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Chen, Zupeng ; Savateev, Aleksandr ; Pronkin, Sergey ; Papaefthimiou, Vasiliki ; Wolff, Christian Michael ; Willinger, Marc Georg ; Willinger, Elena ; Neher, Dieter ; Antonietti, Markus ; Dontsova, Dariya
Cost-efficient, visible-light-driven hydrogen production from water is an attractive potential source of clean, sustainable fuel. Here, it is shown that thermal solid state reactions of traditional carbon nitride precursors (cyanamide, melamine) with NaCl, KCl, or CsCl are a cheap and straightforward way to prepare poly(heptazine imide) alkali metal salts, whose thermodynamic stability decreases upon the increase of the metal atom size. The chemical structure of the prepared salts is confirmed by the results of X-ray photoelectron and infrared spectroscopies, powder X-ray diffraction and electron microscopy studies, and, in the case of sodium poly(heptazine imide), additionally by atomic pair distribution function analysis and 2D powder X-ray diffraction pattern simulations. In contrast, reactions with LiCl yield thermodynamically stable poly(triazine imides). Owing to the metastability and high structural order, the obtained heptazine imide salts are found to be highly active photo-catalysts in Rhodamine B and 4-chlorophenol degradation, and Pt-assisted sacrificial water reduction reactions under visible light irradiation. The measured hydrogen evolution rates are up to four times higher than those provided by a benchmark photocatalyst, mesoporous graphitic carbon nitride. Moreover, the products are able to photocatalytically reduce water with considerable reaction rates, even when glycerol is used as a sacrificial hole scavenger.
Ran, Niva A. ; Roland, Steffen ; Love, John A. ; Savikhin, Victoria ; Takacs, Christopher J. ; Fu, Yao-Tsung ; Li, Hong ; Coropceanu, Veaceslav ; Liu, Xiaofeng ; Bredas, Jean-Luc ; Bazan, Guillermo C. ; Toney, Michael F. ; Neher, Dieter ; Thuc-Quyen Nguyen
A long standing question in organic electronics concerns the effects of molecular orientation at donor/acceptor heterojunctions. Given a well-controlled donor/acceptor bilayer system, we uncover the genuine effects of molecular orientation on charge generation and recombination. These effects are studied through the point of view of photovoltaics-however, the results have important implications on the operation of all optoelectronic devices with donor/ acceptor interfaces, such as light emitting diodes and photodetectors. Our findings can be summarized by two points. First, devices with donor molecules face-on to the acceptor interface have a higher charge transfer state energy and less non-radiative recombination, resulting in larger open-circuit voltages and higher radiative efficiencies. Second, devices with donor molecules edge-on to the acceptor interface are more efficient at charge generation, attributed to smaller electronic coupling between the charge transfer states and the ground state, and lower activation energy for charge generation.
Ortiz-Amezcua, Pablo ; Guerrero-Rascado, Juan Luis ; Jose Granados-Munoz, Maria ; Benavent-Oltra, Jose Antonio ; Böckmann, Christine ; Samaras, Stefanos ; Stachlewska, Iwona Sylwia ; Janicka, Lucja ; Baars, Holger ; Bohlmann, Stephanie ; Alados-Arboledas, Lucas
Strong events of long-range transported biomass burning aerosol were detected during July 2013 at three EARLINET (European Aerosol Research Lidar Network) stations, namely Granada (Spain), Leipzig (Germany) and Warsaw (Poland). Satellite observations from MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instruments, as well as modeling tools such as HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) and NAAPS (Navy Aerosol Analysis and Prediction System), have been used to estimate the sources and transport paths of those North American forest fire smoke particles. A multiwavelength Raman lidar technique was applied to obtain vertically resolved particle optical properties, and further inversion of those properties with a regularization algorithm allowed for retrieving microphysical information on the studied particles. The results highlight the presence of smoke layers of 1-2 km thickness, located at about 5 km a.s.l. altitude over Granada and Leipzig and around 2.5 km a.s.l. at Warsaw. These layers were intense, as they accounted for more than 30% of the total AOD (aerosol optical depth) in all cases, and presented optical and microphysical features typical for different aging degrees: color ratio of lidar ratios (LR532/LR355) around 2, alpha-related angstrom exponents of less than 1, effective radii of 0.3 mu m and large values of single scattering albedos (SSA), nearly spectrally independent. The intensive microphysical properties were compared with columnar retrievals form co-located AERONET (Aerosol Robotic Network) stations. The intensity of the layers was also characterized in terms of particle volume concentration, and then an experimental relationship between this magnitude and the particle extinction coefficient was established.
