The exchange bias phenomenon, inherent in exchange-coupled ferromagnetic and antiferromagnetic systems, has intrigued researchers for decades. Van der Waals materials, with their layered structure, provide an optimal platform for probing such physical phenomena. However, achieving a facile and effective means to manipulate exchange bias in van der Waals heterostructures remains challenging. In this study, we investigate the origin of exchange bias in MnPS3/Fe3GeTe2 van der Waals heterostructures. Our work demonstrates a method to modulate unidirectional exchange anisotropy, achieving an unprecedented nearly 1000% variation through simple thermal cycling. Despite the compensated interfacial spin configuration of MnPS3, magneto-transport measurements reveal a huge 170 mT exchange bias at 5 K, one of the largest observed in van der Waals antiferromagnet-ferromagnet interfaces. This substantial magnitude of the exchange bias is linked to an anomalous weak ferromagnetic ordering in MnPS3 below 40 K. On the other hand, the tunability of exchange bias during thermal cycling is ascribed to the modified arrangement of interfacial atoms and changes in the vdW gap during field cooling. Our findings highlight a robust and easily adjustable exchange bias in van der Waals antiferromagnetic/ferromagnetic heterostructures, presenting a straightforward approach to enhance other interface-related spintronic phenomena for practical applications. A detailed study of the interface reveals migration of atoms between the layers, leading to the formation of amorphous region on either side of the van der Waals gap, underscoring the importance of precise characterization of interfaces in van der Waals heterostructures, which are often presumed to have pristine interfaces.

cond-mat.mtrl-sci↗