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This study investigates the 5$f$-electron-conduction electron hybridization process in the heavy fermion superconductor UPd$_2$Al$_3$ using a combination of angle-resolved photoemission spectroscopy (ARPES) and time-resolved photoemission spectroscopy (tr-PES). ARPES measurements reveal the formation of a hybridization gap at a temperature of approximately 75 K, which becomes more pronounced as the temperature decreases. Notably, the persistence of a flat U 5$f$ band at temperatures well above the hybridization onset challenges conventional understanding. Our findings demonstrate a non-monotonic temperature dependence of the quasiparticle relaxation time, with an anomalous decrease at 20 K, suggesting complex electronic and magnetic interactions. These findings provide detailed insights into the 5$f$-electron hybridization process in UPd$_2$Al$_3$, with significant implications for the understanding of heavy fermion superconductivity and the role of 5$f$-electron hybridization in uranium-based materials., Comment: 5 pages, 4 figures

We propose differential phase contrast (DPC) imaging using energy-filtered electrons to image the magnetic properties of materials at the atomic scale. Compared to DPC measurements with elastic electrons, our simulations predict about two orders of magnitude higher relative magnetic signal intensities and sensitivity to all three vector components of magnetization., Comment: 6 pages, 5 figures

Conversion of charge to orbital angular momentum through the orbital Hall effect (OHE) holds transformative potential for the development of orbital-based electronics, however, it is challenging to directly observe the electrically generated orbital accumulation. Here, we detect the OHE by directly quantifying the orbital accumulation along the edges of a titanium thin film using a scanning transmission electron microscope. We measure the Ti L-edge using electron energy-loss spectroscopy with nanometer resolution and find a sizable orbital accumulation at the sample's outer perimeters, consistent with all signatures expected for the OHE, and determine an orbital diffusion length $\ell_o \approx 7.3$ nm. Our data points to a surprising dependence of the orbital diffusion length on the nano-structural morphology., Comment: 13 pages, 3 figures

Phonon dispersion is widely used to elucidate the vibrational properties of materials. As an emerging technique, momentum-resolved vibrational spectroscopy in scanning transmission electron microscopy (STEM) offers an unparalleled approach to explore q-dependent phonon behavior at local structures. In this study, we systematically investigate the phonon dispersion of monolayer graphene across several Brillouin zones (BZs) using momentum-resolved vibrational spectroscopy and find that the optical phonon signals vanish at the {\Gamma} points with indices (hk0) satisfying h+2k=3n (n denoted integers). Theoretical analysis reveals that the observed phenomena arise from the complete destructive interference of the scattered waves from different basis atoms. This observation, corroborated by the study of diamond, should be a general characteristic of materials composed of symmetrically equivalent pairs of the same elements. Moreover, our results emphasize the importance of multiple scattering in interpreting the vibrational signals in bulk materials. We demonstrate that the systematic absences and dynamic effects, which have not been much appreciated before, offer new insights into the experimental assessment of local vibrational properties of materials.

We present a method for computing angle-resolved electron-energy-loss and gain spectroscopies for phonon and magnon excitations in transmission electron microscopy. Fractional scattering intensities are derived from the temperature-dependent time auto-correlation of the electron beam wave function. This method captures both single and multiple scattering processes, as well as dynamical diffraction effects. Our method remains computationally efficient, and it is easy to parallelize., Comment: We include simulations of relevant systems and compare with existing experimental results

We report the discovery of a boundary-induced body-centered tetragonal (bct) iron phase in thin films deposited on MgAl$_{2}$O$_{4}$ ($001$) substrates. We present evidence for this phase using detailed x-ray analysis and ab-initio density functional theory calculations. A lower magnetic moment and a rotation of the easy magnetisation direction are observed, as compared to body-centered cubic (bcc) iron. Our findings expand the range of known crystal and magnetic phases of iron, providing valuable insights for the development of heterostructure devices using ultra-thin iron layers., Comment: Main text: 4 pages, 3 figures. Supplemental Material: 9 pages, 11 figures

We explore the inelastic electron scattering in SrTiO3, PbTiO3, and SiC in their phonon energy range, challenging the assumption that phonon polaritons are excluded at large angles in high-resolution transmission electron energy-loss spectroscopy. We demonstrate that through multiple scattering, the electron beam can excite both phonons and phonon polaritons, and the relative proportion of each varies depending on the structure factor and scattering angle. Integrating dielectric theory, density functional theory, and multi-slice simulations, we provide a comprehensive framework for understanding these interactions in materials with polar optical phonons.

