arXiv subjects

Rafal E. Dunin-Borkowski

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

At least 37 records · Page 2Linked to original sources

arXiv2025

Model-Based Iterative Reconstruction of Three-Dimensional Magnetisation in a Nanowire Structure Using Electron Holographic Vector Field Tomography

Methods for characterisation of 3D magnetic spin structures are necessary to advance the performance of 3D magnetic nanoscale technologies. However, as the component dimensions approach the nanometre range, it becomes more challenging to analyse 3D magnetic configurations with the appropriate spatial resolution. In this paper, we present a method based on Lorentz transmission electron microscopy in which model-based iterative reconstruction (MBIR) is used to reconstruct the most probable magnetisation in an exemplar nanostructure. This method is based on relating electron phase measurements to the magnetic configuration of the nanostructure, and therefore, the method is subject to certain limitations. In this proof-of-concept experiment, MBIR was tested on an L-shaped ferromagnetic cobalt nanowire, fabricated using focused electron beam induced deposition. Off-axis electron holography was used to acquire a tomographic tilt series of electron holograms, which were analysed to measure magnetic electron phase shift over two tilt arcs with up to $ \pm 60$ degree tilt range. Then, a 3D magnetisation vector field consistent with the tomographic phase measurements was reconstructed, revealing multiple magnetic domains within the nanowire. The reconstructed magnetisation is accurate for magnetic domains larger than 50 nm, and higher resolution can be achieved by the continued development of tomographic reconstruction algorithms.

cond-mat.mes-hall↗

arXiv2025

Unraveling the dynamics of conductive filaments in MoS${_2}$ based memristors by operando transmission electron microscopy

Advanced operando transmission electron microscopy (TEM) techniques enable the observation of nanoscale phenomena in electrical devices during operation. They can be used to study the switching mechanisms in two-dimensional (2D) materials-based memristive devices, which is crucial to tailor their operating regimes and improve reliability and variability. Here, we investigate lateral memristive devices composed of 2D layered molybdenum disulfide (MoS${_2}$) with palladium (Pd) and silver (Ag) electrodes. We visualized the formation and migration of Ag conductive filaments (CFs) between the two electrodes under external bias voltage and their complete dissolution upon reversing the bias voltage polarity. The CFs exhibited a wide range of sizes, ranging from several Ångströms to tens of nanometers, and followed diverse pathways: along the MoS${_2}$ surfaces, within the van der Waals gap between MoS${_2}$ layers, and through the spacing between MoS${_2}$ bundles. Notably, the Ag electrode functioned as a reservoir for the CFs, as evidenced by the shrinking and growing of the Ag electrode upon switching. Our method enabled correlating the current-voltage responses with real-time TEM imaging, offering insights into failed and anomalous switching behavior, and providing clarity on the cycle-to-cycle variabilities. Our findings provide solid evidence for the electrochemical metallization mechanism, elucidate the formation dynamics of CFs, and reveal key parameters influencing the switching performance. Our approach can be extended to investigate similar memristive devices.

cond-mat.mtrl-sci↗

arXiv2025

All-optical stochastic switching of magnetization textures in Fe$_3$Sn$_2$

The all-optical control of magnetization at room temperature broadens the scope of applications of spin degrees-of-freedom in data storage, spintronics, and quantum computing. Topological magnetic spin structures, such as skyrmions, are of particular interest due to their particle-like properties, small size and inherent stability. Controlling skyrmion states without strong magnetic fields or large current densities would create new possibilities for their application. In this work, we utilize femtosecond optical pulses to alter the helicity of the spin configuration in dipolar skyrmions formed in the kagome magnet Fe$_3$Sn$_2$ in the absence of an external magnetic field and at room temperature. In situ Lorentz transmission electron microscopy is used to visualize the stochastic, light-induced switching process of chiral Néel caps, while the internal Bloch component of the dipolar skyrmions remain unchanged. In addition to this switching process, we observe the interconversion between type I skyrmionic and type II bubble configurations depending on the external magnetic field and illumination conditions. To corroborate the spin states and the light-induced magnetization dynamics, micromagnetic modelling and simulations of the resulting electron phase shift maps are conducted to elucidate the spin rearrangement induced by individual femtosecond optical pulses.

physics.optics↗

arXiv2024

Interfacial spin-orbitronic effects controlled with different oxidation levels at the Co|Al interface

Perpendicular magnetic anisotropy (PMA) and Dzyaloshinskii-Moriya interactions are key interactions in modern spintronics. These interactions are thought to be dominated by the oxidation of the Co|Al interface in the archetypal Platinum-Cobalt-Aluminum oxide system. Here, we observe a double sign change in the anisotropy and about threefold variation in interfacial chiral interaction, influenced not only by the oxidation, but also by the metallic Al thickness. Contrary to previous assumptions about negligible spin-orbit effects at light metal interfaces, we not only observe strong PMA with fully oxidized Al, decreasing and turning negative (in-plane) with less oxygen at the Co|Al interface, we also observe that the magnetic anisotropy reverts to positive (out-of-plane) values at fully metallic Co|Al interface. These findings suggest modification in Co d band via Co|Al orbital hybridization, an effect supported by X-ray absorption spectroscopy and ab initio theory calculations, highlighting the key impact of strain on interfacial mechanisms at fully metallic Co|Al interface.

cond-mat.mtrl-sci↗

arXiv2024

Electrostatic interference control of a high-energy coherent electron beam using a three-element Boersch phase shifter

In contrast to static holographic phase shifters, which are restricted to specific electron beam energies and microscope settings, Boersch phase shifters are promising for creating programmable arrays for generating two- and three-dimensional electron beam patterns. We recently demonstrated a three-element Boersch phase shifter device [Thakkar et al., J. Appl. Phys. 128 (2020), 134502], which was fabricated by electron beam lithography and is compatible with up-scaling. However, it suffers from parasitic beam deflection and resulting cross-talk. Here, we report a five-layer phase shifter device, which is based on a metal-insulator-metal-insulator-metal structure (as originally envisioned by Boersch) that reduces cross-talk. We demonstrate a three-element Boersch phase shifter that shows minimal beam deflection of voltage-controlled three-electron-beam interference patterns in a transmission electron microscope operated at 200 keV. The feasibility of using such multi-element phase shifter arrays is discussed.

physics.app-ph↗

arXiv2024

Automated detection and mapping of crystal tilt using thermal diffuse scattering in transmission electron microscopy

Quantitative interpretation of transmission electron microscopy (TEM) data of crystalline specimens often requires the accurate knowledge of the local crystal orientation. A method is presented which exploits momentum-resolved scanning TEM (STEM) data to determine the local mistilt from a major zone axis. It is based on a geometric analysis of Kikuchi bands within a single diffraction pattern, yielding the centre of the Laue circle. Whereas the approach is not limited to convergent illumination, it is here developed using unit-cell averaged diffraction patterns corresponding to high-resolution STEM settings. In simulation studies, an accuracy of approximately 0.1mrad is found. The method is implemented in automated software and applied to crystallographic tilt and in-plane rotation mapping in two experimental cases. In particular, orientation maps of high-Mn steel and an epitaxially grown La$_{\text{0.7}}$Sr$_{\text{0.3}}$MnO$_{\text{3}}$-SrTiO$_{\text{3}}$ interface are presented. The results confirm the estimates of the simulation study and indicate that tilt mapping can be performed consistently over a wide field of view with diameters well above 100nm at unit cell real space sampling.

cond-mat.mtrl-sci↗

arXiv2024

Insights into the defect-driven heterogeneous structural evolution of Ni-rich layered cathode in lithium-ion batteries

Recently, considerable efforts have been made on research and improvement for Ni-rich lithium-ion batteries to meet the demand from vehicles and grid-level large-scale energy storage. Development of next-generation high-performance lithium-ion batteries requires a comprehensive understanding on the underlying electrochemical mechanisms associated with its structural evolution. In this work, advanced operando neutron diffraction and four-dimensional scanning transmission electron microscopy techniques are applied to clarify the structural evolution of electrodes in two distinct full cells with identical LiNi0.8Co0.1Mn0.1O2 cathode but different anode counterparts. It is found that both of cathodes in two cells exhibit non-intrinsic two-phase-like behavior at the early charge stage, indicating selective Li+ extraction from cathodes. But the heterogeneous evolution of cathode is less serious with graphite-silicon blended anode than that with graphite anode due to the different delithiation rate. Moreover, it is revealed that the formation of heterogeneous structure is led by the distribution of defects including Li/Ni disordering and microcracks, which should be inhibited by assembling appropriate anode to avoid potential threaten on cell performance. The present work unveils the origin of inhomogeneity in Ni-rich lithium-ion batteries and highlights the significance of kinetics control in electrodes for batteries with higher capacity and longer life.

cond-mat.mtrl-sci↗

arXiv2024

Embedded skyrmion bags in thin films of chiral magnets

Magnetic skyrmions are topologically nontrivial spin configurations that possess particle-like properties. Earlier research was mainly focused on a specific type of skyrmion with topological charge Q = -1. However, theoretical analyses of two-dimensional chiral magnets have predicted the existence of skyrmion bags -- solitons with arbitrary positive or negative topological charge. Although such spin textures are metastable states, recent experimental observations have confirmed the stability of isolated skyrmion bags in a limited range of applied magnetic fields. Here, by utilizing Lorentz transmission electron microscopy, we show the extraordinary stability of skyrmion bags in thin plates of B20-type FeGe. In particular, we show that skyrmion bags embedded within a skyrmion lattice remain stable even in zero or inverted external magnetic fields. A robust protocol for nucleating such embedded skyrmion bags is provided. Our results agree perfectly with micromagnetic simulations and establish thin plates of cubic chiral magnets as a powerful platform for exploring a broad spectrum of topological magnetic solitons.

cond-mat.mes-hall↗

arXiv2024

Calibrating coordinate system alignment in a scanning transmission electron microscope using a digital twin

In four-dimensional scanning transmission electron microscopy (4D STEM) a focused beam is scanned over a specimen and a diffraction pattern is recorded at each position using a pixelated detector. During the experiment, it must be ensured that the scan coordinate system of the beam is correctly calibrated relative to the detector coordinate system. Various simplified and approximate models are used implicitly and explicitly for understanding and analyzing the recorded data, requiring translation between the physical reality of the instrument and the abstractions used in data interpretation. Here, we introduce a calibration method where interactive live data processing in combination with a digital twin is used to match a set of models and their parameters with the action of a real-world instrument.

physics.ins-det↗

arXiv2024

Simultaneous mapping of magnetic and atomic structure for direct visualization of nanoscale magnetoelastic coupling

Achieving a correlative measurement of both magnetic and atomic structures at the nanoscale is imperative to understand the fundamental magnetism of matters and for fostering the development of new magnetic nanomaterials. Conventional microscopy methods fall short in providing the two information simultaneously. Here, we develop a new approach to simultaneously map the magnetic field and atomic structure at the nanoscale using Lorentz 4-dimensional scanning transmission electron microscopy (Ltz-4D-STEM). This method enables precise measurement of the characteristic atomic and magnetic structures across an extensive field of view, a critical aspect for investigating real-world ferromagnetic materials. It offers a comprehensive visualization and statistical evaluation of the different structural information at a pixel-by-pixel correlation. The new method allows to directly visualize the magnetoelastic coupling and the resulting complex magnetization arrangement as well as the competition between magnetoelastic and magnetostatic energy. This approach opens new avenues for in-depth studying the structure-property correlation of nanoscale magnetic materials.

cond-mat.mtrl-sci↗

arXiv2024

Direct observation of altermagnetic band splitting in CrSb thin films

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spinintegrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the signifcance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to external magnetic fields and possessing THz dynamics, akin to antiferromagnets.

cond-mat.mtrl-sci↗

arXiv2024

Harnessing van der Waals CrPS4 and Surface Oxides for non-monotonic pre-set field induced Exchange Bias in Fe3GeTe2

Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that naturally oxidized vdW ferromagnetic Fe3GeTe2 exhibits exchange bias, attributed to the antiferromagnetic coupling of its ultrathin surface oxide layer (O-FGT) with the underlying unoxidized Fe3GeTe2. Anomalous Hall measurements are employed to scrutinize the exchange bias within the CrPS4/(O-FGT)/Fe3GeTe2 heterostructure. This analysis takes into account the contributions from both the perfectly uncompensated interfacial CrPS4 layer and the interfacial oxide layer. Intriguingly, a distinct and non-monotonic exchange bias trend is observed as a function of temperature below 140 K. The occurrence of exchange bias induced by a 'pre-set field' implies that the prevailing phase in the polycrystalline surface oxide is ferrimagnetic Fe3O4. Moreover, the exchange bias induced by the ferrimagnetic Fe3O4 is significantly modulated by the presence of the van der Waals antiferromagnetic CrPS4 layer, forming a heterostructure, along with additional iron oxide phases within the oxide layer. These findings underscore the intricate and complex nature of exchange bias in van der Waals heterostructures, highlighting their potential for tailored manipulation and control.

cond-mat.mtrl-sci↗

arXiv2023

Atomically resolved phase coexistence in VO2 thin films

Concurrent structural and electronic transformations in VO2 thin films are of twofold importance: enabling fine-tuning of the emergent electrical properties in functional devices, yet creating an intricate interfacial domain structure of transitional phases. Despite the importance of understanding the structure of VO2 thin films, a detailed real space atomic structure analysis in which also the oxygen atomic columns are resolved is lacking. Moreover, intermediate atomic structures have remained elusive due to the lack of robust atomically resolved quantitative analysis. Here, we directly resolve both V and O atomic columns and discover the presence of the strain-stabilized intermediate monoclinic (M2) phase nanolayers (less than 2 nm thick) in epitaxially grown VO2 films on a TiO2 (001) substrate, where the dominant part of VO2 undergoes a transition from the tetragonal (rutile) phase to the monoclinic M1 phase. We unfold the crucial role of imaging the spatial configurations of the oxygen anions (in addition to V cations) utilizing atomic-resolution electron microscopy. Our approach sets a direct pathway to unravel the structural transitions in wide range of correlated oxides, offering substantial implications for e.g. optoelectronics and ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2023

