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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., 14 pages, 4 figures

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.

Metallic/intermetalic materials with BCC structures hold an intrinsic instability due to phonon softening along [110] dirrection, causing BCC to lower-symmetry phases transformation when the BCC structures are thermally or mechanically stressed. Fe50Rh50 binary system is one of the exceptional BCC structures (ordered-B2) that has not been yet showing such transformation upon application of thermal stress, although mechanical deformation results in B2 to disordered FCC (gamma) and L10 phases transformation. Here, a comprehensive transmission electron microscopy (TEM) study is conducted on thermally-stressed samples of Fe50Rh50 aged at water and liquid nitrogen from 1150 degree C and 1250 degree C. The results show that, samples quenched from 1150 degree C into water and liquid nitrogen show presence of 1/4{110} and 1/2{110} satellite reflections, the latter of which is expected from phonon dispersion curves obtained by density functional theory calculation. Therefore, it is believed that Fe50Rh50 maintains the B2 structure that is in premartensite state. Once Fe50Rh50 is quenched from 1250 degree C into liquid nitrogen, formation of two short-range ordered tetragonal phases with various c/a ratios (~1.15 and 1.4) is observed in line with phases formed from mechanically deformed (30%) sample. According to our observations, an accurate atomistic shear model ({110}) is presented that describes the martensitic transformation of B2 to these tetragonal phases. These findings offer implications useful for understanding of magnetic and physical characteristics of metallic/intermetallic materials.

Physical review materials 7(5), L052401 (2023). doi:10.1103/PhysRevMaterials.7.L052401, We demonstrate the presence of a hysteresis in tunneling spectra acquired at 4.3 K on cleaved MA-Br terminated (001) surfaces of MAPbBr3 single crystals. Simulations of the tunneling spectra reveal an underlying polarization-voltage (P-V) hysteresis, which is caused by an interplay of subsurface field-induced rotation and alignment of the MA molecules, stabilized by dipole-dipole interactions, and an ion-lattice relaxation. The resulting subsurface polarization is counteracted by a compensating surface polarization, detectable by surface-sensitive tunneling spectroscopy., Published by APS, College Park, MD

Characterisation of the electron beams trajectory in an electron microscope is possible in a few select commercial software packages, but these tools and their source code are not available in a free and accessible manner. This paper introduces the free and open-source software TEMGYM Advanced, which implements ray tracing methods that calculate the path of electrons through a magnetic or electrostatic lens and allow evaluation of the first-order properties and third-order geometric aberrations. Validation of the aberration coefficient calculations is performed by implementing two independent methods – the aberration integral and differential algebra (DA) methods and by comparing the results of each. This paper also demonstrates parallelised electron ray tracing through a series of magnetic components, which enables near real-time generation of a physically accurate beam-spot including aberrations and brings closer the realisation of a digital twin of an electron microscope. TEMGYM Advanced represents a valuable resource for the electron microscopy community, providing an accessible and open source means of characterising electron lenses. This software utilises the Python programming language to complement the growing ecosystem of free and open-source software within the electron microscopy community, and to facilitate the application of machine learning to an electron microscope digital twin for instrument automation. The software is available under GNU Public License number Three (GPL 3).

For energy efficient and fast magnetic memories, switching of perpendicular magnetization by the spin-orbit torque (SOT) appears as a very promising solution, even more using magnetic insulators that suppress electrical shunting. This SOT switching generally requires the assistance of an in-plane magnetic field to break the symmetry. Here, we present experiments demonstrating the field-free SOT switching of perpendicularly magnetized layers of the thulium iron garnet (Tm_{3}Fe_{5}O_{12}) magnetic insulator. The polarity of the switching loops, clockwise (CW) or counter-clockwise (CCW), is determined by the direction of the initial current pulses, in contrast with field-assisted switchings in which this polarity is controlled by the direction of the field. After an independent determination of Dzyaloshinskii-Moriya interaction (DMI), we relate the field free switching to the interplay of SOT and DMI and the polarity of the loops to the imprint of a N\'eel domain wall induced by the first pulse, in agreement with Kerr imaging. Our observation and interpretation of field-free electrical switching of a magnetic insulator is an important milestone for future low power spintronic devices., Comment: 11 pages, 4 figures

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.