We investigate the antiferromagnetic heavy fermion superconductor UPd$_2$Al$_3$, employing angle-resolved photoemission spectroscopy to unravel the complex electronic structure of its U 5f electrons. We observe unexpected characteristics that challenge the conventional temperature-dependent behavior of heavy fermion systems, revealing unexpected characteristics. At temperatures above the anticipated coherence temperature (T$^*$), we observe itinerant U 5f electrons at temperatures higher than previously postulated. Additionally, a previously unidentified dispersionless band emerges around 600 meV below the Fermi energy, potentially linked to spin-orbit splitting within the U 5f states. Hybridization between the 5f electrons and conduction band was observed with an energy dispersion of 10 meV at low temperatures, suggesting that U 5f electrons near and at the Fermi surface have an itinerant nature. Temperature-dependent 5d-5f resonance spectra reveal that the 5f electron spectrum weight increases with lowering temperature and begins to decrease at temperatures significantly higher than the Neel temperature (T$_N$). We further show that the competition between the Kondo effect and Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions may be responsible for the relocalization of 5f electrons, making relocalization a precursor to the establishment of magnetic order at lower temperatures. Our experiments also provide evidence that 5f electrons with the same orbital are involved in both the Kondo effect and RKKY interactions, suggesting that the two coexist at lower temperatures., Comment: 6 pages, 4 figures

The underlying dielectric properties of materials, intertwined with intriguing phenomena such as topological polariton modes and anisotropic thermal conductivities, stem from the anisotropy in atomic vibrations. Conventionally, X-ray diffraction techniques have been employed to estimate thermal ellipsoids of distinct elements, albeit lacking the desired spatial and energy resolutions. Here we introduce a novel approach utilizing the dark-field monochromated electron energy-loss spectroscopy for momentum-selective vibrational spectroscopy, enabling the cartographic delineation of variations of phonon polarization vectors. By applying this technique to centrosymmetric cubic-phase strontium titanate, we successfully discern two types of oxygen atoms exhibiting contrasting vibrational anisotropies below and above 60 meV due to their frequency-linked thermal ellipsoids. This method establishes a new pathway to visualize phonon eigenvectors at specific crystalline sites for diverse elements, thus delving into uncharted realms of dielectric, optical, and thermal property investigations with unprecedented spatial resolutions.

Electron magnetic circular dichroism (EMCD) is a powerful technique for estimating element-specific magnetic moments of materials on nanoscale with the potential to reach atomic resolution in transmission electron microscopes. However, the fundamentally weak EMCD signal strength complicates quantification of magnetic moments, as this requires very high precision, especially in the denominator of the sum rules. Here, we employ a statistical resampling technique known as bootstrapping to an experimental EMCD dataset to produce an empirical estimate of the noise dependent error distribution resulting from application of EMCD sum rules to bcc iron in a 3 beam orientation. We observe clear experimental evidence that noisy EMCD signals preferentially bias the estimation of magnetic moments, further supporting this with error distributions produced by Monte-Carlo simulations. Finally, we propose guidelines for the recognition and minimization of this bias in the estimation of magnetic moments.

