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- ItemCrystallization of Ge2Sb2Te5 thin films by nano- and femtosecond single laser pulse irradiation(London : Nature Publishing Group, 2016) Sun, Xinxing; Ehrhardt, Martin; Lotnyk, Andriy; Lorenz, Pierre; Thelander, Erik; Gerlach, Jürgen W.; Smausz, Tomi; Decker, Ulrich; Rauschenbach, BerndThe amorphous to crystalline phase transformation of Ge2Sb2Te5 (GST) films by UV nanosecond (ns) and femtosecond (fs) single laser pulse irradiation at the same wavelength is compared. Detailed structural information about the phase transformation is collected by x-ray diffraction and high resolution transmission electron microscopy (TEM). The threshold fluences to induce crystallization are determined for both pulse lengths. A large difference between ns and fs pulse irradiation was found regarding the grain size distribution and morphology of the crystallized films. For fs single pulse irradiated GST thin films, columnar grains with a diameter of 20 to 60 nm were obtained as evidenced by cross-sectional TEM analysis. The local atomic arrangement was investigated by highresolution Cs-corrected scanning TEM. Neither tetrahedral nor off-octahedral positions of Ge-atoms could be observed in the largely defect-free grains. A high optical reflectivity contrast (~25%) between amorphous and completely crystallized GST films was achieved by fs laser irradiation induced at fluences between 13 and 16 mJ/cm2 and by ns laser irradiation induced at fluences between 67 and 130 mJ/cm2. Finally, the fluence dependent increase of the reflectivity is discussed in terms of each photon involved into the crystallization process for ns and fs pulses, respectively.
- ItemRole of Reaction Intermediate Diffusion on the Performance of Platinum Electrodes in Solid Acid Fuel Cells(Basel : MDPI, 2021) Lorenz, Oliver; Kühne, Alexander; Rudolph, Martin; Diyatmika, Wahyu; Prager, Andrea; Gerlach, Jürgen W.; Griebel, Jan; Winkler, Sara; Lotnyk, Andriy; Anders, André; Abel, BerndUnderstanding the reaction pathways for the hydrogen oxidation reaction (HOR) and the oxygen reduction reaction (ORR) is the key to design electrodes for solid acid fuel cells (SAFCs). In general, electrochemical reactions of a fuel cell are considered to occur at the triple-phase boundary where an electrocatalyst, electrolyte and gas phase are in contact. In this concept, diffusion processes of reaction intermediates from the catalyst to the electrolyte remain unconsidered. Here, we unravel the reaction pathways for open-structured Pt electrodes with various electrode thicknesses from 15 to 240 nm. These electrodes are characterized by a triple-phase boundary length and a thickness-depending double-phase boundary area. We reveal that the double-phase boundary is the active catalytic interface for the HOR. For Pt layers ≤ 60 nm, the HOR rate is rate-limited by the processes at the gas/catalyst and/or the catalyst/electrolyte interface while the hydrogen surface diffusion step is fast. For thicker layers (>60 nm), the diffusion of reaction intermediates on the surface of Pt be-comes the limiting process. For the ORR, the predominant reaction pathway is via the triple-phase boundary. The double-phase boundary contributes additionally with a diffusion length of a few nanometers. Based on our results, we propose that the molecular reaction mechanism at the electrode interfaces based upon the triple-phase boundary concept may need to be extended to an effective area near the triple-phase boundary length to include all catalytically relevant diffusion processes of the reaction intermediates. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemLocal atomic arrangements and lattice distortions in layered Ge-Sb-Te crystal structures(London : Nature Publishing Group, 2016) Lotnyk, Andriy; Ross, Ulrich; Bernütz, Sabine; Thelander, Erik; Rauschenbach, BerndInsights into the local atomic arrangements of layered Ge-Sb-Te compounds are of particular importance from a fundamental point of view and for data storage applications. In this view, a detailed knowledge of the atomic structure in such alloys is central to understanding the functional properties both in the more commonly utilized amorphous–crystalline transition and in recently proposed interfacial phase change memory based on the transition between two crystalline structures. Aberration-corrected scanning transmission electron microscopy allows direct imaging of local arrangement in the crystalline lattice with atomic resolution. However, due to the non-trivial influence of thermal diffuse scattering on the high-angle scattering signal, a detailed examination of the image contrast requires comparison with theoretical image simulations. This work reveals the local atomic structure of trigonal Ge-Sb-Te thin films by using a combination of direct imaging of the atomic columns and theoretical image simulation approaches. The results show that the thin films are prone to the formation of stacking disorder with individual building blocks of the Ge2Sb2Te5, Ge1Sb2Te4 and Ge3Sb2Te6 crystal structures intercalated within randomly oriented grains. The comparison with image simulations based on various theoretical models reveals intermixed cation layers with pronounced local lattice distortions, exceeding those reported in literature.
