TY - JOUR A1 - Schreck, Simon A1 - Pietzsch, Annette A1 - Kunnus, Kristjan A1 - Kennedy, Brian A1 - Quevedo, Wilson A1 - Miedema, Piter S. A1 - Wernet, Philippe A1 - Föhlisch, Alexander T1 - Dynamics of the OH group and the electronic structure of liquid alcohols JF - Structural dynamics N2 - In resonant inelastic soft x-ray scattering (RIXS) from molecular and liquid systems, the interplay of ground state structural and core-excited state dynamical contributions leads to complex spectral shapes that partially allow for ambiguous interpretations. In this work, we dissect these contributions in oxygen K-edge RIXS from liquid alcohols. We use the scattering into the electronic ground state as an accurate measure of nuclear dynamics in the intermediate core-excited state of the RIXS process. We determine the characteristic time in the core-excited state until nuclear dynamics give a measurable contribution to the RIXS spectral profiles to tau(dyn) = 1.2 +/- 0.8 fs. By detuning the excitation energy below the absorption resonance we reduce the effective scattering time below sdyn, and hence suppress these dynamical contributions to a minimum. From the corresponding RIXS spectra of liquid methanol, we retrieve the "dynamic-free" density of states and find that it is described solely by the electronic states of the free methanol molecule. From this and from the comparison of normal and deuterated methanol, we conclude that the split peak structure found in the lone-pair emission region at non-resonant excitation originates from dynamics in the O-H bond in the core-excited state. We find no evidence that this split peak feature is a signature of distinct ground state structural complexes in liquid methanol. However, we demonstrate how changes in the hydrogen bond coordination within the series of linear alcohols from methanol to hexanol affect the split peak structure in the liquid alcohols. (C) 2014 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution 3.0 Unported License. Y1 - 2014 U6 - https://doi.org/10.1063/1.4897981 SN - 2329-7778 VL - 1 IS - 5 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Goychuk, Igor A1 - Kharchenko, Vasyl O. T1 - Anomalous features of diffusion in corrugated potentials with spatial correlations: Faster than normal, and other surprises JF - Physical review letters N2 - Normal diffusion in corrugated potentials with spatially uncorrelated Gaussian energy disorder famously explains the origin of non-Arrhenius exp[-sigma(2)/(k(B)T(2))] temperature dependence in disordered systems. Here we show that unbiased diffusion remains asymptotically normal also in the presence of spatial correlations decaying to zero. However, because of a temporal lack of self-averaging, transient subdiffusion emerges on the mesoscale, and it can readily reach macroscale even for moderately strong disorder fluctuations of sigma similar to 4 - 5k(B)T. Because of its nonergodic origin, such subdiffusion exhibits a large scatter in single-trajectory averages. However, at odds with intuition, it occurs essentially faster than one expects from the normal diffusion in the absence of correlations. We apply these results to diffusion of regulatory proteins on DNA molecules and predict that such diffusion should be anomalous, but much faster than earlier expected on a typical length of genes for a realistic energy disorder of several room k(B)T, or merely 0.05-0.075 eV. Y1 - 2014 U6 - https://doi.org/10.1103/PhysRevLett.113.100601 SN - 0031-9007 SN - 1079-7114 VL - 113 IS - 10 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Gehrig, Dominik W. A1 - Roland, Steffen A1 - Howard, Ian A. A1 - Kamm, Valentin A1 - Mangold, Hannah A1 - Neher, Dieter A1 - Laquai, Frederic T1 - Efficiency-limiting processes in low-bandgap polymer:Perylene diimide photovoltaic blends JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - The charge generation and recombination processes following photo-excitation of a low-bandgap polymer:perylene diimide photovoltaic blend are investigated by transient absorption pump-probe spectroscopy covering a dynamic range from femto-to microseconds to get insight into the efficiency-limiting photophysical processes. The several tens of picoseconds, and its efficiency is only half of that in a polymer:fullerene photoinduced electron transfer from the polymer to the perylene acceptor takes up to blend. This reduces the short-circuit current. Time-delayed collection field experiments reveal that the subsequent charge separation is strongly field-dependent, limiting the fill factor and lowering the short-circuit current in polymer:PDI devices. Upon excitation of the acceptor in the low-bandgap polymer blend, the PDI exciton undergoes charge transfer on a time scale of several tens of picoseconds. However, a significant fraction of the charges generated at the interface are quickly lost because of fast geminate recombination. This reduces the short-circuit current even further, leading to a scenario in which only around 2596 of the initial photoexcitations generate free charges that can potentially contribute to the photocurrent. In summary, the key photophysical limitations of perylene diimide as an acceptor in low-bandgap polymer blends appear at the interface between the materials, with the kinetics of both charge generation and separation inhibited as compared to that of fullerenes. Y1 - 2014 U6 - https://doi.org/10.1021/jp503366m SN - 1932-7447 VL - 118 IS - 35 SP - 20077 EP - 20085 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Kliem, Bernhard A1 - Toeroek, Tibor A1 - Titov, Viacheslav S. A1 - Lionello, Roberto A1 - Linker, Jon A. A1 - Liu, Rui A1 - Liu, Chang A1 - Wang, Haimin T1 - Slow rise and partial eruption of a double-decker filament. II. A double flux rope model JF - The astrophysical journal : an international review of spectroscopy and astronomical physics N2 - Force-free equilibria containing two vertically arranged magnetic flux ropes of like chirality and current direction are considered as a model for split filaments/prominences and filament-sigmoid systems. Such equilibria are constructed analytically through an extension of the methods developed in Titov & Demoulin and numerically through an evolutionary sequence including shear flows, flux emergence, and flux cancellation in the photospheric boundary. It is demonstrated that the analytical equilibria are stable if an external toroidal (shear) field component exceeding a threshold value is included. If this component decreases sufficiently, then both flux ropes turn unstable for conditions typical of solar active regions, with the lower rope typically becoming unstable first. Either both flux ropes erupt upward, or only the upper rope erupts while the lower rope reconnects with the ambient flux low in the corona and is destroyed. However, for shear field strengths staying somewhat above the threshold value, the configuration also admits evolutions which lead to partial eruptions with only the upper flux rope becoming unstable and the lower one remaining in place. This can be triggered by a transfer of flux and current from the lower to the upper rope, as suggested by the observations of a split filament in Paper I. It can also result from tether-cutting reconnection with the ambient flux at the X-type structure between the flux ropes, which similarly influences their stability properties in opposite ways. This is demonstrated for the numerically constructed equilibrium. KW - instabilities KW - magnetohydrodynamics (MHD) KW - Sun: coronal mass ejections (CMEs) KW - Sun: filaments, prominences KW - Sun: flares Y1 - 2014 U6 - https://doi.org/10.1088/0004-637X/792/2/107 SN - 0004-637X SN - 1538-4357 VL - 792 IS - 2 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Nishikawa, Ken-Ichi A1 - Hardee, P. E. A1 - Dutan, I. A1 - Niemiec, J. A1 - Medvedev, M. A1 - Mizuno, Y. A1 - Meli, A. A1 - Sol, H. A1 - Zhang, B. A1 - Pohl, Martin A1 - Hartmann, D. H. T1 - Magnetic agnetic field generation in core-sheath jets via the kinetic Kelvin-Helmholtz instability JF - The astrophysical journal : an international review of spectroscopy and astronomical physics N2 - We have investigated magnetic field generation in velocity shears via the kinetic Kelvin-Helmholtz instability (kKHI) using a relativistic plasma jet core and stationary plasma sheath. Our three-dimensional particle-in-cell simulations consider plasma jet cores with Lorentz factors of 1.5, 5, and 15 for both electron-proton and electron-positron plasmas. For electron-proton plasmas, we find generation of strong large-scale DC currents and magnetic fields that extend over the entire shear surface and reach thicknesses of a few tens of electron skin depths. For electron-positron plasmas, we find generation of alternating currents and magnetic fields. Jet and sheath plasmas are accelerated across the shear surface in the strong magnetic fields generated by the kKHI. The mixing of jet and sheath plasmas generates a transverse structure similar to that produced by the Weibel instability. KW - acceleration of particles