Origin of giant enhancement of phase contrast in electron holography of modulation-doped n-type GaN.

The electron optical phase contrast probed by electron holography at n-n+ GaN doping steps is found to exhibit a giant enhancement, in sharp contrast to the always smaller than expected phase contrast reported for p-n junctions. We unravel the physical origin of the giant enhancement by combining off-axis electron holography data with self-consistent electrostatic potential calculations. The predominant contribution to the phase contrast is shown to arise from the doping dependent screening length of the surface Fermi-level pinning, which is induced by FIB-implanted carbon point defects below the outer amorphous shell. The contribution of the built-in potential is negligible for modulation doping and only relevant for large built-in potentials at e.g. p-n junctions. This work provides a quantitative approach to so-called dead layers at TEM lamellas.

Current-driven writing process in antiferromagnetic Mn2Au for memory applications.

Current pulse driven Néel vector rotation in metallic antiferromagnets is one of the most promising concepts in antiferromagnetic spintronics. We show microscopically that the Néel vector of epitaxial thin films of the prototypical compound Mn2Au can be reoriented reversibly in the complete area of cross shaped device structures using single current pulses. The resulting domain pattern with aligned staggered magnetization is long term stable enabling memory applications. We achieve this switching with low heating of ≈20 K, which is promising regarding fast and efficient devices without the need for thermal activation. Current polarity dependent reversible domain wall motion demonstrates a Néel spin-orbit torque acting on the domain walls.

Effect of surface gallium termination on the formation and emission energy of an InGaAs wetting layer during the growth of InGaAs quantum dots by droplet epitaxy.

Self-assembled quantum dots (QDs) based on III-V semiconductors have excellent properties for applications in quantum optics. However, the presence of a 2D wetting layer (WL) which forms during the Stranski-Krastanov growth of QDs can limit their performance. Here, we investigate WL formation during QD growth by the droplet epitaxy technique. We use a combination of photoluminescence excitation spectroscopy, lifetime measurements, and transmission electron microscopy to identify the presence of an InGaAs WL in these droplet epitaxy QDs, even in the absence of distinguishable WL luminescence. We observe that increasing the amount of Ga deposited on a GaAs (100) surface prior to the growth of InGaAs QDs leads to a significant reduction in the emission wavelength of the WL to the point where it can no longer be distinguished from the GaAs acceptor peak emission in photoluminescence measurements. However increasing the amount of Ga deposited does not suppress the formation of a WL under the growth conditions used here.

Alignment of electron optical beam shaping elements using a convolutional neural network.

A convolutional neural network is used to align an orbital angular momentum sorter in a transmission electron microscope. The method is demonstrated using simulations and experiments. As a result of its accuracy and speed, it offers the possibility of real-time tuning of other electron optical devices and electron beam shaping configurations.

Non-topographic current contrast in scanning field emission microscopy.

In scanning field emission microscopy (SFEM), a tip (the source) is approached to few (or a few tens of) nanometres distance from a surface (the collector) and biased to field-emit electrons. In a previous study (Zanin et al. 2016 Proc. R. Soc. A 472, 20160475. (doi:10.1098/rspa.2016.0475)), the field-emitted current was found to change by approximately 1% at a monatomic surface step (approx. 200 pm thick). Here we prepare surface domains of adjacent different materials that, in some instances, have a topographic contrast smaller than 15 pm. Nevertheless, we observe a contrast in the field-emitted current as high as 10%. This non-topographic collector material dependence is a yet unexplored degree of freedom calling for a new understanding of the quantum mechanical tunnelling barrier at the source site that takes into account the properties of the material at the collector site.

Experimental realization of a π/2 vortex mode converter for electrons using a spherical aberration corrector.

In light optics, beams with orbital angular momentum (OAM) can be produced by employing a properly-tuned two-cylinder-lens arrangement, also called π/2 mode converter. It is not possible to convey this concept directly to the beam in an electron microscope due to the non-existence of cylinder lenses in commercial transmission electron microscopes (TEMs). A viable work-around are readily-available electron optical elements in the form of quadrupole lenses. In a proof-of-principle experiment in 2012, it has been shown that a single quadrupole in combination with a Hilbert phase-plate produces a spatially-confined, transient vortex mode. Here, an analogue to an optical π/2 mode converter is realized by repurposing a CEOS DCOR probe corrector in an aberration corrected TEM in a way that it resembles a dual cylinder lens using two quadrupoles. In order to verify the presence of OAM in the output beam, a fork dislocation grating is used as an OAM analyser. The possibility to use magnetic quadrupole fields instead of, e.g., prefabricated fork dislocation gratings to produce electron beams carrying OAM enhances the beam brightness by almost an order of magnitude and delivers switchable high-mode purity vortex beams without unwanted side-bands.