Lechleitner, Franziska A. ; Breitenbach, Sebastian Franz Martin ; Rehfeld, Kira ; Ridley, Harriet E. ; Asmerom, Yemane ; Prufer, Keith M. ; Marwan, Norbert ; Goswami, Bedartha ; Kennett, Douglas J. ; Aquino, Valorie V. ; Polyak, Victor ; Haug, Gerald H. ; Eglinton, Timothy I. ; Baldini, James U. L.
The presence of a low-to mid-latitude interhemispheric hydrologic seesaw is apparent over orbital and glacial-interglacial timescales, but its existence over the most recent past remains unclear. Here we investigate, based on climate proxy reconstructions from both hemispheres, the inter-hemispherical phasing of the Intertropical Convergence Zone (ITCZ) and the low-to mid-latitude teleconnections in the Northern Hemisphere over the past 2000 years. A clear feature is a persistent southward shift of the ITCZ during the Little Ice Age until the beginning of the 19th Century. Strong covariation between our new composite ITCZ-stack and North Atlantic Oscillation (NAO) records reveals a tight coupling between these two synoptic weather and climate phenomena over decadal-to-centennial timescales. This relationship becomes most apparent when comparing two precisely dated, high-resolution paleorainfall records from Belize and Scotland, indicating that the low-to mid-latitude teleconnection was also active over annual-decadal timescales. It is likely a combination of external forcing, i.e., solar and volcanic, and internal feedbacks, that drives the synchronous ITCZ and NAO shifts via energy flux perturbations in the tropics.
We discuss generalized integro-differential diffusion equations whose integral kernels are not of a simple power law form, and thus these equations themselves do not belong to the family of fractional diffusion equations exhibiting a monoscaling behavior. They instead generate a broad class of anomalous nonscaling patterns, which correspond either to crossovers between different power laws, or to a non-power-law behavior as exemplified by the logarithmic growth of the width of the distribution. We consider normal and modified forms of these generalized diffusion equations and provide a brief discussion of three generic types of integral kernels for each form, namely, distributed order, truncated power law and truncated distributed order kernels. For each of the cases considered we prove the non-negativity of the solution of the corresponding generalized diffusion equation and calculate the mean squared displacement. (C) 2017 Elsevier Ltd. All rights reserved.
