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- ItemTiOx/Pt3Ti(111) surface-directed formation of electronically responsive supramolecular assemblies of tungsten oxide clusters(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2021) Moors, Marco; An, Yun; Kuc, Agnieszka; Monakhov, Kirill YuHighly ordered titanium oxide films grown on a Pt3Ti(111) alloy surface were utilized for the controlled immobilization and tip-induced electric field-triggered electronic manipulation of nanoscopic W3O9 clusters. Depending on the operating conditions, two different stable oxide phases, z'-TiO x and w'-TiO x , were produced. These phases show a strong effect on the adsorption characteristics and reactivity of W3O9 clusters, which are formed as a result of thermal evaporation of WO3 powder on the complex TiO x /Pt3Ti(111) surfaces under ultra-high vacuum conditions. The physisorbed tritungsten nano-oxides were found as isolated single units located on the metallic attraction points or as supramolecular self-assemblies with a W3O9-capped hexagonal scaffold of W3O9 units. By applying scanning tunneling microscopy to the W3O9-(W3O9)6 structures, individual units underwent a tip-induced reduction to W3O8. At elevated temperatures, agglomeration and growth of large WO3 islands, which thickness is strongly limited to a maximum of two unit cells, were observed. The findings boost progress toward template-directed nucleation, growth, networking, and charge state manipulation of functional molecular nanostructures on surfaces using operando techniques.
- ItemComparative study of sculptured metallic thin films deposited by oblique angle deposition at different temperatures(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2018) Liedtke, Susann; Grüner, Christoph; Gerlach, Jürgen W.; Rauschenbach, BerndMetals with a wide range of melting points are deposited by electron beam evaporation under oblique deposition geometry on thermally oxidized Si substrates. During deposition the sample holder is cooled down to 77 K. It is observed that all obliquely deposited metals grow as tilted, high aspect ratio columns and hence with a similar morphology. A comparison of such columns with those deposited at room temperature (300 K) reveals that shadowing dominates the growth process for columns deposited at 77 K, while the impact of surface diffusion is significantly increased at elevated substrate temperatures. Furthermore, it is discussed how the incidence angle of the incoming particle flux and the substrate temperature affect the columnar tilt angles and the porosity of the sculptured thin films. Exemplarily for tilted Al columns deposited at 77 K and at 300 K, in-plane pole figure measurements are carried out. A tendency to form a biaxial texture as well as a change in the crystalline structure depending on the substrate temperature is found for those films.
- ItemDeposition of exchange-coupled dinickel complexes on gold substrates utilizing ambidentate mercapto-carboxylato ligands(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2017) Börner, Martin; Blömer, Laura; Kischel, Marcus; Richter, Peter; Salvan, Georgeta; Zahn, Dietrich R. T.; Siles, Pablo F.; Fuentes, Maria E. N.; Bufon, Carlos C. B.; Grimm, Daniel; Schmidt, Oliver G.; Breite, Daniel; Abel, Bernd; Kersting, BertholdThe chemisorption of magnetically bistable transition metal complexes on planar surfaces has recently attracted increased scientific interest due to its potential application in various fields, including molecular spintronics. In this work, the synthesis of mixed-ligand complexes of the type [NiII2L(L’)](ClO4), where L represents a 24-membered macrocyclic hexaazadithiophenolate ligand and L’ is a ω-mercapto-carboxylato ligand (L’ = HS(CH2)5CO2− (6), HS(CH2)10CO2− (7), or HS(C6H4)2CO2− (8)), and their ability to adsorb on gold surfaces is reported. Besides elemental analysis, IR spectroscopy, electrospray ionization mass spectrometry (ESIMS), UV–vis spectroscopy, and X-ray crystallography (for 6 and 7), the compounds were also studied by temperature-dependent magnetic susceptibility measurements (for 7 and 8) and (broken symmetry) density functional theory (DFT) calculations. An S = 2 ground state is demonstrated by temperature-dependent susceptibility and magnetization measurements, achieved by ferromagnetic coupling between the spins of the Ni(II) ions in 7 (J = +22.3 cm−1) and 8 (J = +20.8 cm−1; H = −2JS1S2). The reactivity of complexes 6–8 is reminiscent of that of pure thiolato ligands, which readily chemisorb on Au surfaces as verified by contact angle, atomic force microscopy (AFM) and spectroscopic ellipsometry measurements. The large [Ni2L] tail groups, however, prevent the packing and self-assembly of the hydrocarbon chains. The smaller film thickness of 7 is attributed to the specific coordination mode of the coligand. Results of preliminary transport measurements utilizing rolled-up devices are also reported.
- ItemHeterobimetallic conducting polymers based on salophen complexes via electrosynthesis(London [u.a.] : RSC, 2023) Bia, Francesca; Gualandi, Isacco; Griebel, Jan; Rasmussen, Leon; Hallak, Bassam; Tonelli, Domenica; Kersting, BertholdIn this work, we report the first electrochemical synthesis of two copolymeric bimetallic conducting polymers by a simple anodic electropolymerization method. The adopted precursors are electroactive transition metal (M = Ni, Cu and Fe) salophen complexes, which can be easily obtained by direct chemical synthesis. The resulting films, labeled poly-NiCu and poly-CuFe, were characterized by cyclic voltammetry in both organic and aqueous media, attenuated total reflectance Fourier transform infrared spectroscopy, UV-vis spectroscopy, scanning electron microscopy, and coupled energy dispersive X-ray spectroscopy. The films are conductive and exhibit great electrochemical stability in both organic and aqueous media (resistant over 100 cycles without significant loss in current response or changes in electrochemical behavior), which makes them good candidates for an array of potential applications. Electrochemical detection of ascorbic acid was performed using both materials.
- 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.
- ItemPhotoemission electron microscopy of magneto-ionic effects in La0.7Sr0.3MnO3(Melville, NY : AIP Publ., 2020) Wilhelm, Marek; Giesen, Margret; Duchoň, Tomáš; Moors, Marco; Mueller, David N.; Hackl, Johanna; Baeumer, Christoph; Hamed, Mai Hussein; Cao, Lei; Zhang, Hengbo; Petracic, Oleg; Glöß, Maria; Cramm, Stefan; Nemšák, Slavomír; Wiemann, Carsten; Dittmann, Regina; Schneider, Claus M.; Müller, MartinaMagneto-ionic control of magnetism is a promising route toward the realization of non-volatile memory and memristive devices. Magneto-ionic oxides are particularly interesting for this purpose, exhibiting magnetic switching coupled to resistive switching, with the latter emerging as a perturbation of the oxygen vacancy concentration. Here, we report on electric-field-induced magnetic switching in a La0.7Sr0.3MnO3 (LSMO) thin film. Correlating magnetic and chemical information via photoemission electron microscopy, we show that applying a positive voltage perpendicular to the film surface of LSMO results in the change in the valence of the Mn ions accompanied by a metal-to-insulator transition and a loss of magnetic ordering. Importantly, we demonstrate that the voltage amplitude provides granular control of the phenomena, enabling fine-tuning of the surface electronic structure. Our study provides valuable insight into the switching capabilities of LSMO that can be utilized in magneto-ionic devices. © 2020 Author(s).
- ItemFlexible Transparent Barrier Applications of Oxide Thin Films Prepared by Photochemical Conversion at Low Temperature and Ambient Pressure(Lausanne : Frontiers Media, 2020) With, Patrick C.; Helmstedt, Ulrike; Prager, LutzPhotoconversion of metal-organic precursors to thin film metal oxides using ultraviolet (UV) radiation in oxidative atmosphere is an attractive technology because it can be applied at temperatures <80°C and at ambient pressure. Thus, it enables preparing this class of thin films in a cost-efficient manner on temperature sensitive substrates such as polymer films. In this article, various aspects of research and development in the field of photochemical thin-film fabrication, with particular focus to the application of the produced films as gas permeation barriers for the encapsulation of optoelectronic devices are reviewed. Thereby, it covers investigations on fundamental photochemically initiated reactions for precursor classes containing metal-oxygen and metal-nitrogen bonds, and emphazises the relevance of that understanding for applicative considerations like integration of the single-layer barrier films into relevant encapsulation films. Further perspectives are given concerning integration of additional functionalities like electrical conductivity to the flexible and transparent barrier films. © Copyright © 2020 With, Helmstedt and Prager.
- 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
- ItemAntiphase Boundaries Constitute Fast Cation Diffusion Paths in SrTiO3 Memristive Devices(Weinheim : Wiley-VCH, 2020) Heisig, Thomas; Kler, Joe; Du, Hongchu; Baeumer, Christoph; Hensling, Felix; Glöß, Maria; Moors, Marco; Locatelli, Andrea; Menteş, Tevfik Onur; Genuzio, Francesca; Mayer, Joachim; De Souza, Roger A.; Dittmann, ReginaResistive switching in transition metal oxide-based metal-insulator-metal structures relies on the reversible drift of ions under an applied electric field on the nanoscale. In such structures, the formation of conductive filaments is believed to be induced by the electric-field driven migration of oxygen anions, while the cation sublattice is often considered to be inactive. This simple mechanistic picture of the switching process is incomplete as both oxygen anions and metal cations have been previously identified as mobile species under device operation. Here, spectromicroscopic techniques combined with atomistic simulations to elucidate the diffusion and drift processes that take place in the resistive switching model material SrTiO3 are used. It is demonstrated that the conductive filament in epitaxial SrTiO3 devices is not homogenous but exhibits a complex microstructure. Specifically, the filament consists of a conductive Ti3+-rich region and insulating Sr-rich islands. Transmission electron microscopy shows that the Sr-rich islands emerge above Ruddlesden–Popper type antiphase boundaries. The role of these extended defects is clarified by molecular static and molecular dynamic simulations, which reveal that the Ruddlesden–Popper antiphase boundaries constitute diffusion fast-paths for Sr cations in the perovskites structure. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemFinishing of metal optics by ion beam technologies(Bellingham, Wash. : SPIE, 2019) Bauer, Jens; Frost, Frank; Lehmann, Antje; Ulitschka, Melanie; Li, Yaguo; Arnold, ThomasUltraprecise mirror devices show considerable potential with view to applications in the visible and the ultraviolet spectral ranges. Aluminum alloys gather good mechanical and excellent optical properties and thus they emerge as important mirror construction materials. However, ultraprecision machining and polishing of optical aluminum surfaces are challenging, which originates from the high chemical reactivity and the heterogeneous matrix structure. Recently, several ion beam-based techniques have been developed to qualify aluminum mirrors for short-wavelength applications. We give an overview of the state-of-the-art ion beamprocessing techniques for figure error correction and planarization, either by direct aluminum machining or with the aid of polymer or inorganic, amorphous surface films. © The Authors.