Off-axis electron holography of Néel-type skyrmions in multilayers of heavy metals and ferromagnets.

Magnetic skyrmions are complex swirling spin structures that are of interest for applications in energy-efficient memories and logic technologies. Multilayers of heavy metals and ferromagnets have been shown to host magnetic skyrmions at room temperature. Lorentz transmission electron microscopy is often used to study magnetic domain structures in multilayer samples using mainly Fresnel defocus imaging. Here, off-axis electron holography is used to obtain in-focus electron optical phase images of Néel-type domains and skyrmions in an Ir/Fe/Co/Pt multilayer sample. The preparation of the sample, reconstruction of the holograms and influence of sample tilt angle on the signal-to-noise ratio in the phase images are discussed. A good agreement is found between images of individual skyrmions that are stabilized using an external magnetic field and simulated images based on theoretical models of Néel-type skyrmions.

STEM electron beam-induced current measurements of organic-inorganic perovskite solar cells.

We describe a new approach for preparing organic-inorganic perovskite solar cells for electron beam-induced current (EBIC) measurements in plan-view geometry. This method substantially reduces sample preparation artefacts, provides good electrical contact and keeps the preparation steps as close as possible to those for real devices. Our EBIC images were acquired simultaneously with annular dark-field scanning transmission electron microscopy images using a home-made highly sensitive EBIC amplifier. High-angle annular dark-field images and energy dispersive X-ray maps were recorded from the same area immediately afterwards. This allowed the EBIC contrast to be correlated with regions containing N and a deficiency of O. The EBIC contrast was also found to be similar to secondary electron contrast recorded with a scanning electron microscope. By identifying the generation and absorption electron processes, we determine that EBIC cannot be separated from the secondary electron and absorbed currents. This means that careful analysis needs to be performed before conclusions can be made on the origin of the current measured across p-n or p-i-n junctions.

Energy-level quantization and single-photon control of phase slips in YBa2Cu3O7-x nanowires.

Significant progress has been made in superconducting quantum circuits. However new quantum devices that have longer decoherence times at higher temperatures are urgently required for quantum technologies. Superconducting nanowires with quantum phase slips are promising candidates for use in novel quantum devices. Here, we demonstrate YBa2Cu3O7-x nanowires with phase-slip dynamics and study their switching-current statistics at temperatures below 20 K. We apply theoretical models developed for Josephson junctions and show that our results provide strong evidence for energy-level quantization in the nanowires. The crossover temperature to the quantum regime of 12-13 K and the lifetime in the excited state exceeding 20 ms at 5.4 K are superior to those in conventional Josephson junctions. We also show how the absorption of a single photon changes the phase-slip and quantum state of a nanowire, which is important for the development of single-photon detectors with high operating temperature and superior temporal resolution.

Effect of annealing on the magnetic states of FEBID-grown cobalt nanopatterns examined by off-axis electron holography.

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. LAY DESCRIPTION: In this paper, electron microscopy is used to deposit magnetic cobalt nanopatterns and characterise the effect of in-situ heating on their chemistry, structure and magnetic properties. The electron beam of the secondary electron microscope is used to dissociate an injected precursor gas near the SiN membrane substrate of in-situ transmission electron microscopy (TEM) chips and locally deposit the elemental Co in circular patterns ∼ 90 nm in diameter. TEM reveals formation of a Co-oxide shell and embedding of carbon from the precursor gas during growth. The technique of electron holography is used to image the magnetism of the core-shell Co / Co-oxide nanopatterns, which are shown to exhibit magnetic vortex states. In-situ annealing results in migration of the Co overspray to increase their height and carbon diffusion from their surface, as well as change in their original magnetic state through change of orientation. It is found that the change in the morphology and chemistry of Co nanopatterns under heating limits their use for studying the effect of temperature on their magnetism in isolation.

Iuliacumite: A Novel Chemical Short-Range Order in a Two-Dimensional Wurtzite Single Monolayer InAs1-xSbx Shell on InAs Nanowires.

A chemical short-range order is found in single monolayer InAs1-xSbx shells, which inherit a wurtzite structure from the underlying InAs nanowire, instead of crystallizing in the energetically preferred zincblende structure. The chemical order is characterized by an anticorrelation ordering vector in the ⟨112̅0⟩ direction and arises from strong Sb-Sb repulsive interactions along the atomic chains in the ⟨112̅0⟩ direction.