Two-dimensional van der Waals heterostructures are an attractive platform for studying exchange bias due to their defect free and atomically flat interfaces. Chromium thiophosphate (CrPS4), an antiferromagnet, has uncompensated magnetic spins in a single layer that make it an excellent candidate for studying exchange bias. In this study, we examined the exchange bias in CrPS4/Fe3GeTe2 van der Waals heterostructures using anomalous Hall measurements. Our results show that the exchange bias strength is robust for clean interfaces, with a hysteresis loop shift of about 55 mT at 5 K for few-layer Fe3GeTe2, which is larger than that obtained in most van der Waals AFM/FM heterostructures. However, when exposed to air, the ferromagnetic Fe3GeTe2 layer develops a thin surface oxide layer that significantly modulates the exchange bias. Remarkably, this surface oxide layer can induce exchange bias without any field-cooling, but merely by applying a 'preset field' from 5 K up to 140K due to the presence of ferrimagnetic magnetite. We also observed exchange bias beyond the N\'eel temperature of CrPS4, with two local minima due to contributions from CrPS4 and surface oxides. These results illustrate the complex behaviour of exchange bias in van der Waals heterostructures and its potential for tailored control.

Nature Communications 14(1), 3963 (2023). doi:10.1038/s41467-023-39650-8, Published by Nature Publishing Group UK, [London]

The European research and innovation infrastructure ecosystem is diverse in its scale and scope, comprising facilities and services that include major scientific research equipment, resources such as collections, archives of scientific data, e-infrastructures such as data storage and computing systems, communication networks, as well as pilot and demonstration sites and living labs...

The Fe–Cr alloy system is the basis of ferritic steels, which are important structural materials for many applications, including their use in future fusion reactors. However, when exposed to elevated temperatures and radiation, the Fe–Cr system can undergo phase separation, resulting in Fe-rich (α) and Cr-rich (α’) nanoscale regions. This in turn generates the so-called “475 °C embrittlement” and modifies the magnetic properties. The correlation between the microstructural and magnetic changes is however poorly understood, which currently prevents the possibility of assessing the material in a non-destructive way by magnetometry. Here, we study the microstructural decomposition of an Fe–40Cr alloy induced by annealing at 500 °C for extensive time scales and its impact on the magnetic properties using magnetometry and advanced experimental methods, such as atom probe tomography, transmission electron microscopy (TEM), and micromagnetic simulations. Upon annealing, the alloy rapidly exhibits a spinodal decomposition morphology with a typical length scale of about 10 nm. With increasing annealing time, the hardness assessed by Vickers testing, the magnetic saturation, and the coercivity increase, which correlates with an increase in α-volume fraction and the system's heterogeneity. The magnetic domain patterns imaged by TEM and interpreted with the help of micromagnetic simulations reveal at the nanometer scale the impact of decomposition on the magnetic response of Fe–Cr., Acta Materialia, 240, ISSN:1359-6454

Self-assembled quantum dots based on III-V semiconductors have excellent properties for applications in quantum optics. However, the presence of a 2D wetting layer which forms during the Stranski-Krastanov growth of quantum dots can limit their performance. Here, we investigate wetting layer formation during quantum dot growth by the alternative droplet epitaxy technique. We use a combination of photoluminescence excitation spectroscopy, lifetime measurements, and transmission electron microscopy to identify the presence of an InGaAs wetting layer in these droplet epitaxy quantum dots, even in the absence of distinguishable wetting layer photoluminescence. We observe that increasing the amount of Ga deposited on a GaAs (100) surface prior to the growth of InGaAs quantum dots leads to a significant reduction in the emission wavelength of the wetting layer to the point where it can no longer be distinguished from the GaAs acceptor peak emission in photoluminescence measurements.

We report the use of an electrostatic MEMS-based device to produce high quality electron vortex beams with more than 1000 quanta of orbital angular momentum (OAM). Diffraction and off-axis electron holography experiments are used to show that the diameter of the vortex in the diffraction plane increases linearly with OAM, thereby allowing the angular momentum content of the vortex to be calibrated. The realization of electron vortex beams with even larger values of OAM is currently limited by the breakdown voltage of the device. Potential solutions to overcome this problem are discussed.

MEMS based electron optics are a promising approach for a new generation of experiments in electron microscopy. In this contribution we improve analytically the modelling of the MEMS based phase plates with thin electrodes with accurate account of the fringing fields. As a result we are able to improve the design and the boundary conditions in MEMS-based spiral phase plates acting on the control parameters. We checked the quality of the generated vortex beam.

