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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
- ItemBiomaterial based strategies to reconstruct the nigrostriatal pathway in organotypic slice co-cultures(Amsterdam [u.a.] : Elsevier, 2021) Ucar, Buket; Kajtez, Janko; Foidl, Bettina M.; Eigel, Dimitri; Werner, Carsten; Long, Katherine R.; Emnéus, Jenny; Bizeau, Joëlle; Lomora, Mihai; Pandit, Abhay; Newland, Ben; Humpel, ChristianProtection or repair of the nigrostriatal pathway represents a principal disease-modifying therapeutic strategy for Parkinson's disease (PD). Glial cell line-derived neurotrophic factor (GDNF) holds great therapeutic potential for PD, but its efficacious delivery remains difficult. The aim of this study was to evaluate the potential of different biomaterials (hydrogels, microspheres, cryogels and microcontact printed surfaces) for reconstructing the nigrostriatal pathway in organotypic co-culture of ventral mesencephalon and dorsal striatum. The biomaterials (either alone or loaded with GDNF) were locally applied onto the brain co-slices and fiber growth between the co-slices was evaluated after three weeks in culture based on staining for tyrosine hydroxylase (TH). Collagen hydrogels loaded with GDNF slightly promoted the TH+ nerve fiber growth towards the dorsal striatum, while GDNF loaded microspheres embedded within the hydrogels did not provide an improvement. Cryogels alone or loaded with GDNF also enhanced TH+ fiber growth. Lines of GDNF immobilized onto the membrane inserts via microcontact printing also significantly improved TH+ fiber growth. In conclusion, this study shows that various biomaterials and tissue engineering techniques can be employed to regenerate the nigrostriatal pathway in organotypic brain slices. This comparison of techniques highlights the relative merits of different technologies that researchers can use/develop for neuronal regeneration strategies. © 2020
- 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
- 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
- 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
- ItemPolysulfide driven degradation in lithium–sulfur batteries during cycling – quantitative and high time-resolution operando X-ray absorption study for dissolved polysulfides probed at both electrode sides(London [u.a.] : RSC, 2021) Zech, Claudia; Hönicke, Philipp; Kayser, Yves; Risse, Sebastian; Grätz, Olga; Stamm, Manfred; Beckhoff, BurkhardThe development of operando characterization techniques on realistic batteries is essential for an advanced mechanistic understanding in battery chemistry and, therefore, contributes to their further performance improvement. This manuscript presents operando Near-Edge X-ray Absorption Spectroscopy (NEXAFS) traceable to the SI units (SI is the abbreviation for the International System of Units) during multiple charge–discharge cycles on both electrodes of lithium–sulfur (Li/S) coin cells which enables an absolute quantification of dissolved polysulfides with no need for calibration samples or reference material. We could reveal that during the charging process, polysulfide (PS) movement from the negative to the positive electrode is inhibited. This leads to a steady increase of dissolved polysulfides at the anode side and, therefore, is one of the key points for capacity fading. We quantitatively track the polysulfides dissolved in the electrolyte and correlate for the first time their evolution with the capacity fading of the cell. We analyze the appearance of PS during cell operation at the cathode and anode side to characterize the transport mechanisms of the polysulfide shuttle phenomena and to reveal quantitative information about their evolution at different states of charge and states of health. Our cell design suppresses the contribution of cathodic sulfur, which is mandatory for reference-sample-free quantification in X-ray spectrometry and allows us to use only slightly modified standard coin cell batteries.
- ItemComparison and uncertainty evaluation of two centrifugal separators for microplastic sampling(New York, NY [u.a.] : Science Direct, 2021) Hildebrandt, Lars; Zimmermann, Tristan; Primpke, Sebastian; Fischer, Dieter; Gerdts, Gunnar; Pröfrock, DanielFor commonly applied microplastic sampling approaches based on filtration, high throughput and no size-discrimination are conflicting goals. Therefore, we propose two efficient centrifugal separators for small microplastic sampling, namely the utilization of a hydrocyclone as well as a continuous flow centrifuge. Thorough method optimization was followed by application in an extensive sampling study to investigate the separators' retention behavior for particulate plastics from estuarine waters. Microplastic concentrations ranged from 193 to 2072 particles m-3. The most dominant identified polymer types were polypropylene, acrylates, polyvinyl chloride and polyethylene. More than 95% of particles were < 100 µm. For the first time in microplastic research, an expanded uncertainty was calculated according to the "Guide to the expression of Uncertainty in Measurement" (JCGM 100:2008). Bottom-up uncertainty evaluation revealed the different sampling methods (~ 44%), sample replicates (~ 26%) and the different detection techniques (~ 16%) as the major sources of uncertainty. Depending on the number of particles detected in the samples, the relative expanded uncertainty (Urel (k = 2)) ranged from 24% up to > 200% underpinning tremendous importance of sound uncertainty evaluation. Our results indicate that scientist should rethink many "observed patterns" in the literature due to being insignificant and herewith not real.