KW - magnetic fields KW - plasmas KW - radiation mechanisms: non-thermal KW - relativistic processes KW - stars: jets Y1 - 2014 U6 - https://doi.org/10.1088/0004-637X/793/1/60 SN - 0004-637X SN - 1538-4357 VL - 793 IS - 1 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Godec, Aljaz A1 - Bauer, Maximilian A1 - Metzler, Ralf T1 - Collective dynamics effect transient subdiffusion of inert tracers in flexible gel networks JF - New journal of physics : the open-access journal for physics N2 - Based on extensive Brownian dynamics simulations we study the thermal motion of a tracer bead in a cross-linked, flexible gel in the limit when the tracer particle size is comparable to or even larger than the equilibrium mesh size of the gel. The analysis of long individual trajectories of the tracer demonstrates the existence of pronounced transient anomalous diffusion. From the time averaged mean squared displacement and the time averaged van Hove correlation functions we elucidate the many-body origin of the non-Brownian tracer bead dynamics. Our results shed new light onto the ongoing debate over the physical origin of steric tracer interactions with structured environments. KW - anomalous diffusion KW - gel network KW - van Hove correlation Y1 - 2014 U6 - https://doi.org/10.1088/1367-2630/16/9/092002 SN - 1367-2630 VL - 16 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Miedema, P. S. A1 - Beye, Martin A1 - Koennecke, R. A1 - Schiwietz, G. A1 - Föhlisch, Alexander T1 - The angular- and crystal-momentum transfer through electron-phonon coupling in silicon and silicon-carbide: similarities and differences JF - New journal of physics : the open-access journal for physics N2 - Electron-phonon scattering has been studied for silicon carbide (6H-SiC) with resonant inelastic x-ray scattering at the silicon 2p edge. The observed electron-phonon scattering yields a crystal momentum transfer rate per average phonon in 6H-SiC of 1.8 fs(-1) while it is 0.2 fs(-1) in crystalline silicon. The angular momentum transfer rate per average phonon for 6H-SiC is 0.1 fs(-1), which is much higher than 0.0035 fs(-1) obtained for crystalline silicon in a previous study. The higher electron-phonon scattering rates in 6H-SiC are a result of the larger electron localization at the silicon atoms in 6H-SiC as compared to crystalline silicon. While delocalized valence electrons can screen effectively (part of) the electron-phonon interaction, this effect is suppressed for 6H-SiC in comparison to crystalline silicon. Smaller contributions to the difference in electron-phonon scattering rates between 6H-SiC and silicon arise from the lower atomic mass of carbon versus silicon and the difference in local symmetry. KW - electron-phonon scattering KW - 6H-SiC KW - RIXS Y1 - 2014 U6 - https://doi.org/10.1088/1367-2630/16/9/093056 SN - 1367-2630 VL - 16 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Xu, Jingsan A1 - Brenner, Thomas J. K. A1 - Chabanne, Laurent A1 - Neher, Dieter A1 - Antonietti, Markus A1 - Shalom, Menny T1 - Liquid-Based growth of polymeric carbon nitride layers and their use in a mesostructured polymer solar cell with V-oc exceeding 1 V JF - Journal of the American Chemical Society N2 - Herein we report a general liquid-mediated pathway for the growth of continuous polymeric carbon nitride (C3N4) thin films. The deposition method consists of the use of supramolecular complexes that transform to the liquid state before direct thermal condensation into C3N4 solid films. The resulting films exhibit continuous porous C3N4 networks on various substrates. Moreover, the optical absorption can be easily tuned to cover the solar spectrum by the insertion of an additional molecule into the starting complex. The strength of the deposition method is demonstrated by the use of the C3N4 layer as the electron acceptor in a polymer solar cell that exhibits a remarkable open-circuit voltage exceeding 1 V. The easy, safe, and direct synthesis of carbon nitride in a continuous layered architecture on different functional substrates opens new possibilities for the fabrication of many energy-related devices. Y1 - 2014 U6 - https://doi.org/10.1021/ja508329c SN - 0002-7863 VL - 136 IS - 39 SP - 13486 EP - 13489 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Di Florio, G. A1 - Bruendermann, E. A1 - Yadavalli, Nataraja Sekhar A1 - Santer, Svetlana A1 - Havenith, Martina T1 - Graphene multilayer as nanosized optical strain gauge for polymer surface relief gratings JF - Nano letters : a journal dedicated to