Chemical communications : ChemComm 10(19), 3130-3133 (2022). doi:10.1039/D1CC07172F, Published by Royal Society of Chemistry, Cambridge

Ultramicroscopy 241, 113593 (2022). doi:10.1016/j.ultramic.2022.113593, Published by Elsevier Science, Amsterdam

A fundamental property of particles and antiparticles, such as electrons and positrons, is their ability to annihilate one another. Similar behavior is predicted for magnetic solitons -- localized spin textures that can be distinguished by their topological index $Q$. Theoretically, magnetic topological solitons with opposite values of $Q$, such as skyrmions and their antiparticles -- antiskyrmions -- are expected to be able to merge continuously and to annihilate. However, experimental verification of such particle-antiparticle pair production and annihilation processes has been lacking. Here, we report the creation and annihilation of skyrmion-antiskyrmion pairs in an exceptionally thin film of the cubic chiral magnet B20-type FeGe observed using transmission electron microscopy. Our observations are highly reproducible and are fully consistent with micromagnetic simulations. Our findings provide a new platform for fundamental studies of particles and antiparticles based on magnetic solids and open new perspectives for practical applications of thin films of isotropic chiral magnets., 16 pages, 14 figures

This deliverable is meant to summarise the final results regarding the plasmon analysis based on OAM sorter. The aim is to prove that we can achieve a substantial scientific advancement using the OAM-sorter that was not possible without it. We document here both the actual scientific results and the partial attempts that could not be brought to conclusions. The deliverable is separated into 2 main chapters. Chapter 1 reports the efforts to produce the Q-SORT setup for different kinds of plasmon observation and explains why the setup has to be different for every specific experiment. Chapter 2 reports the actual scientific results, of high fundamental relevance, that we obtained for volume plasmons. The experimental results are qualitatively and quantitatively compared with simulation. Conclusions are drawn at the end. It is worth highlighting here that the OAM sorter allowed us to better understand the characteristics of plasmon loss excitation and to find a new phenomenon consisting of the ‘spontaneous Emission’ of quanta of OAM in the interaction with plasmon. Surprising theoretical results were also obtained thanks to the definition of coherence through innovative density matrix formalism: we showed that the coherence of the initial OAM state superposition of the electron is partially preserved after the electron-plasmon scattering, which is reflected mathematically by the possibility of expressing the post-scattering electron density matrix as the sum of one fully coherent term containing the initial OAM values and another term which is characterised by full OAM decoherence. The theory was confirmed by experiment in this case as well.

This deliverable reports the comprehensive results and activities aimed to demonstrate Electron Magnetic Circular Dichroism (EMCD). It is difficult to keep the delicate OAM sorter alignment at the large energy-loss of the iron L-edge (about 700 eV). Considering also the slowdowns due to COVID-19 pandemic we opted for an equally and similar problem by looking at the difference in the σ* and π* transition in 2D material in the energy range of 200eV energy loss. The kind of information and the OAM–EELS theory is fundamentally the same as real EMCD but the difficulty in the alignment is reduced. The experiment therefore succeeds in demonstrating the importance of the combination of OAM-EELS experiment also to study atomic transitions. Considering the similarities of the two experiments this work demonstrate that EMCD is feasible and that automatic alignment procedure should soon allow to explore the energy loss range of EMCD. For these reasons, most of this work will be of quite general interest and only a small part will regard the case of h-BN. Given the rising importance of 2D material that are now receiving even more attention than magnetic structure the result has also a large importance in its own right and fully demonstrates the potentialities of a OAM sorter in material science. Chapter 1 will explain all the improvements we carried out in the direction of EMCD and in OAM–EELS experiments. A large space has been dedicated to the automatic control of the microscope by means of a neural network. Given the difficulties to control the many parameters, this will probably be the best way to carry out the most difficult future experiments. Chapter 2 will explain all problems of localization and decoherence. Once again this theoretical framework is valid for all OAM–EELS experiments and is of general interest to understand our data and to design future experiments. Chapter 3 is dedicated to effective manuscript draft with experiments and data analysis. As for the setup also the deconvolution method used in this section can be easily transported to the case of EMCD.

