Browsing by Author "Solodenko, Helena"

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    ItemOpen Access
    A complementary experimental and theoretical approach for probing the surface functionalization of ZnO with molecular catalyst linkers
    (2023) Kousik, Shravan R.; Solodenko, Helena; YazdanYar, Azade; Kirchhof, Manuel; Schützendübe, Peter; Richter, Gunther; Laschat, Sabine; Fyta, Maria; Schmitz, Guido; Bill, Joachim; Atanasova, Petia
    The application of ZnO materials as solid-state supports for molecular heterogeneous catalysis is contingent on the functionalization of the ZnO surface with stable self-assembled monolayers (SAMs) of catalyst linker molecules. Herein, experimental and theoretical methods are used to study SAMs of azide-terminated molecular catalyst linkers with two different anchor groups (silane and thiol) on poly and monocrystalline (0001, ) ZnO surfaces. Angle-resolved and temperature-dependent X-ray photoelectron spectroscopy (XPS) is used to study SAM binding modes, thermal stabilities, and coverages. The binding strengths and atomistic ordering of the SAMs are determined via atom-probe tomography (APT). Density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations provide insights on the influence of the ZnO surface polarity on the interaction affinity and conformational behavior of the SAMs. The investigations show that SAMs based on 3-azidopropyltriethoxysilane possess a higher binding strength and thermal stability than the corresponding thiol. SAM surface coverage is strongly influenced by the surface polarity of ZnO, and the highest coverage is observed on the polycrystalline surface. To demonstrate the applicability of linker-modified polycrystalline ZnO as a catalyst support, a chiral Rh diene complex is immobilized on the azide-terminal of the SAM and its coverage is evaluated via XPS.
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    ItemOpen Access
    Nanoscale analysis of frozen honey by atom probe tomography
    (2022) Schwarz, Tim M.; Ott, Jonas; Solodenko, Helena; Schmitz, Guido; Stender, Patrick
    Three-dimensional reconstruction of the analysed volume is one of the main goals of atom probe tomography (APT) and can deliver nearly atomic resolution (~ 0.2 nm spatial resolution) and chemical information with a mass sensitivity down to the ppm range. Extending this technique to frozen biological systems would have an enormous impact on the structural analysis of biomolecules. In previous works, we have shown that it is possible to measure frozen liquids with APT. In this paper, we demonstrate the ability of APT to trace nanoscale precipitation in frozen natural honey. While the mass signals of the common sugar fragments CxHy and CxOyHz overlap with (H2O)nH from water, we achieved correct stoichiometric values via different interpretation approaches for the peaks and thus determined the water content reliably. Next, we use honey to investigate the spatial resolution capabilities as a step toward the measurement of biological molecules in solution in 3D with sub-nanometer resolution. This may take analytical techniques to a new level, since methods of chemical characterization for cryogenic samples, especially biological samples, are still limited.
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    Optimizing the plasma oxidation of aluminum gate electrodes for ultrathin gate oxides in organic transistors
    (2021) Geiger, Michael; Hagel, Marion; Reindl, Thomas; Weis, Jürgen; Weitz, R. Thomas; Solodenko, Helena; Schmitz, Guido; Zschieschang, Ute; Klauk, Hagen; Acharya, Rachana
    A critical requirement for the application of organic thin-film transistors (TFTs) in mobile or wearable applications is low-voltage operation, which can be achieved by employing ultrathin, high-capacitance gate dielectrics. One option is a hybrid dielectric composed of a thin film of aluminum oxide and a molecular self-assembled monolayer in which the aluminum oxide is formed by exposure of the surface of the aluminum gate electrode to a radio-frequency-generated oxygen plasma. This work investigates how the properties of such dielectrics are affected by the plasma power and the duration of the plasma exposure. For various combinations of plasma power and duration, the thickness and the capacitance of the dielectrics, the leakage-current density through the dielectrics, and the current–voltage characteristics of organic TFTs in which these dielectrics serve as the gate insulator have been evaluated. The influence of the plasma parameters on the surface properties of the dielectrics, the thin-film morphology of the vacuum-deposited organic-semiconductor films, and the resulting TFT characteristics has also been investigated.