- ItemStructural Transitions in Ge2Sb2Te5 Phase Change Memory Thin Films Induced by Nanosecond UV Optical Pulses(Basel : MDPI, 2020) Behrens, Mario; Lotnyk, Andriy; Bryja, Hagen; Gerlach, Jürgen W.; Rauschenbach, BerndGe-Sb-Te-based phase change memory alloys have recently attracted a lot of attention due to their promising applications in the fields of photonics, non-volatile data storage, and neuromorphic computing. Of particular interest is the understanding of the structural changes and underlying mechanisms induced by short optical pulses. This work reports on structural changes induced by single nanosecond UV laser pulses in amorphous and epitaxial Ge2Sb2Te5 (GST) thin films. The phase changes within the thin films are studied by a combined approach using X-ray diffraction and transmission electron microscopy. The results reveal different phase transitions such as crystalline-to-amorphous phase changes, interface assisted crystallization of the cubic GST phase and structural transformations within crystalline phases. In particular, it is found that crystalline interfaces serve as crystallization templates for epitaxial formation of metastable cubic GST phase upon phase transitions. By varying the laser fluence, GST thin films consisting of multiple phases and different amorphous to crystalline volume ratios can be achieved in this approach, offering a possibility of multilevel data storage and realization of memory devices with very low resistance drift. In addition, this work demonstrates amorphization and crystallization of GST thin films by using only one UV laser with one single pulse duration and one wavelength. Overall, the presented results offer new perspectives on switching pathways in Ge-Sb-Te-based materials and show the potential of epitaxial Ge-Sb-Te thin films for applications in advanced phase change memory concepts.
- ItemPhase and grain size engineering in Ge-Sb-Te-O by alloying with La-Sr-Mn-O towards improved material properties(Oxford : Elsevier Science, 2020) Kraft, Nikolas; Wang, Guoxiang; Bryja, Hagen; Prager, Andrea; Griebel, Jan; Lotnyk, AndriyGe-Sb-Te alloys are promising materials for non-volatile memory applications. Alloying of the materials with various elements is considered as prospective approach to enhance material properties. This work reports on the preparation and characterization of pure Ge-Sb-Te-O (GSTO) and alloyed with La-Sr-Mn-O (LSMO) thin films. Thermal heating of amorphous thin films to different temperatures show distinct crystallization behavior. A general trend is the decrease in the size of GSTO crystallites and the suppression in the formation of stable trigonal GSTO phase with increasing content of LSMO. Microstructural studies by transmission electron microscopy show the formation of metastable GSTO nanocrystallites dispersed in the amorphous matrix. Analysis of local chemical bonding by X-ray spectroscopy reveal the presence of different oxides in the GSTO-LSMO composites. Moreover, the composites with a high LSMO content exhibit higher crystallization temperature and significant larger sheet resistance in amorphous and crystalline phase, while a memory device made of GSTO-LSMO alloy reveals bipolar switching and synaptic behavior. In addition, the amount of LSMO in GSTO-LSMO thin films influences their optical properties and band gap. Overall, the results of this work reveal the highly promising potential of GSTO-LSMO nanocomposites for data storage and reconfigurable photonic applications as well as neuro-inspired computing.
- ItemInfluence of substrate dimensionality on the growth mode of epitaxial 3D-bonded GeTe thin films: From 3D to 2D growth(Amsterdam [u.a.] : Elsevier Science, 2019) Hilmi, Isom; Lotnyk, Andriy; Gerlach, Jürgen W.; Schumacher, Philipp; Rauschenbach, BerndThe pseudo-binary line of Sb2Te3-GeTe contains alloys featuring different crystalline characteristics from two-dimensionally (2D-) bonded Sb2Te3 to three-dimensionally (3D-) bonded GeTe. Here, the growth scenario of 3D-bonded GeTe is investigated by depositing epitaxial GeTe thin films on Si(111) and Sb2Te3-buffered Si(111) substrates using pulsed laser deposition (PLD). GeTe thin films were grown in trigonal structure within a temperature window for epitaxial growth of 210–270 °C on unbuffered Si(111) substrates. An unconventional growth onset was characterized by the formation of a thin amorphous GeTe layer. Nonetheless, the as-grown film is found to be crystalline. Furthermore, by employing a 2D-bonded Sb2Te3 thin film as a seeding layer on Si(111), a 2D growth of GeTe is harnessed. The epitaxial window can substantially be extended especially towards lower temperatures down to 145 °C. Additionally, the surface quality is significantly improved. The inspection of the local structure of the epitaxial films reveals the presence of a superposition of twinned domains, which is assumed to be an intrinsic feature of such thin films. This work might open a way for an improvement of an epitaxy of a 3D-bonded material on a highly-mismatched substrate (e.g. Si (111)) by employing a 2D-bonded seeding layer (e.g. Sb2Te3).
- ItemIon Beam Assisted Deposition of Thin Epitaxial GaN Films(Basel : MDPI, 2017-6-23) Rauschenbach, Bernd; Lotnyk, Andriy; Neumann, Lena; Poppitz, David; Gerlach, Jürgen W.The assistance of thin film deposition with low-energy ion bombardment influences their final properties significantly. Especially, the application of so-called hyperthermal ions (energy <100 eV) is capable to modify the characteristics of the growing film without generating a large number of irradiation induced defects. The nitrogen ion beam assisted molecular beam epitaxy (ion energy <25 eV) is used to deposit GaN thin films on (0001)-oriented 6H-SiC substrates at 700 °C. The films are studied in situ by reflection high energy electron diffraction, ex situ by X-ray diffraction, scanning tunnelling microscopy, and high-resolution transmission electron microscopy. It is demonstrated that the film growth mode can be controlled by varying the ion to atom ratio, where 2D films are characterized by a smooth topography, a high crystalline quality, low biaxial stress, and low defect density. Typical structural defects in the GaN thin films were identified as basal plane stacking faults, low-angle grain boundaries forming between w-GaN and z-GaN and twin boundaries. The misfit strain between the GaN thin films and substrates is relieved by the generation of edge dislocations in the first and second monolayers of GaN thin films and of misfit interfacial dislocations. It can be demonstrated that the low-energy nitrogen ion assisted molecular beam epitaxy is a technique to produce thin GaN films of high crystalline quality.
- ItemBiaxially Textured Titanium Thin Films by Oblique Angle Deposition: Conditions and Growth Mechanisms(Weinheim : Wiley-VCH, 2020) Liedtke-Grüner, Susann; Grüner, Christoph; Lotnyk, Andriy; Gerlach, Juergen W.; Rauschenbach, BerndGrowing highly crystalline nanowires over large substrate areas remains an ambiguous task nowadays. Herein, a time-efficient and easy-to-handle bottom-up approach is demonstrated that enables the self-assembled growth of biaxially textured Ti thin films composed of single-crystalline nanowires in a single-deposition step. Ti thin films are deposited under highly oblique incidence angles by electron beam evaporation on amorphous substrates. Substrate temperature, angle of the incoming particle flux, and working pressure are varied to optimize the crystallinity in those films. Height-resolved structure information of individual nanowires is provided by a transmission electron microscopy (TEM) nanobeam, high-resolution TEM, and electron diffraction. Ti nanowires are polycrystalline at 77 K, whereas for ≥300 K, single-crystalline nanowires are tendentially found. The Ti crystals grow along the thermodynamically favored c-direction, but the nanowires’ tilt angle is determined by shadowing. Biaxially textured Ti thin films require a certain temperature range combined with highly oblique deposition angles, which is proved by X-ray in-plane pole figures. A general correlation between average activation energy for surface self-diffusion and melting point of metals is given to estimate the significant influence of surface self-diffusion on the evolution of obliquely deposited metal thin films.
- ItemResearch Update: Van-der-Waals epitaxy of layered chalcogenide Sb2Te3 thin films grown by pulsed laser deposition(Melville, NY : AIP Publ., 2017) Hilmi, Isom; Lotnyk, Andriy; Gerlach, Jürgen W.; Schumacher, Philipp; Rauschenbach, BerndAn attempt to deposit a high quality epitaxial thin film of a two-dimensionally bonded (layered) chalcogenide material with van-der-Waals (vdW) epitaxy is of strong interest for non-volatile memory application. In this paper, the epitaxial growth of an exemplary layered chalcogenide material, i.e., stoichiometric Sb2Te3 thin films, is reported. The films were produced on unreconstructed highly lattice-mismatched Si(111) substrates by pulsed laser deposition (PLD). The films were grown by vdW epitaxy in a two-dimensional mode. X-ray diffraction measurements and transmission electron microscopy revealed that the films possess a trigonal Sb2Te3 structure. The single atomic Sb/Te termination layer on the Si surface was formed initializing the thin film growth. This work demonstrates a straightforward method to deposit vdW-epitaxial layered chalcogenides and, at the same time, opens up the feasibility to fabricate chalcogenide vdW heterostructures by PLD.
- ItemCompositional Patterning in Carbon Implanted Titania Nanotubes(Weinheim : Wiley-VCH, 2021) Kupferer, Astrid; Holm, Alexander; Lotnyk, Andriy; Mändl, Stephan; Mayr, Stefan G.Ranging from novel solar cells to smart biosensors, titania nanotube arrays constitute a highly functional material for various applications. A promising route to modify material characteristics while preserving the amorphous nanotube structure is present when applying low-energy ion implantation. In this study, the interplay of phenomenological effects observed upon implantation of low fluences in the unique 3D structure is reported: sputtering versus readsorption and plastic flow, amorphization versus crystallization and compositional patterning. Patterning within the oxygen and carbon subsystem is revealed using transmission electron microscopy. By applying a Cahn–Hilliard approach within the framework of driven alloys, characteristic length scales are derived and it is demonstrated that compositional patterning is expected on free enthalpy grounds, as predicted by density functional theory based ab initio calculations. Hence, an attractive material with increased conductivity for advanced devices is provided. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH