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Institute
- Institut für Physik und Astronomie (312) (remove)
Advancing charge selective contacts for efficient monolithic perovskite-silicon tandem solar cells
(2019)
Hybrid organic-inorganic perovskites are one of the most promising material classes for photovoltaic energy conversion. In solar cells, the perovskite absorber is sandwiched between n- and p-type contact layers which selectively transport electrons and holes to the cell’s cathode and anode, respectively. This thesis aims to advance contact layers in perovskite solar cells and unravel the impact of interface and contact properties on the device performance. Further, the contact materials are applied in monolithic perovskite-silicon heterojunction (SHJ) tandem solar cells, which can overcome the single junction efficiency limits and attract increasing attention. Therefore, all contact layers must be highly transparent to foster light harvesting in the tandem solar cell design. Besides, the SHJ device restricts processing temperatures for the selective contacts to below 200°C.
A comparative study of various electron selective contact materials, all processed below 180°C, in n-i-p type perovskite solar cells highlights that selective contacts and their interfaces to the absorber govern the overall device performance. Combining fullerenes and metal-oxides in a TiO2/PC60BM (phenyl-C60-butyric acid methyl ester) double-layer contact allows to merge good charge extraction with minimized interface recombination. The layer sequence thereby achieved high stabilized solar cell performances up to 18.0% and negligible current-voltage hysteresis, an otherwise pronounced phenomenon in this device design. Double-layer structures are therefore emphasized as a general concept to establish efficient and highly selective contacts.
Based on this success, the concept to combine desired properties of different materials is transferred to the p-type contact. Here, a mixture of the small molecule Spiro-OMeTAD [2,2’,7,7’-tetrakis(N,N-di-p-methoxyphenylamine)-9,9’-spirobifluoren] and the doped polymer PEDOT [poly(3,4-ethylenedioxythiophene)] is presented as a novel hole selective contact. PEDOT thereby remarkably suppresses charge recombination at the perovskite surface, allowing an increase of quasi-Fermi level splitting in the absorber. Further, the addition of Spiro-OMeTAD into the PEDOT layer is shown to enhance charge extraction at the interface and allow high efficiencies up to 16.8%.
Finally, the knowledge on contact properties is applied to monolithic perovskite-SHJ tandem solar cells. The main goal is to optimize the top contact stack of doped Spiro-OMeTAD/molybdenum oxide(MoOx)/ITO towards higher transparency by two different routes. First, fine-tuning of the ITO deposition to mitigate chemical reduction of MoOx and increase the transmittance of MoOx/ITO stacks by 25%. Second, replacing Spiro-OMeTAD with the alternative hole transport materials PEDOT/Spiro-OMeTAD mixtures, CuSCN or PTAA [poly(triaryl amine)]. Experimental results determine layer thickness constrains and validate optical simulations, which subsequently allow to realistically estimate the respective tandem device performances. As a result, PTAA represents the most promising replacement for Spiro-OMeTAD, with a projected increase of the optimum tandem device efficiency for the herein used architecture by 2.9% relative to 26.5% absolute. The results also reveal general guidelines for further performance gains of the technology.
The unceasing impact of intense sunlight on earth constitutes a continuous source of energy fueling countless natural processes. On a molecular level, the energy contained in the electromagnetic radiation is transferred through photochemical processes into chemical or thermal energy. In the course of such processes, photo-excitations promote molecules into thermally inaccessible excited states. This induces adaptations of their molecular geometry according to the properties of the excited state. Decay processes towards energetically lower lying states in transient molecular geometries result in the formation of excited state relaxation pathways. The photo-chemical relaxation mechanisms depend on the studied system itself, the interactions with its chemical environment and the character of the involved states. This thesis focuses on systems in which photo-induced deprotonation processes occur at specific atomic sites.
To detect these excited-state proton dynamics at the affected atoms, a local probe of molecular electronic structure is required. Therefore, site-selective and orbital-specific K-edge soft X-ray spectroscopy techniques are used here to detect photo-induced proton dynamics in gaseous and liquid sample environments. The protonation of nitrogen (N) sites in organic molecules and the oxygen (O) atom in the water molecule are probed locally through transitions between 1s orbitals and the p-derived molecular valence electronic structure. The used techniques are X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS). Both yield access to the unoccupied local valence electronic structure, whereas the latter additionally probes occupied states.