Controlling Near-Surface Ni Composition in Octahedral PtNi(Mo) Nanoparticles by Mo Doping for a Highly Active Oxygen Reduction Reaction Catalyst.

We report and study the translation of exceptionally high catalytic oxygen electroreduction activities of molybdenum-doped octahedrally shaped PtNi(Mo) nanoparticles from conventional thin-film rotating disk electrode screenings (3.43 ± 0.35 A mgPt-1 at 0.9 VRHE) to membrane electrode assembly (MEA)-based single fuel cell tests with sustained Pt mass activities of 0.45 A mgPt-1 at 0.9 Vcell, one of the highest ever reported performances for advanced shaped Pt alloys in real devices. Scanning transmission electron microscopy with energy dispersive X-ray analysis (STEM-EDX) reveals that Mo preferentially occupies the Pt-rich edges and vertices of the element-anisotropic octahedral PtNi particles. Furthermore, by combining in situ wide-angle X-ray spectroscopy, X-ray fluorescence, and STEM-EDX elemental mapping with electrochemical measurements, we finally succeeded to realize high Ni retention in activated PtNiMo nanoparticles even after prolonged potential-cycling stability tests. Stability losses at the anodic potential limits were mainly attributed to the loss of the octahedral particle shape. Extending the anodic potential limits of the tests to the Pt oxidation region induced detectable Ni losses and structural changes. Our study shows on an atomic level how Mo adatoms on the surface impact the Ni surface composition, which, in turn, gives rise to the exceptionally high experimental catalytic ORR reactivity and calls for strategies on how to preserve this particular surface composition to arrive at performance stabilities comparable with state-of-the-art spherical dealloyed Pt core-shell catalysts.

Structural characterization of bulk and nanoparticle lead halide perovskite thin films by (S)TEM techniques.

Lead halide (APbX3) perovskites, in polycrystalline thin films but also perovskite nanoparticles (NPs) has demonstrated excellent performance to implement a new generation of photovoltaic and photonic devices. The structural characterization of APbX3 thin films using (scanning) transmission electron microscopy ((S)TEM) techniques can provide valuable information that can be used to understand and model their optoelectronic performance and device properties. However, since APbX3 perovskites are soft materials, their characterization using (S)TEM is challenging. Here, we study and compare the structural properties of two different metal halide APbX3 perovskite thin films: bulk CH3NH3PbI3 prepared by spin-coating of the precursors in solution and CsPbBr3 colloidal NPs synthetized and deposited by doctor blading. Both specimen preparation methods and working conditions for analysis by (S)TEM are properly optimized. We show that CH3NH3PbI3 thin films grown by a one-step method are composed of independent grains with random orientations. The growth method results in the formation of tetragonal perovskite thin films with good adherence to an underlying TiO2 layer, which is characterized by a photoluminescence (PL) emission band centered at 775 nm. The perovskite thin films based on CsPbBr3 colloidal NPs, which are used as the building blocks of the film, are preserved by the deposition process, even if small gaps are observed between adjacent NPs. The crystal structure of CsPbBr3 NPs is cubic, which is beneficial for optical properties due to its optimal band gap. The absorption and PL spectra measured in both the thin film and the colloidal solution of CsPbBr3 NPs are very similar, indicating a good homogeneity of the thin films and the absence of aggregation of NPs. However, a particular care was required to avoid long electron irradiation times during our structural studies, even at a low voltage of 80 kV, as the material was observed to decompose through Pb segregation.

Composition modulation by twinning in InAsSb nanowires.

We observe a composition modulated axial heterostructure in zincblende (ZB) InAs0.90Sb0.10 nanowires initiated by pseudo-periodic twin boundaries using scanning tunneling microscopy. The twin boundaries exhibit four planes with reduced Sb concentration due to a lower Sb incorporation during lateral overgrowth of a 4H wurtzite as compared to a ZB stacking sequence. We anticipate that this leads to compositional band offsets in addition to known structural band offsets present between 4H and ZB polytypes, changing the band alignment from type II to type I.

Resistive switching in optoelectronic III-V materials based on deep traps.

Resistive switching random access memories (ReRAM) are promising candidates for energy efficient, fast, and non-volatile universal memories that unite the advantages of RAM and hard drives. Unfortunately, the current ReRAM materials are incompatible with optical interconnects and wires. Optical signal transmission is, however, inevitable for next generation memories in order to overcome the capacity-bandwidth trade-off. Thus, we present here a proof-of-concept of a new type of resistive switching realized in III-V semiconductors, which meet all requirements for the implementation of optoelectronic circuits. This resistive switching effect is based on controlling the spatial positions of vacancy-induced deep traps by stimulated migration, opening and closing a conduction channel through a semi-insulating compensated surface layer. The mechanism is widely applicable to opto-electronically usable III-V compound semiconductors.

