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- 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.
- ItemWeak electron irradiation suppresses the anomalous magnetization of N-doped diamond crystals(Weinheim : Wiley-VCH, 2021) Setzer, Annette; Esquinazi, Pablo D.; Daikos, Olesya; Scherzer, Tom; Pöppl, Andreas; Staacke, Robert; Lühmann, Tobias; Pezzagna, Sebastien; Knolle, Wolfgang; Buga, Sergei; Abel, Bernd; Meijer, JanSeveral diamond bulk crystals with a concentration of electrically neutral single substitutional nitrogen atoms of ≲80 ppm, the so-called C or P1 centers, are irradiated with electrons at 10 MeV energy and low fluence. The results show a complete suppression of the irreversible behavior in field and temperature of the magnetization below 30 K, after a decrease in ≲40 ppm in the concentration of C centers produced by the electron irradiation. This result indicates that magnetic C centers are at the origin of the large hysteretic behavior found recently in nitrogen-doped diamond crystals. This is remarkable because of the relatively low density of C centers, stressing the extraordinary role of the C centers in triggering those phenomena in diamond at relatively high temperatures. After annealing the samples at high temperatures in vacuum, the hysteretic behavior is partially recovered.
- ItemMolecular Beam Epitaxy Growth and Characterization of Germanium-Doped Cubic AlxGa1−xN(Weinheim : Wiley-VCH, 2020) Deppe, Michael; Henksmeier, Tobias; Gerlach, Jürgen W.; Reuter, Dirk; As, Donat J.In cubic (c-)GaN Ge has emerged as a promising alternative to Si for n-type doping, offering the advantage of slightly improved electrical properties. Herein, a study on Ge doping of the ternary alloy c-AlxGa1−xN is presented. Ge-doped c-AlxGa1−xN layers are grown by plasma-assisted molecular beam epitaxy. In two sample series, both the Al mole fraction x and the doping level are varied. The incorporation of Ge is verified by time-of-flight secondary ion mass spectrometry. Ge incorporation and donor concentrations rise exponentially with increasing Ge cell temperature. A maximum donor concentration of 1.4 × 1020 cm−3 is achieved. While the incorporation of Ge is almost independent of x, incorporation of O, which acts as an unintentional donor, increases for higher x. Dislocation densities start increasing when doping levels of around 3 × 1019 cm−3 are exceeded. Also photoluminescence intensities begin to drop at these high doping levels. Optical emission of layers with x > 0.25 is found to originate from a defect level 0.9 eV below the indirect bandgap, which is not related to Ge. In the investigated range 0 ≤ x ≤ 0.6, Ge is a suitable donor in c-AlxGa1−xN up to the low 1019 cm−3 range.
- ItemDefect-Induced Magnetism in Nonmagnetic Oxides: Basic Principles, Experimental Evidence, and Possible Devices with ZnO and TiO2(Weinheim : Wiley-VCH, 2020) Esquinazi, Pablo David; Hergert, Wolfram; Stiller, Markus; Botsch, Lukas; Ohldag, Hendrik; Spemann, Daniel; Hoffmann, Martin; Adeagbo, Waheed A.; Chassé, Angelika; Nayak, Sanjeev K.; Ben Hamed, HichemThe magnetic moment and the magnetic order induced by localized defects, like vacancies, interstitials, and/or nonmagnetic (NM) ions, in a NM oxide atomic lattice are discussed. When the defect concentration is of the order of or larger than ≈3 at%, magnetic order at room temperature can appear. Herein, the theoretical basic principles needed to understand and compute this new magnetic phenomenon in solids are developed in detail. In particular, the main results of density functional theory (DFT) calculations are used to estimate the magnetization and X-ray magnetic circular dichroism (XMCD) values. The main experimental evidences on this phenomenon are reviewed, especially magnetization, the element-specific XMCD, and transport properties in two selected oxides, ZnO and TiO2. Emphasis is given on the simplicity and efficiency ion irradiation methods have to trigger magnetic order in these oxides as well as a very sensitive method to characterize magnetic impurities. Two possible applications of this phenomenon are discussed, namely spin filtering at magnetic/NM interfaces in ZnO and perpendicular magnetic anisotropy triggered in TiO2 anatase microstructures. The existing literature on defect-induced magnetism in oxides is shortly reviewed, which provides further evidence on the robustness of this phenomenon in solids.
