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Die Femtosekundendynamik nach resonanten Photoanregungen mit optischen und Röntgenpulsen ermöglicht eine selektive Verformung von chemischen N‐H‐ und N‐C‐Bindungen in 2‐Thiopyridon in wässriger Lösung. Die Untersuchung der orbitalspezifischen elektronischen Struktur und ihrer Dynamik auf ultrakurzen Zeitskalen mit resonanter inelastischer Röntgenstreuung an der N1s‐Resonanz am Synchrotron und dem Freie‐Elektronen‐Laser LCLS in Kombination mit quantenchemischen Multikonfigurationsberechnungen erbringen den direkten Nachweis dieser kontrollierten photoinduzierten Molekülverformungen und ihrer ultrakurzen Zeitskala.
Permafrost is a distinct feature of the terrestrial Arctic and is vulnerable to climate warming. Permafrost degrades in different ways, including deepening of a seasonally unfrozen surface and localized but rapid development of deep thaw features. Pleistocene ice-rich permafrost with syngenetic ice-wedges, termed Yedoma deposits, are widespread in Siberia, Alaska, and Yukon, Canada and may be especially prone to rapid-thaw processes. Freeze-locked organic matter in such deposits can be re-mobilized on short time-scales and contribute to a carbon-cycle climate feedback. Here we synthesize the characteristics and vulnerability of Yedoma deposits by synthesizing studies on the Yedoma origin and the associated organic carbon pool. We suggest that Yedoma deposits accumulated under periglacial weathering, transport, and deposition dynamics in non-glaciated regions during the late Pleistocene until the beginning of late glacial warming. The deposits formed due to a combination of aeolian, colluvial, nival, and alluvial deposition and simultaneous ground ice accumulation. We found up to 130 gigatons organic carbon in Yedoma, parts of which are well-preserved and available for fast decomposition after thaw. Based on incubation experiments, up to 10% of the Yedoma carbon is considered especially decomposable and may be released upon thaw. The substantial amount of ground ice in Yedoma makes it highly vulnerable to disturbances such as thermokarst and thermo-erosion processes. Mobilization of permafrost carbon is expected to increase under future climate warming. Our synthesis results underline the need of accounting for Yedoma carbon stocks in next generation Earth-System-Models for a more complete representation of the permafrost-carbon feedback.
The femtosecond excited-state dynamics following resonant photoexcitation enable the selective deformation of N-H and N-C chemical bonds in 2-thiopyridone in aqueous solution with optical or X-ray pulses. In combination with multiconfigurational quantum-chemical calculations, the orbital-specific electronic structure and its ultrafast dynamics accessed with resonant inelastic X-ray scattering at the N 1s level using synchrotron radiation and the soft X-ray free-electron laser LCLS provide direct evidence for this controlled photoinduced molecular deformation and its ultrashort time-scale.
In this combined theoretical and experimental study we report a full analysis of the resonant inelastic X-ray scattering (RIXS) spectra of H2O, D2O and HDO. We demonstrate that electronically-elastic RIXS has an inherent capability to map the potential energy surface and to perform vibrational analysis of the electronic ground state in multimode systems. We show that the control and selection of vibrational excitation can be performed by tuning the X-ray frequency across core-excited molecular bands and that this is clearly reflected in the RIXS spectra. Using high level ab initio electronic structure and quantum nuclear wave packet calculations together with high resolution RIXS measurements, we discuss in detail the mode coupling, mode localization and anharmonicity in the studied systems.
The valence orbitals of aqueous histidine under basic, neutral and acidic conditions and their X-ray induced transformations have been monitored through N 1s resonant inelastic X-ray scattering. Using density functional ab initio molecular dynamics simulations in the core-hole state within the Z + 1 approximation, core-excitation-induced molecular transformations are quantified. Spectroscopic evidence for a highly directional X-ray-induced local N-H dissociation within the scattering duration is presented for acidic histidine. Our report demonstrates a protonation-state and chemical-environment dependent propensity for a molecular dissociation, which is induced by the absorption of high energy photons. This case study indicates that structural deformations in biomolecules under exposure to ionizing radiation, yielding possible alteration or loss of function, is highly dependent on the physiological state of the molecule upon irradiation.
The dynamics of fragmentation and vibration of molecular systems with a large number of coupled degrees of freedom are key aspects for understanding chemical reactivity and properties. Here we present a resonant inelastic X-ray scattering (RIXS) study to show how it is possible to break down such a complex multidimensional problem into elementary components. Local multimode nuclear wave packets created by X-ray excitation to different core-excited potential energy surfaces (PESs) will act as spatial gates to selectively probe the particular ground-state vibrational modes and, hence, the PES along these modes. We demonstrate this principle by combining ultra-high resolution RIXS measurements for gas-phase water with state-of-the-art simulations.