nanoscience and nanotechnology N2 - In this paper, we show how graphene can be utilized as a nanoscopic probe in order to characterize local opto-mechanical forces generated within photosensitive azobenzene containing polymer films. Upon irradiation with light interference patterns, photosensitive films deform according to the spatial intensity variation, leading to the formation of periodic topographies such as surface relief gratings (SRG). The mechanical driving forces inscribing a pattern into the films are supposedly fairly large, because the deformation takes place without photofluidization; the polymer is in a glassy state throughout. However, until now there has been no attempt to characterize these forces by any means. The challenge here is that the forces vary locally on a nanometer scale. Here, we propose to use Raman analysis of the stretching of the graphene layer adsorbed on top of polymer film under deformation in order to probe the strength of the material transport spatially resolved. With the well-known mechanical properties of graphene, we can obtain lower bounds on the forces acting within the film. Upon the basis of our experimental results, we can deduce that the internal pressure in the film due to grating formation can exceed 1 GPa. The graphene-based nanoscopic gauge opens new possibilities to characterize opto-mechanical forces generated within photosensitive polymer films. KW - Surface relief grating KW - optomechanical forces KW - photosensitive polymer films KW - multilayer graphene deformation KW - confocal Raman microscopy Y1 - 2014 U6 - https://doi.org/10.1021/nl502631s SN - 1530-6984 SN - 1530-6992 VL - 14 IS - 10 SP - 5754 EP - 5760 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Steffen, M. A1 - Hubrig, Swetlana A1 - Todt, Helge Tobias A1 - Schoeller, M. A1 - Hamann, Wolf-Rainer A1 - Sandin, Christer A1 - Schönberner, Detlef T1 - Weak magnetic fields in central stars of planetary nebulae? JF - Astronomy and astrophysics : an international weekly journal N2 - Context. It is not yet clear whether magnetic fields play an essential role in shaping planetary nebulae (PNe), or whether stellar rotation alone and/or a close binary companion, stellar or substellar, can account for the variety of the observed nebular morphologies. Aims. In a quest for empirical evidence verifying or disproving the role of magnetic fields in shaping planetary nebulae, we follow up on previous attempts to measure the magnetic field in a representative sample of PN central stars. Methods. We obtained low-resolution polarimetric spectra with FORS2 installed on the Antu telescope of the VLT for a sample of 12 bright central stars of PNe with different morphologies, including two round nebulae, seven elliptical nebulae, and three bipolar nebulae. Two targets are Wolf-Rayet type central stars. Results. For the majority of the observed central stars, we do not find any significant evidence for the existence of surface magnetic fields. However, our measurements may indicate the presence of weak mean longitudinal magnetic fields of the order of 100 Gauss in the central star of the young elliptical planetary nebula IC 418 as well as in the Wolf-Rayet type central star of the bipolar nebula Hen 2-113 and the weak emission line central star of the elliptical nebula Hen 2-131. A clear detection of a 250 G mean longitudinal field is achieved for the A-type companion of the central star of NGC 1514. Some of the central stars show a moderate night-to-night spectrum variability, which may be the signature of a variable stellar wind and/or rotational modulation due to magnetic features. Conclusions. Since our analysis indicates only weak fields, if any, in a few targets of our sample, we conclude that strong magnetic fields of the order of kG are not widespread among PNe central stars. Nevertheless, simple estimates based on a theoretical model of magnetized wind bubbles suggest that even weak magnetic fields below the current detection limit of the order of 100 G may well be sufficient to contribute to the shaping of the surrounding nebulae throughout their evolution. Our current sample is too small to draw conclusions about a correlation between nebular morphology and the presence of stellar magnetic fields. KW - planetary nebulae: general KW - stars: magnetic field KW - stars: AGB and post-AGB KW - binaries: close KW - techniques: polarimetric Y1 - 2014 U6 - https://doi.org/10.1051/0004-6361/201423842 SN - 0004-6361 SN - 1432-0746 VL - 570 PB - EDP Sciences CY - Les Ulis ER -