- ItemEnhancing sub-bandgap external quantum efficiency by photomultiplication for narrowband organic near-infrared photodetectors([London] : Nature Publishing Group UK, 2021) Kublitski, Jonas; Fischer, Axel; Xing, Shen; Baisinger, Lukasz; Bittrich, Eva; Spoltore, Donato; Benduhn, Johannes; Vandewal, Koen; Leo, KarlDetection of electromagnetic signals for applications such as health, product quality monitoring or astronomy requires highly responsive and wavelength selective devices. Photomultiplication-type organic photodetectors have been shown to achieve high quantum efficiencies mainly in the visible range. Much less research has been focused on realizing near-infrared narrowband devices. Here, we demonstrate fully vacuum-processed narrow- and broadband photomultiplication-type organic photodetectors. Devices are based on enhanced hole injection leading to a maximum external quantum efficiency of almost 2000% at −10 V for the broadband device. The photomultiplicative effect is also observed in the charge-transfer state absorption region. By making use of an optical cavity device architecture, we enhance the charge-transfer response and demonstrate a wavelength tunable narrowband photomultiplication-type organic photodetector with external quantum efficiencies superior to those of pin-devices. The presented concept can further improve the performance of photodetectors based on the absorption of charge-transfer states, which were so far limited by the low external quantum efficiency provided by these devices.
- ItemAn Improved Conservative Direct Re-Initialization Method (ICDR) for Two-Phase Flow Simulations(Basel ; Beijing ; Wuhan ; Barcelona ; Belgrade : MDPI, 2021) Mostafaiyan, Mehdi; Wießner, Sven; Heinrich, Gert; Hosseini, Mahdi SalamiWe introduce an improved conservative direct re-initialization (ICDR) method (for two-phase flow problems) as a new and efficient geometrical re-distancing scheme. The ICDR technique takes advantage of two mass-conserving and fast re-distancing schemes, as well as a global mass correction concept to reduce the extent of the mass loss/gain in two- and three-dimensional (2D and 3D) problems. We examine the ICDR method, at the first step, with two 2D benchmarks: the notched cylinder and the swirling flow vortex problems. To do so, we (for the first time) extensively analyze the dependency of the regenerated interface quality on both time-step and element sizes. Then, we quantitatively assess the results by employing a defined norm value, which evaluates the deviation from the exact solution. We also present a visual assessment by graphical demonstration of original and regenerated interfaces. In the next step, we investigate the performance of the ICDR in three-dimensional (3D) problems. For this purpose, we simulate drop deformation in a simple shear flow field. We describe our reason for this choice and show that, by employing the ICDR scheme, the results of our analysis comply with the existing numerical and experimental data in the literature
- ItemSelf-Replication of Deeply Buried Doped Silicon Structures, which Remotely Control the Etching Process: A New Method for Forming a Silicon Pattern from the Bottom Up(Weinheim : Wiley-VCH, 2021) Schutzeichel, Christopher; Kiriy, Nataliya; Kiriy, Anton; Voit, BrigitteA typical microstructuring process utilizes photolithographic masks to create arbitrary patterns on silicon substrates in a top-down approach. Herein, a new, bottom-up microstructuring method is reported, which enables the patterning of n-doped silicon substrates to be performed without the need for application of etch-masks or stencils during the etching process. Instead, the structuring process developed herein involves a simple alkaline etching performed under illumination and is remotely controlled by the p-doped micro-sized implants, buried beneath a homogeneous n-doped layer at depths of 0.25 to 1 µm. The microstructuring is realized because the buried implants act upon illumination as micro-sized photovoltaic cells, which generate a flux of electrons and increase the negative surface charge in areas above the implants. The locally increased surface charge causes a local protection of the native silicon oxide layer from alkaline etching, which ultimately leads to the microstructuring of the substrate. In this way, substrates having at their top a thick layer of homogeneously n-doped silicon can be structured, reducing the need for costly, time-consuming photolithography steps. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH