Qucosa – Hemholtz-Zentrum Dresden-Rossendorf
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On the Effect of Thin Film Growth Mechanisms on the Specular Reflectance of Aluminium Thin Films Deposited via Filtered Cathodic Vacuum Arc
The optimisation of the specular reflectance of solar collectors is a key parameter to increase the global yield of concentrated solar power (CSP) plants. In this work, the influence of filtered cathodic vacuum arc deposition parameters, particularly working pressure and deposition time, on the specular and diffuse reflectance of aluminium thin films, was studied. Changes in specular reflectance, measured by ultraviolet–visible and near-infrared spectroscopy (UV-vis-NIR) spectrophotometry, were directly correlated with thin film elemental concentration depth profiles, obtained by Rutherford backscattering spectrometry (RBS), and surface and cross-sectional morphologies as measured by scanning electron microscopy (SEM) and profilometry. Finally, atomic force microscopy (AFM) provided information on the roughness and growth mechanism of the films. The two contributions to the total reflectance of the films, namely diffuse and specular reflectance, were found to be deeply influenced by deposition conditions. It was proven that working pressure and deposition time directly determine the predominant factor. Specular reflectance varied from 12 to 99.8% of the total reflectance for films grown at the same working pressure of 0.1 Pa and with different deposition times. This transformation could not be attributed to an oxidation of the films as stated by RBS, but was correlated with a progressive modification of the roughness, surface, and bulk morphology of the samples over the deposition time. Hence, the evolution in the final optical properties of the films is driven by different growth mechanisms and the resulting microstructures. In addition to the originally addressed CSP applications the potential of the developed aluminium films for other application rather than CSP, such as, for example, reference material for spectroscopic diffuse reflectance measurements, is also discussed
Design of high-temperature solar-selective coatings based on aluminium titanium oxynitrides AlyTi1-y(OxN1-x). Part 1: Advanced microstructural characterisation and optical simulation
Aluminium titanium oxynitrides were studied as candidate materials for high temperature absorbers in solar selective coatings due to their excellent stability and their tuneable optical behaviour. A set of individual AlyTi1-y(OxN1-x) layers with different oxygen content was prepared by cathodic vacuum arc (CVA) deposition. The composition, morphology, phase structure and microstructure of the films were characterized by elastic recoil detection (ERD), scanning and transmission electron microscopy and X-ray diffraction. An fcc phase structure is found in a broad compositional range of AlyTi1-y(OxN1-x). Simultaneously, sample microstructure and morphology undergo systematic changes from a columnar growth to the development of a heterogeneous structure with spherical nanoparticle inclusions when the oxygen concentration is increased. The optical properties were determined by spectroscopic ellipsometry and UV–Vis–NIR and FTIR spectrophotometry. A comprehensive analysis of the film properties allowed an accurate modelling of the optical constants of the AlyTi1-y(OxN1-x) in the whole wavelength range of solar interest (from 190 nm to 25 µm). It points to a transition from metallic to dielectric behaviour with increasing oxygen content. Consequently, it is demonstrated that the optical properties of these AlyTi1-y(OxN1-x) deposited films can be controlled in a wide range from metallic to dielectric character by adjusting the oxygen concentration, opening a huge range of possibilities for the design of solar selective coatings (SSC) based on this material. Complete SSC, including a TiN layer as IR reflector, were designed by applying optical simulations, obtaining excellent optical selective properties of α=94.0% and εRT = 4.8%
Transverse electron beam dynamics in the beam loading regime
GeV electron bunches accelerated on a centimeter scale device exemplify the extraordinary advances of laser-plasma acceleration. The combination of high charges from optimized injection schemes and intrinsic femtosecond short bunch duration yields kiloampere peak currents. Further enhancing the current while reducing the energy spread will pave the way for future application, e.g. the driver for compact secondary radiation sources such as high-field THz, high-brightness x-ray or gamma-ray sources. One essential key for beam transport to a specific application is an electron bunch with high quality beam parameters such as low energy spread as well as small divergence and spot size. The inherent micrometer size at the plasma exit is typically sufficient for an efficient coupling into a conventional beamline. However, energy spread and beam divergence require