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- ItemDesign of biomimetic collagen matrices by reagent-free electron beam induced crosslinking: Structure-property relationships and cellular response(Amsterdam [u.a.] : Elsevier Science, 2019) Riedel, Stefanie; Hietschold, Philine; Krömmelbein, Catharina; Kunschmann, Tom; Konieczny, Robert; Knolle, Wolfgang; Mierke, Claudia T.; Zink, Mareike; Mayr, Stefan G.Novel strategies to mimic mammalian extracellular matrix (ECM) in vitro are desirable to study cell behavior, diseases and new agents in drug delivery. Even though collagen represents the major constituent of mammalian ECM, artificial collagen hydrogels with characteristic tissue properties such as network size and stiffness are difficult to design without application of chemicals which might be even cytotoxic. In our study we investigate how high energy electron induced crosslinking can be utilized to precisely tune collagen properties for ECM model systems. Constituting a minimally invasive approach, collagen residues remain intact in the course of high energy electron treatment. Quantification of the 3D pore size of the collagen network as a function of irradiation dose shows an increase in density leading to decreased pore size. Rheological measurements indicate elevated storage and loss moduli correlating with an increase in crosslinking density. In addition, cell tests show well maintained viability of NIH 3T3 cells for irradiated collagen gels indicating excellent cellular acceptance. With this, our investigations demonstrate that electron beam crosslinked collagen matrices have a high potential as precisely tunable ECM-mimetic systems with excellent cytocompatibility.
- 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.
- ItemMagnetic field and angle-dependent photoluminescence of a fiber-coupled nitrogen vacancy rich diamond(Melville, NY : American Inst. of Physics, 2021) Wunderlich, Ralf; Staacke, Robert; Knolle, Wolfgang; Abel, Bernd; Meijer, JanHere, we investigate the magnetic field dependent photoluminescence (PL) of a fiber-coupled diamond single crystal with a high density of nitrogen vacancy (NV) centers. Angle-dependent magnetic field sweep measurements between 0 and 111 mT were performed using an oscillating illumination combined with lock-in techniques. Besides the expected superposed PL of differently oriented NV centers, a zoo of features in the PL are found. These features can be associated with level anti-crossings and cross relaxations. In particular, PL measurements allowed us to detect auto-cross relaxation between coupled NV centers. Moreover, the PL measurements at low magnetic fields show dips suggesting an interaction of NV centers with additional spin defects. The results presented here are not only a study for NV-based fiber-coupled sensors made of diamond, but also show a way to investigate with manageable effort and purely an optical multispin interaction with at least one NV center as a constituent.
- ItemRobust nuclear hyperpolarization driven by strongly coupled nitrogen vacancy centers(Melville, NY : American Inst. of Physics, 2021) Wunderlich, Ralf; Staacke, Robert; Knolle, Wolfgang; Abel, Bernd; Haase, Jürgen; Meijer, JanNuclear magnetic resonance techniques are widely used in the natural sciences but they lack sensitivity. Therefore, large sample volumes or long measurement times are necessary. In this work, we investigate the polarization of bulk 13C nuclei in a diamond above the thermal equilibrium at room temperature. Previously studied mechanisms utilize direct coupling to nitrogen vacancy centers or the additional assistance of substitutional nitrogen impurities for this purpose. We exploit strongly coupled nitrogen vacancy centers as polarization sources. We study two approaches to transfer the optically induced polarization of the electron spins of the nitrogen vacancy centers to nearby nuclear spins. First, the electron-nuclear polarization transfer is achieved by energy matching conditions or, second, by magnetic field sweeps inducing Landau–Zener-like transitions. Simulations according to a quantum mechanical system consisting of two coupled nitrogen vacancy centers and a weakly coupled 13C spin show an excellent agreement with the experimental data. Both approaches allow a reduction of the measurement time by roughly three orders of magnitude.
- ItemRadiation-Induced Graft Immobilization (RIGI): Covalent Binding of Non-Vinyl Compounds on Polymer Membranes(Basel : MDPI, 2021) Schmidt, Martin; Zahn, Stefan; Gehlhaar, Florian; Prager, Andrea; Griebel, Jan; Kahnt, Axel; Knolle, Wolfgang; Konieczny, Robert; Gläser, Roger; Schulze, AgnesRadiation-induced graft immobilization (RIGI) is a novel method for the covalent binding of substances on polymeric materials without the use of additional chemicals. In contrast to the well-known radiation-induced graft polymerization (RIGP), RIGI can use non-vinyl compounds such as small and large functional molecules, hydrophilic polymers, or even enzymes. In a one-step electron-beam-based process, immobilization can be performed in a clean, fast, and continuous operation mode, as required for industrial applications. This study proposes a reaction mechanism using polyvinylidene fluoride (PVDF) and two small model molecules, glycine and taurine, in aqueous solution. Covalent coupling of single molecules is achieved by radical recombination and alkene addition reactions, with water radiolysis playing a crucial role in the formation of reactive solute species. Hydroxyl radicals contribute mainly to the immobilization, while solvated electrons and hydrogen radicals play a minor role. Release of fluoride is mainly induced by direct ionization of the polymer and supported by water. Hydrophobic chains attached to cations appear to enhance the covalent attachment of solutes to the polymer surface. Computational work is complemented by experimental studies, including X-ray photoelectron spectroscopy (XPS) and fluoride high-performance ion chromatography (HPIC).
- ItemIn situ Gelling Amphotericin B Nanofibers: A New Option for the Treatment of Keratomycosis(Lausanne : Frontiers Media, 2020) Göttel, Benedikt; Lucas, Henrike; Syrowatka, Frank; Knolle, Wolfgang; Kuntsche, Judith; Heinzelmann, Joana; Viestenz, Arne; Mäder, KarstenThe purpose of our research was the development of Amphotericin B-loaded in situ gelling nanofibers for the treatment of keratomycosis. Different formulation strategies were applied to increase the drug load of the sparingly water-soluble Amphotericin B in electrospun Gellan Gum/Pullulan fibers. These include bile salt addition, encapsulation in poly(lactic-co-glycolic acid) (PLGA) nanoparticles and formation of a polymeric Amphotericin B polyelectrolyte complex. The Amphotericin B polyelectrolyte complex (AmpB-Eu L) performed best and was very effective against the fungal strain Issatchenkia orientalis in vitro. The complex was characterized in detail by attenuated total reflection infrared spectroscopy, X-ray powder diffraction, and differential scanning calorimetry. A heat induced stress test was carried out to ensure the stability of the polyelectrolyte complex. To gain information about the cellular tolerance of the developed polyelectrolyte complex a new, innovative multilayered-stratified human cornea cell model was used for determination of the cellular toxicity in vitro. For a safe therapy, the applied ophthalmic drug delivery system has to be sterile. Sterilization by electron irradiation caused not degradation of pure Amphotericin B and also for the bile salt complex. Furthermore, the developed Amphotericin B polyelectrolyte complex was not degraded by the irradiation process. In conclusion, a new polyelectrolyte Amphotericin B complex has been found which retains the antifungal activity of the drug with sufficient stability against irradiation-sterilization induced drug degradation. Furthermore, in comparison with the conventional used eye drop formulation, the new AmpB-complex loaded nanofibers were less toxic to cornea cells in vitro. Electrospinning of the Amphotericin B polyelectrolyte complex with Gellan Gum/ Pullulan leads to the formation of nanofibers with in situ gelling properties, which is a new and promising option for the treatment of keratomycosis. © Copyright © 2020 Göttel, Lucas, Syrowatka, Knolle, Kuntsche, Heinzelmann, Viestenz and Mäder.