Parkinson's disease (PD) is a neurological disorder impacting a person's speech. Among automatic PD assessment methods, deep learning models have gained particular interest. Recently, the community has explored cross-pathology and cross-language models which can improve diagnostic accuracy even further. However, strict patient data privacy regulations largely prevent institutions from sharing patient speech data with each other. In this paper, we employ federated learning (FL) for PD detection using speech signals from 3 real-world language corpora of German, Spanish, and Czech, each from a separate institution. Our results indicate that the FL model outperforms all the local models in terms of diagnostic accuracy, while not performing very differently from the model based on centrally combined training sets, with the advantage of not requiring any data sharing among collaborators. This will simplify inter-institutional collaborations, resulting in enhancement of patient outcomes., Comment: INTERSPEECH 2023, pp. 5003--5007, Dublin, Ireland

We compare the Frequency-Resolved Frozen Phonon Multislice (FRFPMS) method, introduced in Phys. Rev. Lett. 124, 025501 (2020), with other theoretical approaches used to account for the inelastic scattering of high energy electrons, namely the first-order Born approximation and the quantum excitation of phonons model. We show, that these theories lead to similar expressions for the single inelastically scattered intensity as a function of momentum transfer for an anisotropic quantum harmonic oscillator in a weak phase object approximation of the scattered waves, except for a too small smearing of the scattering potential by the effective Debye-Waller factor (DWF) in the FRFPMS method. We propose that this issue can be fixed by including an explicit DWF smearing into the potential and demonstrate numerically, that in any realistic situation, a FRFPMS approach revised in this way, correctly accounts for the single inelastically scattered intensity and the correct elastic scattering intensity. Furthermore our simulations illustrate that the only requirement for such a revised FRFPMS method is the smallness of mean squared displacements for all atomic species in all frequency bins. The analytical considerations for the FRFPMS method also explain the $1/\omega^2$-scaling of FRFPMS spectra observed in Phys. Rev. B 104, 104301 (2021) by the use of classical statistics in the molecular dynamics simulation. Moreover, we find that the FRFPMS method inherently adds the contributions of phonon loss and gain within each frequency bin. Both of these issues related to the frequency-scaling can be fixed by a system-independent post-processing step.

We investigated the electronic structure of the antiferromagnetic Kondo lattice CePd5Al2 using high-resolution angle-resolved photoemission spectroscopy. The experimentally determined band structure of the conduction electrons is predominated by the Pd 4d character. It contains multiple hole and electron Fermi pockets, in good agreement with density functional theory calculations. The Fermi surface is folded over Q0 = (0, 0, 1), manifested by Fermi surface reconstruction and band folding. Our results suggest that Fermi surface nesting drives the formation of antiferromagnetic order in CePd5Al2., Comment: 6 pages,3 figure

The isotopic mass of constituent elements of materials has a well-known effect on the energy of vibrational modes. By means of monochromated scanning transmission electron microscopy we have experimentally studied the phonon bandstructure of hexagonal BN, where a phonon band gap appears between in-plane optical phonon modes and the lower energy part of the phonon spectrum. The size of the phonon band gap can be manipulated by the isotopic mass of the boron. While in $^{11}$BN the phonon band gap is about 7 meV wide, in $^{10}$BN the gap nearly closes, being an order of magnitude smaller (below 0.5 meV). This opens exciting options for manipulating terahertz wave propagation through isotopically structured devices having otherwise no interfaces between chemically distinct components., Comment: 5 pages, 3 figures

