arXiv subjects

Axel Lubk

Publications and source records attributed to Axel Lubk.

At least 37 records · Page 2Linked to original sources

arXiv2020

Autocorrected Off-axis Holography of 2D Materials

The reduced dimensionality in two-dimensional materials leads a wealth of unusual properties, which are currently explored for both fundamental and applied sciences. In order to study the crystal structure, edge states, the formation of defects and grain boundaries, or the impact of adsorbates, high resolution microscopy techniques are indispensible. Here we report on the development of an electron holography (EH) transmission electron microscopy (TEM) technique, which facilitates high spatial resolution by an automatic correction of geometric aberrations. Distinguished features of EH beyond conventional TEM imaging are the gap-free spatial information signal transfer and higher dose efficiency for certain spatial frequency bands as well as direct access to the projected electrostatic potential of the 2D material. We demonstrate these features at the example of h-BN, at which we measure the electrostatic potential as a function of layer number down to the monolayer limit and obtain evidence for a systematic increase of the potential at the zig-zag edges.

cond-mat.mes-hall↗

arXiv2020

Investigation of potassium-intercalated bulk MoS$_2$ using transmission electron energy-loss spectroscopy

We have investigated the effect of potassium (K) intercalation on $2H$-MoS$_2$ using transmission electron energy-loss spectroscopy. For K concentrations up to approximately 0.4, the crystals appear to be inhomogeneous with a mix of structural phases and irregular potassium distribution. Above this intercalation level, MoS$_2$ exhibits a $2a \times 2a$ superstructure in the $ab$ plane and unit cell parameters of a = 3.20 $\unicode{x212B}$ and c = 8.23 $\unicode{x212B}$ indicating a conversion from the $2H$ to the $1T'$ or $1T''$ polytypes. The diffraction patterns also show a $\sqrt{3}a \times \sqrt{3}a$ and a much weaker $2\sqrt{3}a \times 2\sqrt{3}a$ superstructure that is very likely associated with the ordering of the potassium ions. A semiconductor-to-metal transition occurs signified by the disappearance of the excitonic features from the electron energy-loss spectra and the emergence of a charge carrier plasmon with an unscreened plasmon frequency of 2.78 eV. The plasmon has a positive, quadratic dispersion and appears to be superimposed with an excitation arising from interband transitions. The behavior of the plasmon peak energy positions as a function of potassium concentration shows that potassium stoichiometries of less than $\sim 0.3$ are thermodynamically unstable while higher stoichiometries up to $\sim 0.5$ are thermodynamically stable. Potassium concentrations greater than $\sim 0.5$ lead to the decomposition of MoS$_2$ and the formation of K$_2$S. The real part of the dielectric function and the optical conductivity of K$_{0.41}$MoS$_2$ were derived from the loss spectra via Kramers-Kronig analysis.

cond-mat.mes-hall↗

arXiv2019

Magnetic Nanoparticle Chains in Gelatin Ferrogels: Bioinspiration from Magnetotactic Bacteria

Inspired by chains of ferrimagnetic nanocrystals (NCs) in magnetotactic bacteria (MTB), the synthesis and detailed characterization of ferrimagnetic magnetite NC chain-like assemblies is reported. An easy green synthesis route in a thermoreversible gelatin hydrogel matrix is used. The structure of these magnetite chains prepared with and without gelatin is characterized by means of transmission electron microscopy, including electron tomography (ET). These structures indeed bear resemblance to the magnetite assemblies found in MTB, known for their mechanical flexibility and outstanding magnetic properties and known to crystallographically align their magnetite NCs along the strongest <111> magnetization easy axis. Using electron holography (EH) and angular dependent magnetic measurements, the magnetic interaction between the NCs and the generation of a magnetically anisotropic material can be shown. The electro- and magnetostatic modeling demonstrates that in order to precisely determine the magnetization (by means of EH) inside chain-like NCs assemblies, their exact shape, arrangement and stray-fields have to be considered (ideally obtained using ET).

cond-mat.mtrl-sci↗

arXiv2019

Direct Observation of Plasmon Band Formation and Delocalization in Quasi-Infinite Nanoparticle Chains

