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DDC: 660 × Type: article × WGL Institute: IPHT ×

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Now showing 1 - 10 of 23
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    Excited-State Dynamics in Borylated Arylisoquinoline Complexes in Solution and in cellulo
    (Weinheim : Wiley-VCH, 2023) Yang, Tingxiang; Valavalkar, Abha; Romero‐Arenas, Antonio; Dasgupta, Anindita; Then, Patrick; Chettri, Avinash; Eggeling, Christian; Ros, Abel; Pischel, Uwe; Dietzek‐Ivanšić, Benjamin
    Two four-coordinate organoboron N,C-chelate complexes with different functional terminals on the PEG chains are studied with respect to their photophysical properties within human MCF-7 cells. Their excited-state properties are characterized by time-resolved pump-probe spectroscopy and fluorescence lifetime microscopy. The excited-state relaxation dynamics of the two complexes are similar when studied in DMSO. Aggregation of the complexes with the carboxylate terminal group is observed in water. When studying the light-driven excited-state dynamics of both complexes in cellulo, i. e., after being taken up into human MCF-7 cells, both complexes show different features depending on the nature of the anchoring PEG chains. The lifetime of a characteristic intramolecular charge-transfer state is significantly shorter when studied in cellulo (360±170 ps) as compared to in DMSO (∼960 ps) at 600 nm for the complexes with an amino group. However, the kinetics of the complexes with the carboxylate group are in line with those recorded in DMSO. On the other hand, the lifetimes of the fluorescent state are almost identical for both complexes in cellulo. These findings underline the importance to evaluate the excited-state properties of fluorophores in a complex biological environment in order to fully account for intra- and intermolecular effects governing the light-induced processes in functional dyes.
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    Towards on-site testing of Phytophthora species
    (Cambridge : RSC Publ., 2014) Schwenkbier, Lydia; Pollok, Sibyll; König, Stephan; Urban, Matthias; Werres, Sabine; Cialla-May, Dana; Weber, Karina; Popp, Jürgen
    Rapid detection and accurate identification of plant pathogens in the field is an ongoing challenge. In this study, we report for the first time on the development of a helicase-dependent isothermal amplification (HDA) in combination with on-chip hybridization for the detection of selected Phytophthora species. The HDA approach allows efficient amplification of the yeast GTP-binding protein (Ypt1) target gene region at one constant temperature in a miniaturized heating device. The assay's specificity was determined by on-chip DNA hybridization and subsequent silver nanoparticle deposition. The silver deposits serve as stable endpoint signals that enable the visual as well as the electrical readout. Our promising results point to the direction of a near future on-site application of the combined techniques for a reliable detection of Phytophthora species.
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    Shape-Memory Metallopolymers Based on Two Orthogonal Metal–Ligand Interactions
    (Weinheim : Wiley-VCH, 2021) Meurer, Josefine; Hniopek, Julian; Bätz, Thomas; Zechel, Stefan; Enke, Marcel; Vitz, Jürgen; Schmitt, Michael; Popp, Jürgen; Hager, Martin D.; Schubert, Ulrich S.
    A new shape-memory polymer is presented, in which both the stable phase as well as the switching unit consist of two different metal complexes. Suitable metal ions, which simultaneously form labile complexes with histidine and stable ones with terpyridine ligands, are identified via isothermal titration calorimetry (ITC) measurements. Different copolymers are synthesized, which contain butyl methacrylate as the main monomer and the metal-binding ligands in the side chains. Zn(TFMS)2 and NiCl2 are utilized for the dual crosslinking, resulting in the formation of metallopolymer networks. The switching temperature can simply be tuned by changing the composition as well as by the choice of the metal ion. Strain fixity rates (about 99%) and very high strain recovery rates (up to 95%) are achieved and the mechanism is revealed using different techniques such as Raman spectroscopy. © 2021 The Authors. Advanced Materials published by Wiley-VCH GmbH
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    1,7,9,10-Tetrasubstituted PMIs Accessible through Decarboxylative Bromination: Synthesis, Characterization, Photophysical Studies, and Hydrogen Evolution Catalysis
    (Weinheim : Wiley-VCH, 2020) Costabel, Daniel; Skabeev, Artem; Nabiyan, Afshin; Luo, Yusen; Max, Johannes B.; Rajagopal, Ashwene; Kowalczyk, Daniel; Dietzek, Benjamin; Wächtler, Maria; Görls, Helmar; Ziegenbalg, Dirk; Zagranyarski, Yulian; Streb, Carsten; Schacher, Felix H.; Peneva, Kalina
    In this work, we present a new synthetic strategy for fourfold-substituted perylene monoimides via tetrabrominated perylene monoanhydrides. X-ray diffraction analysis unveiled the intramolecular stacking orientation between the substituents and semicircular packing behavior. We observed the remarkable influence of the substituent on the longevity and nature of the excited state upon visible light excitation. In the presence of poly(dehydroalanine)-graft-poly(ethylene glycol) graft copolymers as solubilizing template, the chromophores are capable of sensitizing [Mo3S13]2− clusters in aqueous solution for stable visible light driven hydrogen evolution over three days. © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH
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    Nanoparticles Can Wrap Epithelial Cell Membranes and Relocate Them Across the Epithelial Cell Layer
    (Washington, DC : ACS Publ., 2018-7-24) Urbančič, Iztok; Garvas, Maja; Kokot, Boštjan; Majaron, Hana; Umek, Polona; Cassidy, Hilary; Škarabot, Miha; Schneider, Falk; Galiani, Silvia; Arsov, Zoran; Koklic, Tilen; Matallanas, David; Čeh, Miran; Muševič, Igor; Eggeling, Christian; Štrancar, Janez
    Although the link between the inhalation of nanoparticles and cardiovascular disease is well established, the causal pathway between nanoparticle exposure and increased activity of blood coagulation factors remains unexplained. To initiate coagulation tissue factor bearing epithelial cell membranes should be exposed to blood, on the other side of the less than a micrometre thin air-blood barrier. For the inhaled nanoparticles to promote coagulation, they need to bind lung epithelial-cell membrane parts and relocate them into the blood. To assess this hypothesis, we use advanced microscopy and spectroscopy techniques to show that the nanoparticles wrap themselves with epithelial-cell membranes, leading to the membrane’s disruption. The membrane-wrapped nanoparticles are then observed to freely diffuse across the damaged epithelial cell layer relocating epithelial cell membrane parts over the epithelial layer. Proteomic analysis of the protein content in the nanoparticles wraps/corona finally reveals the presence of the coagulation-initiating factors, supporting the proposed causal link between the inhalation of nanoparticles and cardiovascular disease.
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    Comparison of novel semi-airborne electromagnetic data with multi-scale geophysical, petrophysical and geological data from Schleiz, Germany
    (Amsterdam [u.a.] : Elsevier Science, 2020) Steuer, Annika; Smirnova, Maria; Becken, Michael; Schiffler, Markus; Günther, Thomas; Rochlitz, Raphael; Yogeshwar, Pritam; Mörbe, Wiebke; Siemon, Bernhard; Costabel, Stephan; Preugschat, Benedikt; Ibs-von Seht, Malte; Zampa, Luigi Sante; Müller, Franz
    In the framework of the Deep Electromagnetic Sounding for Mineral EXploration (DESMEX) project, we carried out multiple geophysical surveys from regional to local scales in a former mining area in the state of Thuringia, Germany. We prove the applicability of newly developed semi-airborne electromagnetic (EM) systems for mineral exploration by cross-validating inversion results with those of established airborne and ground-based investigation techniques. In addition, supporting petrophysical and geological information to our geophysical measurements allowed the synthesis of all datasets over multiple scales. An initial regional-scale reconnaissance survey was performed with BGR's standard helicopter-borne geophysical system deployed with frequency-domain electromagnetic (HEM), magnetic and radiometric sensors. In addition to geological considerations, the HEM results served as base-line information for the selection of an optimal location for the intermediate-scale semi-airborne EM experiments. The semi-airborne surveys utilized long grounded transmitters and two independent airborne receiver instruments: induction coil magnetometers and SQUID sensors. Due to the limited investigation depth of the HEM method, local-scale electrical resistivity tomography (ERT) and long-offset transient electromagnetic (LOTEM) measurements were carried out on a reference profile, enabling the validation of inversion results at greater depths. The comparison of all inversion results provided a consistent overall resistivity distribution. It further confirmed that both semi-airborne receiver instruments achieve the bandwidth and sensitivity required for the investigation of the resistivity structure down to 1 km depth and therewith the detection of deeply seated earth resources. A 3D geological model, lithological and geophysical borehole logs as well as petrophysical investigations were integrated to interpret of the geophysical results. Distinct highly-conductive anomalies with resistivities of less than 10 Om were identified as alum shales over all scales. Apart from that, the petrophysical investigations exhibited that correlating geophysical and geological information using only one single parameter, such as the electrical resistivity, is hardly possible. Therefore, we developed a first approach based on clustering methods and self-organizing maps (SOMs) that allowed us to assign geological units at the surface to a given combination of geophysical and petrophysical parameters, obtained on different scales. © 2020 The Authors
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    Plasticity, crack initiation and defect resistance in alkali-borosilicate glasses: From normal to anomalous behavior
    (Amsterdam [u.a.] : Elsevier Science, 2015) Limbach, R.; Winterstein-Beckmann, A.; Dellith, J.; Möncke, D.; Wondraczek, L.