In quantum mechanics, each conserved quantity (e.g., energy, position, linear momentum and angular momentum) is associated with a Hermitian operator. Its expected value can then be determined by performing a measurement on the wavefunction. In modern electron microscopy, one can select the initial and final states of the electron and the measurement basis by performing measurements of scattering processes. For example, the orbital angular momentum (OAM) of an electron can be used to reveal the n-fold symmetry of a wavefunction scattered by a sample. Here, we introduce a new composite planar chirality operator that can be used to measure a spiral-like feature in a sample. This concept develops the concept of chirality to highlight a specific roto-scale symmetry. We show that planar chirality can be characterized using an electron OAM sorter to uncover the atomic structures of biomolecules in cryo electron microscopy, either in a stand-alone analysis for fast identification of protein structures or in the context of conventional cryo electron microscopy to produce faster and more detailed 3D reconstructions by solving upside-down orientation ambiguities., available also at arXiv:2110.03391 This project has received fundings also from the Deutsche Forschungsgemeinschaft (Project-ID 405553726 – TRR 270), from the DARPA TEE program (Grant MIPR# HR0011831554) and from an Ontario Early Researcher Award (ERA) and a Canada Research Chair (CRC).

Beam shaping - the ability to engineer the phase and the amplitude of massive and massless particles - has long interested scientists working on communication, imaging and the foundations of quantum mechanics. In light optics, the shaping of electromagnetic waves (photons) can be achieved using techniques that include, but are not limited to, direct manipulation of the beam source (as in X-ray Free Electron Lasers (XFELs) and Synchrotrons), deformable mirrors, spatial light modulators, mode converters and holograms. The recent introduction of holographic masks for electrons provides new possibilities for electron beam shaping. Their fabrication has been made possible by advances in micrometric and nanometric device production using lithography and focused ion beam patterning. This article provides a tutorial on the generation, production and analysis of synthetic holograms for transmission electron microscopy. It begins with an introduction to synthetic holograms, outlining why they are useful for beam shaping to study material properties. It then focuses on the fabrication of the required devices from theoretical and experimental perspectives, with examples taken from both simulations and experimental results. Applications of synthetic electron holograms as aberration correctors, electron vortex generators and spatial mode sorters are then presented., This project has received funding from the European Union's Horizon 2020 research and innovation programme (Grant No. 766970, project "Q-SORT"; Grant No. 856538, project "3D MAGiC"; Grant No. 823717, project "ESTEEM3"), from the Deutsche Forschungsgemeinschaft (Project-ID 405553726 – TRR 270), from the DARPA TEE program (Grant MIPR# HR0011831554) and from an Ontario Early Researcher Award (ERA) and a Canada Research Chair (CRC).

Nanomaterials : open access journal 11(2), 466 (2021). doi:10.3390/nano11020466 special issue: "Special Issue "Characterization of Quantum Effects in Nanomaterials, Nano-Devices, and Nanophotonics" / Special Issue Editor: Prof. Dr. Jeong Ryeol Cho, Guest Editor", Published by MDPI, Basel

Magnetic high entropy alloys (HEAs) are a new category of high-performance magnetic materials, with multi-component concentrated compositions and complex multi-phase structures. Although there have been numerous reports of their interesting magnetic properties, there is very limited understanding about the interplay between their hierarchical multi-phase structures and their local magnetic structures. By employing high spatial resolution correlative magnetic, structural and chemical studies, we reveal the influence of a hierarchically decomposed B2 + A2 structure in an AlCo0.5Cr0.5FeNi HEA on the formation of magnetic vortex states within individual A2 (disordered BCC) precipitates, which are distributed in an ordered B2 matrix that is weakly ferromagnetic. Non-magnetic or weakly ferromagnetic B2 precipitates in large magnetic domains of the A2 phase, and strongly magnetic Fe-Co-rich interphase A2 regions, are also observed. These results provide important insight into the origin of coercivity in this HEA, which can be attributed to a complex magnetization process that includes the successive reversal of magnetic vortices.

Advanced functional materials 2008306 (2021). doi:10.1002/adfm.202008306, Published by Wiley-VCH, Weinheim

Magnetic skyrmions are stable topological solitons with complex non-coplanar spin structures. Their nanoscopic size and the low electric currents required to initiate and control their motion has opened a new field of research, skyrmionics, that aims at using skyrmions as information carriers for data storage and manipulation. Recent advances in skyrmionics prompt for a thorough understanding of the detailed three-dimensional (3D) spin texture of a skyrmion including skyrmion-skyrmion interactions and their coupling to surfaces and interfaces. These properties crucially affect application-related aspects such as the stability and mobility of skyrmions in confined structures. To date, however, experimental techniques to measure the three-dimensional spin texture with nanometer resolution are largely missing. We therefore adapt holographic vector field electron tomography to the problem and report on the first quantitative reconstruction of the 3D spin texture of skyrmions with sub-10 nanometer resolution. The reconstructed textures reveal a variety of previously unseen local deviations from a homogeneous Bloch character within the skyrmion tubes (SkTs), details of the collapse of the skyrmion texture at surfaces, and a correlated modulation of the SkT in FeGe along their tube axes. The quantitative 3D data of the magnetic induction also allow to experimentally confirm some principles of skyrmion formation by deriving spatially resolved maps of the magnetic energy density across these magnetic solitons.

Phase transition describes a mutational behavior of matter states at a critical transition temperature or external field. Despite the phase-transition orders are well sorted by classic thermodynamic theory, ambiguous situations interposed between the first- and second-order transitions were exposed one after another. Here, we report discovery of phase-transition frustration near a tricritical composition point in ferroelectric Pb(Zr1-xTix)O3. Our multi-scale transmission electron microscopy characterization reveals a number of geometrically frustrated microstructure features such as self-assembled hierarchical domain structure, degeneracy of mesoscale domain tetragonality and decoupled polarization-strain relationship. Associated with deviation from the classic mean-field theory, dielectric critical exponent anomalies and temperature dependent birefringence data unveil that the frustrated transition order stems from intricate competition of short-range polar orders and their decoupling to long-range lattice deformation. With supports from effective Hamiltonian Monte Carlo simulations, our findings point out a potentially universal mechanism to comprehend the abnormal critical phenomena occurring in phase-transition materials., Phase transition brings a plethora of exotic phenomena and intriguing effects such as spin and charge frustration. However, the phase transition order is not always explicit. Here, the authors discover phase transition frustration near a tricritical composition point in ferroelectric Pb(Zr,Ti)O3.

Computer simulations are used to assess the influence of a 20-nm-thick SiNx membrane on the quantification of atomic-resolution annular dark-field (ADF) scanning transmission electron microscopy images of Pt nanoparticles. The discussions include the effect of different nanoparticle/membrane arrangements, accelerating voltage, nanoparticle thickness and the presence of adjacent atomic columns on the accuracy with which the number of Pt atoms in each atom column can be counted. The results, which are based on the use of ADF scattering cross-sections, show that an accuracy of better than a single atom is attainable at 200 and 300 kV. At 80kV, the scattering in a typical SiNx membrane is sufficiently strong that the best possible atom counting accuracy is reduced to +/- 2 atoms. The implications of the work for quantitative studies of Pt nanoparticles imaged through SiNx membranes are discussed.

This deliverable reports on the progress that has been achieved in the direction of the dose-effective imaging of organic molecules. We report several essential experimental advancements, including a successful experimental scheme of ghost imaging that could be realised in Modena without the need of travelling. Overall this deliverable includes material for at least 3 papers and a patent. The restriction on travels due to Covid-19 imposed hard constraints on the performance of the intended experiment. The complete experiment on proteins would, in fact, have required the simultaneous presence of three groups at the microscope in Jülich: FZJ personnel for main operation on the microscope, people from MU for the cryomicroscopy part, and people from CNR for the lateral control of software and for the coordination of the experiment. Moreover, the preparation of the experiment required the intervention of FEI personnel. Unfortunately, in spite of the partial release of the restrictions during the extra 6 months allotted to Q-SORT, for the reasons given above these conditions were impossible to meet. This was unforeseeable at the moment the project extension was asked. Given these hard constraints, we chose the combination of experimental activities that allowed us to achieve the greatest possible amount of project goals. In fact, Q-SORT scientists achieved more than what was foreseen; novel results include: 1) the first patentable phase plates of different design ( designed in WP3 D3.4 for protein recognition) able to control up to 24 electrodes by multiplexing the initial 8 inputs. 2) the first computational ghost imaging experiment in microscopy and its optimization for low dose regime 3) a state of the art neural network control for an efficient prediction of the generated caustic pattern. Two approaches to the protein recognition were chosen at the end of WP3: a) the extension of the OAM sorter with an additional programmable phase plate. Such approach is referred to as GOAMS (generalised OAM sorter) in D3.2 as b) the computational ghost imaging with increasingly complex masks. Under the given constraints, it was found that the computational ghost imaging approach (D3.2, task 3.1 & 3.2) was the most appropriate and effective to pursue - enabling the greatest advancement. This development is also consistent with contingency plan #6 “Test random or Hadamard sparse sampling”. The results have been also written as a manuscript that is going to be submitted soon. The hardware for the 3-element GOAMS (i.e. the second approach that was found to be most promising in WP3) was also developed, with the design of an additional element that allowed the recognition of the radial degree of freedom. Such extended “protein specific” phase modulator (D3.4) was also finished and tested as one of the design of the programmable phase plates. [...]

Magnetoelectric (ME) coupling in La0.7Sr0.3MnO3/Pb(Mg1/3Nb2/3)0.7Ti0.3O3 (LSMO/PMN–PT (001)) has been probed in the past years to identify the underlying mechanism behind it. PMN–PT, which is well known for its excellent piezoelectric properties, also exhibits ferroelectricity. This motivates our interest to differentiate which effect is dominant for this 'voltage control of magnetism'. Here, we present results for the ME coupling at different temperatures: 300 K and 80 K. In this article we discuss and explain, how the nature of ME coupling is influenced by different parameters such as magnetic field, electric field, directional dependence (hard axis, easy axis) and temperature. Owing to large lattice mismatch between LSMO and PMN–PT, the strain-mediated coupling is strongly prevalent, however the change in strain behaviour from butterfly loop to linear loop is observed as a function of temperature. ME measurements are performed along hard axis [100] and easy axis [110] of LSMO in the presence of remanent magnetic field which showcases the pure influence of electric field on the system, resulting in a combination of strain- and charge-mediated coupling. The magnetic depth profile is probed by polarized neutron reflectometry as a function of electric field which demonstrates the existence of an interlayer with reduced nuclear scattering length density and reduced magnetic scattering length density at the interface. From transmission electron microscopy, stoichiometric variations are observed due to the presence of Mn3O4 particles at the interface.

Advanced functional materials 2008609 (2021). doi:10.1002/adfm.202008609, Published by Wiley-VCH, Weinheim

Modern nanotechnology techniques offer new opportunities for fabricating structures and devices at the micron and sub-micron level. Here, we use focused ion beam techniques to realize drift tube Zernike phase plates for electrons, whose operation is based on the presence of contact potentials in Janus bimetallic cylinders, in a similar manner to the electrostatic Aharonov-Bohm effect in bimetallic wires. We use electron Fraunhofer interference to demonstrate that such bimetallic pillar structures introduce phase shifts that can be tuned to desired values by varying their dimensions, in particular their heights., 7 pages, 4 figures, preprint

The growth of cobalt nanopatterns (NPs) using focused electron‐beam induced deposition (FEBID) for localised magnetic studies is presented. The initial FEBID products are shown to be polycrystalline and form hetero‐structured core‐shell NPs through surface oxidation. Off‐axis electron holography is performed to reconstruct their morphology, thickness profile and image their individual magnetic vortex domain states. In situ annealing to 400°C promoted migration of the Co‐overspray to grow the Co NPs and improved their crystallinity through coarsening, as well as induced diffusion of embedded carbon out of their surface. It is found that the change in their morphology and chemical instability under heating restricts their suitability for examining thermally induced magnetic variations.

Arrays of interacting 2D nanomagnets display unprecedented electromagnetic properties via collective effects, demonstrated in artificial spin ices and magnonic crystals. Progress toward 3D magnetic metamaterials is hampered by two challenges: fabricating 3D structures near intrinsic magnetic length scales (sub-100 nm) and visualizing their magnetic configurations. Here, we fabricate and measure nanoscale magnetic gyroids, periodic chiral networks comprising nanowire-like struts forming three-connected vertices. Via block copolymer templating, we produce Ni75Fe25 single-gyroid and double-gyroid (an inversion pair of single-gyroids) nanostructures with a 42 nm unit cell and 11 nm diameter struts, comparable to the exchange length in Ni-Fe. We visualize their magnetization distributions via off-axis electron holography with nanometer spatial resolution and interpret the patterns using finite-element micromagnetic simulations. Our results suggest an intricate, frustrated remanent state which is ferromagnetic but without a unique equilibrium configuration, opening new possibilities for collective phenomena in magnetism, including 3D magnonic crystals and unconventional computing.

Nanoscale horizons 5(7), 1065 - 1072 (2020). doi:10.1039/D0NH00117A, The self-assembly of nanoparticles into highly ordered crystals is largely influenced by variations in the size and shape of the constituent particles, with crystallization generally not observed if their polydispersity is too large. Here, we report on size selectivity in the self-assembly of rounded cubic maghemite nanoparticles into three-dimensional mesocrystals. Different X-ray scattering techniques are used to study and compare a nanoparticle dispersion that is used later for self-assembly, an ensemble of mesocrystals grown on a substrate, as well as an individual mesocrystal. The individual μm-sized mesocrystal is isolated using a focused-ion-beam-based technique and investigated by the diffraction of a micro-focused X-ray beam. Structural analysis reveals that individual mesocrystals have a drastically smaller size dispersity of nanoparticles than that in the initial dispersion, implying very strong size selectivity during self-assembly. The small size dispersity of the nanoparticles within individual mesocrystals is accompanied by a very narrow lattice parameter distribution. In contrast, the lattice parameter distribution within all mesocrystals of an ensemble is about four times wider than that of individual mesocrystals, indicating significant size fractionalization between mesocrystals during self-assembly. The small size dispersity within each mesocrystal has important implications for their physical properties., Published by Royal Society of Chemistry, Cambridge

ACS applied energy materials 3(6), 5101-5106 (2020). doi:10.1021/acsaem.0c00543, Published by ACS Publications, Washington, DC

We use an electron holographic method to determine the charge distribution along a quasi-one-dimensional W5O14 nanowire during in situ field emission in a transmission electron microscope. The results show that the continuous charge distribution along the nanowire is not linear, but that there is an additional accumulation of charge at its apex. An analytical expression for this additional contribution to the charge distribution is proposed and its effect on the field enhancement factor and emission current is discussed.

The Gatan K2 IS direct electron detector (Gatan Inc., 2018), which was introduced in 2014, marked a watershed moment in the development of cameras for transmission electron microscopy (TEM) (Pan & Czarnik, 2016). Its pixel frequency, i.e. the number of data points (pixels) recorded per second, was two orders of magnitude higher than the fastest cameras available only five years before. Starting from 2009, the data rate of TEM cameras has outpaced the development of network, mass storage and memory bandwidth by almost two orders of magnitude. Consequently, solutions based on personal computers (PCs) that were adequate until then are no longer able to handle the resulting data rates. Instead, tailored high-performance setups are necessary. Similar developments have occurred for advanced X-ray sources such as the European XFEL, requiring special information technology (IT) systems for data handling (Sauter, Hattne, Grosse-Kunstleve, & Echols, 2013) (Fangohr, et al., 2018). Information and detector technology are currently under rapid development and involve disruptive technological innovations. This chapter briefly reviews the technological developments of the past 20 years, presents a snapshot of the current situation at the beginning of 2019 with many practical considerations, and looks forward to future developments.

Advances in catalysis rely on the synthesis and characterisation of nanoparticles that have tailored structures and compositions. Although energy-dispersive X-ray (EDX) spectroscopy can be used to study local variations in the compositions of individual supported nanoparticles on the atomic-scale in the scanning transmission electron microscope, electron beam induced damage and contamination can preclude the use of long exposure times and tomographic approaches. Here, we perform simulations of EDX maps of seven different octahedral PtNi nanoparticles for a selection of crystallographic orientations and tilts, to evaluate which of them can be distinguished from elemental mapping performed in only one orientation. Electronic supplementary material The online version of this article (10.1186/s40679-018-0053-x) contains supplementary material, which is available to authorized users.

Advances in fuel cell technology depend strongly on the development of affordable, active, and stable catalysts. For example, octahedral Pt–Ni alloy nanoparticles show exceptional activity for the oxygen reduction reaction in fuel cell cathodes as a result of the presence of highly active {1 1 1} facets. Here, we review a selection of recent transmission electron microscopy studies that address the correlation between the catalytic performance of octahedral Pt–Ni-based nanoparticles and their atomic-scale structure and composition. We begin by describing strategies for the growth of binary Pt–Ni and ternary Pt–Ni–TM (TM = transition metal) nanoparticles, with a focus on understanding how their structure and compositional anisotropy is related to their catalytic activity and stability. We then describe the morphological changes and compositional degradation effects that can occur in electrochemical environments. Changes in nanoparticle shape, including the loss of highly active {1 1 1} facets due to dealloying from Ni-rich facets and Pt surface diffusion, are discussed as important reasons for catalyst degradation. Finally, strategies to prevent degradation, e.g. by surface doping, are addressed. The growth, segregation, and degradation mechanisms that we describe highlight the complexity with which octahedral alloy nanoparticles form and evolve under reaction conditions.