optimization before the beam can be transported efficiently. Induced by the high peak current, the beam loading regime can be used in order to achieve optimized beam parameters for beam transport.In this thesis, the impact of beam loading on the transverse electron dynamic is systematically studied by investigating betatron radiation and electron beam divergence. For this reason, the bubble regime with self-truncated ionization injection (STII) is applied to set up a nanocoulomb-class laser wakefield accelerator. The accelerator is driven by 150TW laser pulses from the DRACO high power laser system. A supersonic gas jet provides a 3mm long acceleration medium with electron densities from 3 × 10^18 cm^−3 to 5 × 10^18 cm^−3. The STII scheme together with the employed setup yields highly reproducible injections with bunch charges of up to 0.5 nC. The recorded betatron radius at the accelerator exit is about one micron and reveals that the beam size stays at the same value. The optimal beam loading, which is observed at around 250 pC to 300 pC, leads to the minimum energy spread of ~40MeV and a 20% smaller divergence. It is demonstrated that an incomplete betatron phase mixing due to the small energy spread can explain the experimentally observed minimum beam divergence
Infrared nanospectroscopy at cryogenic temperatures and on semiconductor nanowires
This PhD thesis concentrates on scattering scanning near-field infrared microscopy (s-SNIM) which utilizes the radiation from the free-electron laser (FEL) at the Helmholtz-Zentrum Dresden-Rossendorf. The FEL is an intense, narrow-band radiation source, tunable from the mid- to far-infrared spectral range (5 meV to 250 meV). The s-SNIM technique enables infrared microscopy and spectroscopy with a wavelength-independent spatial resolution of about 10nm. The first part demonstrates the extension of s-SNIM at the FEL towards cryogenic temperatures as low as 5K. To this end, we show the functionality of our low-temperature s-SNIM apparatus on different samples such as Au, structured Si/SiO2, as well as the multiferroic material gallium vanadium sulfide (GaV4S8). The latter material recently attracted a lot of interest since it hosts a Néel-type skyrmion lattice – a periodic array of spin vortices. Below T = 42K, GaV4S8 undergoes a structural phase transition and then forms ferroelectric domains, which we can map out by low-tempererature s-SNIM. Notably, we found a strong impact on the ferroelectric domains upon infrared irradiation, which we further utilize to calibrate the local heat contribution of the focused infrared beam beneath the s-SNIM probe.The second part of this thesis contains comprehensive s-SNIM investigations of high-quality semiconductor nanowires (NWs) rown by molecular beam epitaxy. Such NWs are promising building blocks for fast (opto-)electronic nanodevices, amongst thers due to their high carrier mobility. We have examined highly doped GaAs/InGaAs core/shell NWs and observed a strong and spectrally sharp plasmonic resonance at about hw = 125 meV, using a continuous wave CO2 laser for probing. If we probe the same NWs utilizing the intense, pulsed FEL radiation, we observe a pronounced redshift to hw < 100 meV and a broading of the plasmonic response. This nonlinear response is most likely induced by heating of the electron gas upon irradiation by the strong FEL pulses. Our observations open up the possibility to actively induce and observe non-equilibrium states in s-SNIM directly by the mid-infrared beam. Beside the nonlinear effect, we prepared and measured cross sections of both homogeneously-doped and modulation-doped core/shell NWs
Annual Report 2018 - Institute of Resource Ecology
Annual Report 2018 of the scientific activities of the Institute of Resource Ecology of the Helmholtz-Zentrum Dresden-Rossendor
Transparent Conductive Tantalum Doped Tin Oxide as Selectively Solar-Transmitting Coating for High Temperature Solar Thermal Applications
The transparent conductive oxide (TCO) SnO2:Ta is developed as a selectively solar-transmitting coating for concentrated solar power (CSP) absorbers. Upon covering with an antireflective layer, a calculated absorptivity of 95% and an emissivity of 30% are achieved for the model configuration of SnO2:Ta on top of a perfect black body (BB). High-temperature stability of the developed TCO up to 1073 K is shown in situ by spectroscopic ellipsometry and Rutherford backscattering spectrometry. The universality of the concept is demonstrated by transforming silicon and glassy carbon from non-selective into solar-selective absorbers by depositing the TCO on top of them. Finally, the energy conversion efficiencies of SnO2:Ta on top of a BB and an ideal non-selective BB absorber are extensively compared as a function of solar concentration factor C and absorber temperature TH. Equal CSP efficiencies can be achieved by the TCO on BB configuration with approximately 50% lower solar concentration. This improvement could be used to reduce the number of mirrors in a solar plant, and thus, the levelized costs of electricity for CSP technology
