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- ItemMerging Top-Down and Bottom-Up Approaches to Fabricate Artificial Photonic Nanomaterials with a Deterministic Electric and Magnetic Response(Weinheim : Wiley-VCH Verlag, 2020) Dietrich K.; Zilk M.; Steglich M.; Siefke T.; Hübner U.; Pertsch T.; Rockstuhl C.; Tünnermann A.; Kley E.-B.Artificial photonic nanomaterials made from densely packed scatterers are frequently realized either by top-down or bottom-up techniques. While top-down techniques offer unprecedented control over achievable geometries for the scatterers, by trend they suffer from being limited to planar and periodic structures. In contrast, materials fabricated with bottom-up techniques do not suffer from such disadvantages but, unfortunately, they offer only little control on achievable geometries for the scatterers. To overcome these limitations, a nanofabrication strategy is introduced that merges both approaches. A large number of scatterers are fabricated with a tailored optical response by fast character projection electron-beam lithography and are embedded into a membrane. By peeling-off this membrane from the substrate, scrambling, and densifying it, a bulk material comprising densely packed and randomly arranged scatterers is obtained. The fabrication of an isotropic material from these scatterers with a strong electric and magnetic response is demonstrated. The approach of this study unlocks novel opportunities to fabricate nanomaterials with a complex optical response in the bulk but also on top of arbitrarily shaped surfaces. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemPinning of the Fermi Level in CuFeO2 by Polaron Formation Limiting the Photovoltage for Photochemical Water Splitting(Weinheim : Wiley-VCH Verlag, 2020) Hermans Y.; Klein A.; Sarker H.P.; Huda M.N.; Junge H.; Toupance T.; Jaegermann W.CuFeO2 is recognized as a potential photocathode for photo(electro)chemical water splitting. However, photocurrents with CuFeO2-based systems are rather low so far. In order to optimize charge carrier separation and water reduction kinetics, defined CuFeO2/Pt, CuFeO2/Ag, and CuFeO2/NiOx(OH)y heterostructures are made in this work through a photodeposition procedure based on a 2H CuFeO2 hexagonal nanoplatelet shaped powder. However, water splitting performance tests in a closed batch photoreactor show that these heterostructured powders exhibit limited water reduction efficiencies. To test whether Fermi level pinning intrinsically limits the water reduction capacity of CuFeO2, the Fermi level tunability in CuFeO2 is evaluated by creating CuFeO2/ITO and CuFeO2/H2O interfaces and analyzing the electronic and chemical properties of the interfaces through photoelectron spectroscopy. The results indicate that Fermi level pinning at the Fe3+/Fe2+ electron polaron formation level may intrinsically prohibit CuFeO2 from acquiring enough photovoltage to reach the water reduction potential. This result is complemented with density functional theory calculations as well. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim