Energy and Charge Transfer in Dimers and Trimers of Xenon

The goal of this thesis is the investigation of decay processes in innershell ionised xenon dimers and trimers. To this end, the small clusters were ionised using 100 eV photons from a Free-Electron Laser and the momenta of the created ion fragments and electrons were measured using the Reaction Microscope at FLASH2. Employing an XUV/XUV pump-probe scheme, the timescale to distribute energy or charge throughout the cluster following local excitation was determined to below (186+-6) fs for dimers decaying into Xe^{1+} / Xe^{2+} and (84+-13) fs for trimers decaying into Xe^{1+}/Xe^{1+}/Xe^{1+}. The kinetic energy distributions yield clear evidence that Xe_2^{2+} decays by a slow CT process after bond contraction and Xe_3^{2+*} decays by ETMD(3) before the nuclei can move. Furthermore, we see signatures of frustrated ionisation in Xe_2 dimers

Atomic, Molecular and Cluster Science with the Reaction Microscope Endstation at FLASH2

The reaction microscope (REMI) endstation for atomic and molecular science at the free-electron laser FLASH2 at DESY in Hamburg is presented together with a brief overview of results recently obtained. The REMI allows coincident detection of electrons and ions that emerge from atomic or molecular fragmentation reactions in the focus of the extreme-ultraviolet (XUV) free-electron laser (FEL) beam. A large variety of target species ranging from atoms and molecules to small clusters can be injected with a supersonic gas-jet into the FEL focus. Their ionization and fragmentation dynamics can be studied either under single pulse conditions, or for double pulses as a function of their time delay by means of FEL-pump–FEL-probe schemes and also in combination with a femtosecond infrared (IR) laser. In a recent upgrade, the endstation was further extended by a light source based on high harmonic generation (HHG), which is now available for upcoming FEL/HHG pump–probe experiments

High heparin content surface-modified polyurethane discs promote rapid and stable angiogenesis in full thickness skin defects through VEGF immobilization

Three-dimensional scaffolds have the capacity to serve as an architectural framework to guide and promote tissue regeneration. Parameters such as the type of material, growth factors, and pore dimensions are therefore critical in the scaffold's success. In this study, heparin has been covalently bound to the surface of macroporous polyurethane (PU) discs via two different loading methods to determine if the amount of heparin content had an influence on the therapeutic affinity loading and release of (VEGF165 ) in full thickness skin defects. PU discs (5.4 mm diameter, 300 µm thickness, and interconnected pore size of 150 µm) were produced with either a low (2.5 mg/g) or high (6.6 mg/g) heparin content (LC and HC respectively), and were implanted into the modified dorsal skin chamber (MDSC) of C57BL/6 J mice with and without VEGF. Both low- and high-content discs with immobilized VEGF165 (LCV and HCV, respectively) presented accelerated neovascularization and tissue repair in comparison to heparin discs alone. However, the highest angiogenetic peak was on day 7 with subsequent stabilization for HCV, whereas other groups displayed a delayed peak on day 14. We therefore attribute the superior performance of HCV due to its ability to hold more VEGF165, based on its increased heparin surface coverage, as also demonstrated in VEGF elution dynamics. © 2017 Wiley Periodicals, Inc. J Biomed Mater Res Part A: 105A: 2543-2550, 2017

Surface-Structured Bacterial Cellulose with Guided Assembly-Based Biolithography (GAB)

A powerful replica molding methodology to transfer on-demand functional topographies to the surface of bacterial cellulose nanofiber textures is presented. With this method, termed guided assembly-based biolithography (GAB), a surface-structured polydimethylsiloxane (PDMS) mold is introduced at the gas-liquid interface of an Acetobacter xylinum culture. Upon bacterial fermentation, the generated bacterial cellulose nanofibers are assembled in a three-dimensional network reproducing the geometric shape imposed by the mold. Additionally, GAB yields directional alignment of individual nanofibers and memory of the transferred geometrical features upon dehydration and rehydration of the substrates. Scanning electron and atomic force microscopy are used to establish the good fidelity of this facile and affordable method. Interaction of surface-structured bacterial cellulose substrates with human fibroblasts and keratinocytes illustrates the efficient control of cellular activities which are fundamental in skin wound healing and tissue regeneration. The deployment of surface-structured bacterial cellulose substrates in model animals as skin wound dressing or body implant further proves the high durability and low inflammatory response to the material over a period of 21 days, demonstrating beneficial effects of surface structure on skin regeneration

