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- ItemSelf-Regenerating Soft Biophotovoltaic Devices(Washington, DC : ACS Publications, 2018) Qiu, Xinkai; Castañeda Ocampo, Olga; de Vries, Hendrik W.; van Putten, Maikel; Loznik, Mark; Herrmann, Andreas; Chiechi, Ryan C.This paper describes the fabrication of soft, stretchable biophotovoltaic devices that generate photocurrent from photosystem I (PSI) complexes that are self-assembled onto Au electrodes with a preferred orientation. Charge is collected by the direct injection of electrons into the Au electrode and the transport of holes through a redox couple to liquid eutectic gallium-indium (EGaIn) electrodes that are confined to microfluidic pseudochannels by arrays of posts. The pseudochannels are defined in a single fabrication step that leverages the non-Newtonian rheology of EGaIn. This strategy is extended to the fabrication of reticulated electrodes that are inherently stretchable. A simple shadow evaporation technique is used to increase the surface area of the Au electrodes by a factor of approximately 106 compared to planar electrodes. The power conversion efficiency of the biophotovoltaic devices decreases over time, presumably as the PSI complexes denature and/or detach from the Au electrodes. However, by circulating a solution of active PSI complexes the devices self-regenerate by mass action/self-assembly. These devices leverage simple fabrication techniques to produce complex function and prove that photovoltaic devices comprising PSI can retain the ability to regenerate, one of the most important functions of photosynthetic organisms. © 2018 American Chemical Society.
- ItemSeeded Growth Synthesis of Gold Nanotriangles: Size Control, SAXS Analysis, and SERS Performance(Washington, DC : Soc., 2018) Kuttner, Christian; Mayer, Martin; Dulle, Martin; Moscoso, Ana; López-Romero, Juan Manuel; Förster, Stephan; Fery, Andreas; Pérez-Juste, Jorge; Contreras-Cáceres, RafaelWe studied the controlled growth of triangular prismatic Au nanoparticles with different beveled sides for surface-enhanced Raman spectroscopy (SERS) applications. First, in a seedless synthesis using 3-butenoic acid (3BA) and benzyldimethylammonium chloride (BDAC), gold nanotriangles (AuNTs) were synthesized in a mixture with gold nanooctahedra (AuNOCs) and separated by depletion-induced flocculation. Here, the influence of temperature, pH, and reducing agent on the reaction kinetics was initially investigated by UV–vis and correlated to the size and yield of AuNT seeds. In a second step, the AuNT size was increased by seed-mediated overgrowth with Au. We show for the first time that preformed 3BA-synthesized AuNT seeds can be overgrown up to a final edge length of 175 nm and a thickness of 80 nm while maintaining their triangular shape and tip sharpness. The NT morphology, including edge length, thickness, and tip rounding, was precisely characterized in dispersion by small-angle X-ray scattering and in dry state by transmission electron microscopy and field-emission scanning electron microscopy. For sensor purposes, we studied the size-dependent SERS performance of AuNTs yielding analytical enhancement factors between 0.9 × 104 and 5.6 × 104 and nanomolar limit of detection (10–8–10–9 M) for 4-mercaptobenzoic acid and BDAC. These results confirm that the 3BA approach allows the fabrication of AuNTs in a whole range of sizes maintaining the NT morphology. This enables tailoring of localized surface plasmon resonances between 590 and 740 nm, even in the near-infrared window of a biological tissue, for use as colloidal SERS sensing agents or for optoelectronic applications.
- ItemStatistical Analysis of Scanning Fluorescence Correlation Spectroscopy Data Differentiates Free from Hindered Diffusion(Washington, DC : Soc., 2018-7-20) Schneider, Falk; Waithe, Dominic; Lagerholm, B. Christoffer; Shrestha, Dilip; Sezgin, Erdinc; Eggeling, Christian; Fritzsche, MarcoCells rely on versatile diffusion dynamics in their plasma membrane. Quantification of this often heterogeneous diffusion is essential to the understanding of cell regulation and function. Yet such measurements remain a major challenge in cell biology, usually due to low sampling throughput, a necessity for dedicated equipment, sophisticated fluorescent label strategies, and limited sensitivity. Here, we introduce a robust, broadly applicable statistical analysis pipeline for large scanning fluorescence correlation spectroscopy data sets, which uncovers the nanoscale heterogeneity of the plasma membrane in living cells by differentiating free from hindered diffusion modes of fluorescent lipid and protein analogues.
