@phdthesis{Anders2017, author = {Anders, Friedrich}, title = {Disentangling the chemodynamical history of the Milky Way disc with asteroseismology and spectroscopy}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-396681}, school = {Universit{\"a}t Potsdam}, pages = {121}, year = {2017}, abstract = {Galaxies are among the most complex systems that can currently be modelled with a computer. A realistic simulation must take into account cosmology and gravitation as well as effects of plasma, nuclear, and particle physics that occur on very different time, length, and energy scales. The Milky Way is the ideal test bench for such simulations, because we can observe millions of its individual stars whose kinematics and chemical composition are records of the evolution of our Galaxy. Thanks to the advent of multi-object spectroscopic surveys, we can systematically study stellar populations in a much larger volume of the Milky Way. While the wealth of new data will certainly revolutionise our picture of the formation and evolution of our Galaxy and galaxies in general, the big-data era of Galactic astronomy also confronts us with new observational, theoretical, and computational challenges. This thesis aims at finding new observational constraints to test Milky-Way models, primarily based on infra-red spectroscopy from the Apache Point Observatory Galactic Evolution Experiment (APOGEE) and asteroseismic data from the CoRoT mission. We compare our findings with chemical-evolution models and more sophisticated chemodynamical simulations. In particular we use the new powerful technique of combining asteroseismic and spectroscopic observations that allows us to test the time dimension of such models for the first time. With CoRoT and APOGEE (CoRoGEE) we can infer much more precise ages for distant field red-giant stars, opening up a new window for Galactic archaeology. Another important aspect of this work is the forward-simulation approach that we pursued when interpreting these complex datasets and comparing them to chemodynamical models. The first part of the thesis contains the first chemodynamical study conducted with the APOGEE survey. Our sample comprises more than 20,000 red-giant stars located within 6 kpc from the Sun, and thus greatly enlarges the Galactic volume covered with high-resolution spectroscopic observations. Because APOGEE is much less affected by interstellar dust extinction, the sample covers the disc regions very close to the Galactic plane that are typically avoided by optical surveys. This allows us to investigate the chemo-kinematic properties of the Milky Way's thin disc outside the solar vicinity. We measure, for the first time with high-resolution data, the radial metallicity gradient of the disc as a function of distance from the Galactic plane, demonstrating that the gradient flattens and even changes its sign for mid-plane distances greater than 1 kpc. Furthermore, we detect a gap between the high- and low-[\$\alpha\$/Fe] sequences in the chemical-abundance diagram (associated with the thin and thick disc) that unlike in previous surveys can hardly be explained by selection effects. Using 6D kinematic information, we also present chemical-abundance diagrams cleaned from stars on kinematically hot orbits. The data allow us to confirm without doubt that the scale length of the (chemically-defined) thick disc is significantly shorter than that of the thin disc. In the second part, we present our results of the first combination of asteroseismic and spectroscopic data in the context of Galactic Archaeology. We analyse APOGEE follow-up observations of 606 solar-like oscillating red giants in two CoRoT fields close to the Galactic plane. These stars cover a large radial range of the Galactic disc (4.5 kpc \$\lesssim R_{\rm Gal}\lesssim15\$ kpc) and a large age baseline (0.5 Gyr \$\lesssim \tau\lesssim\$ 13 Gyr), allowing us to study the age- and radius-dependence of the [\$\alpha\$/Fe] vs. [Fe/H] distributions. We find that the age distribution of the high-[\$\alpha\$/Fe] sequence appears to be broader than expected from a monolithically-formed old thick disc that stopped to form stars 10 Gyr ago. In particular, we discover a significant population of apparently young, [\$\alpha\$/Fe]-rich stars in the CoRoGEE data whose existence cannot be explained by standard chemical-evolution models. These peculiar stars are much more abundant in the inner CoRoT field LRc01 than in the outer-disc field LRc01, suggesting that at least part of this population has a chemical-evolution rather than a stellar-evolution origin, possibly due to a peculiar chemical-enrichment history of the inner disc. We also find that strong radial migration is needed to explain the abundance of super-metal-rich stars in the outer disc. Finally, we use the CoRoGEE sample to study the time evolution of the radial metallicity gradient in the thin disc, an observable that has been the subject of observational and theoretical debate for more than 20 years. By dividing the CoRoGEE dataset into six age bins, performing a careful statistical analysis of the radial [Fe/H], [O/H], and [Mg/Fe] distributions, and accounting for the biases introduced by the observation strategy, we obtain reliable gradient measurements. The slope of the radial [Fe/H] gradient of the young red-giant population (\$-0.058\pm0.008\$ [stat.] \$\pm0.003\$ [syst.] dex/kpc) is consistent with recent Cepheid data. For the age range of \$1-4\$ Gyr, the gradient steepens slightly (\$-0.066\pm0.007\pm0.002\$ dex/kpc), before flattening again to reach a value of \$\sim-0.03\$ dex/kpc for stars with ages between 6 and 10 Gyr. This age dependence of the [Fe/H] gradient can be explained by a nearly constant negative [Fe/H] gradient of \$\sim-0.07\$ dex/kpc in the interstellar medium over the past 10 Gyr, together with stellar heating and migration. Radial migration also offers a new explanation for the puzzling observation that intermediate-age open clusters in the solar vicinity (unlike field stars) tend to have higher metallicities than their younger counterparts. We suggest that non-migrating clusters are more likely to be kinematically disrupted, which creates a bias towards high-metallicity migrators from the inner disc and may even steepen the intermediate-age cluster abundance gradient.}, language = {en} } @article{BelasriTopalHeydenreichetal.2020, author = {Belasri, Khadija and Topal, Leila and Heydenreich, Matthias and Koch, Andreas and Kleinpeter, Erich and Fulop, Ferenc and Szatmari, Istvan}, title = {Synthesis and conformational analysis of naphthoxazine-fused phenanthrene derivatives}, series = {Molecules}, volume = {25}, journal = {Molecules}, number = {11}, publisher = {MDPI}, address = {Basel}, issn = {1420-3049}, doi = {10.3390/molecules25112524}, pages = {15}, year = {2020}, abstract = {The synthesis of new phenanthr[9,10-e][1,3]oxazines was achieved by the direct coupling of 9-phenanthrol with cyclic imines in the modified aza-Friedel-Crafts reaction followed by the ring closure of the resulting bifunctional aminophenanthrols with formaldehyde. Aminophenanthrol-type Mannich bases were synthesised and transformed to phenanthr[9,10-e][1,3]oxazines via [4 + 2] cycloaddition. Detailed NMR structural analyses of the new polyheterocycles as well as conformational studies including Density Functional Theory (DFT) modelling were performed. The relative stability of ortho-quinone methides (o-QMs) was calculated, the geometries obtained were compared with the experimentally determined NMR structures, and thereby, the regioselectivity of the reactions has been assigned.}, language = {en} } @phdthesis{Brosinsky2015, author = {Brosinsky, Arlena}, title = {Spectral fingerprinting}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-83369}, school = {Universit{\"a}t Potsdam}, pages = {VI, 117}, year = {2015}, abstract = {Current research on runoff and erosion processes, as well as an increasing demand for sustainable watershed management emphasize the need for an improved understanding of sediment dynamics. This involves the accurate assessment of erosion rates and sediment transfer, yield and origin. A variety of methods exist to capture these processes at the catchment scale. Among these, sediment fingerprinting, a technique to trace back the origin of sediment, has attracted increasing attention by the scientific community in recent years. It is a two-step procedure, based on the fundamental assumptions that potential sources of sediment can be reliably discriminated based on a set of characteristic 'fingerprint' properties, and that a comparison of source and sediment fingerprints allows to quantify the relative contribution of each source. This thesis aims at further assessing the potential of spectroscopy to assist and improve the sediment fingerprinting technique. Specifically, this work focuses on (1) whether potential sediment sources can be reliably identified based on spectral features ('fingerprints'), whether (2) these spectral fingerprints permit the quantification of relative source contribution, and whether (3) in situ derived source information is sufficient for this purpose. Furthermore, sediment fingerprinting using spectral information is applied in a study catchment to (4) identify major sources and observe how relative source contributions change between and within individual flood events. And finally, (5) spectral fingerprinting results are compared and combined with simultaneous sediment flux measurements to study sediment origin, transport and storage behaviour. For the sediment fingerprinting approach, soil samples were collected from potential sediment sources within the Is{\´a}bena catchment, a meso-scale basin in the central Spanish Pyrenees. Undisturbed samples of the upper soil layer were measured in situ using an ASD spectroradiometer and subsequently sampled for measurements in the laboratory. Suspended sediment was sampled automatically by means of ISCO samplers at the catchment as well as at the five major subcatchment outlets during flood events, and stored fine sediment from the channel bed was collected from 14 cross-sections along the main river. Artificial mixtures of known contributions were