Magnetic Phase Imaging using Lorentz Near-field Electron Ptychography

Over the past few years, the combination of diffuser and near-field electron ptychography has drawn more attention by its ability to recover large field of view with few diffraction patterns. In this paper, we purpose a novel design and implementation of amplitude diffuser. The amplitude diffuser introduces structures to the illumination while reducing the inelastic scattering. And the amplitude diffuser is implemented at the condenser lens aperture, allowing us to vary the illumination size under the same microscope setup. We demonstrate the reconstruction results under both conventional Transmission Electron Microscopy (TEM) mode as well as Lorentz mode.

cond-mat.mtrl-sci↗

arXiv2023

A quantum logic gate for free electrons

The topological charge $m$ of vortex electrons spans an infinite-dimensional Hilbert space. Selecting a two-dimensional subspace spanned by $m=\pm 1$, a beam electron in a transmission electron microscope (TEM) can be considered as a quantum bit (qubit) freely propagating in the column. A combination of electron optical quadrupole lenses can serve as a universal device to manipulate such qubits at the experimenter's discretion. We set up a TEM probe forming lens system as a quantum gate and demonstrate its action numerically and experimentally. High-end TEMs with aberration correctors are a promising platform for such experiments, opening the way to study quantum logic gates in the electron microscope.

quant-ph↗

arXiv2023

Driving skyrmions in flow regime in synthetic ferrimagnets

Despite significant advances in the last decade regarding the room temperature stabilization of skyrmions or their current induced dynamics, the impact of local material inhomogeneities still remains an important issue that impedes to reach the regime of steady state motion of these spin textures. Here, we study the spin-torque driven motion of skyrmions in synthetic ferrimagnetic multilayers with the aim of achieving high mobility and reduced skyrmion Hall effect. We consider Pt|Co|Tb multilayers of various thicknesses with antiferromagnetic coupling between the Co and Tb magnetization. The increase of Tb thickness in the multilayers allows to reduce the total magnetic moment and increases the spin-orbit torques allowing to reach velocities up to 400 m.s-1 for skyrmions with diameters of about 160 nm. We demonstrate that due to reduced skyrmion Hall effect, combined with the edge repulsion of the magnetic track making the skyrmions moving along the track without any transverse deflection. Further, by comparing the field-induced domain wall motion and current-induced skyrmion motion, we demonstrate that the skyrmions at the largest current densities present all the characteristics of a dynamical flow regime.

cond-mat.mtrl-sci↗

arXiv2023

Influence of amorphous phase on coercivity in SmCo5-Cu nanocomposites

Severe plastic deformation of powder blends consisting of SmCo5-Cu results in magnetically hardened nanocomposite bulk materials. The microstructure is continuously refined with increasing torsional deformation, yet, coercivity saturates at a certain level of strain. Transmission electron microscopy (TEM) investigation of the microstructure reveals a partial amorphization of the SmCo5 phase due to high-pressure torsion by 20 applied rotations. In this amorphous matrix nanocrystals are embedded. The effect of these experimentally observed microstructural features on the magnetic properties are investigated by micromagnetic simulations, which show that an increasing volume fraction of nanocrystals is beneficial for higher coercivities. For a fixed volume fraction of nanocrystals the simulations reveal an increasing coercivity with decreasing the size of the nanocrystals due to increasing number of interfaces acting as pinning sites. Furthermore, our micromagnetic simulations disclose the mechanisms of the saturation and decline of magnetic hardening due to the strain induced by high-pressure torsion. The calculated coercivity fits very well to the experimentally observed coercivity of Hc=1.34 T. The knowledge can also be used to develop and provide optimization strategies from the microstructure perspective.

cond-mat.mtrl-sci↗

arXiv2023

Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo$_{5-x}$Cu$_{x}$ Thin Films

This work investigates the effect of copper substitution on the magnetic properties of SmCo$_{5}$ thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co$_{3g}$ sites not only stabilizes the formation of the SmCo$_{5}$ structure but enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co$_4$Cu$_{3g}$)$_5$ possesses a higher single-ion anisotropy as compared to pure SmCo$_{5}$. In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4\textit{f} and Co 3\textit{d} moments. Scanning transmission electron microscopy confirms predominantly SmCo$_{5}$ phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare earth-based magnets, \textit{i.e.} the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

cond-mat.mtrl-sci↗