Superconducting Quantum Interferometers for Nondestructive Evaluation.

We review stationary and mobile systems that are used for the nondestructive evaluation of room temperature objects and are based on superconducting quantum interference devices (SQUIDs). The systems are optimized for samples whose dimensions are between 10 micrometers and several meters. Stray magnetic fields from small samples (10 µm-10 cm) are studied using a SQUID microscope equipped with a magnetic flux antenna, which is fed through the walls of liquid nitrogen cryostat and a hole in the SQUID's pick-up loop and returned sidewards from the SQUID back to the sample. The SQUID microscope does not disturb the magnetization of the sample during image recording due to the decoupling of the magnetic flux antenna from the modulation and feedback coil. For larger samples, we use a hand-held mobile liquid nitrogen minicryostat with a first order planar gradiometric SQUID sensor. Low-Tc DC SQUID systems that are designed for NDE measurements of bio-objects are able to operate with sufficient resolution in a magnetically unshielded environment. High-Tc DC SQUID magnetometers that are operated in a magnetic shield demonstrate a magnetic field resolution of ~4 fT/√Hz at 77 K. This sensitivity is improved to ~2 fT/√Hz at 77 K by using a soft magnetic flux antenna.

Atomic resolution elemental mapping using energy-filtered imaging scanning transmission electron microscopy with chromatic aberration correction.

This paper addresses a novel approach to atomic resolution elemental mapping, demonstrating a method that produces elemental maps with a similar resolution to the established method of electron energy-loss spectroscopy in scanning transmission electron microscopy. Dubbed energy-filtered imaging scanning transmission electron microscopy (EFISTEM) this mode of imaging is, by the quantum mechanical principle of reciprocity, equivalent to tilting the probe in energy-filtered transmission electron microscopy (EFTEM) through a cone and incoherently averaging the results. In this paper we present a proof-of-principle EFISTEM experimental study on strontium titanate. The present approach, made possible by chromatic aberration correction, has the advantage that it provides elemental maps which are immune to spatial incoherence in the electron source, coherent aberrations in the probe-forming lens and probe jitter. The veracity of the experiment is supported by quantum mechanical image simulations, which provide an insight into the image-forming process. Elemental maps obtained in EFTEM suffer from the effect known as preservation of elastic contrast, which, for example, can lead to a given atomic species appearing to be in atomic columns where it is not to be found. EFISTEM very substantially reduces the preservation of elastic contrast and yields images which show stability of contrast with changing thickness. The experimental application is demonstrated in a proof-of-principle study on strontium titanate.

Interface-driven formation of a two-dimensional dodecagonal fullerene quasicrystal.

Since their discovery, quasicrystals have attracted continuous research interest due to their unique structural and physical properties. Recently, it was demonstrated that dodecagonal quasicrystals could be used as bandgap materials in next-generation photonic devices. However, a full understanding of the formation mechanism of quasicrystals is necessary to control their physical properties. Here we report the formation of a two-dimensional dodecagonal fullerene quasicrystal on a Pt3Ti(111) surface, which can be described in terms of a square-triangle tiling. Employing density functional theory calculations, we identify the complex adsorption energy landscape of the Pt-terminated Pt3Ti surface that is responsible for the quasicrystal formation. We demonstrate the presence of quasicrystal-specific phason strain, which provides the degree of freedom required to accommodate the quasicrystalline structure on the periodic substrate. Our results reveal detailed insight into an interface-driven formation mechanism and open the way to the creation of tailored fullerene quasicrystals with specific physical properties.

Temperature and Magnetic Field Dependence of the Internal and Lattice Structures of Skyrmions by Off-Axis Electron Holography.

The internal and lattice structures of magnetic Skyrmions in B20-type FeGe are investigated using off-axis electron holography. The temperature, magnetic field, and angular dependence of the magnetic moments of individual Skyrmions are analyzed. The internal Skyrmion shape is found to vary with applied magnetic field. In contrast, the inter-Skyrmion distance remains almost unchanged in the lattice phase over the studied range of applied field. The amplitude of the local magnetic moment is found to vary with temperature, while the Skyrmion shape does not change significantly. Deviations from a circular to a hexagonal Skyrmion structure are observed in the lattice phase, in agreement with the results of micromagnetic simulations.