Magnon diffuse scattering (MDS) signals could be studied with high spatial resolution in scanning transmission electron microscopy (STEM), thanks to recent technological progress in electron energy loss spectroscopy. However, detecting MDS signals in STEM is challenging due to their overlap with stronger thermal diffuse scattering (TDS) signals. In bcc Fe at 300 K, MDS signals greater than or comparable to TDS signals occur under the central Bragg disk, into a currently inaccesible energy-loss region. Therefore, to detect MDS in STEM, it is necessary to find conditions in which TDS and MDS signals can be separated. Temperature may be a key factor due to the distinct thermal signatures of magnon and phonon signals. In this work, we present a study on the effects of temperature on MDS and TDS in bcc Fe -- considering a detector outside the central Bragg disk and a fixed convergent electron probe -- using the frozen phonon and frozen magnon multislice methods. Our study reveals that neglecting the effects of atomic vibrations causes the MDS signal to grow approximately linearly up to the Curie temperature of Fe, after which it exhibits less variation. The MDS signal displays an alternating behavior due to dynamical diffraction, instead of increasing monotonically as a function of thickness. Including the effects of atomic vibrations through a complex atomic electrostatic potential causes the linear growth of the MDS signal to change to a non-linear behavior that exhibits a predominant peak for a sample of thickness 16.072 nm at 1100 K. In contrast, the TDS signal grows more linearly than the MDS signal but still exhibits appreciable dynamical diffraction effects. An analysis of the signal-to-noise ratio (SNR) shows that the MDS signal can be a statistically significant contribution to the total scattering intensity under realizable measurement conditions and acquisition times., Comment: *) Changed title to "Unveiling the impact of temperature on magnon diffuse scattering detection in the transmission electron microscope." *) Incorporated the effects of absorption due to phonons in the magnon-diffuse-scattering calculations through a complex atomic electrostatic potential

The need to acquire multiple angle-resolved electron energy loss spectra (EELS) is one of the several critical challenges associated with electron magnetic circular dichroism (EMCD) experiments. If the experiments are performed by scanning a nanometer to atomic-sized electron probe on a specific region of a sample, the precision of the local magnetic information extracted from such data highly depends on the accuracy of the spatial registration between multiple scans. For an EMCD experiment in a 3-beam orientation, this means that the same specimen area must be scanned four times while keeping all the experimental conditions same. This is a non-trivial task as there is a high chance of morphological and chemical modification as well as non-systematic local orientation variations of the crystal between the different scans due to beam damage, contamination and spatial drift. In this work, we employ a custom-made quadruple aperture to acquire the four EELS spectra needed for the EMCD analysis in a single electron beam scan, thus removing the above-mentioned complexities. We demonstrate a quantitative EMCD result for a beam convergence angle corresponding to sub-nm probe size and compare the EMCD results for different detector geometries., Comment: 10 pages, 7 figures

We have simulated the magnetic Bragg scattering in transmission electron microscopy in two antiferromagnetic compounds, NiO and LaMnAsO. This weak magnetic phenomenon was experimentally observed in NiO by Loudon. We have computationally reproduced Loudon's experimental data, and for comparison we have performed calculations for the LaMnAsO compound as a more challenging case, containing lower concentration of magnetic elements and strongly scattering heavier non-magnetic elements. We have also described thickness and voltage dependence of the intensity of the antiferromagnetic Bragg spot for both compounds. We have considered lattice vibrations within two computational approaches, one assuming a static lattice with Debye-Waller smeared potentials, and another explicitly considering the atomic vibrations within the quantum excitations of phonons model (thermal diffuse scattering). The structural analysis shows that the antiferromagnetic Bragg spot appears in between (111) and (000) reflections for NiO, while for LaMnAsO the antiferromagnetic Bragg spot appears at the position of the (010) reflection in the diffraction pattern, which corresponds to a forbidden reflection of the crystal structure. Calculations predict that the intensity of the magnetic Bragg spot in NiO is significantly stronger than thermal diffuse scattering at room temperature. For LaMnAsO, the magnetic Bragg spot is weaker than the room-temperature thermal diffuse scattering, but its detection can be facilitated at reduced temperatures.

Electrons can form a two-dimensional electron gas at metal surfaces, where lateral confinement leads to quantum-well states. Such states have been observed for highly itinerant electrons, but it remains an open question whether quantum-well states can be formed from strongly correlated electrons. Here we study atomically flat terraces on surfaces of the heavy-fermion superconductor URu$_2$Si$_2$ using millikelvin scanning tunneling spectroscopy. We observe two-dimensional heavy fermions (2DHF) with an effective mass 17 times the free electron mass that form quantized states separated by a fraction of a meV. Superconductivity at the surface is induced by the bulk into the 2DHF. Our results provide a new route to realize quantum well states in correlated quantum materials.