We apply these probes in optical pump X-ray probe experiments to investigate valence excited-state proton transfer capabilities of aqueous 2-thiopyridone. A characteristic shift of N K-edge X-ray absorption resonances as well as a distinct X-ray emission line are established by us as spectral fingerprints of N deprotonation in the system. We utilize them to identify photo-induced N deprotonation of 2-thiopyridone on femtosecond timescales, in optical pump N K-edge RIXS probe measurements. We further establish excited state proton transfer mechanisms on picosecond and nanosecond timescales along the dominant relaxation pathways of 2-thiopyridone using transient N K-edge XAS.
Despite being an excellent probe mechanism for valence excited-state proton dynamics, the K-edge core-excitation itself also disturbs the electronic structure at specific sites of a molecule. The rapid reaction of protons to 1s photo-excitations can yield directional structural distortions within the femtosecond core-excited state lifetime. These directional proton dynamics can change the energetic separation of eigenstates of the system and alter probabilities for radiative decay between them. Both effects yield spectral signatures of the dynamics in RIXS spectra.
Using these signatures of RIXS transitions into electronically excited states, we investigate proton dynamics induced by N K-edge excitation in the amino-acid histidine. The minor core-excited state dynamics of histidine in basic and neutral chemical environments allow us to establish XAS and RIXS spectral signatures of different N protonation states at its imidazole N sites. Based on these signatures, we identify an excitation-site-independent N-H dissociation for N K-edge excitation under acidic conditions.
Such directional structural deformations, induced by core-excitations, also make proton dynamics in electronic ground states accessible through RIXS transitions into vibrationally excited states. In that context, we interpret high resolution RIXS spectra of the water molecule for three O K-edge resonances based on quantum-chemical wave packet propagation simulations. We show that highly oriented ground state vibrational modes of coupled nuclear motion can be populated through RIXS processes by preparation of core-excited state nuclear wave packets with the same directionality. Based on that, we analytically derive the possibility to extract one-dimensional directional cuts through potential energy surfaces of molecular systems from the corresponding RIXS spectra. We further verify this concept through the extraction of the gas-phase water ground state potential along three coordinates from experimental data in comparison to quantum-chemical simulations of the potential energy surface.
This thesis also contains contributions to instrumentation development for investigations of photo-induced molecular dynamics at high brilliance X-ray light sources. We characterize the setup used for the transient valence-excited state XAS measurements of 2-thiopyridone. Therein, a sub-micrometer thin liquid sample environment is established employing in-vacuum flat-jet technology, which enables a transmission experimental geometry. In combination with a MHz-laser system, we achieve a high detection sensitivity for photo-induced X-ray absorption changes. Additionally, we present conceptual improvements for temporal X-ray optical cross-correlation techniques based on transient changes of multilayer optical properties, which are crucial for the realization of femtosecond time-resolved studies at synchrotrons and free-electron lasers.
The nitrogen and sulfur K-edge X-ray absorption spectra of aqueous 2-thiopyridone, a model system for excited-state proton transfer in several recent time-resolved measurements, have been simulated from ab initio molecular dynamics. Spectral signatures of the local intra- and inter-molecular structure are identified and rationalized, which facilitates experimental interpretation and optimization. In particular, comparison of aqueous and gas phase spectrum simulations assesses the previously unquantified solvatization effects, where hydrogen bonding is found to yield solvatochromatic shifts up to nearly 1 eV of the main peak positions. Thereby, while each K-edge can still decisively determine the local protonation of its core-excited site, only their combined, complementary fingerprints allow separating all of the three relevant molecular forms, giving a complete picture of the proton transfer.