- ItemA Diverse View of Science to Catalyse Change(Weinheim : Wiley-VCH, 2020) Urbina-Blanco, César A.; Jilani, Safia Z.; Speight, Isaiah R.; Bojdys, Michael J.; Friščić, Tomislav; Stoddart, J. Fraser; Nelson, Toby L.; Mack, James; Robinson, Renã A.S.; Waddell, Emanuel A.; Lutkenhaus, Jodie L.; Godfrey, Murrell; Abboud, Martine I.; Aderinto, Stephen O.; Aderohunmu, Damilola; Bibič, Lučka; Borges, João; Dong, Vy M.; Ferrins, Lori; Fung, Fun Man; John, Torsten; Lim, Felicia P.L.; Masters, Sarah L.; Mambwe, Dickson; Thordarson, Pall; Titirici, Maria-Magdalena; Tormet-González, Gabriela D.; Unterlass, Miriam M.; Wadle, Austin; Yam, Vivian W.-W.; Yang, Ying-WeiValuing diversity leads to scientific excellence, the progress of science and most importantly, it is simply the right thing to do. We can value diversity not only in words, but also in actions. From the structure of DNA,1 to computer science,2 and space-station batteries,3 several key scientific discoveries that enhance our lives today, were made by marginalized scientists. These three scientists, Rosalind E. Franklin, Alan M. Turing and Olga D. González-Sanabria, did not conform to the cultural expectations of how scientists should look and behave. Unfortunately, marginalized scientists are often viewed as just a resource rather than the lifeblood that constitutes science itself. We need to embrace scientists from all walks of life and corners of the globe; this will also mean that nobody is excluded from tackling the life-threatening societal challenges that lie ahead. An awareness of science policy is essential to safeguarding our future. Science policy deals with creating the framework and codes of conduct that determine how science can best serve society.4-6 Discussions around science policy are often accompanied by anecdotes of “good” and “bad” practices regarding the merits of diversity and inclusion. Excellence and truth, which flow inexorably from diversity and inclusion, are the bedrocks upon which science should influence political and economic outcomes. A vital area of science policy is to support the professional development of marginalized scientists, an objective that must be acted upon by scientific leaders and communicators...
- ItemSynthesis of Modified Poly(vinyl Alcohol)s and Their Degradation Using an Enzymatic Cascade(Weinheim : Wiley-VCH, 2023) von Haugwitz, Gerlis; Donnelly, Kian; Di Filippo, Mara; Breite, Daniel; Phippard, Max; Schulze, Agnes; Wei, Ren; Baumann, Marcus; Bornscheuer, Uwe T.Poly(vinyl alcohol) (PVA) is a water-soluble synthetic vinyl polymer with remarkable physical properties including thermostability and viscosity. Its biodegradability, however, is low even though a large amount of PVA is released into the environment. Established physical-chemical degradation methods for PVA have several disadvantages such as high price, low efficiency, and secondary pollution. Biodegradation of PVA by microorganisms is slow and frequently involves pyrroloquinoline quinone (PQQ)-dependent enzymes, making it expensive due to the costly cofactor and hence unattractive for industrial applications. In this study, we present a modified PVA film with improved properties as well as a PQQ-independent novel enzymatic cascade for the degradation of modified and unmodified PVA. The cascade consists of four steps catalyzed by three enzymes with in situ cofactor recycling technology making this cascade suitable for industrial applications.
- ItemFibroblast Response to Nanocolumnar TiO2 Structures Grown by Oblique Angle Sputter Deposition(Weinheim : Wiley-VCH, 2021) Kapprell, Uta; Friebe, Sabrina; Grüner, Susann; Grüner, Christoph; Kupferer, Astrid; Rauschenbach, Bernd; Mayr, Stefan G.Cells are established to sense and respond to the properties, including nano- and microscale morphology, of the substrate they adhere to, which opens up the possibility to tailor bioactivity. With this background, the potential of tilted TiO2 nanostructures grown by oblique angle sputtering to affect fibroblasts with particular focus on inducing anisotropy in cell behavior is explored. By depositing TiO2 at different oblique angles relative to the substrate normal, morphologies, columnar tilt angle, roughness, and distances between neighbored nanocolumns can be adjusted. To assess bioactivity of the resulting structures, L929-mouse fibroblasts are seeded in vitro on TiO2 nanostructured substrates. Angle-dependent movement and velocity distributions of the cells on differently tilted columns and a smooth reference sample are studied. Cell proliferation rates and cell areas are additional factors which provide information about viability and the well-being of cells. It could be shown that the local topography of the surface has an influence on the directed movement of the cells. © 2021 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
- ItemFour-Step Domino Reaction Enables Fully Controlled Non-Statistical Synthesis of Hexaarylbenzene with Six Different Aryl Groups*(Weinheim : Wiley-VCH, 2021) Grau, Benedikt W.; Dill, Maximilian; Hampel, Frank; Kahnt, Axel; Jux, Norbert; Tsogoeva, Svetlana B.Hexaarylbenzene (HAB) derivatives are versatile aromatic systems playing a significant role as chromophores, liquid crystalline materials, molecular receptors, molecular-scale devices, organic light-emitting diodes and candidates for organic electronics. Statistical synthesis of simple symmetrical HABs is known via cyclotrimerization or Diels–Alder reactions. By contrast, the synthesis of more complex, asymmetrical systems, and without involvement of statistical steps, remains an unsolved problem. Here we present a generally applicable synthetic strategy to access asymmetrical HAB via an atom-economical and high-yielding metal-free four-step domino reaction using nitrostyrenes and α,α-dicyanoolefins as easily available starting materials. Resulting domino product—functionalized triarylbenzene (TAB)—can be used as a key starting compound to furnish asymmetrically substituted hexaarylbenzenes in high overall yield and without involvement of statistical steps. This straightforward domino process represents a distinct approach to create diverse and still unexplored HAB scaffolds, containing six different aromatic rings around central benzene core. © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
- ItemLong-Living Holes in Grey Anatase TiO2 Enable Noble-Metal-Free and Sacrificial-Agent-Free Water Splitting(Weinheim : Wiley-VCH, 2020) Liu, Ning; Mohajernia, Shiva; Nguyen, Nhat Truong; Hejazi, Seyedsina; Plass, Fabian; Kahnt, Axel; Yokosawa, Tadahiro; Osvet, Andres; Spiecker, Erdmann; Guldi, Dirk M.; Schmuki, PatrikTitanium dioxide has been the benchmark semiconductor in photocatalysis for more than 40 years. Full water splitting, that is, decomposing water into H2 and O2 in stoichiometric amounts and with an acceptable activity, still remains a challenge, even when TiO2-based photocatalysts are used in combination with noble-metal co-catalysts. The bottleneck of anatase-type TiO2 remains the water oxidation, that is, the hole transfer reaction from pristine anatase to the aqueous environment. In this work, we report that “grey” (defect engineered) anatase can provide a drastically enhanced lifetime of photogenerated holes, which, in turn, enables an efficient oxidation reaction of water to peroxide via a two-electron pathway. As a result, a Ni@grey anatase TiO2 catalyst can be constructed with an impressive performance in terms of photocatalytic splitting of neutral water into H2 and a stoichiometric amount of H2O2 without the need of any noble metals or sacrificial agents. The finding of long hole lifetimes in grey anatase opens up a wide spectrum of further photocatalytic applications of this material. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemSynthesis, Electronic Properties and Reactivity of [B12X11(NO2)]2− (X=F–I) Dianions(Weinheim : Wiley-VCH, 2020) Asmis, Knut R.; Beele, Björn B.; Jenne, Carsten; Kawa, Sebastian; Knorke, Harald; Nierstenhöfer, Marc C.; Wang, Xue-Bin; Warneke, Jonas; Warneke, Ziyan; Yuan, QinqinNitro-functionalized undecahalogenated closo-dodecaborates [B12X11(NO2)]2− were synthesized in high purities and characterized by NMR, IR, and Raman spectroscopy, single crystal X-diffraction, mass spectrometry, and gas-phase ion vibrational spectroscopy. The NO2 substituent leads to an enhanced electronic and electrochemical stability compared to the parent perhalogenated [B12X12]2− (X=F–I) dianions evidenced by photoelectron spectroscopy, cyclic voltammetry, and quantum-chemical calculations. The stabilizing effect decreases from X=F to X=I. Thermogravimetric measurements of the salts indicate the loss of the nitric oxide radical (NO.). The homolytic NO. elimination from the dianion under very soft collisional excitation in gas-phase ion experiments results in the formation of the radical [B12X11O]2−.. Theoretical investigations suggest that the loss of NO. proceeds via the rearrangement product [B12X11(ONO)]2−. The O-bonded nitrosooxy structure is thermodynamically more stable than the N-bonded nitro structure and its formation by radical recombination of [B12X11O]2−. and NO. is demonstrated. © 2020 The Authors. Published by Wiley-VCH GmbH