Background: An early diagnosis together with an accurate disease progression monitoring of multiple sclerosis is an important component of successful disease management. Prior studies have established that multiple sclerosis is correlated with speech discrepancies. Early research using objective acoustic measurements has discovered measurable dysarthria. Objective: To determine the potential clinical utility of machine learning and deep learning/AI approaches for the aiding of diagnosis, biomarker extraction and progression monitoring of multiple sclerosis using speech recordings. Methods: A corpus of 65 MS-positive and 66 healthy individuals reading the same text aloud was used for targeted acoustic feature extraction utilizing automatic phoneme segmentation. A series of binary classification models was trained, tuned, and evaluated regarding their Accuracy and area-under-curve. Results: The Random Forest model performed best, achieving an Accuracy of 0.82 on the validation dataset and an area-under-curve of 0.76 across 5 k-fold cycles on the training dataset. 5 out of 7 acoustic features were statistically significant. Conclusion: Machine learning and artificial intelligence in automatic analyses of voice recordings for aiding MS diagnosis and progression tracking seems promising. Further clinical validation of these methods and their mapping onto multiple sclerosis progression is needed, as well as a validating utility for English-speaking populations.

We systemically investigate the nature of Ce 4f electrons in structurally layered heavy-fermion compounds CcmMnIn3m+2n (with M =Co, Rh, Ir, and Pt, m=l, 2, n=0 - 2), at low temperature using on-resonance angle-resolved photoemission spectroscopy. Three heavy quasiparticle bands f^0, f^1_7/2 and f^1_5/2 are observed in all compounds, but their intensities and energy locations vary greatly with materials. The strong f^0 states imply that the localized electron behavior dominates the Ce 4f states. The Ce 4f electrons are partially hybridized with the conduction electrons, making them have the dual nature of localization and itinerant. Our quantitative comparison reveals that the f^1_5/2 / f^0 intensity ratio is more suitable to reflect the 4f-state hybridization strength., Comment: 7 pages, 4 figures

We present a theory and a simulation of thermal diffuse scattering due to the excitation of magnons in scanning transmission electron microscopy. The calculations indicate that magnons can present atomic contrast when detected by electron energy-loss spectroscopy using atomic-size electron beams. The results presented here indicate that the intensity of the magnon diffuse scattering in bcc iron at 300~K is 4 orders of magnitude weaker than the intensity of thermal diffuse scattering arising from atomic vibrations. In an energy range where the phonon and magnon dispersions do not overlap, a monochromated scanning transmission electron microscope equipped with direct electron detectors for spectroscopy is expected to resolve the magnon spectral signatures., Comment: 6 pages, 3 figures

The multislice method, which simulates the propagation of the incident electron wavefunction through a crystal, is a well-established method for analyzing the multiple scattering effects that an electron beam may undergo. The inclusion of magnetic effects into this method proves crucial towards simulating magnetic differential phase contrast images at atomic resolution, enhanced magnetic interaction of vortex beams with magnetic materials, calculating magnetic Bragg spots, or searching for magnon signatures, to name a few examples. Inclusion of magnetism poses novel challenges to the efficiency of the multislice method for larger systems, especially regarding the consistent computation of magnetic vector potentials and magnetic fields over large supercells. We present in this work a tabulation of parameterized magnetic values for the first three rows of transition metal elements computed from atomic density functional theory calculations, allowing for the efficient computation of approximate magnetic vector fields across large crystals using only structural and magnetic moment size and direction information. Ferromagnetic bcc Fe and tetragonal FePt are chosen as examples in this work to showcase the performance of the parameterization versus directly obtaining magnetic vector fields from the unit cell spin density by density functional theory calculations, both for the quantities themselves and the resulting magnetic signal from their respective use in multislice calculations., Comment: 27 pages, 1 table, 6 figures

Recent developments in experiments with vibrational electron energy loss spectroscopy (EELS) have revealed spectral shape variations at spatial resolutions down to sub-atomic scale. Interpretation in terms of local phonon density of states enables their qualitative understanding, yet a more detailed analysis is calling for advances in theoretical methods. In Zeiger and Rusz, Phys. Rev. Lett. 124, 025501 (2020) we have presented a frequency resolved frozen phonon multislice method for simulations of vibrational EELS. Detailed simulations for a plane wave electron beam scattering on a vibrating hexagonal boron nitride are presented in a companion manuscript (Zeiger and Rusz, arXiv:2104.03197). Here we present simulations of vibrational EELS assuming a convergent electron probe of nanometer size and atomic size on a hexagonal boron nitride structure model with a planar defect. With a nanometer beam we observe spectral shape modifications in the presence of the defect, which are correlated with local changes of the phonon density of states. With an atomic size electron beam, we observe the same, although with better contrast. In addition, we observe atomic level contrast and sub-atomic scale spectral shape modifications, which are particularly strong for small detector collection angles., Comment: 11 pages, 13 figures

We explore the capabilities of the frequency-resolved frozen phonon multislice method introduced in Phys. Rev. Lett. 124, 025501 (2020) to model inelastic vibrational scattering in transmission electron microscopy. We review the method in detail and discuss advantages of using a so called hotspot thermostat instead of the $\delta$-thermostat used in our first report. We apply the method to simulate vibrational electron energy loss spectra of hexagonal boron nitride under plane wave illumination. Simulated spectroscopic information well represents the theoretical phonon bandstructure of the studied material, both in terms of energies as well as polarization vectors of individual phonon modes.

The interest in understanding scaling limits of magnetic textures such as domain walls spans the entire field of magnetism from its relativistic quantum fundamentals to applications in information technologies. The traditional focus of the field on ferromagnets has recently started to shift towards antiferromagnets which offer a rich materials landscape and utility in ultra-fast and neuromorphic devices insensitive to magnetic field perturbations. Here we report the observation that domain walls in an epitaxial crystal of antiferromagnetic CuMnAs can be atomically sharp. We reveal this ultimate domain wall scaling limit using differential phase contrast imaging within aberrationcorrected scanning transmission electron microscopy, which we complement by X-ray magnetic dichroism microscopy and ab initio calculations. We highlight that the atomically sharp domain walls are outside the remits of established spin-Hamiltonian theories and can offer device functionalities unparalleled in ferromagnets., Comment: 8 pages, 4 figures, Supplementary information

The presence of a quantum critical point separating two distinct zero-temperature phases is thought to underlie the `strange' metal state of many high-temperature superconductors. The nature of this quantum critical point, as well as a description of the resulting strange metal, are central open problems in condensed matter physics. In large part, the controversy stems from the lack of a clear broken symmetry to characterize the critical phase transition, and this challenge is no clearer than in the example of the unconventional superconductor CeCoIn$_5$. Through Hall effect and Fermi surface measurements of CeCoIn$_5$, in comparison to ab initio calculations, we find evidence for a critical point that connects two Fermi surfaces with different volumes without apparent symmetry-breaking, indicating the presence of a transition that involves an abrupt localization of one sector of the charge degrees of freedom. We present a model for the anomalous electrical Hall resistivity of this material based on the conductivity of valence charge fluctuations., Comment: 17 pages, 4 figures, Supplement included

When magnetic properties are analysed in a TEM using the technique of electron magnetic circular dichroism (EMCD), one of the critical parameters is the sample orientation, and this, independently on the chosen acquisition geometry. Since small orientation changes can have a strong impact on the EMCD measurement, it is experimentally non trivial to measure the EMCD signal as a function of sample orientation. The classical EMCD experimental setup requires to tilt the crystal in a 2 beam orientation and to acquire two electron energy loss spectra at two conjugate scattering angles. The effect of a mistilt from the perfect 2-beam orientation on the measured EMCD signals has not been explored yet due to different experimental constraints. In order to maintain the exact sample location and orientation for the acquisition of the EMCD signal, we have developed a methodology to simultaneously map the quantitative EMCD signals and the local orientation of the crystal. We analyse, both experimentally and with simulations, how the measured magnetic signals evolve with a change in the crystal tilt from the exact 2-beam orientation. Based on this analysis, we establish an accurate relationship between the crystal orientations and the EMCD signals. Our results demonstrate that a small crystal tilt away from the 2-beam orientation can significantly alter the strength and the distribution of the EMCD signals. From an optimisation of the crystal orientation, we obtain quantitative EMCD measurements., Comment: 13 pages, 8 figures, 1 table

In this work we derive sum rules for orbital angular momentum(OAM) resolved electron magnetic chiral dichroism (EMCD) which enable the evaluation of the strength of spin and orbital components of the atomic magnetic moments in a crystalline sample. We also demonstrate through numerical simulations that these rules appear to be only slightly dependent from the dynamical diffraction of the electron beam in the sample, making possible their application without the need of additional dynamical diffraction calculations., Comment: 7 pages, 4 figures

The three-dimensional electronic structure and Ce 4f electrons of the heavy fermion superconductor CePt2In7 is investigated. Angle-resolved photoemission spectroscopy using variable photon energy establishes the existence of quasi-two and three dimensional Fermi surface topologies. Temperature-dependent 4d-4f on-resonance photoemission spectroscopies reveal that heavy quasiparticle bands begin to form at a temperature well above the characteristic (coherence) temperature T*. T* emergence may be closely related to crystal electric field splitting, particularly the low-lying heavy band formed by crystal electric field splitting., Comment: 6 pages, 4 figures

We introduce a novel method for the simulation of the impact scattering in vibrational scanning transmission electron microscopy electron energy loss spectroscopy (STEM-EELS) simulations. The phonon-loss process is modeled by a combination of molecular dynamics and elastic multislice calculations within a modified frozen phonon approximation. The key idea is thereby to use a so-called $\delta$-thermostat in the classical molecular dynamics simulation to generate frequency dependent configurations of the vibrating specimen's atomic structure. The method includes correlated motion of atoms and provides vibrational spectrum images at the cost comparable to standard frozen phonon calculations. We demonstrate good agreement of our method with simulations and experiments for a 15nm flake of hexagonal boron-nitride (hBN).

We give an experimental demonstration of two types of recently proposed ventilator apertures which can be used to acquire electron magnetic circular dichroic (EMCD) signals in zone axis orientation with high spatial resolution. To simplify the experimental procedures, we propose a third type of aperture and experimentally demonstrate the use of this modified ventilator aperture for the case of multiple symmetries in the diffraction patterns. To show the feasibility of the atomic resolution EMCD, EMCD signals are acquired for a range of beam convergence angles. High quality EMCD signals with convergence angles corresponding to atomic resolution electron probes are obtained., Comment: 10 pages including 5 figures and 1 table

We use high-resolution angle-resolved photoemission spectroscopy to investigate the electronic structure of the antiferromagnetic heavy fermion compound CePt2In7, which is a member of the CeIn3-derived heavy fermion material family. Weak hybridization among 4f electron states and conduction bands was identified in CePt2In7 at low temperature much weaker than that in the other heavy fermion compounds like CeIrIn5 and CeRhIn5. The Ce 4f spectrum shows fine structures near the Fermi energy, reflecting the crystal electric field splitting of the 4f^1_5/2 and 4f^1_7/2 states. Also, we find that the Fermi surface has a strongly three-dimensional topology, in agreement with density-functional theory calculations., Comment: 7 pages, 4 figures

Measuring magnetic moments in ferromagnetic materials with atomic column resolution is theoretically possible using the electron magnetic circular dichroism (EMCD) technique in a (scanning) transmission electron microscope ((S)TEM). However, experimental and data processing hurdles currently hamper the realization of this goal. Experimentally, the sample must be tilted to a zone-axis orientation, yielding a complex distribution of magnetic scattering intensity, and the same sample region must be scanned multiple times with sub-atomic spatial registration necessary at each pass. Furthermore, the weak nature of the EMCD signal requires advanced data processing techniques to reliably detect and quantify the result. In this manuscript, we detail our experimental and data processing progress towards achieving single-pass zone-axis EMCD using a patterned aperture. First, we provide a comprehensive data acquisition and analysis strategy for this and other EMCD experiments that should scale down to atomic resolution experiments. Second, we demonstrate that, at low spatial resolution, promising EMCD candidate signals can be extracted, and that these are sensitive to both crystallographic orientation and momentum transfer., Comment: 17 pages, 9 figures. Data available at DOI: 10.5281/zenodo.3361582 Code available at DOI: 10.5281/zenodo.3374648