Room temperature deposition of highly dense TiO2 thin films by Filtered Cathodic Vacuum Arc
A systematic study of TiO2 films deposited by dc filtered cathodic vacuum arc (FCVA) was carried out by varying the deposition parameters in a reactive oxygen atmosphere. The influence of the oxygen partial pressure on film properties is analyzed. Composition was obtained by Rutherford backscattering spectroscopy (RBS) measurements, which also allow us to obtain the density of the films. Morphology of the samples was studied by scanning electron microscopy (SEM) and their optical properties by ellipsometry. Transparent, very dense and stoichiometric TiO2 films were obtained by FCVA at room temperatur
Ultrafast Response of Photoexcited Carriers in Transition Metal Oxides under High Pressure
In this work, optical pump – near-infrared probe and near-infrared pump – mid-infrared probe spectroscopy are used for the investigation of pressure-induced insulator-tometal transitions in transition metal oxide compounds. The materials under study are a-Fe₂O₃, also known as hematite, and VO₂. Both materials undergo pressureinduced metallization. However, the physical mechanisms of this phase transition are very different for these systems and have not been fully understood up to now. Using ultrafast pump-probe spectroscopy we obtain an insight into the evolution of the band structure and electron dynamics across the insulator-to-metal transition.
In the case of VO₂, our near-infrared pump – mid-infrared probe experiments reveal a non-vanishing pumping threshold for photo-induced metallization even at our highest pressures around 20 GPa. This demonstrates the existence of localized charge carriers and the corresponding persistence of a band gap. Besides the threshold behaviour for photo-induced metallization, the carrier relaxation time scale, and the linear reflectivity and transmissivity have been studied under pressure increase. An anomaly in the threshold behaviour as well as the linear reflectivity and transmissivity at a critical pressure around 7 GPa indicates band gap filling under pressure. This is further supported by results obtained under decompression, where the changes of the linear reflectivity turned out to be almost fully reversible. The observations on VO₂ are highly reproducible and can be explained in terms of a pressure-induced bandwidth-driven insulator-to-metal transition.
Fe₂O₃ has been studied via optical pump – near-infrared probe spectroscopy up to pressures of 60 GPa. In the pressure range up to 40 GPa, the changes of the response can be explained by photo-induced absorption and bleaching. The pressure-dependent study of the relaxation dynamics allows to identify cooling of the electron system as origin of the picosecond relaxation process
Radiotherapy Beamline Design for Laser-driven Proton Beams
Motivation: Radiotherapy is an important modality in cancer treatment commonly using photon beams from compact electron linear accelerators. However, due to the inverse depth dose profile (Bragg peak) with maximum dose deposition at the end of their path, proton beams allow a dose escalation within the target volume and reduction in surrounding normal tissue. Up to 20% of all radiotherapy patients could benefit from proton therapy (PT). Conventional accelerators are utilized to obtain proton beams with therapeutic energies of 70 – 250 MeV. These beams are then transported to the patient via magnetic transferlines and a rotatable beamline, called gantry, which are large and bulky. PT requires huge capex, limiting it to only a few big centres worldwide treating much less than 1% of radiotherapy patients. The new particle acceleration by ultra-intense laser pulses occurs on micrometer scales, potentially enabling more compact PT facilities and increasing their widespread. These laser-accelerated proton (LAP) bunches have been observed recently with energies of up to 90 MeV and scaling models predict LAP with therapeutic energies with the next generation petawatt laser systems
Cluster tool for in situ processing and comprehensive characterization of thin films at high temperatures
A new cluster tool for in situ real-time processing and depth-resolved compositional, structural and optical characterization of thin films at temperatures from -100 to 800 °C is described. The implemented techniques comprise magnetron sputtering, ion irradiation, Rutherford backscattering spectrometry, Raman spectroscopy and spectroscopic ellipsometry. The capability of the cluster tool is demonstrated for a layer stack MgO/ amorphous Si (~60 nm)/ Ag (~30 nm), deposited at room temperature and crystallized with partial layer exchange by heating up to 650°C. Its initial and final composition, stacking order and structure were monitored in situ in real time and a reaction progress was defined as a function of time and temperature