Gamma-ray bursts (GRBs) are brief flashes of gamma-rays and are considered to be the most energetic explosive phenomena in the Universe(1). The emission from GRBs comprises a short (typically tens of seconds) and bright prompt emission, followed by a much longer afterglow phase. During the afterglow phase, the shocked outflow-produced by the interaction between the ejected matter and the circumburst medium-slows down, and a gradual decrease in brightness is observed(2). GRBs typically emit most of their energy via.-rays with energies in the kiloelectronvolt-to-megaelectronvolt range, but a few photons with energies of tens of gigaelectronvolts have been detected by space-based instruments(3). However, the origins of such high-energy (above one gigaelectronvolt) photons and the presence of very-high-energy (more than 100 gigaelectronvolts) emission have remained elusive(4). Here we report observations of very-high-energy emission in the bright GRB 180720B deep in the GRB afterglow-ten hours after the end of the prompt emission phase, when the X-ray flux had already decayed by four orders of magnitude. Two possible explanations exist for the observed radiation: inverse Compton emission and synchrotron emission of ultrarelativistic electrons. Our observations show that the energy fluxes in the X-ray and gamma-ray range and their photon indices remain comparable to each other throughout the afterglow. This discovery places distinct constraints on the GRB environment for both emission mechanisms, with the inverse Compton explanation alleviating the particle energy requirements for the emission observed at late times. The late timing of this detection has consequences for the future observations of GRBs at the highest energies.
Context. Galactic globular clusters (GCs) are now known to host multiple populations displaying particular abundance variations. The different populations within a GC can be well distinguished following their position in the pseudo two-colors diagrams, also referred to as "chromosome maps". These maps are constructed using optical and near-UV photometry available from the Hubble Space Telescope (HST) UV survey of GCs. However, the chemical tagging of the various populations in the chromosome maps is hampered by the fact that HST photometry and elemental abundances are both only available for a limited number of stars. Aims. The spectra collected as part of the MUSE survey of globular clusters provide a spectroscopic counterpart to the HST photometric catalogs covering the central regions of GCs. In this paper, we use the MUSE spectra of 1115 red giant branch (RGB) stars in NGC 2808 to characterize the abundance variations seen in the multiple populations of this cluster. Methods. We used the chromosome map of NGC 2808 to divide the RGB stars into their respective populations. We then combined the spectra of all stars belonging to a given population, resulting in one high signal-to-noise ratio spectrum representative of each population. Results. Variations in the spectral lines of O, Na, Mg, and Al are clearly detected among four of the populations. In order to quantify these variations, we measured equivalent width differences and created synthetic populations spectra that were used to determine abundance variations with respect to the primordial population of the cluster. Our results are in good agreement with the values expected from previous studies based on high-resolution spectroscopy. We do not see any significant variations in the spectral lines of Ca, K, and Ba. We also do not detect abundance variations among the stars belonging to the primordial population of NGC 2808. Conclusions. We demonstrate that in spite of their low resolution, the MUSE spectra can be used to investigate abundance variations in the context of multiple populations.
We utilise multi-epoch MUSE spectroscopy to study binary stars in the core of the Galactic globular cluster NGC 3201. Our sample consists of 3553 stars with 54 883 spectra in total comprising 3200 main-sequence stars up to 4 magnitudes below the turn-off. Each star in our sample has between 3 and 63 (with a median of 14) reliable radial velocity measurements within five years of observations. We introduce a statistical method to determine the probability of a star showing radial velocity variations based on the whole inhomogeneous radial velocity sample. Using HST photometry and an advanced dynamical MOCCA simulation of this specific cluster we overcome observational biases that previous spectroscopic studies had to deal with. This allows us to infer a binary frequency in the MUSE field of view and enables us to deduce the underlying true binary frequency of (6.75 +/- 0.72)% in NGC 3201. The comparison of the MUSE observations with the MOCCA simulation suggests a large portion of primordial binaries. We can also confirm a radial increase in the binary fraction towards the cluster centre due to mass segregation. We discovered that in the core of NGC 3201 at least (57.5 +/- 7.9)% of blue straggler stars are in a binary system. For the first time in a study of globular clusters, we were able to fit Keplerian orbits to a significant sample of 95 binaries. We present the binary system properties of eleven blue straggler stars and the connection to SX Phoenicis-type stars. We show evidence that two blue straggler formation scenarios, the mass transfer in binary (or triple) star systems and the coalescence due to binary-binary interactions, are present in our data. We also describe the binary and spectroscopic properties of four sub-subgiant (or red straggler) stars. Furthermore, we discovered two new black hole candidates with minimum masses (M sin i) of (7.68 +/- 0.50)M-circle dot, (4.4 +/- 2.8)M-circle dot, and refine the minimum mass estimate on the already published black hole to (4.53 +/- 0.21)M-circle dot, These black holes are consistent with an extensive black hole subsystem hosted by NGC 3201.
A stellar census in globular clusters with MUSE: A spectral catalogue of emission-line sources
(2019)
Aims. Globular clusters produce many exotic stars due to a much higher frequency of dynamical interactions in their dense stellar environments. Some of these objects were observed together with several hundred thousand other stars in our MUSE survey of 26 Galactic globular clusters. Assuming that at least a few exotic stars have exotic spectra (i.e. spectra that contain emission lines), we can use this large spectroscopic data set of over a million stellar spectra as a blind survey to detect stellar exotica in globular clusters. Methods. To detect emission lines in each spectrum, we modelled the expected shape of an emission line as a Gaussian curve. This template was used for matched filtering on the di fferences between each observed 1D spectrum and its fitted spectral model. The spectra with the most significant detections of H alpha emission are checked visually and cross-matched with published catalogues. Results. We find 156 stars with H alpha emission, including several known cataclysmic variables (CV) and two new CVs, pulsating variable stars, eclipsing binary stars, the optical counterpart of a known black hole, several probable sub-subgiants and red stragglers, and 21 background emission-line galaxies. We find possible optical counterparts to 39 X-ray sources, as we detected H alpha emission in several spectra of stars that are close to known positions of Chandra X-ray sources. This spectral catalogue can be used to supplement existing or future X-ray or radio observations with spectra of potential optical counterparts to classify the sources.
Over large coastal regions in Greenland and Antarctica the ice sheet calves directly into the ocean. In contrast to ice-shelf calving, an increase in calving from grounded glaciers contributes directly to sea-level rise. Ice cliffs with a glacier freeboard larger than approximate to 100 m are currently not observed, but it has been shown that such ice cliffs are increasingly unstable with increasing ice thickness. This cliff calving can constitute a self-amplifying ice loss mechanism that may significantly alter sea-level projections both of Greenland and Antarctica. Here we seek to derive a minimalist stress-based parametrization for cliff calving from grounded glaciers whose freeboards exceed the 100m stability limit derived in previous studies. This will be an extension of existing calving laws for tidewater glaciers to higher ice cliffs. To this end we compute the stress field for a glacier with a simplified two-dimensional geometry from the two-dimensional Stokes equation. First we assume a constant yield stress to derive the failure region at the glacier front from the stress field within the glacier. Secondly, we assume a constant response time of ice failure due to exceedance of the yield stress. With this strongly constraining but very simple set of assumptions we propose a cliff-calving law where the calving rate follows a power-law dependence on the freeboard of the ice with exponents between 2 and 3, depending on the relative water depth at the calving front. The critical freeboard below which the ice front is stable decreases with increasing relative water depth of the calving front. For a dry water front it is, for example, 75 m. The purpose of this study is not to provide a comprehensive calving law but to derive a particularly simple equation with a transparent and minimalist set of assumptions.
A Search for Pulsed Very High-energy Gamma-Rays from 13 Young Pulsars in Archival VERITAS Data
(2019)
We conduct a search for periodic emission in the very high-energy (VHE) gamma-ray band (E > 100 GeV) from a total of 13 pulsars in an archival VERITAS data set with a total exposure of over 450 hr. The set of pulsars includes many of the brightest young gamma-ray pulsars visible in the Northern Hemisphere. The data analysis resulted in nondetections of pulsed VHE gamma-rays from each pulsar. Upper limits on a potential VHE gamma-ray flux are derived at the 95% confidence level above three energy thresholds using two methods. These are the first such searches for pulsed VHE emission from each of the pulsars, and the obtained limits constrain a possible flux component manifesting at VHEs as is seen for the Crab pulsar.
Aims. We investigated the ionisation conditions and distances of Galactic high-velocity clouds (HVCs) in the Galactic halo and beyond in the direction of the Local Group (LG) barycentre and anti-barycentre, by studying spectral data of 29 extragalactic background sources obtained with the Cosmic Origins Spectropgraph (COS) installed on the Hubble Space Telescope (HST). Methods. We model column-densities of low, intermediate, and high ions such as Si ii, C ii, Si iii, Si vi, and C iv, and use these data to construct a set of Cloudy ionisation models. Results. In total, we found 69 high-velocity absorption components along the 29 lines of sight. The components in the direction of the LG barycentre span the entire range of studied velocities, 100 less than or similar to vertical bar nu(LSR)vertical bar less than or similar to 400 km s(-1), while those in the anti-barycentre sample have velocities up to about 300 km s(-1). For 49 components, we infer the gas densities. In the direction of the LG barycentre, the gas densities exhibit a wide range from log nH = -3.96 to -2.55, while in the anti-barycentre direction the densities are systematically higher, log nH > -3.25. The barycentre absorbers can be split into two groups based on their density: a high-density group with log nH > -3.54, which can be affected by the Milky Way radiation field, and a low-density group (log nH <= -3.54). The latter has very low thermal pressures of P/k < 7.3 Kcm(-3). Conclusions. Our study shows that part of the absorbers in the LG barycentre direction trace gas at very low gas densities and thermal pressures. These properties indicate that the absorbers are located beyond the virial radius of the Milky Way. Our study also confirms results from earlier, single-sightline studies, suggesting the presence of a metal-enriched intragroup medium filling the LG near its barycentre.
Additive Manufacturing (AM) in terms of laser powder-bed fusion (L-PBF) offers new prospects regarding the design of parts and enables therefore the production of lattice structures. These lattice structures shall be implemented in various industrial applications (e.g. gas turbines) for reasons of material savings or cooling channels. However, internal defects, residual stress, and structural deviations from the nominal geometry are unavoidable.
In this work, the structural integrity of lattice structures manufactured by means of L-PBF was non-destructively investigated on a multiscale approach.
A workflow for quantitative 3D powder analysis in terms of particle size, particle shape, particle porosity, inter-particle distance and packing density was established. Synchrotron computed tomography (CT) was used to correlate the packing density with the particle size and particle shape. It was also observed that at least about 50% of the powder porosity was released during production of the struts.
Struts are the component of lattice structures and were investigated by means of laboratory CT. The focus was on the influence of the build angle on part porosity and surface quality. The surface topography analysis was advanced by the quantitative characterisation of re-entrant surface features. This characterisation was compared with conventional surface parameters showing their complementary information, but also the need for AM specific surface parameters.
The mechanical behaviour of the lattice structure was investigated with in-situ CT under compression and successive digital volume correlation (DVC). The deformation was found to be knot-dominated, and therefore the lattice folds unit cell layer wise.
The residual stress was determined experimentally for the first time in such lattice structures. Neutron diffraction was used for the non-destructive 3D stress investigation. The principal stress directions and values were determined in dependence of the number of measured directions. While a significant uni-axial stress state was found in the strut, a more hydrostatic stress state was found in the knot. In both cases, strut and knot, seven directions were at least needed to find reliable principal stress directions.
Already for decades it has been known that the winds of massive stars are inhomogeneous (i.e. clumped). To properly model observed spectra of massive star winds it is necessary to incorporate the 3-D nature of clumping into radiative transfer calculations. In this paper we present our full 3-D Monte Carlo radiative transfer code for inhomogeneous expanding stellar winds. We use a set of parameters to describe dense as well as the rarefied wind components. At the same time, we account for non-monotonic velocity fields. We show how the 3-D density and velocity wind inhomogeneities strongly affect the resonance line formation. We also show how wind clumping can solve the discrepancy between P v and H alpha mass-loss rate diagnostics.