produced from source soil samples. Then, all source, sediment and mixture samples were dried and spectrally measured in the laboratory. Subsequently, colour coefficients and physically based features with relation to organic carbon, iron oxide, clay content and carbonate, were calculated from all in situ and laboratory spectra. Spectral parameters passing a number of prerequisite tests were submitted to principal component analyses to study natural clustering of samples, discriminant function analyses to observe source differentiation accuracy, and a mixing model for source contribution assessment. In addition, annual as well as flood event based suspended sediment fluxes from the catchment and its subcatchments were calculated from rainfall, water discharge and suspended sediment concentration measurements using rating curves and Quantile Regression Forests. Results of sediment flux monitoring were interpreted individually with respect to storage behaviour, compared to fingerprinting source ascriptions and combined with fingerprinting to assess their joint explanatory potential. In response to the key questions of this work, (1) three source types (land use) and five spatial sources (subcatchments) could be reliably discriminated based on spectral fingerprints. The artificial mixture experiment revealed that while (2) laboratory parameters permitted source contribution assessment, (3) the use of in situ derived information was insufficient. Apparently, high discrimination accuracy does not necessarily imply good quantification results. When applied to suspended sediment samples of the catchment outlet, the spectral fingerprinting approach was able to (4) quantify the major sediment sources: badlands and the Villacarli subcatchment, respectively, were identified as main contributors, which is consistent with field observations and previous studies. Thereby, source contribution was found to vary both, within and between individual flood events. Also sediment flux was found to vary considerably, annually as well as seasonally and on flood event base. Storage was confirmed to play an important role in the sediment dynamics of the studied catchment, whereas floods with lower total sediment yield tend to deposit and floods with higher yield rather remove material from the channel bed. Finally, a comparison of flux measurements with fingerprinting results highlighted the fact that (5) immediate transport from sources to the catchment outlet cannot be assumed. A combination of the two methods revealed different aspects of sediment dynamics that none of the techniques could have uncovered individually. In summary, spectral properties provide a fast, non-destructive, and cost-efficient means to discriminate and quantify sediment sources, whereas, unfortunately, straight-forward in situ collected source information is insufficient for the approach. Mixture modelling using artificial mixtures permits valuable insights into the capabilities and limitations of the method and similar experiments are strongly recommended to be performed in the future. Furthermore, a combination of techniques such as e.g. (spectral) sediment fingerprinting and sediment flux monitoring can provide comprehensive understanding of sediment dynamics.}, language = {en} } @misc{CoutoCruzErtanetal.2017, author = {Couto, Rafael C. and Cruz, Vinicius V. and Ertan, Emelie and Eckert, Sebastian and Fondell, Mattis and Dantz, Marcus and Kennedy, Brian and Schmitt, Thorsten and Pietzsch, Annette and Guimar{\~a}es, Freddy F. and {\AA}gren, Hans and Gel'mukhanov, Faris and Odelius, Michael and Kimberg, Victor and F{\"o}hlisch, Alexander}, title = {Selective gating to vibrational modes through resonant X-ray scattering}, series = {Postprints der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam : Mathematisch-Naturwissenschaftliche Reihe}, number = {1124}, issn = {1866-8372}, doi = {10.25932/publishup-43692}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-436926}, pages = {9}, year = {2017}, abstract = {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.}, language = {en} } @article{EhlertKlamroth2020, author = {Ehlert, Christopher and Klamroth, Tillmann}, title = {PSIXAS: A Psi4 plugin for efficient simulations of X-ray absorption spectra based on the transition-potential and Delta-Kohn-Sham method}, series = {Journal of computational chemistry : organic, inorganic, physical, biological}, volume = {41}, journal = {Journal of computational chemistry : organic, inorganic, physical, biological}, number = {19}, publisher = {Wiley}, address = {Hoboken}, issn = {0192-8651}, doi = {10.1002/jcc.26219}, pages = {1781 -- 1789}, year = {2020}, abstract = {Near edge X-ray absorption fine structure (NEXAFS) spectra and their pump-probe extension (PP-NEXAFS) offer insights into valence- and core-excited states. We present PSIXAS, a recent implementation for simulating NEXAFS and PP-NEXAFS spectra by means of the transition-potential and the Delta-Kohn-Sham method. The approach is implemented in form of a software plugin for the Psi4 code, which provides access to a wide selection of basis