State‐of‐the‐art water‐oxidation catalysts (WOCs) in acidic electrolytes usually contain expensive noble metals such as ruthenium and iridium. However, they too expensive to be implemented broadly in semiconductor photoanodes for photoelectrochemical (PEC) water splitting devices. Here, an Earth‐abundant CoFe Prussian blue analogue (CoFe‐PBA) is incorporated with core–shell Fe2O3/Fe2TiO5 type II heterojunction nanowires as composite photoanodes for PEC water splitting. Those deliver a high photocurrent of 1.25 mA cm−2 at 1.23 V versus reversible reference electrode in acidic electrolytes (pH = 1). The enhancement arises from the synergic behavior between the successive decoration of the hematite surface with nanolayers of Fe2TiO5 and then, CoFe‐PBA. The underlying physical mechanism of performance enhancement through formation of the Fe2O3/Fe2TiO5/CoFe‐PBA heterostructure reveals that the surface states’ electronic levels of hematite are modified such that an interfacial charge transfer becomes kinetically favorable. These findings open new pathways for the future design of cheap and efficient hematite‐based photoanodes in acidic electrolytes.

The thermal demagnetization of pseudo‐single‐domain (PSD) magnetite (Fe3O4) particles, which govern the magnetic signal in many igneous rocks, is examined using off‐axis electron holography. Visualization of a vortex structure held by an individual Fe3O4 particle (~250 nm in diameter) during in situ heating is achieved through the construction and examination of magnetic‐induction maps. Stepwise demagnetization of the remanence‐induced Fe3O4 particle upon heating to above the Curie temperature, performed in a similar fashion to bulk thermal demagnetization measurements, revealed that its vortex state remains stable under heating close to its unblocking temperature and is recovered upon cooling with the same or reversed vorticity. Hence, the PSD Fe3O4 particle exhibits thermomagnetic behavior comparable to a single‐domain carrier, and thus, vortex states are considered reliable magnetic recorders for paleomagnetic investigations., Key Points Thermal demagnetization of nonideal magnetite particlesVisualized magnetization of vortex state with temperatureVortex structures are reliable paleomagnetic signal recorders

Electron waves give an unprecedented enhancement to the field of microscopy by providing higher resolving power compared to their optical counterpart. Further information about a specimen, such as electric and magnetic features, can be revealed in electron microscopy because electrons possess both a magnetic moment and charge. In-plane magnetic structures in materials can be studied experimentally using the effect of the Lorentz force. On the other hand, full mapping of the magnetic field has hitherto remained challenging. Here we measure a nanoscale out-of-plane magnetic field by interfering a highly twisted electron vortex beam with a reference wave. We implement a recently developed holographic technique to manipulate the electron wavefunction, which gives free electrons an additional unbounded quantized magnetic moment along their propagation direction. Our finding demonstrates that full reconstruction of all three components of nanoscale magnetic fields is possible without tilting the specimen., Beyond high resolving power, electron microscopy can be used to study both the electronic and magnetic properties of a sample. Here, Grillo et al. combine electron vortex beams with holographic detection to measure out-of-plane nanoscale magnetic fields.

A novel device that can be used as a tunable support-free phase plate for transmission electron microscopy of weakly scattering specimens is described. The device relies on the generation of a controlled phase shift by the magnetic field of a segment of current-carrying wire that is oriented parallel or antiparallel to the electron beam. The validity of the concept is established using both experimental electron holographic measurements and a theoretical model based on Ampere's law. Computer simulations are used to illustrate the resulting contrast enhancement for studies of biological cells and macromolecules.

The use of chiral skyrmions, which are nanoscale vortex-like spin textures, as movable data bit carriers forms the basis of a recently proposed concept for magnetic solid-state memory. In this concept, skyrmions are considered to be unique localized spin textures, which are used to encode data through the quantization of different distances between identical skyrmions on a guiding nanostripe. However, the conservation of distances between highly mobile and interacting skyrmions is difficult to implement in practice. Here, we report the direct observation of another type of theoretically-predicted localized magnetic state, which is referred to as a chiral bobber (ChB), using quantitative off-axis electron holography. We show that ChBs can coexist together with skyrmions. Our results suggest a novel approach for data encoding, whereby a stream of binary data representing a sequence of ones and zeros can be encoded via a sequence of skyrmions and bobbers. The need to maintain defined distances between data bit carriers is then not required. The proposed concept of data encoding promises to expedite the realization of a new generation of magnetic solid-state memory.