Chains of metallic nanoparticles sustain strongly confined surface plasmons with relatively low dielectric losses. To exploit these properties in applications,such as waveguides, the fabrication of long chains of low disorder and a thorough understanding of the plasmon-mode properties, such as dispersion relations, are indispensable. Here, we use a wrinkled template for directed self-assembly to assemble chains of gold nanoparticles. With this up-scalable method, chain lengths from two particles (140 nm) to 20 particles (1500 nm) and beyond can be fabricated. Electron energy-loss spectroscopy supported by boundary element simulations, finite-difference time-domain, and a simplified dipole coupling model reveal the evolution of a band of plasmonic waveguide modes from degenerated single-particle modes in detail. In striking difference from plasmonic rod-like structures, the plasmon band is confined in excitation energy, which allows light manipulations below the diffraction limit. The non-degenerated surface plasmon modes show suppressed radiative losses for efficient energy propagation over a distance of 1500 nm.

cond-mat.mes-hall↗

arXiv2019

Three-dimensional imaging of beam-induced biasing of InP/GaInP tunnel diodes

Electron Holographic Tomography was used to obtain 3-dimensional reconstructions of the morphology and electrostatic potential gradient of axial GaInP/InP nanowire tunnel diodes. Crystal growth was carried out in two opposite directions: GaInP:Zn/InP:S and InP:Sn/GaInP:Zn, using Zn as the p-type dopant in the GaInP, but with changes to the n-type dopant (S or Sn) in the InP. Secondary electron and electron beam induced current images obtained using scanning electron microscopy indicated the presence of p-n junctions in both cases and current-voltage characteristics measured via lithographic contacts showed the negative differential resistance, characteristic of band-to-band tunneling, for both diodes. EHT measurements confirmed a short depletion width in both cases ($21 \pm 3$ nm), but different built-in potentials, $V_{bi}$, of 1.0 V for the p-type (Zn) to n-type (S) transition, and 0.4 V for both were lower than the expected 1.5 V for these junctions, if degenerately-doped. Charging induced by the electron beam was evident in phase images which showed non-linearity in the surrounding vacuum, most severe in the case of the nanowire grounded at the \emph{p}-type Au contact. We attribute their lower $V_{bi}$ to asymmetric secondary electron emission, beam-induced current biasing and poor grounding contacts.

physics.app-ph↗

arXiv2019

Optimal principal component Analysis of STEM XEDS spectrum images

STEM XEDS spectrum images can be drastically denoised by application of the principal component analysis (PCA). This paper looks inside the PCA workflow step by step on an example of a complex semiconductor structure consisting of a number of different phases. Typical problems distorting the principal components decomposition are highlighted and solutions for the successful PCA are described. Particular attention is paid to the optimal truncation of principal components in the course of reconstructing denoised data. A novel accurate and robust method, which overperforms the existing truncation methods is suggested for the first time and described in details.

eess.IV↗

arXiv2019

Holographic Vector Field Electron Tomography of Three-Dimensional Nanomagnets

Complex 3D magnetic textures in nanomagnets exhibit rich physical properties, for example in their dynamic interaction with external fields and currents, and play an increasing role for current technological challenges such as energy-efficient memory devices. To study these magnetic nanostructures including their dependency on geometry, composition and crystallinity, a 3D characterization of the magnetic field with nanometer spatial resolution is indispensable. Here we show how holographic vector field electron tomography can reconstruct all three components of magnetic induction as well as the electrostatic potential of a Co/Cu nanowire with sub 10\,nm spatial resolution. We address the workflow from acquisition, via image alignment to holographic and tomographic reconstruction. Combining the obtained tomographic data with micromagnetic considerations we derive local key magnetic characteristics, such as magnetization current or exchange stiffness, and demonstrate how magnetization configurations, such as vortex states in the Co-disks, depend on small structural variations of the as-grown nanowire.

cond-mat.mes-hall↗

arXiv2019

The Dresden in-situ (S)TEM special with a continuous-flow liquid-helium cryostat

Fundamental solid state physics phenomena typically occur at very low temperatures, requiring liquid helium cooling in experimental studies. Transmission electron microscopy is a well-established characterization method, which allows probing crucial materials properties down to nanometer and even atomic resolution. Due to the limited space in the object plane, however, suitable liquid-helium cooling is very challenging. To overcome this limitation, resolving power was sacrificed in our Dresden in-situ (S)TEM special, resulting in more than 60 mm usable experimental space in all directions with the specimen in the center. With the installation of a continuous-flow liquid-helium cryostat, any temperature between 6.5 K and 400 K can be set precisely and kept for days. The information limit of the Dresden in-situ (S)TEM special is about 5 nm. It is shown that the resolution of the Dresden in-situ (S)TEM special is currently not limited by aberrations, but by external instabilities, that are currently addressed.

physics.ins-det↗

arXiv2019

Quantum-mechanical treatment of atomic resolution differential phase contrast imaging of magnetic materials

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.

