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- ItemBlind Super-Resolution Approach for Exploiting Illumination Variety in Optical-Lattice Illumination Microscopy(Washington, DC : ACS Publications, 2021) Samanta, Krishnendu; Sarkar, Swagato; Acuña, Sebastian; Joseph, Joby; Ahluwalia, Balpreet Singh; Agarwal, KrishnaOptical-lattice illumination patterns help in pushing high spatial frequency components of the sample into the optical transfer function of a collection microscope. However, exploiting these high-frequency components require precise knowledge of illumination if reconstruction approaches similar to structured illumination microscopy are employed. Here, we present an alternate blind reconstruction approach that can provide super-resolution without the requirement of extra frames. For this, the property of exploiting temporal fluctuations in the sample emissions using “multiple signal classification algorithm” is extended aptly toward using spatial fluctuation of phase-modulated lattice illuminations for super-resolution. The super-resolution ability is shown for sinusoidal and multiperiodic lattice with approximately 3- and 6-fold resolution enhancements, respectively, over the diffraction limit. © 2021 The Authors. Published by American Chemical Society
- ItemRemarkable Mechanochromism in Blends of a π-Conjugated Polymer P3TEOT: The Role of Conformational Transitions and Aggregation(Weinheim : Wiley-VCH, 2020) Zessin, Johanna; Schnepf, Max; Oertel, Ulrich; Beryozkina, Tetyana; König, Tobias A.F.; Fery, Andreas; Mertig, Michael; Kiriy, AntonA novel mechanism for well-pronounced mechanochromism in blends of a π-conjugated polymer based on reversible conformational transitions of a chromophore rather than caused by its aggregation state, is exemplified. Particularly, a strong stretching-induced bathochromic shift of the light absorption, or hypsochromic shift of the emission, is found in blends of the water-soluble poly(3-tri(ethylene glycol)) (P3TEOT) embedded into the matrix of thermoplastic polyvinyl alcohol. This counterintuitive phenomenon is explained in terms of the concentration dependency of the P3TEOT's aggregation state, which in turn results in different molecular conformations and optical properties. A molecular flexibility, provided by low glass transition temperature of P3TEOT, and the fact that P3TEOT adopts an intermediate, moderately planar conformation in the solid state, are responsible for the unusual complex mechanochromic behavior. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemPlasmonic Properties of Colloidal Assemblies(Weinheim : Wiley-VCH, 2021) Rossner, Christian; König, Tobias A.F.; Fery, AndreasThe assembly of metal nanoparticles into supracolloidal structures unlocks optical features, which can go beyond synergistic combinations of the properties of their primary building units. This is due to inter-particle plasmonic coupling effects, which give rise to emergent properties. The motivation for this progress report is twofold: First, it is described how simulation approaches can be used to predict and understand the optical properties of supracolloidal metal clusters. These simulations may form the basis for the rational design of plasmonic assembly architectures, based on the desired functional cluster properties, and they may also spark novel material designs. Second, selected scalable state-of-the-art preparative strategies based on synthetic polymers to guide the supracolloidal assembly are discussed. These routes also allow for equipping the assembly structures with adaptive properties, which in turn enables (inter-)active control over the cluster optical properties. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemLightweight polymer-carbon composite current collector for lithium-ion batteries(Basel : MDPI, 2020) Fritsch, Marco; Coeler, Matthias; Kunz, Karina; Krause, Beate; Marcinkowski, Peter; Pötschke, Petra; Wolter, Mareike; Michaelis, AlexanderA hermetic dense polymer-carbon composite-based current collector foil (PCCF) for lithium-ion battery applications was developed and evaluated in comparison to state-of-the-art aluminum (Al) foil collector. Water-processed LiNi0.5Mn1.5O4 (LMNO) cathode and Li4Ti5O12 (LTO) anode coatings with the integration of a thin carbon primer at the interface to the collector were prepared. Despite the fact that the laboratory manufactured PCCF shows a much higher film thickness of 55 µm compared to Al foil of 19 µm, the electrode resistance was measured to be by a factor of 5 lower compared to the Al collector, which was attributed to the low contact resistance between PCCF, carbon primer and electrode microstructure. The PCCF-C-primer collector shows a sufficient voltage stability up to 5 V vs. Li/Li+ and a negligible Li-intercalation loss into the carbon primer. Electrochemical cell tests demonstrate the applicability of the developed PCCF for LMNO and LTO electrodes, with no disadvantage compared to state-of-the-art Al collector. Due to a 50% lower material density, the lightweight and hermetic dense PCCF polymer collector offers the possibility to significantly decrease the mass loading of the collector in battery cells, which can be of special interest for bipolar battery architectures. © 2020 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemCell-Instructive Multiphasic Gel-in-Gel Materials(Weinheim : Wiley-VCH, 2020) Kühn, Sebastian; Sievers, Jana; Stoppa, Aukha; Träber, Nicole; Zimmermann, Ralf; Welzel, Petra B.; Werner, CarstenDeveloping tissue is typically soft, highly hydrated, dynamic, and increasingly heterogeneous matter. Recapitulating such characteristics in engineered cell-instructive materials holds the promise of maximizing the options to direct tissue formation. Accordingly, progress in the design of multiphasic hydrogel materials is expected to expand the therapeutic capabilities of tissue engineering approaches and the relevance of human 3D in vitro tissue and disease models. Recently pioneered methodologies allow for the creation of multiphasic hydrogel systems suitable to template and guide the dynamic formation of tissue- and organ-specific structures across scales, in vitro and in vivo. The related approaches include the assembly of distinct gel phases, the embedding of gels in other gel materials and the patterning of preformed gel materials. Herein, the capabilities and limitations of the respective methods are summarized and discussed and their potential is highlighted with some selected examples of the recent literature. As the modularity of the related methodologies facilitates combinatorial and individualized solutions, it is envisioned that multiphasic gel-in-gel materials will become a versatile morphogenetic toolbox expanding the scope and the power of bioengineering technologies. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemNanoimprint Lithography Facilitated Plasmonic-Photonic Coupling for Enhanced Photoconductivity and Photocatalysis(Weinheim : Wiley-VCH, 2021) Gupta, Vaibhav; Sarkar, Swagato; Aftenieva, Olha; Tsuda, Takuya; Kumar, Labeesh; Schletz, Daniel; Schultz, Johannes; Kiriy, Anton; Fery, Andreas; Vogel, Nicolas; König, Tobias A.F.Imprint lithography has emerged as a reliable, reproducible, and rapid method for patterning colloidal nanostructures. As a promising alternative to top-down lithographic approaches, the fabrication of nanodevices has thus become effective and straightforward. In this study, a fusion of interference lithography (IL) and nanosphere imprint lithography on various target substrates ranging from carbon film on transmission electron microscope grid to inorganic and dopable polymer semiconductor is reported. 1D plasmonic photonic crystals are printed with 75% yield on the centimeter scale using colloidal ink and an IL-produced polydimethylsiloxane stamp. Atomically smooth facet, single-crystalline, and monodisperse colloidal building blocks of gold (Au) nanoparticles are used to print 1D plasmonic grating on top of a titanium dioxide (TiO2) slab waveguide, producing waveguide-plasmon polariton modes with superior 10 nm spectral line-width. Plasmon-induced hot electrons are confirmed via two-terminal current measurements with increased photoresponsivity under guiding conditions. The fabricated hybrid structure with Au/TiO2 heterojunction enhances photocatalytic processes like degradation of methyl orange (MO) dye molecules using the generated hot electrons. This simple colloidal printing technique demonstrated on silicon, glass, Au film, and naphthalenediimide polymer thus marks an important milestone for large-scale implementation in optoelectronic devices. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemTuning the Local Availability of VEGF within Glycosaminoglycan-Based Hydrogels to Modulate Vascular Endothelial Cell Morphogenesis(Weinheim : Wiley-VCH, 2020) Limasale, Yanuar Dwi Putra; Atallah, Passant; Werner, Carsten; Freudenberg, Uwe; Zimmermann, RalfIncorporation of sulfated glycosaminoglycans (GAGs) into cell-instructive polymer networks is shown to be instrumental in controlling the diffusivity and activity of growth factors. However, a subtle balance between local retention and release of the factors is needed to effectively direct cell fate decisions. To quantitatively unravel material characteristics governing these key features, the GAG content and the GAG sulfation pattern of star-shaped poly(ethylene glycol) (starPEG)–GAG hydrogels are herein tuned to control the local availability and bioactivity of GAG-affine vascular endothelial growth factor (VEGF165). Hydrogels containing varying concentrations of heparin or heparin derivatives with different sulfation pattern are prepared and thoroughly characterized for swelling, mechanical properties, and growth factor transport. Mathematical models are developed to predict the local concentration and spatial distribution of free and bound VEGF165 within the gel matrices. The results of simulation and experimental studies concordantly reveal how the GAG concentration and sulfation pattern determine the local availability of VEGF165 within the cell-instructive hydrogels and how the factor—in interplay with cell-instructive gel properties—determines the formation and spatial organization of capillary networks of embedded human vascular endothelial cells. Taken together, this study exemplifies how mathematical modeling and rational hydrogel design can be combined to pave the way for precision tissue engineering. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemExploiting Combinatorics to Investigate Plasmonic Properties in Heterogeneous Ag-Au Nanosphere Chain Assemblies(Weinheim : Wiley-VCH, 2021) Schletz, Daniel; Schultz, Johannes; Potapov, Pavel L.; Steiner, Anja Maria; Krehl, Jonas; König, Tobias A.F.; Mayer, Martin; Lubk, Axel; Fery, AndreasChains of coupled metallic nanoparticles are of special interest for plasmonic applications because they can sustain highly dispersive plasmon bands, allowing strong ballistic plasmon wave transport. Whereas early studies focused on homogeneous particle chains exhibiting only one dominant band, heterogeneous assemblies consisting of different nanoparticle species came into the spotlight recently. Their increased configuration space principally allows engineering multiple bands, bandgaps, or topological states. Simultaneously, the challenge of the precise arrangement of nanoparticles, including their distances and geometric patterns, as well as the precise characterization of the plasmonics in these systems, persists. Here, the surface plasmon resonances in heterogeneous Ag-Au nanoparticle chains are reported. Wrinkled templates are used for directed self-assembly of monodisperse gold and silver nanospheres as chains, which allows assembling statistical combinations of more than 109 particles. To reveal the spatial and spectral distribution of the plasmonic response, state-of-the-art scanning transmission electron microscopy coupled with electron energy loss spectroscopy accompanied by boundary element simulations is used. A variety of modes in the heterogeneous chains are found, ranging from localized surface plasmon modes occurring in single gold or silver spheres, respectively, to modes that result from the hybridization of the single particles. This approach opens a novel avenue toward combinatorial studies of plasmonic properties in heterosystems. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemMWCNT induced negative real permittivity in a copolyester of Bisphenol-A with terephthalic and isophthalic acids(Bristol : IOP Publ., 2020) Özdemir, Zeynep Güven; Daşdan, Dolunay Şakar; Kavak, Pelin; Pionteck, Jürgen; Pötschke, Petra; Voit, Brigitte; SüngüMısırlıoğlu, BanuIn the present study, the negative real permittivity behavior of a copolyester of bisphenol-A with terephthalic acid and isophthalic acid (PAr) containing 1.5 to 7.5 wt% multi-walled carbon nanotubes (MWCNTs) have been investigated in detail. The structural and morphological analysis of the melt-mixed composites was performed by Fourier transform infrared spectroscopy using attenuated total reflection (FTIR-ATR), atomic force microscopy (AFM), X-ray diffraction (XRD), and light microscopy. The influences of the MWCNT filler on the AC impedance, complex permittivity, and AC conductivity of the PAr polymer matrix were investigated at different operating temperatures varied between 296 K and 373 K. The transition from a negative to positive real permittivity was observed at different crossover frequencies depending on the MWCNT content of the composites whereas pure PAr showed positive values at all frequencies. The negative real permittivity characteristic of the composites was discussed in the context of Drude model. © 2020 The Author(s). Published by IOP Publishing Ltd.
- ItemA non-cytotoxic resin for micro-stereolithography for cell cultures of HUVECs(Basel : MDPI, 2020) Männel, Max J.; Fischer, Carolin; Thiele, JulianThree-dimensional (3D) printing of microfluidic devices continuously replaces conventional fabrication methods. A versatile tool for achieving microscopic feature sizes and short process times is micro-stereolithography (µSL). However, common resins for µSL lack biocompatibility and are cytotoxic. This work focuses on developing new photo-curable resins as a basis for µSL fabrication of polymer materials and surfaces for cell culture. Different acrylate-and methacrylate-based compositions are screened for material characteristics including wettability, surface roughness, and swelling behavior. For further understanding, the impact of photo-absorber and photo-initiator on the cytotoxicity of 3D-printed substrates is studied. Cell culture experiments with human umbilical vein endothelial cells (HUVECs) in standard polystyrene vessels are compared to 3D-printed parts made from our library of homemade resins. Among these, after optimizing material composition and post-processing, we identify selected mixtures of poly(ethylene glycol) diacrylate (PEGDA) and poly(ethylene glycol) methyl ethyl methacrylate (PEGMEMA) as most suitable to allow for fabricating cell culture platforms that retain both the viability and proliferation of HUVECs. Next, our PEGDA/PEGMEMA resins will be further optimized regarding minimal feature size and cell adhesion to fabricate microscopic (microfluidic) cell culture platforms, e.g., for studying vascularization of HUVECs in vitro. © 2020 by the authors.