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- Fakultät II - Maschinenbau und Bioverfahrenstechnik (77) (remove)
The use of vibrational sum-frequency spectroscopy (VSFS) to study transferred graphene, produced by chemical vapour deposition, is presented. The VSF spectrum shows a clear CeH stretching mode at ~2924 cm⁻¹, which is attributed to residue of the polymer used for the transfer. This makes VSFS a powerful tool to identify adsorbates and contaminants affecting the properties of graphene.
We report velocity-dependent internal energy distributions of nitric oxide molecules, NO, scattered off graphene supported on gold to further explore the dynamics of the collision process between NO radicals and graphene. These experiments were performed by directing a molecular beam of NO onto graphene in a surface-velocity map imaging setup, which allowed us to record internal energy distributions of the NO radicals as a function of their velocity. We do not observe bond formation but (1) major contributions from direct inelastic scattering and (2) a smaller trapping–desorption component where some physisorbed NO molecules have residence times on the order of microseconds. This is in agreement with our classical molecular dynamics simulations which also observe a small proportion of two- and multi-bounce collisions events but likewise a small proportion of NO radicals trapped at the surface for the entire length of the molecular dynamics simulations (a few picoseconds). Despite a collision energy of 0.31 eV, which would be sufficient to populate NO(v = 1), we do not detect vibrationally excited nitric oxide.
Worldwide, seagrass meadows are under threat. Consequently, there is a strong need for seagrass restoration to guarantee the provision of related ecosystem services such as nutrient cycling, carbon sequestration and habitat provision. Seagrass often grows in vast meadows in which the presence of seagrass itself leads to a reduction of hydrodynamic energy. By modifying the environment, seagrass thus serves as foundation species and ecosystem engineer improving habitat quality for itself and other species as well as positively affecting its own fitness. On the downside, this positive feedback mechanism can render natural recovery of vanished and destroyed seagrass meadows impossible. An innovative approach to promote positive feedback mechanisms in seagrass restoration is to create an artificial seagrass (ASG) that mimics the facilitation function of natural seagrass. ASG could provide a window of opportunity with respect to suitable hydrodynamic and light conditions as well as sediment stabilization to allow natural seagrass to re-establish. Here, we give an overview of challenges and open questions for the application of ASG to promote seagrass restoration based on experimental studies and restoration trials and we propose a general approach for the design of an ASG produced from biodegradable materials. Considering positive feedback mechanisms is crucial to support restoration attempts. ASG provides promising benefits when habitat conditions are too harsh for seagrass meadows to re-establish themselves.
We have combined the velocity map imaging technique with time-of-flight measurements to study the surface photochemistry of KBr single crystals. This approach yields 3-dimensional velocity distributions of Br atoms resulting from 193 nm photodesorption. The velocity distributions indicate that at least two non-thermal mechanisms contribute to the photodesorption dynamics. Our experimental geometry also allows us to measure the Br(²P₃⁄₂):Br(²P₁⁄₂) branching ratio, which is found to be 24:1.
The effects of surface temperature on the gas-liquid interfacial reaction dynamics of O(³P)+squalane
(2005)
OH/OD product state distributions arising from the reaction of gas-phase O(³P) atoms at the surface of the liquid hydrocarbon squalane C₃₀H₆₂/C₃₀D₆₂ have been measured. The O(³P) atoms were generated by 355 nm laser photolysis of NO₂ at a low pressure above the continually refreshed liquid. It has been shown unambiguously that the hydroxyl radicals detected by laser-induced fluorescence originate from the squalane surface. The gas-phase OH/OD rotational populations are found to be partially sensitive to the liquid temperature, but do not adapt to it completely. In addition, rotational temperatures for OH/OD(v′=1) are consistently colder (by 34±5 K) than those for OH/OD(v′=0). This is reminiscent of, but less pronounced than, a similar effect in the well-studied homogeneous gas-phase reaction of O(³P) with smaller hydrocarbons. We conclude that the rotational distributions are composed of two different components. One originates from a direct abstraction mechanism with product characteristics similar to those in the gas phase. The other is a trapping-desorption process yielding a thermal, Boltzmann-like distribution close to the surface temperature. This conclusion is consistent with that reached previously from independent measurements of OH product velocity distributions in complementary molecular-beam scattering experiments. It is further supported by the temporal profiles of OH/OD laser-induced fluorescence signals as a function of distance from the surface observed in the current experiments. The vibrational branching ratios for (v′=1)/(v′=0) for OH and OD have been found to be (0.07±0.02) and (0.30±0.10), respectively. The detection of vibrationally excited hydroxyl radicals suggests that secondary and/or tertiary hydrogen atoms may be accessible to the attacking oxygen atoms.
Background: The topographical correlations between certain extracranial and intracranial osseous points of interest (POIs), and their age-related changes, are indispensable to know for a diagnostical or surgical access to intracranial structures; however, they are difficult to assess with conventional devices.
Materials and methods: In this pilot study, the 3-dimensional coordinates of extra-/intracranial POIs were determined, thus avoiding perspective distortions that used to be intrinsic problems in 2-dimensional morphometry. The data sets were then analysed by creating virtual triangles. The sizes, shapes, and positions of these triangles described the extent and the directions of the age-related shifts of the POIs. A selection of extracranial and intracranial POIs were marked on half skulls of four warmblood horses in two age groups (young: 6 weeks, n = 2; old: 14 and 17 years, n = 2). The x-, y-, and z-coordinates of these POIs were determined with a measurement arm (FaroArm Fusion, FARO Europe®). Direct distances between the POIs as well as their indirect distances on the x-, y-, and z-axis, and angles were calculated.