cond-mat.mtrl-sci↗

arXiv2018

Chemical Aspects of the Antiferromagnetic Topological Insulator MnBi$_{2}$Te$_{4}$

Crystal growth of MnBi$_{2}$Te$_{4}$ has delivered the first experimental corroboration of the 3D antiferromagnetic topological insulator state. Our present results confirm that the synthesis of MnBi$_{2}$Te$_{4}$ can be scaled-up and strengthen it as a promising experimental platform for studies of a crossover between magnetic ordering and non-trivial topology. High-quality single crystals of MnBi$_{2}$Te$_{4}$ are grown by slow cooling within a narrow range between the melting points of Bi$_{2}$Te$_{3}$ (586 °C) and MnBi$_{2}$Te$_{4}$ (600 °C). Single crystal X-ray diffraction and electron microscopy reveal ubiquitous antisite defects in both cation sites and, possibly, Mn vacancies. Powders of MnBi$_{2}$Te$_{4}$ can be obtained at subsolidus temperatures, and a complementary thermochemical study establishes a limited high-temperature range of phase stability. Nevertheless, quenched powders are stable at room temperature and exhibit long-range antiferromagnetic ordering below 24 K. The expected Mn(II) out-of-plane magnetic state is confirmed by the magnetization, X-ray photoemission, X-ray absorption and linear dichroism data. MnBi$_{2}$Te$_{4}$ exhibits a metallic type of resistivity in the range 4.5-300 K. The compound is an n-type conductor that reaches a thermoelectric figure of merit up to ZT = 0.17. Angle-resolved photoemission experiments provide evidence for a surface state forming a gapped Dirac cone.

cond-mat.mtrl-sci↗

arXiv2018

Fully nonlocal inelastic scattering computations for spectroscopical transmission electron microscopy methods

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.

cond-mat.mes-hall↗

arXiv2018

Three-dimensional composition and electric potential mapping of III-V core-multishell nanowires by correlative STEM and holographic tomography

The non-destructive characterization of nanoscale devices, such as those based on semiconductor nanowires, in terms of functional potentials is crucial for correlating device properties with their morphological/materials features, as well as for precisely tuning and optimizing their growth process. Electron holographic tomography (EHT) has been used in the past to reconstruct the total potential distribution in 3D but hitherto lacked a quantitative approach to separate potential variations due to chemical composition changes (mean inner potential - MIP) and space charges. In this letter, we combine and correlate EHT and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) tomography on an individual <111> oriented GaAs-AlGaAs core-multishell nanowire (NW). We obtain excellent agreement between both methods in terms of the determined Al concentration within the AlGaAs shell, as well as thickness variations of the few nanometer thin GaAs shell acting as quantum well tube. Subtracting the MIP determined from the STEM tomogram, enables us to observe functional potentials at the NW surfaces and at the Au-NW interface, both ascribed to surface/interface pinning of the semiconductor Fermi level.

cond-mat.mes-hall↗

arXiv2018

$\mathrm{Fe}_{1-x}\mathrm{Ni}_x$ Alloy Nanoparticles Encapsulated inside Carbon Nanotubes: Controlled Synthesis, Structure and Magnetic Properties

In the present work, different synthesis procedures have been demonstrated to fill carbon nanotubes (CNTs) with $\mathrm{Fe}_{1-x}\mathrm{Ni}_x$ alloy nanoparticles (x = 0.33, 0.5). CNTs act as templates for the encapsulation of magnetic nanoparticles, and provide a protective shield against oxidation as well as prevent nanoparticles agglomeration. By variation of the reaction parameters, the purity of the samples, degree of filling, the composition and size of filling nanoparticles have been tailored and therefore the magnetic properties. The samples were analyzed by scanning electron microscopy (SEM), transmission electron microscopy (TEM), Bright-field (BF) TEM tomography, X-ray powder diffraction, superconducting quantum interference device (SQUID) and thermogravimetric analysis (TGA). The Fe1-xNix-filled CNTs show a huge enhancement in the coercive fields compared to the corresponding bulk materials, which make them excellent candidates for several applications such as magnetic storage devices.

cond-mat.mtrl-sci↗

arXiv2018

Induction Mapping of the 3D-Modulated Spin Texture of Skyrmions in Thin Helimagnets

