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    Background Reduction in STED-FCS Using a Bivortex Phase Mask
    (Washington, DC : ACS Publications, 2020) Barbotin, Aurélien; Urbančič, Iztok; Galiani, Silvia; Eggeling, Christian; Booth, Martin
    Fluorescence correlation spectroscopy (FCS) is a valuable tool to study the molecular dynamics in living cells. When used together with a super-resolution stimulated emission depletion (STED) microscope, STED-FCS can measure diffusion processes on the nanoscale in living cells. In two-dimensional (2D) systems like the cellular plasma membrane, a ring-shaped depletion focus is most commonly used to increase the lateral resolution, leading to more than 25-fold decrease in the observation volume, reaching the relevant scale of supramolecular arrangements. However, STED-FCS faces severe limitations when measuring diffusion in three dimensions (3D), largely due to the spurious background contributions from undepleted areas of the excitation focus that reduce the signal quality and ultimately limit the resolution. In this paper, we investigate how different STED confinement modes can mitigate this issue. By simulations as well as experiments with fluorescent probes in solution and in cells, we demonstrate that the coherent-hybrid (CH) depletion pattern created by a bivortex phase mask reduces background most efficiently and thus provides superior signal quality under comparable reduction of the observation volume. Featuring also the highest robustness to common optical aberrations, CH-STED can be considered the method of choice for reliable STED-FCS-based investigations of 3D diffusion on the subdiffraction scale. Copyright © 2020 American Chemical Society.
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    1D p–n Junction Electronic and Optoelectronic Devices from Transition Metal Dichalcogenide Lateral Heterostructures Grown by One-Pot Chemical Vapor Deposition Synthesis
    (Weinheim : Wiley-VCH, 2021) Najafidehaghani, Emad; Gan, Ziyang; George, Antony; Lehnert, Tibor; Ngo, Gia Quyet; Neumann, Christof; Bucher, Tobias; Staude, Isabelle; Kaiser, David; Vogl, Tobias; Hübner, Uwe; Kaiser, Ute; Eilenberger, Falk; Turchanin, Andrey
    Lateral heterostructures of dissimilar monolayer transition metal dichalcogenides provide great opportunities to build 1D in-plane p–n junctions for sub-nanometer thin low-power electronic, optoelectronic, optical, and sensing devices. Electronic and optoelectronic applications of such p–n junction devices fabricated using a scalable one-pot chemical vapor deposition process yielding MoSe2-WSe2 lateral heterostructures are reported here. The growth of the monolayer lateral heterostructures is achieved by in situ controlling the partial pressures of the oxide precursors by a two-step heating protocol. The grown lateral heterostructures are characterized structurally and optically using optical microscopy, Raman spectroscopy/microscopy, and photoluminescence spectroscopy/microscopy. High-resolution transmission electron microscopy further confirms the high-quality 1D boundary between MoSe2 and WSe2 in the lateral heterostructure. p–n junction devices are fabricated from these lateral heterostructures and their applicability as rectifiers, solar cells, self-powered photovoltaic photodetectors, ambipolar transistors, and electroluminescent light emitters are demonstrated. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    Photodoping and Fast Charge Extraction in Ionic Carbon Nitride Photoanodes
    (Weinheim : Wiley-VCH, 2021) Adler, Christiane; Selim, Shababa; Krivtsov, Igor; Li, Chunyu; Mitoraj, Dariusz; Dietzek, Benjamin; Durrant, James R.; Beranek, Radim
    Ionic carbon nitrides based on poly(heptazine imides) (PHI) represent a vigorously studied class of materials with possible applications in photocatalysis and energy storage. Herein, for the first time, the photogenerated charge dynamics in highly stable and binder-free PHI photoanodes using in operando transient photocurrents and spectroelectrochemical photoinduced absorption measurements is studied. It is discovered that light-induced accumulation of long-lived trapped electrons within the PHI film leads to effective photodoping of the PHI film, resulting in a significant improvement of photocurrent response due to more efficient electron transport. While photodoping is previously reported for various semiconductors, it has not been shown before for carbon nitride materials. Furthermore, it is found that the extraction kinetics of untrapped electrons are remarkably fast in these PHI photoanodes, with electron extraction times (ms) comparable to those measured for commonly employed metal oxide semiconductors. These results shed light on the excellent performance of PHI photoanodes in alcohol photoreforming, including very negative photocurrent onset, outstanding fill factor, and the possibility to operate under zero-bias conditions. More generally, the here reported photodoping effect and fast electron extraction in PHI photoanodes establish a strong rationale for the use of PHI films in various applications, such as bias-free photoelectrochemistry or photobatteries. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
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    Impact of rare earth doping on the luminescence of lanthanum aluminum silicate glasses for radiation sensing
    (Washington, DC : OSA, 2022) Shaw, Ruth E.; Kalnins, Christopher A. G.; Whittaker, Carly A.; Moffatt, Jillian E.; Tsiminis, Georgios; Klantsataya, Elizaveta; Ottaway, David; Spooner, Nigel A.; Litzkendorf, Doris; Matthes, Anne; Schwuchow, Anka; Wondraczek, Katrin; Ebendorff-Heidepriem, Heike
    Large core soft glass fibers have been demonstrated to be promising candidates as intrinsic fiber sensors for radiation detection and dosimetry applications. Doping with rare earth ions enhanced their radiation sensitivity. SiO2-Al2O3-La2O3 (SAL) glasses offer easy fabrication of large core fibers with high rare earth concentration and higher mechanical strength than soft glasses. This paper evaluates the suitability of the SAL glass type for radiation dosimetry based on optically stimulated luminescence (OSL) via a comprehensive investigation of the spectroscopic and dosimetric properties of undoped and differently rare earth doped bulk SAL glass samples. Due to the low intensity of the rare earth luminescence peaks in the 250–400 nm OSL detection range, the OSL response for all the SAL glasses is not caused by the rare earth ions but by radiation-induced defects that act as intrinsic centers for the recombination of electrons and holes produced by the ionizing radiation, trapped in fabrication induced defect centers, and then released via stimulation with 470 nm light. The rare earth ions interfere with these processes involving intrinsic centers. This dosimetric behavior of highly rare earth doped SAL glasses suggests that enhancement of OSL response requires lower rare earth concentrations and/or longer wavelength OSL detection range.
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    Noise Sources and Requirements for Confocal Raman Spectrometers in Biosensor Applications
    (Basel : MDPI, 2021) Jahn, Izabella J.; Grjasnow, Alexej; John, Henry; Weber, Karina; Popp, Jürgen; Hauswald, Walter
    Raman spectroscopy probes the biochemical composition of samples in a non-destructive, non-invasive and label-free fashion yielding specific information on a molecular level. Nevertheless, the Raman effect is very weak. The detection of all inelastically scattered photons with highest efficiency is therefore crucial as well as the identification of all noise sources present in the system. Here we provide a study for performance comparison and assessment of different spectrometers for confocal Raman spectroscopy in biosensor applications. A low-cost, home-built Raman spectrometer with a complementary metal-oxide-semiconductor (CMOS) camera, a middle price-class mini charge-coupled device (CCD) Raman spectrometer and a laboratory grade confocal Raman system with a deeply cooled CCD detector are compared. It is often overlooked that the sample itself is the most important “optical” component in a Raman spectrometer and its properties contribute most significantly to the signal-to-noise ratio. For this purpose, different representative samples: a crystalline silicon wafer, a polypropylene sample and E. coli bacteria were measured under similar conditions using the three confocal Raman spectrometers. We show that biosensor applications do not in every case profit from the most expensive equipment. Finally, a small Raman database of three different bacteria species is set up with the middle price-class mini CCD Raman spectrometer in order to demonstrate the potential of a compact setup for pathogen discrimination.
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    A wideband cryogenic microwave low-noise amplifier
    (Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2020) Ivanov, Boris I.; Volkhin, Dmitri I.; Novikov, Ilya L.; Pitsun, Dmitri K.; Moskalev, Dmitri O.; Rodionov, Ilya A.; Il'ichev, Evgeni; Vostretsov, Aleksey G.
    A broadband low-noise four-stage high-electron-mobility transistor amplifier was designed and characterized in a cryogen-free dilution refrigerator at the 3.8 K temperature stage. The obtained power dissipation of the amplifier is below 20 mW. In the frequency range from 6 to 12 GHz its gain exceeds 30 dB. The equivalent noise temperature of the amplifier is below 6 K for the presented frequency range. The amplifier is applicable for any type of cryogenic microwave measurements. As an example we demonstrate here the characterization of the superconducting X-mon qubit coupled to an on-chip coplanar waveguide resonator. ©2020 Ivanov et al.; licensee Beilstein-Institut.License and terms: see end of document.
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    Morphology and Microstructure Evolution of Gold Nanostructures in the Limited Volume Porous Matrices
    (Basel : MDPI, 2020) Yakimchuk, Dzmitry V.; Bundyukova, Victoria D.; Ustarroz, Jon; Terryn, Herman; Baert, Kitty; Kozlovskiy, Artem L.; Zdorovets, Maxim V.; Khubezhov, Soslan A.; Trukhanov, Alex V.; Trukhanov, Sergei V.; Panina, Larissa V.; Arzumanyan, Grigory M.; Mamatkulov, Kahramon Z.; Tishkevich, Daria I.; Kaniukov, Egor Y.; Sivakov, Vladimir
    The modern development of nanotechnology requires the discovery of simple approaches that ensure the controlled formation of functional nanostructures with a predetermined morphology. One of the simplest approaches is the self-assembly of nanostructures. The widespread implementation of self-assembly is limited by the complexity of controlled processes in a large volume where, due to the temperature, ion concentration, and other thermodynamics factors, local changes in diffusion-limited processes may occur, leading to unexpected nanostructure growth. The easiest ways to control the diffusion-limited processes are spatial limitation and localized growth of nanostructures in a porous matrix. In this paper, we propose to apply the method of controlled self-assembly of gold nanostructures in a limited pore volume of a silicon oxide matrix with submicron pore sizes. A detailed study of achieved gold nanostructures' morphology, microstructure, and surface composition at different formation stages is carried out to understand the peculiarities of realized nanostructures. Based on the obtained results, a mechanism for the growth of gold nanostructures in a limited volume, which can be used for the controlled formation of nanostructures with a predetermined geometry and composition, has been proposed. The results observed in the present study can be useful for the design of plasmonic-active surfaces for surface-enhanced Raman spectroscopy-based detection of ultra-low concentration of different chemical or biological analytes, where the size of the localized gold nanostructures is comparable with the spot area of the focused laser beam.
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    On the stability of microwave-fabricated SERS substrates - chemical and morphological considerations
    (Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2021) Wang, Limin; Womiloju, Aisha Adebola; Höppener, Christiane; Schubert, Ulrich Sigmar; Hoeppener, Stephanie
    The stability of surface-enhanced Raman spectroscopy (SERS) substrates in different organic solvents and different buffer solutions was investigated. SERS substrates were fabricated by a microwave-assisted synthesis approach and the morphological as well as chemical changes of the SERS substrates were studied. It was demonstrated that the SERS substrates treated with methanol, ethanol, or N,N-dimethylformamide (DMF) were comparable and showed overall good stability and did not show severe morphological changes or a strong decrease in their Raman activity. Toluene treatment resulted in a strong decrease in the Raman activity whereas dimethyl sulfoxide (DMSO) treatment completely preserved or even slightly improved the Raman enhancement capabilities. SERS substrates immersed into phosphate-buffered saline (PBS) solutions were observed to be rather instable in low and neutral pH buffer solutions. Other buffer systems showed less severe influences on the SERS activity of the substrates and a carbonate buffer at pH 10 was found to even improve SERS performance. This study represents a guideline on the stability of microwave-fabricated SERS substrates or other SERS substrates consisting of non-stabilized silver nanoparticles for the application of different organic solvents and buffer solutions.
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    Polarization-resolved second-harmonic generation imaging through a multimode fiber
    (Washington, DC : OSA, 2021) Cifuentes, Angel; Pikálek, Tomáš; Ondráčková, Petra; Amezcua-Correa, Rodrigo; Antonio-Lopez, José Enrique; Čižmár, Tomáš; Trägårdh, Johanna
    Multimode fiber-based endoscopes have recently emerged as a tool for minimally invasive endoscopy in tissue, at depths well beyond the reach of multiphoton imaging. Here, we demonstrate label-free second-harmonic generation (SHG) microscopy through such a fiber endoscope. We simultaneously fully control the excitation polarization state and the spatial distribution of the light at the fiber tip, and we use this to implement polarization-resolved SHG imaging, which allows imaging and identification of structural proteins such as collagen and myosin. We image mouse tail tendon and heart tissue, employing the endoscope at depths up to 1 mm, demonstrating that we can differentiate these structural proteins. This method has the potential for enabling instant and in situ diagnosis of tumors and fibrotic conditions in sensitive tissue with minimal damage.
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    Preparation, analysis, and application of coated glass targets for the Wendelstein 7-X laser blow-off system
    (Melville, NY : American Inst. of Physics, 2020) Wegner, Th.; Geiger, B.; Foest, R.; Jansen van Vuuren, A.; Winters, V. R.; Biedermann, C.; Burhenn, R.; Buttenschön, B.; Cseh, G.; Joda, I.; Kocsis, G.; Kunkel, F.; Quade, A.; Schäfer, J.; Schmitz, O.; Szepesi, T.
    Coated glass targets are a key component of the Wendelstein 7-X laser blow-off system that is used for impurity transport studies. The preparation and analysis of these glass targets as well as their performance is examined in this paper. The glass targets have a high laser damage threshold and are coated via physical vapor deposition with μm thick films. In addition, nm-thin layers of Ti are used as an interface layer for improved ablation efficiency and reduced coating stress. Hence, the metallic or ceramic coating has a lateral homogeneity within 2% and contaminants less than 5%, being optimal for laser ablation processing. With this method, a short (few ms) and well defined pulse of impurities with about 1017 particles can be injected close to the last closed flux surface of Wendelstein 7-X. In particular, a significant amount of atoms with a velocity of about 1 km/s enters the plasma within 1 ms. The atoms are followed by a negligible concentration of slower clusters and macro-particles. This qualifies the use of the targets and applied laser settings for impurity transport studies with the laser blow-off system in Wendelstein 7-X. © 2020 Author(s).