- ItemStructural and mechanical characterization of heterogeneities in a CuZr-based bulk metallic glass processed by high pressure torsion(Amsterdam [u.a.] : Elsevier Science, 2018) Ebner, Christian; Escher, Benjamin; Gammer, Christoph; Eckert, Jürgen; Pauly, Simon; Rentenberger, ChristianCu45Zr45Al5Ag5 bulk metallic glass samples, processed by high pressure torsion (HPT) under various conditions, were characterized using synchrotron X-ray diffraction, nanoindentation, differential scanning calorimetry, atomic force and transmission electron microscopy. The experimental results clearly show that HPT modifies the amorphous structure by increasing the mean atomic volume. The level of rejuvenation, correlated with the excess mean atomic volume, is enhanced at higher shear strains as inferred from relaxation enthalpies. By mapping of structural and mechanical quantities, the strain-induced rejuvenated state is characterized on cross-sectional HPT samples on a local scale. A clear correlation both between elastic and plastic softening and between softening and excess mean atomic volume is obtained. But also the heterogeneity of the HPT induced rejuvenation is revealed, resulting in the formation of highly strain-softened regions next to less-deformed ones. A hardness drop of up to 20% is associated with an estimated increase of the mean atomic volume of up to 0.75%. Based on synchrotron X-ray diffraction and nanoindentation measurements it is concluded that elastic fluctuations are enhanced in the rejuvenated material on different length scales down to atomic scale. Furthermore, the calculated flexibility volume and the corresponding average mean square atomic displacement is increased. The plastic response during nanoindentation indicates that HPT processing promotes a more homogeneous-like deformation.
- ItemApplication of the transferred matrix method to a unified evaluation of the cathodic electron emission(New York, NY : American Inst. of Physics, 2018) Baeva, M.The work is concerned with the Transfer Matrix Method for solving the steady-state Schrödinger equation applied for a unified evaluation of the emission current density from non-refractory cathodes. The method is applicable to arbitrary shapes of the potential barrier and its transmission probability is obtained without any analytical approximations. The Fermi-Dirac distribution for the free electrons in the metal is considered as a supply function. The results, obtained for a work function of the cathode material of 4.5 eV over a wide range of values of the surface temperature and the electric field strength, clearly show a growing deviation from those obtained by the classical Jeffreys-Wentzel-Kramers-Brillouin approximation with the increase of the electric field strength. Preliminary results are obtained to demonstrate the applicability of the Transfer Matrix method to the evaluation of the ion-assisted electron emission. A significant local enhancement of the emission current density is obtained as a result of the presence of an ion at a fixed position near the metal surface. The effect becomes very strongly pronounced at an appropriate value of the electric field strength, for which a resonant ion contribution appears.
- ItemHigh-resolution vertical velocities and their power spectrum observed with the MAARSY radar – Part 1: frequency spectrum(Katlenburg, Lindau : Copernicus, 2018-4-3) Li, Qiang; Rapp, Markus; Stober, Gunter; Latteck, RalphThe Middle Atmosphere Alomar Radar System (MAARSY) installed at the island of Andøya has been run for continuous probing of atmospheric winds in the upper troposphere and lower stratosphere (UTLS) region. In the current study, we present high-resolution wind measurements during the period between 2010 and 2013 with MAARSY. The spectral analysis applying the Lomb–Scargle periodogram method has been carried out to determine the frequency spectra of vertical wind velocity. From a total of 522 days of observations, the statistics of the spectral slope have been derived and show a dependence on the background wind conditions. It is a general feature that the observed spectra of vertical velocity during active periods (with wind velocity > 10 m s−1) are much steeper than during quiet periods (with wind velocity < 10 m s−1). The distribution of spectral slopes is roughly symmetric with a maximum at −5/3 during active periods, whereas a very asymmetric distribution with a maximum at around −1 is observed during quiet periods. The slope profiles along altitudes reveal a significant height dependence for both conditions, i.e., the spectra become shallower with increasing altitudes in the upper troposphere and maintain roughly a constant slope in the lower stratosphere. With both wind conditions considered together the general spectra are obtained and their slopes are compared with the background horizontal winds. The comparisons show that the observed spectra become steeper with increasing wind velocities under quiet conditions, approach a spectral slope of −5/3 at a wind velocity of 10 m s−1 and then roughly maintain this slope (−5/3) for even stronger winds. Our findings show an overall agreement with previous studies; furthermore, they provide a more complete climatology of frequency spectra of vertical wind velocities under different wind conditions.
- ItemUltrahigh Power Factor in Thermoelectric System Nb0.95M0.05FeSb (M = Hf, Zr, and Ti)(Chichester : John Wiley and Sons Ltd, 2018) Ren, W.; Zhu, H.; Zhu, Q.; Saparamadu, U.; He, R.; Liu, Z.; Mao, J.; Wang, C.; Nielsch, K.; Wang, Z.; Ren, Z.Conversion efficiency and output power are crucial parameters for thermoelectric power generation that highly rely on figure of merit ZT and power factor (PF), respectively. Therefore, the synergistic optimization of electrical and thermal properties is imperative instead of optimizing just ZT by thermal conductivity reduction or just PF by electron transport enhancement. Here, it is demonstrated that Nb0.95Hf0.05FeSb has not only ultrahigh PF over ≈100 µW cm−1 K−2 at room temperature but also the highest ZT in a material system Nb0.95M0.05FeSb (M = Hf, Zr, Ti). It is found that Hf dopant is capable to simultaneously supply carriers for mobility optimization and introduce atomic disorder for reducing lattice thermal conductivity. As a result, Nb0.95Hf0.05FeSb distinguishes itself from other outstanding NbFeSb-based materials in both the PF and ZT. Additionally, a large output power density of ≈21.6 W cm−2 is achieved based on a single-leg device under a temperature difference of ≈560 K, showing the realistic prospect of the ultrahigh PF for power generation.
- ItemAssessment of climate change and associated impact on selected sectors in Poland(Warsaw : De Gruyter Open, 2018) Kundzewicz, Zbigniew W.; Piniewski, Mikołaj; Mezghani, Abdelkader; Okruszko, Tomasz; Pińskwar, Iwona; Kardel, Ignacy; Hov, Øystein; Szcześniak, Mateusz; Szwed, Małgorzata; Benestad, Rasmus E.; Marcinkowski, Paweł; Graczyk, Dariusz; Dobler, Andreas; Førland, Eirik J.; O’Keefe, Joanna; Choryński, Adam; Parding, Kajsa M.; Haugen, Jan ErikThe present paper offers a brief assessment of climate change and associated impact in Poland, based on selected results of the Polish–Norwegian CHASE-PL project. Impacts are examined in selected sectors, such as water resources, natural hazard risk reduction, environment, agriculture and health. Results of change detection in long time series of observed climate and climate impact variables in Poland are presented. Also, projections of climate variability and change are provided for time horizons of 2021–2050 and 2071–2100 for two emission scenarios, RCP4.5 and RCP8.5 in comparison with control period, 1971–2000. Based on climate projections, examination of future impacts on sectors is also carried out. Selected uncertainty issues relevant to observations, understanding and projections are tackled as well.
- ItemSynthesis and crystallographic characterization of [2,2-bis(η5-pentamethylcyclopentadienyl)-3,4-bis(trimethylsilyl)-2-zirconafuran-5-one-κO5]triisobutylaluminium(Chester : International Union of Crystallography, 2018-3-27) Burlakov, Vladimir V.; Bogdanov, Vyacheslav S.; Arndt, Perdita; Spannenberg, Anke; Rosenthal, Uwe; Beweries, Torsten; Shur, Vladimir B.The crystal structure of the title zwitterionic zirconocene complex containing a furanone unit, [AlZr(C10H15)2(C4H9)3(C9H18O2Si2)], is reported. On reacting a zirconafuranone with two equivalents of HAl(i-Bu)2, disproportionation of the Lewis acid results in the formation of a triisobutylaluminium fragment, Al(i-Bu)3, which coordinates to the exocyclic carbonyl O atom of the zirconafuranone ring. Single-crystal X-ray diffraction reveals that the zirconafuranone ring remains intact with coordination of the aluminium to the exocyclic O atom. One of the i-butyl groups is disordered over two sets of sites, with an occupancy ratio of 0.731 (3):0.269 (3).
- ItemTwo new magnetic cataclysmic variables discovered in the 3XMM catalogue(Les Ulis : EDP Sciences, 2018) Webb, N.A.; Schwope, A.; Zolotukhin, I.; Lin, D.; Rosen, S.R.Context. X-ray catalogues provide a wealth of information on many source types, ranging from compact objects to galaxies, clusters of galaxies, stars, and even planets. Thanks to the huge volume of X-ray sources provided in the 3XMM catalogue, along with many source specific products, many new examples from rare classes of sources can be identified. Aims. Through visualising spectra and lightcurves from about 80 observations included in the incremental part of the 3XMM catalogue, 3XMM-DR5, as part of the quality control of the catalogue, we identified two new X-ray sources, 3XMM J183333.1+225136 and 3XMM J184916.1+652943, that were highly variable. This work aims to investigate their nature. Methods. Through simple model fitting of the X-ray spectra and analysis of the X-ray lightcurves of 3XMM J183333.1+225136 and 3XMM J184916.1+652943, along with complementary photometry from the XMM-Newton Optical Monitor, Pan-STARRS and the Stella/WiFSIP and Large Binocular Telescope (LBT) spectra, we suggest that the two sources might be magnetic cataclysmic variables (CVs) of the polar type and we determine some of their properties. Results. Both CVs have very hard spectra, showing no soft excess. They are both situated in the local neighbourhood, located within ∼1 kpc. 3XMM J183333.1+225136 has an orbital period of 2.15 h. It shows features in the lightcurve that may be a total eclipse of the white dwarf. 3XMM J184916.1+652943 has an orbital period of 1.6 h. Given that only a small sky area was searched to identify these CVs, future sensitive all sky surveys such as the eROSITA project should be very successful at uncovering large numbers of such sources.