Linear dichroism in few-photon ionization of laser-dressed helium

Abstract: Ionization of laser-dressed atomic helium is investigated with focus on photoelectron angular distributions stemming from two-color multi-photon excited states. The experiment combines extreme ultraviolet (XUV) with infrared (IR) radiation, while the relative polarization and the temporal delay between the pulses can be varied. By means of an XUV photon energy scan over several electronvolts, we get access to excited states in the dressed atom exhibiting various binding energies, angular momenta, and magnetic quantum numbers. Furthermore, varying the relative polarization is employed as a handle to switch on and off the population of certain states that are only accessible by two-photon excitation. In this way, photoemission can be suppressed for specific XUV photon energies. Additionally, we investigate the dependence of the photoelectron angular distributions on the IR laser intensity. At our higher IR intensities, we start leaving the simple multi-photon ionization regime. The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation. Graphic abstract: [Figure not available: see fulltext.

Photoelectron spectroscopy of laser-dressed atomic helium

© 2020 authors. Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color exteme ultraviolet (XUV)-infrared (IR) measurement, the XUV photon energy is scanned between 20.4 eV and the ionization threshold at 24.6 eV, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse (≈1012Wcm-2). The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation

Differential Measurement of Electron Ejection after Two-Photon Two-Electron Excitation of Helium

We report the measurement of the photoelectron angular distribution of two-photon single-ionization near the $2p^2$ $^1D^e$ double-excitation resonance in helium, benchmarking the fundamental nonlinear interaction of two photons with two correlated electrons. This observation is enabled by the unique combination of intense extreme ultraviolet pulses, delivered at the high-repetition-rate free-electron laser in Hamburg (FLASH), ionizing a jet of cryogenically cooled helium atoms in a reaction microscope. The spectral structure of the intense self-amplified spontaneous emission free-electron laser pulses has been resolved on a single-shot level to allow for post selection of pulses, leading to an enhanced spectral resolution, and introducing a new experimental method. The measured angular distribution is directly compared to state-of-the-art theory based on multichannel quantum defect theory and the streamlined $R$-matrix method. These results and experimental methodology open a promising route for exploring fundamental interactions of few photons with few electrons in general

Surface-Structured Bacterial Cellulose with Guided Assembly-Based Biolithography (GAB)

A powerful replica molding methodology to transfer on-demand functional topographies to the surface of bacterial cellulose nanofiber textures is presented. With this method, termed guided assembly-based biolithography (GAB), a surface-structured polydimethylsiloxane (PDMS) mold is introduced at the gas–liquid interface of an <i>Acetobacter xylinum</i> culture. Upon bacterial fermentation, the generated bacterial cellulose nanofibers are assembled in a three-dimensional network reproducing the geometric shape imposed by the mold. Additionally, GAB yields directional alignment of individual nanofibers and memory of the transferred geometrical features upon dehydration and rehydration of the substrates. Scanning electron and atomic force microscopy are used to establish the good fidelity of this facile and affordable method. Interaction of surface-structured bacterial cellulose substrates with human fibroblasts and keratinocytes illustrates the efficient control of cellular activities which are fundamental in skin wound healing and tissue regeneration. The deployment of surface-structured bacterial cellulose substrates in model animals as skin wound dressing or body implant further proves the high durability and low inflammatory response to the material over a period of 21 days, demonstrating beneficial effects of surface structure on skin regeneration

Ultrafast Roaming Mechanisms in Ethanol Probed by Intense Extreme Ultraviolet Free-Electron Laser Radiation: Electron Transfer versus Proton Transfer

Ultrafast H$_2$$^+$ and H$_3$$^+$ formation from ethanol is studied using pump-probe spectroscopy with an extreme ultraviolet (XUV) free-electron laser. The first pulse creates a dication, triggering H2 roaming that leads to H$_2$$^+$ and H$_3$$^+$ formation, which is disruptively probed by a second pulse. At photon energies of 28 and 32 eV, the ratio of H$_2$$^+$ to H$_3$$^+$ increases with time delay, while it is flat at a photon energy of 70 eV. The delay-dependent effect is ascribed to a competition between electron and proton transfer. High-level quantum chemistry calculations show a flat potential energy surface for H$_2$ formation, indicating that the intermediate state may have a long lifetime. The ab initio molecular dynamics simulation confirms that, in addition to the direct emission, a small portion of H$_2$ undergoes a roaming mechanism that leads to two competing pathways: electron transfer from H2 to C$_2$H$_4$O$_2$$^+$ and proton transfer from C$_2$H$_4$O$_2$$^+$ to H$_2$