Results: The analysed virtual triangles revealed that some parts of the skull grew in size, but did not change in shape/relative proportions (proportional type of growth, as displayed by POI A and POI B at the Arcus zygomaticus). The same POIs (A and B) remained in a very stable relationship to their closest intracranial POI at the Basis cranii on the longitudinal axis, however, shifted markedly in the dorso-lateral direction. In contrast, a disproportional growth of other parts of the cranium was, for example, related to POI C at the Crista nuchae, which shifted strongly in the caudal direction with age. A topographically stable reference point (so-called anchor point) at the Basis cranii was difficult to determine.
Conclusions: Two candidates (one at the Synchondrosis intersphenoidalis, another one at the Synchondrosis sphenooccipitalis) were relatively stable in their positions. However, the epicentre of (neuro-)cranial growth could only be pinpointed to an area between them.
The authors describe the application of a combination of velocity map imaging and time-of-flight (TOF) techniques to obtain three-dimensional velocity distributions for surface photodesorption. They have established a systematic alignment procedure to achieve correct and reproducible experimental conditions. It includes four steps: (1) optimization of the velocity map imaging ion optics’ voltages to achieve optimum velocity map imaging conditions; (2) alignment of the surface normal with the symmetry axis (ion flight axis) of the ion optics; (3) determination of TOF distance between the surface and the ionizing laser beam; (4) alignment of the position of the ionizing laser beam with respect to the ion optics. They applied this set of alignment procedures and then measured Br(²P₃/₂) (Br) and Br(²P₁/₂) (Br∗) atoms photodesorbing from a single crystal of KBr after exposure to 193 nm light. They analyzed the velocity flux and energy flux distributions for motion normal to the surface. The Br∗ normal energy distribution shows two clearly resolved peaks at approximately 0.017 and 0.39 eV, respectively. The former is slightly faster than expected for thermal desorption at the surface temperature and the latter is hyperthermal. The Br normal energy distribution shows a single broad peak that is likely composed of two hyperthermal components. The capability that surface three-dimensional velocity map imaging provides for measuring state-specific velocity distributions in all three dimensions separately and simultaneously for the products of surface photodesorption or surface reactions holds great promise to contribute to our understanding of these processes.
Surface atomic relaxation and magnetism on hydrogen-adsorbed Fe(110) surfaces from first principles
(2016)
We have computed adsorption energies, vibrational frequencies, surface relaxation and buckling for hydrogen adsorbed on a body-centred-cubic Fe(110) surface as a function of the degree of H coverage. This adsorption system is important in a variety of technological processes such as the hydrogen embrittlement in ferritic steels, which motivated this work, and the Haber–Bosch process. We employed spin-polarised density functional theory to optimise geometries of a six-layer Fe slab, followed by frozen mode finite displacement phonon calculations to compute Fe–H vibrational frequencies. We have found that the quasi-threefold (3f) site is the most stable adsorption site, with adsorption energies of ∼3.0 eV/H for all coverages studied. The long-bridge (lb) site, which is close in energy to the 3f site, is actually a transition state leading to the stable 3f site. The calculated harmonic vibrational frequencies collectively span from 730 to 1220 cm−1, for a range of coverages. The increased first-to-second layer spacing in the presence of adsorbed hydrogen, and the pronounced buckling observed in the Fe surface layer, may facilitate the diffusion of hydrogen atoms into the bulk, and therefore impact the early stages of hydrogen embrittlement in steels.
The ability to functionalize graphene with several methods, such as radical reactions, cycloadditions, hydrogenation, and oxidations, allows this material to be used in a large range of applications. In this framework, it is essential to be able to control the efficiency and stability of the functionalization process—this requires understanding how the graphene reactivity is affected by the environment, including the substrate. In this work we provide an insight on the substrate dependence of graphene reactivity towards hydrogenation by comparing three different substrates: silicon, hexagonal boron nitride (h-BN), and molybdenum disulfide (MoS2). Although MoS2 and h-BN have flatter surfaces than silicon, we found that the H coverage of graphene on h-BN is about half of the H coverage on graphene on both silicon and MoS2. Therefore, graphene shows strongly reduced reactivity towards hydrogenation when placed on h-BN. The difference in hydrogenation reactivity between h-BN and MoS2 may indicate a stronger van der Waals force between graphene and h-BN, compared to MoS2, or may be related to the chemical properties of MoS2, which is a well-known catalyst for hydrogen evolution reactions.
A proven method to enhance the mechanical properties of additively manufactured plastic parts is the embedding of continuous fibers. Due to its great flexibility, continuous fiber-reinforced material extrusion allows fiber strands to be deposited along optimized paths. Nevertheless, the fibers have so far been embedded in the parts contour-based or on the basis of regular patterns. The outstanding strength and stiffness properties of the fibers in the longitudinal direction cannot be optimally utilized. Therefore, a method is proposed which allows to embed fibers along the principal stresses into the parts in a load-oriented manner. A G-code is generated from the calculated principal stress trajectories and the part geometry, which also takes into account the specific restrictions of the manufacturing technology used. A distinction is made between fiber paths and the matrix so that the average fiber volume content can be set in a defined way. To determine the mechanical properties, tensile and flexural tests are carried out on specimens consisting of carbon fiber-reinforced polyamide. In order to increase the influence of the principal stress-based fiber orientation, open-hole plates are used for the tensile tests, as this leads to variable stresses across the cross section. In addition, a digital image correlation system is used to determine the deformations during the mechanical tests. It was found that the peak load of the optimized open-hole plates was greater by a factor of 3 and the optimized flexural specimens by a factor of 1.9 than the comparison specimens with unidirectional fiber alignment.