    We provide a comprehensive description of the defect tolerance of sodium-borosilicate glasses upon sharp contact loading. This is motivated by the key role which is taken by this particular glass system in a wide variety of applications, ranging from electronic substrates, display covers and substrates for biomedical imaging and sensing to, e.g., radioactive waste vitrification. The present report covers the mechanical properties of glasses in the Na2O–B2O3–SiO2 ternary over the broad range of compositions from pure SiO2 to binary sodium-borates, and crossing the regions of various commercially relevant specialty borosilicate glasses, such as the multi-component Duran-, Pyrex- and BK7-type compositions and typical soda-lime silicate glasses, which are also included in this study. In terms of structure, the considered glasses may be separated into two groups, that is, one series which contains only bridging oxygen atoms, and another series which is designed with an increasing number of non-bridging oxygen ions. Elastic moduli, Poisson ratio, hardness as well as creep and crack resistance were evaluated, as well as the contribution of densification to the overall amount of indentation deformation. Correlations between the mechanical properties and structural characteristics of near- and mid-range order are discussed, from which we obtain a mechanistic view at the molecular reactions which govern the overall deformation reaction and, ultimately, contact cracking.
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    Comparative Analysis of Raman Signal Amplifying Effectiveness of Silver Nanostructures with Different Morphology
    (Basel : MDPI, 2022) Yakimchuk, Dzmitry V.; Khubezhov, Soslan A.; Prigodich, Uladzislau V.; Tishkevich, Daria I.; Trukhanov, Sergei V.; Trukhanov, Alex V.; Sivakov, Vladimir; Kaniukov, Egor Y.
    To increase the attractiveness of the practical application of molecular sensing methods, the experimental search for the optimal shape of silver nanostructures allowing to increase the Raman cross section by several orders of magnitude is of great interest. This paper presents a detailed study of spatially separated plasmon-active silver nanostructures grown in SiO2/Si template pores with crystallite, dendrite, and “sunflower-like” nanostructures shapes. Nile blue and 2-mercaptobenzothiazole were chosen as the model analytes for comparative evaluation of the Raman signal amplification efficiency using these structures. It was discussed the features of the structures for the enhancement of Raman intensity. Finally, we showed that silver crystals, dendrites, and “sunflower-like” nanostructures in SiO2/Si template could be used as the relevant materials for Raman signal amplification, but with different efficiency.
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    Giant persistent photoconductivity in monolayer MoS2 field-effect transistors
    (London : Nature Publishing Group, 2021) George, A.; Fistul, M.V.; Gruenewald, M.; Kaiser, D.; Lehnert, T.; Mupparapu, R.; Neumann, C.; Hübner, U.; Schaal, M.; Masurkar, N.; Arava, L.M.R.; Staude, I.; Kaiser, U.; Fritz, T.; Turchanin, A.
    Monolayer transition metal dichalcogenides (TMD) have numerous potential applications in ultrathin electronics and photonics. The exposure of TMD-based devices to light generates photo-carriers resulting in an enhanced conductivity, which can be effectively used, e.g., in photodetectors. If the photo-enhanced conductivity persists after removal of the irradiation, the effect is known as persistent photoconductivity (PPC). Here we show that ultraviolet light (λ = 365 nm) exposure induces an extremely long-living giant PPC (GPPC) in monolayer MoS2 (ML-MoS2) field-effect transistors (FET) with a time constant of ~30 days. Furthermore, this effect leads to a large enhancement of the conductivity up to a factor of 107. In contrast to previous studies in which the origin of the PPC was attributed to extrinsic reasons such as trapped charges in the substrate or adsorbates, we show that the GPPC arises mainly from the intrinsic properties of ML-MoS2 such as lattice defects that induce a large number of localized states in the forbidden gap. This finding is supported by a detailed experimental and theoretical study of the electric transport in TMD based FETs as well as by characterization of ML-MoS2 with scanning tunneling spectroscopy, high-resolution transmission electron microscopy, and photoluminescence measurements. The obtained results provide a basis for the defect-based engineering of the electronic and optical properties of TMDs for device applications.
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    Photophysics of Anionic Bis(4H-imidazolato)CuI Complexes
    (Weinheim : Wiley-VCH, 2022) Seidler, Bianca; Tran, Jens H.; Hniopek, Julian; Traber, Philipp; Görls, Helmar; Gräfe, Stefanie; Schmitt, Michael; Popp, Jürgen; Schulz, Martin; Dietzek‐Ivanšić, Benjamin
    In this paper, the photophysical behavior of four panchromatically absorbing, homoleptic bis(4H-imidazolato)CuI complexes, with a systematic variation in the electron-withdrawing properties of the imidazolate ligand, were studied by wavelength-dependent time-resolved femtosecond transient absorption spectroscopy. Excitation at 400, 480, and 630 nm populates metal-to-ligand charge transfer, intraligand charge transfer, and mixed-character singlet states. The pump wavelength-dependent transient absorption data were analyzed by a recently established 2D correlation approach. Data analysis revealed that all excitation conditions yield similar excited-state dynamics. Key to the excited-state relaxation is fast, sub-picosecond pseudo-Jahn-Teller distortion, which is accompanied by the relocalization of electron density onto a single ligand from the initially delocalized state at Franck-Condon geometry. Subsequent intersystem crossing to the triplet manifold is followed by a sub-100 ps decay to the ground state. The fast, nonradiative decay is rationalized by the low triplet-state energy as found by DFT calculations, which suggest perspective treatment at the strong coupling limit of the energy gap law.