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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.

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

Despite significant potential as energy storage materials for electric vehicles due to their combination of high energy density per unit cost and reduced environmental and ethical concerns, Co-free lithium ion batteries based off layered Mn oxides presently lack the longevity and stability of their Co-containing counterparts. Here, we demonstrate a reduction in this performance gap via chemical doping, with Li$_{1.1}$Ni$_{0.35}$Mn$_{0.55}$O$_2$ achieving an initial discharge capacity of 159 mAhg$^{-1}$ at C/3 rate and a corresponding capacity retention of 94.3% after 150 cycles. We subsequently explore the nanoscale origins of this improvement through a combination of advanced diffraction, spectroscopy, and electron microscopy techniques, finding that optimized doping profiles lead to an improved structural and chemical compatibility between the two constituent sub-phases that characterize the layered Mn oxide system, resulting in the formation of unobstructed lithium ion pathways between them. We also directly observe a structural stabilization effect of the host compound near the surface using aberration corrected scanning transmission electron microscopy and integrated differential phase contrast imaging., Comment: 20 pages, 8 figures

Modern TEM instrumentation can probe a wide range of structural, optical, and chemical properties with unprecedented resolution. However, each of these properties must be recorded in independent datasets using different detector modes with no unifying framework currently available for quantitatively mapping their relationships onto chemically distinct features, particularly in complex morphologies. Here, we tackle this challenge by proposing a data acquisition and analysis workflow called "hypermodal data fusion," describing how to directly couple an arbitrary number of highly disparate detector modes including spectroscopy and scanning diffraction and jointly analyze them for correlations. We demonstrate this concept on a random collection of anatase and rutile nanoparticles, first detailing how to use core-loss EELS to unmix the different polymorphs despite three-dimensional overlap along the beam direction and then showing how this can be used to extract polymorph-specific composition, bandgaps, and crystal structure. We conclude with a discussion on the applicability of this workflow for a broad range of materials systems., Comment: 18 pages, 8 figures

A DigitalMicrograph script InsteaDMatic has been developed to facilitate rapid automated continuous rotation electron diffraction (cRED) data acquisition. The script coordinates microscope functions, such as stage rotation, camera functions relevant for data collection, and stores the experiment metadata. The script is compatible with any microscope that can be controlled by DigitalMicrograph and has been tested on both JEOL and Thermo Fisher Scientific microscopes. A proof-of-concept has been performed through employing InsteaDMatic for data collection and structure determination of a ZSM-5 zeolite. The influence of illumination settings and electron dose rate on the quality of diffraction data, unit cell determination and structure solution has been investigated in order to optimize the data acquisition procedure.

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 propose a magnetic measurement method utilizing a patterned post-sample aperture in a transmission electron microscope. While utilizing electron magnetic circular dichroism, the method circumvents previous needs to shape the electron probe to an electron vortex beam or astigmatic beam. The method can be implemented in standard scanning transmission electron microscopes by replacing the spectrometer entrance aperture with a specially shaped aperture, hereafter called ventilator aperture. The proposed setup is expected to work across the whole range of beam sizes -- from wide parallel beams down to atomic resolution magnetic spectrum imaging., Comment: 6 pages, 4 figures

Understanding the ramifications of reduced crystalline symmetry on magnetic behavior is a critical step in improving our understanding of nanoscale and interfacial magnetism. However, investigations of such effects are often controversial largely due to the challenges inherent in directly correlating nanoscale stoichiometry and structure to magnetic behavior. Here, we describe how to use Transmission Electron Microscope (TEM) to obtain Electron Magnetic Circular Dichroism (EMCD) signals as a function of scattering angle to locally probe the magnetic behavior of thin oxide layers grown on an Fe (1 1 0) surface. Experiments and simulations both reveal a strong dependence of the magnetic orbital to spin ratio on its scattering vector in reciprocal space. We exploit this variation to extract the magnetic properties of the oxide cladding layer, showing that it locally may exhibit an enhanced orbital to spin moment ratio. This finding is supported here by both spatially and angularly resolved EMCD measurements, opening up the way for compelling investigations into how magnetic properties are affected by nanoscale features., Comment: Accepted in Scientific Reports. 22 pages, 6 figures

First experiments on the growth of oxypnictide F-doped LaFeAsO thin films indicated an incomplete normal-to-superconducting transition and offered a work programme challenging to overcome possible difficulties in their fabrication. In this regard the possibility of an all in-situ epitaxial growth appeared to be a matter of time and growth parameters. The following review clarifies that F-doped oxypnictide thin films are extremely difficult to grow by in-situ PLD due to the formation of very stable impurity phases such as oxyfluorides (LaOF) and oxides (La2O3) and the loss of stoichiometry possibly due to incongruent evaporation of the target or re-evaporation of volatile elements at the substrate surface. However, the review also demonstrates that the employed two-step fabrication process for oxypnictide thin films has been successfully applied in the preparation of clean polycrystalline as well as of epitaxial thin films. Fundamental investigations on the upper critical field, its temperature dependence and its anisotropy contributed to an understanding of multiband superconductivity in oxypnictides., Comment: accepted, pre-print version

Diffusionless phase transitions are at the core of the multifunctionality of (magnetic) shape memory alloys, ferroelectrics and multiferroics. Giant strain effects under external fields are obtained in low symmetric modulated martensitic phases. We outline the origin of modulated phases, their connection with tetragonal martensite and consequences for their functional properties by analysing the martensitic microstructure of epitaxial Ni-Mn-Ga films from the atomic to macroscale. Geometrical constraints at an austenite-martensite phase boundary act down to the atomic scale. Hence a martensitic microstructure of nanotwinned tetragonal martensite can form. Coarsening of twin variants can reduce twin boundary energy, a process we could follow from the atomic to the millimetre scale. Coarsening is a fractal process, proceeding in discrete steps by doubling twin periodicity. The collective defect energy results in a substantial hysteresis, which allows retaining modulated martensite as a metastable phase at room temperature. In this metastable state elastic energy is released by the formation of a 'twins within twins' microstructure which can be observed from the nanometre to millimetre scale. This hierarchical twinning results in mesoscopic twin boundaries which are diffuse, in contrast to the common atomically sharp twin boundaries of tetragonal martensite. We suggest that observed extraordinarily high mobility of such mesoscopic twin boundaries originates from their diffuse nature which renders pinning by atomistic point defects ineffective., Comment: 34 pages, 8 figures

We have successfully grown epitaxial, superconducting films of Ba(Fe1-xCox)2As2 (Ba-122)with x ~ 0.1. The films grow without observable correlated defects parallel to the c-axis, as confirmed by TEM. This is also reflected in the absence of a caxis peak in Jc({\theta}). In contrast to cuprate high-Tc superconductors such as YBa2Cu3O7-d or even Bi2Sr2Ca2Cu3O10-d, the pnictides show a rather low anisotropic behavior in their Jc({\theta}) behavior as well as in their upper critical fields, Hc2. As a multiband superconductor, Ba-122 exhibits a temperature dependent electronic mass anisotropy., Comment: contribution at ASC2010, accepted for publication in IEEE Trans. Appl. Supercond

We demonstrate the growth of epitaxial Fe/Ba(Fe(1-x)Co(x))2As2 (Fe/Ba-122) bilayers on MgO(001) and LSAT(001) single crystal substrates using Pulsed Laser Deposition (PLD). By exploiting the metallic nature of the FeAs tetrahedron in the Ba-122 crystal structure, we achieve a coherent interfacial bond between bcc iron and Co-doped Ba-122. Tc values for both bilayers were close to that of the PLD target. Direct observation of interfacial bonding between Fe and the Ba-122 FeAs sublattice by atomic resolution transmission electron microscopy implies that this bilayer architecture may work for other iron pnictide systems and pave the way for the fabrication of superconducting/ferromagnetic heterostructures., Comment: 3 pages, 4 figures