Envisaged applications of skyrmions in magnetic memory and logic devices crucially depend on the stability and mobility of these topologically non-trivial magnetic textures in thin films. We present for the first time quantitative maps of the magnetic induction that provide evidence for a 3D modulation of the skyrmionic spin texture. The projected in-plane magnetic induction maps as determined from in-line and off-axis electron holography carry the clear signature of Bloch skyrmions. However, the magnitude of this induction is much smaller than the values expected for homogeneous Bloch skyrmions that extend throughout the thickness of the film. This finding can only be understood, if the underlying spin textures are modulated along the out-of-plane z direction. The projection of (the in-plane magnetic induction of) helices is further found to exhibit thickness-dependent lateral shifts, which show that this z modulation is accompanied by an (in-plane) modulation along the x and y directions.

cond-mat.mtrl-sci↗

arXiv2017

The Rytov Approximation in Electron Scattering

In this work we introduce the Rytov approximation in the scope of high-energy electron scattering with the motivation of developing better linear models for electron scattering. Such linear models play an important role in tomography and similar reconstruction techniques. Conventional linear models, such as the Phase Grating Approximation, have reached their limits in current and forsee- able applications, most importantly in achieving three-dimensional atomic resolution using electron holographic tomography. The Rytov approximation incorporates propagation effects which are the most pressing limitation of conventional models. While predominately used in the weak-scattering regime of light microscopy we show that the Rytov approximation can give reasonable results in the inherently strong-scattering regime of transmission electron microscopy.

physics.class-ph↗

arXiv2016

Transport of Intensity Phase Retrieval of Arbitrary Wave Fields Including Vortices

The phase problem can be considered as one of the cornerstones of quantum mechanics intimately connected to the detection process and the uncertainty relation. The latter impose fundamental limits on the manifold phase reconstruction schemes invented to date in particular at small magnitudes of the quantum wave. Here, we show that a rigorous solution of the Transport of Intensity Reconstruction (TIE) scheme in terms of a linear elliptic partial differential equation for the phase provides reconstructions even in the presence of wave zeros if particular boundary conditions (BCs) are given. We furthermore discuss how partial coherence hampers phase reconstruction and show that a modified version of the TIE reconstructs the curl-free current density at arbitrary (in-)coherence. This opens the way for a large variety of new applications in fields as diverse as astrophysics, geophysics, photonics, acoustics, and electron microscopy, where zeros in the respective wave field are a ubiquitous feature.

physics.optics↗

arXiv2016

Investigation into spiral phase plate contrast in optical and electron microscopy

The use of phase plates in the back focal plane of a microscope is a well established technique in optical microscopy to increase the contrast of weakly interacting samples and is gaining interest in electron microscopy as well. In this paper we study the spiral phase plate (SPP), also called helical, vortex, or two-dimensional Hilbert phase plate, that adds an angularly dependent phase of the form $e^{i\ellϕ}$ to the exit wave in Fourier space. In the limit of large collection angles, we analytically calculate that the average of a pair of $\ell=\pm1$ SPP images is directly proportional to the gradient squared of the exit wave, explaining the edge contrast previously seen in optical SPP work. The difference between a clockwise-anticlockwise pair of SPP images and conditions where this difference vanishes and the gradient of the exit wave can be seen from one single SPP image, are discussed. Finally, we demonstrate how with three images, one without and one with each of an $\ell=\pm1$ SPP, may give enough information to reconstruct both the amplitude and the phase of the exit wave. This work provides the theoretical background to interpret images obtained with a SPP and can help enable new experiments to study for example magnetic materials in an electron microscope.

physics.optics↗

arXiv2016

Magnetic Effects in the Paraxial Regime of Elastic Electron Scattering

Based on a recent claim [Phys. Rev. Lett. 116, 127203 (2016)] that electron vortex can be used to image magnetism at the nanoscale in elastic scattering experiments, using transmission electron microscopy, a comprehensive computational study is performed to study magnetic effects in the paraxial regime of elastic electron scattering in magnetic solids. Magnetic interactions from electron vortex beams, spin polarized electron beams and beams with phase aberrations are considered, as they pass through ferromagnetic FePt or antiferromagnetic LaMnAsO. The magnetic signals are obtained by comparing the intensity over a disk in the diffraction plane for beams with opposite angular momentum or aberrations. The strongest magnetic signals are obtained from vortex beams with large orbital angular momentum, where relative magnetic signals above $10^{-3}$ are indicated for $10\hbar$ orbital angular momentum, meaning that relative signals of one percent could be expected with the even larger orbital angular momenta, which have been produced in experimental setups. All results indicate that beams with low acceleration voltage and small convergence angles yield stronger magnetic signals, which is unfortunately problematic for the possibility of high spatial resolution imaging. Nevertheless, under atomic resolution conditions, relative magnetic signals in the order of $10^{-4}$ are demonstrated, corresponding to an increase with one order of magnitude compared to previous work.

cond-mat.mtrl-sci↗