sets as well as density functionals. We briefly outline the theoretical foundation and the key aspects of the plugin. Then, we use the plugin to simulate PP-NEXAFS spectra of thymine, a system already investigated by others and us. It is found that larger, extended basis sets are needed to obtain more accurate absolute resonance positions. We further demonstrate that, in contrast to ordinary NEXAFS simulations, where the choice of the density functional plays a minor role for the shape of the spectrum, for PP-NEXAFS simulations the choice of the density functional is important. Especially hybrid functionals (which could not be used straightforwardly before to simulate PP-NEXAFS spectra) and their amount of "Hartree-Fock like" exact exchange affects relative resonance positions in the spectrum.}, language = {en} } @misc{EllisBauerBacigalupoetal.2018, author = {Ellis, S. C. and Bauer, S. and Bacigalupo, C. and Bland-Hawthorn, J. and Bryant, J. J. and Case, S. and Content, R. and Fechner, T. and Giannone, D. and Haynes, R. and Hernandez, E. and Horton, A. J. and Klauser, U. and Lawrence, J. S. and Leon-Saval, S. G. and Lindley, E. and L{\"o}hmannsr{\"o}ben, Hans-Gerd and Min, S. -S. and Pai, N. and Roth, M. and Shortridge, K. and Waller, L. and Xavier, Pascal and Zhelem, Ross}, title = {PRAXIS: an OH suppression optimised near infrared spectrograph}, series = {Ground-based and Airborne Instrumentation for Astronomy VII}, volume = {10702}, journal = {Ground-based and Airborne Instrumentation for Astronomy VII}, publisher = {SPIE-INT Soc Optical Engineering}, address = {Bellingham}, isbn = {978-1-5106-1958-6}, issn = {0277-786X}, doi = {10.1117/12.2311898}, pages = {16}, year = {2018}, abstract = {The problem of atmospheric emission from OH molecules is a long standing problem for near-infrared astronomy. PRAXIS is a unique spectrograph which is fed by fibres that remove the OH background and is optimised specifically to benefit from OH-Suppression. The OH suppression is achieved with fibre Bragg gratings, which were tested successfully on the GNOSIS instrument. PRAXIS uses the same fibre Bragg gratings as GNOSIS in its first implementation, and will exploit new, cheaper and more efficient, multicore fibre Bragg gratings in the second implementation. The OH lines are suppressed by a factor of similar to 1000, and the expected increase in the signal-to-noise in the interline regions compared to GNOSIS is a factor of similar to 9 with the GNOSIS gratings and a factor of similar to 17 with the new gratings. PRAXIS will enable the full exploitation of OH suppression for the first time, which was not achieved by GNOSIS (a retrofit to an existing instrument that was not OH-Suppression optimised) due to high thermal emission, low spectrograph transmission and detector noise. PRAXIS has extremely low thermal emission, through the cooling of all significantly emitting parts, including the fore-optics, the fibre Bragg gratings, a long length of fibre, and the fibre slit, and an optical design that minimises leaks of thermal emission from outside the spectrograph. PRAXIS has low detector noise through the use of a Hawaii-2RG detector, and a high throughput through a efficient VPH based spectrograph. PRAXIS will determine the absolute level of the interline continuum and enable observations of individual objects via an IFU. In this paper we give a status update and report on acceptance tests.}, language = {en} } @phdthesis{Fritzewski2021, author = {Fritzewski, Dario Jasper}, title = {From fast to slow rotation in the open clusters NGC 2516 and NGC 3532}, doi = {10.25932/publishup-53135}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-531356}, school = {Universit{\"a}t Potsdam}, pages = {viii, 137}, year = {2021}, abstract = {Angular momentum is a particularly sensitive probe into stellar evolution because it changes significantly over the main sequence life of a star. In this thesis, I focus on young main sequence stars of which some feature a rapid evolution in their rotation rates. This transition from fast to slow rotation is inadequately explored observationally and this work aims to provide insights into the properties and time scales but also investigates stellar rotation in young open clusters in general. I focus on the two open clusters NGC 2516 and NGC 3532 which are ~150 Myr (zero-age main sequence age) and ~300 Myr old, respectively. From 42 d-long time series photometry obtained at the Cerro Tololo Inter-American Observatory, I determine stellar rotation periods in both clusters. With accompanying low resolution spectroscopy, I measure radial velocities and chromospheric emission for NGC 3532, the former to establish a clean membership and the latter to probe the rotation-activity connection. The rotation period distribution derived for NGC 2516 is identical to that of four other coeval open clusters, including the Pleiades, which shows the universality of stellar rotation at the zero-age main sequence. Among the similarities (with the Pleiades) the "extended slow rotator sequence" is a new, universal, yet sparse, feature in the colour-period