We investigated experimentally and computationally the concentration dependence of electronic specific heat coefficient $\gamma$ in Y(Fe$_{1-x}$Co$_x$)$_2$ pseudobinary Laves phase system. The experimentally observed maximum in $\gamma$($x$) around the magnetic phase transition was interpreted within the local density approximation (LDA) combined with the virtual crystal approximation (VCA). To explain the formation of the observed maximum, we analyzed theoretically the dependence of the magnetic energy, magnetic moments, densities of states, and Fermi surfaces on the Co concentration. Furthermore, we carried out the calculations of density of states at the Fermi level as a function of fixed spin moment. The calculated Co concentration at which $\gamma$ takes the maximum value ($x_{\mathrm{max-LDA-VCA}}=0.91$) stays in good agreement with the measured value ($x_{\mathrm{max-expt}} = 0.925$). We conclude that the observed maximum in $\gamma(x)$ results from the presence of the sharp DOS peak in the vicinity of the Fermi level.

We propose a highly efficient atomically-resolved mode of electron magnetic chiral dichroism. This method exploits the recently introduced orbital angular momentum spectrometer to analyze the inelastically scattered electrons allowing for simultaneous dispersion in both energy and angular momentum. The technique offers several advantages over previous formulations of electron magnetic chiral dichroism as it requires much simpler experimental conditions in terms of specimen orientation and thickness. A novel simulation algorithm, based on the multislice description of the beam propagation, is used to anticipate the advantages of the new approach over current electron magnetic chiral dichroism implementations. Numerical calculations confirm an increased magnetic signal to noise ratio with in plane atomic resolution., Comment: 14 pages, 5 figures

Utilizing the Pauli equation based multislice method, introduced in Phys. Rev. Lett. 116, 127203 (2016), we study the atomic resolution differential phase contrast (DPC) imaging on an example of a hard magnet FePt with in-plane magnetization. Simulated center of mass pattern in a scanning transmission electron microscopy (STEM) experiment carries information about both electric and magnetic fields. The momentum transfer remains curl-free, which has consequences for interpretation of the integrated DPC technique. The extracted magnetic component of the pattern is compared to the expected projected microscopic magnetic field as obtained by density functional theory calculation. Qualitative agreement is obtained for low sample thicknesses and a suitable range of collection angles., Comment: 9 pages, 8 figures

The complex interplay of elastic and inelastic scattering amenable to different levels of approximation constitutes the major challenge for the computation and hence interpretation of TEM-based spectroscopical methods. The two major approaches to calculate inelastic scattering cross sections of fast electrons on crystals-Yoshioka-equations-based forward propagation and the reciprocal wave method-are founded in two conceptually differing schemes-a numerical forward integration of each inelastically scattered wave function, yielding the exit density matrix, and a computation of inelastic scattering matrix elements using elastically scattered initial and final states (double channeling). Here, we compare both approaches and show that the latter is computationally competitive to the former by exploiting analytical integration schemes over multiple excited states. Moreover, we show how to include full nonlocality of the inelastic scattering event, neglected in the forward propagation approaches, at no additional computing costs in the reciprocal wave method. Detailed simulations show in some cases significant errors due to the z-locality approximation and hence pitfalls in the interpretation of spectroscopical TEM results.

We propose a magnetic measurement method based on combining depth sectioning and electron magnetic circular dichroism in scanning transmission electron microscopy. Electron vortex beams with large convergence angles, as those achievable in current state-of-the-art aberration correctors, could produce atomic lateral resolution and depth resolution below 2~nm., Comment: 5 pages, 3 figures