Kegelmann, Lukas ; Wolff, Christian Michael ; Awino, Celline ; Lang, Felix ; Unger, Eva L. ; Korte, Lars ; Dittrich, Thomas ; Neher, Dieter ; Rech, Bernd ; Albrecht, Steve
Solar cells made from inorganic organic perovskites have gradually approached market requirements as their efficiency and stability have improved tremendously in recent years. Planar low-temperature processed perovskite solar cells are advantageous for possible large-scale production but are more prone to exhibiting photocurrent hysteresis, especially in the regular n-i-p structure. Here, a systematic characterization of different electron selective contacts with a variety of chemical and electrical properties in planar n-i-p devices processed below 180 degrees C is presented. The inorganic metal oxides TiO2 and SnO2, the organic fullerene derivatives C-60, PCBM, and ICMA, as well as double-layers with a metal oxide/PCBM structure are used as electron transport materials (ETMs). Perovskite layers deposited atop, the different ETMs with the herein applied fabrication method show a similar morphology according to scanning electron microscopy. Further, surface photovoltage spectroscopy measurements indicate comparable perovskite absorber qualities on all ETMs, except TiO2, which shows a more prominent influence of defect states. Transient photoluminescence studies together with current voltage scans over a broad range of scan speeds reveal faster charge extraction, less pronounced hysteresis effects, and higher efficiencies for devices with fullerene compared to those with metal oxide ETMs. Beyond this, only double-layer ETM structures substantially diminish hysteresis effects for all performed scan speeds and strongly enhance the power conversion efficiency up to a champion stabilized value of 18.0%. The results indicate reduced recombination losses for a double-layer TiO2/PCBM contact design: First, a reduction of shunt paths through the fullerene to the ITO layer. Second, an improved hole blocking by the wide band gap metal oxide. Third, decreased transport losses due to an energetically more favorable contact, as implied by photoelectron spectroscopy measurements. The herein demonstrated improvements of multilayer selective contacts may serve as a general design guideline for perovskite solar cells.
Jošt, Marko ; Albrecht, Steve ; Kegelmann, Lukas ; Wolff, Christian Michael ; Lang, Felix ; Lipovšek, Benjamin ; Krč, Janez ; Korte, Lars ; Neher, Dieter ; Rech, Bernd ; Topič, Marko
Inorganic-organic perovskites like methylammonium-lead-iodide have proven to be an effective class of 17 materials for fabricating efficient solar cells. To improve their performance, light management techniques using textured surfaces, similar to those used in established solar cell technologies, should be considered. Here, we apply a light management foil created by UV nanoimprint lithography on the glass side of an inverted (p-i-n) perovskite solar cell with 16.3% efficiency. The obtained 1 mA cm(-2) increase in the short-circuit current density translates to a relative improvement in cell performance of 5%, which results in a power conversion efficiency of 17.1%. Optical 3D simulations based on experimentally obtained parameters were used to support the experimental findings. A good match between the simulated and experimental data was obtained, validating the model. Optical simulations reveal that the main improvement in device performance is due to a reduction in total reflection and that relative improvement in the short-circuit current density of up to 10% is possible for large-area devices. Therefore, our results present the potential of light management foils for improving the device performance of perovskite solar cells and pave the way for further use of optical simulations in the field of perovskite solar cells.
Absorption Tails of Donor
(2017)
Vandewal, Koen ; Benduhn, Johannes ; Schellhammer, Karl Sebastian ; Vangerven, Tim ; Rückert, Janna E. ; Piersimoni, Fortunato ; Scholz, Reinhard ; Zeika, Olaf ; Fan, Yeli ; Barlow, Stephen ; Neher, Dieter ; Marder, Seth R. ; Manca, Jean ; Spoltore, Donato ; Cuniberti, Gianaurelio ; Ortmann, Frank
In disordered organic semiconductors, the transfer of a rather localized charge carrier from one site to another triggers a deformation of the molecular structure quantified by the intramolecular relaxation energy. A similar structural relaxation occurs upon population of intermolecular charge-transfer (CT) states formed at organic electron donor (D)-acceptor (A) interfaces. Weak CT absorption bands for D A complexes occur at photon energies below the optical gaps of both the donors and the C-60 acceptor as a result of optical transitions from the neutral ground state to the ionic CT state. In this work, we show that temperature-activated intramolecular vibrations of the ground state play a major role in determining the line shape of such CT absorption bands. This allows us to extract values for the relaxation energy related to the geometry change from neutral to ionic CT complexes. Experimental values for the relaxation energies of 20 D:C-60 CT complexes correlate with values calculated within density functional theory. These results provide an experimental method for determining the polaron relaxation energy in solid-state organic D-A blends and show the importance of a reduced relaxation energy, which we introduce to characterize thermally activated CT processes.
De Angelis, A. ; Tatischeff, V. ; Tavani, M. ; Oberlack, U. ; Grenier, I. ; Hanloni, L. ; Walter, R. ; Argan, A. ; Von Ballmoos, P. ; Bulgarelli, A. ; Donnarumma, I. ; Hernanz, M. ; Kuvvetli, I. ; Pearce, M. ; Zdziarski, A. ; Aboudan, A. ; Ajello, M. ; Ambrosi, G. ; Bernard, D. ; Bernardini, E. ; Bonvicini, V. ; Brogna, A. ; Branchesi, M. ; Budtz-Jorgensen, C. ; Bykov, A. M. ; Campana, R. ; Cardillo, M. ; Coppi, P. ; De Martino, D. ; Diehl, R. ; Doro, M. ; Fioretti, V. ; Funk, S. ; Ghisellini, G. ; Grove, E. ; Hamadache, C. ; Hartmann, D. H. ; Hayashida, M. ; Isern, J. ; Kanbach, G. ; Kiener, J. ; Knodlseder, J. ; Labanti, C. ; Laurent, P. ; Limousin, O. ; Longo, F. ; Mannheim, K. ; Marisaldi, M. ; Martinez, M. ; Mazziotta, Mario Nicola ; McEnery, J. ; Mereghetti, S. ; Minervini, G. ; Moiseev, A. ; Morselli, A. ; Nakazawa, K. ; Orleanski, P. ; Paredes, J. M. ; Patricelli, B. ; Pevre, J. ; Piano, G. ; Pohl, Martin ; Ramarijaona, H. ; Rando, R. ; Reichardt, I. ; Roncadelli, M. ; Silva, R. ; Tavecchio, F. ; Thompson, D. J. ; Turolla, R. ; Ulyanov, A. ; Vacchi, A. ; Wu, X. ; Zoglauer, A.
e-ASTROGAM (‘enhanced ASTROGAM’) is a breakthrough Observatory space mission, with a detector composed by a Silicon tracker, a calorimeter, and an anticoincidence system, dedicated to the study of the non-thermal Universe in the photon energy range from 0.3 MeV to 3 GeV – the lower energy limit can be pushed to energies as low as 150 keV, albeit with rapidly degrading angular resolution, for the tracker, and to 30 keV for calorimetric detection. The mission is based on an advanced space-proven detector technology, with unprecedented sensitivity, angular and energy resolution, combined with polarimetric capability. Thanks to its performance in the MeV-GeV domain, substantially improving its predecessors, e-ASTROGAM will open a new window on the non-thermal Universe, making pioneering observations of the most powerful Galactic and extragalactic sources, elucidating the nature of their relativistic outflows and their effects on the surroundings. With a line sensitivity in the MeV energy range one to two orders of magnitude better than previous generation instruments, e-ASTROGAM will determine the origin of key isotopes fundamental for the understanding of supernova explosion and the chemical evolution of our Galaxy. The mission will provide unique data of significant interest to a broad astronomical community, complementary to powerful observatories such as LIGO-Virgo-GEO600-KAGRA, SKA, ALMA, E-ELT, TMT, LSST, JWST, Athena, CTA, IceCube, KM3NeT, and the promise of eLISA.
We develop a simple two-zone interpretation of the broadband baseline Crab nebula spectrum between 10(-5) eV and similar to 100 TeV by using two distinct log-parabola energetic electrons distributions. We determine analytically the very-high energy photon spectrum as originated by inverse-Compton scattering of the far-infrared soft ambient photons within the nebula off a first population of electrons energized at the nebula termination shock. The broad and flat 200 GeV peak jointly observed by Fermi/LAT and MAGIC is naturally reproduced. The synchrotron radiation from a second energetic electron population explains the spectrum from the radio range up to similar to 10 keV. We infer from observations the energy dependence of the microscopic probability of remaining in proximity of the shock of the accelerating electrons.