diagrams of open clusters. From a membership study, I find NGC 3532 to be one of the richest nearby open clusters with 660 confirmed radial velocity members and to be slightly sub-solar in metallicity. The stellar rotation periods for NGC 3532 are the first published for a 300 Myr-old open cluster, a key age to understand the transition from fast to slow rotation. The fast rotators at this age have significantly evolved beyond what is observed in NGC 2516 which allows to estimate the spin-down timescale and to explore the issues that angular momentum models have in describing this transition. The transitional sequence is also clearly identified in a colour-activity diagram of stars in NGC 3532. The synergies of the chromospheric activity and the rotation periods allow to understand the colour-activity-rotation connection for NGC 3532 in unprecedented detail and to estimate additional rotation periods for members of NGC 3532, including stars on the "extended slow rotator sequence". In conclusion, this thesis probes the transition from fast to slow rotation but has also more general implications for the angular momentum evolution of young open clusters.}, language = {en} } @phdthesis{Haubitz2021, author = {Haubitz, Toni}, title = {Transient absorption spectroscopy}, doi = {10.25932/publishup-53509}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-535092}, school = {Universit{\"a}t Potsdam}, pages = {xiii, 176}, year = {2021}, abstract = {The optical properties of chromophores, especially organic dyes and optically active inorganic molecules, are determined by their chemical structures, surrounding media, and excited state behaviors. The classical optical go-to techniques for spectroscopic investigations are absorption and luminescence spectroscopy. While both techniques are powerful and easy to apply spectroscopic methods, the limited time resolution of luminescence spectroscopy and its reliance on luminescent properties can make its application, in certain cases, complex, or even impossible. This can be the case when the investigated molecules do not luminesce anymore due to quenching effects, or when they were never luminescent in the first place. In those cases, transient absorption spectroscopy is an excellent and much more sophisticated technique to investigate such systems. This pump-probe laser-spectroscopic method is excellent for mechanistic investigations of luminescence quenching phenomena and photoreactions. This is due to its extremely high time resolution in the femto- and picosecond ranges, where many intermediate or transient species of a reaction can be identified and their kinetic evolution can be observed. Furthermore, it does not rely on the samples being luminescent, due to the active sample probing after excitation. In this work it is shown, that with transient absorption spectroscopy it was possible to identify the luminescence quenching mechanisms and thus luminescence quantum yield losses of the organic dye classes O4-DBD, S4-DBD, and pyridylanthracenes. Hence, the population of their triplet states could be identified as the competitive mechanism to their luminescence. While the good luminophores O4-DBD showed minor losses, the S4-DBD dye luminescence was almost entirely quenched by this process. However, for pyridylanthracenes, this phenomenon is present in both the protonated and unprotonated forms and moderately effects the luminescence quantum yield. Also, the majority of the quenching losses in the protonated forms are caused by additional non-radiative processes introduced by the protonation of the pyridyl rings. Furthermore, transient absorption spectroscopy can be applied to investigate the quenching mechanisms of uranyl(VI) luminescence by chloride and bromide. The reduction of the halides by excited uranyl(VI) leads to the formation of dihalide radicals X^(·-2). This excited state redox process is thus identified as the quenching mechanism for both halides, and this process, being diffusion-limited, can be suppressed by cryogenically freezing the samples or by observing these interactions in media with a lower dielectric constant, such as ACN and acetone.}, language = {en} } @phdthesis{Henkel2004, author = {Henkel, Carsten}, title = {Coherence theory of atomic de Broglie waves and electromagnetic near fields}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-0001272}, school = {Universit{\"a}t Potsdam}, year = {2004}, abstract = {Die Arbeit untersucht theoretisch die Wechselwirkung neutraler Teilchen (Atome, Molek{\"u}le) mit Oberfl{\"a}chen, soweit sie durch das elektromagnetische Feld vermittelt wird. Spektrale Energiedichten und Koh{\"a}renzfunktionen werden hergeleitet und liefern eine umfassende Charakterisierung des Felds auf der sub-Wellenl{\"a}ngen-Skala. Die Ergebnisse finden auf zwei Teilgebieten Anwendung: in der integrierten Atomoptik, wo ultrakalte Atome an thermische Oberfl{\"a}chen koppeln, und in der Nahfeldoptik, wo eine Aufl{\"o}sung unterhalb der Beugungsbegrenzung mit einzelnen Molek{\"u}len als Sonden und Detektoren erzielt werden kann.}, language = {en} } @article{JohanssonLeitnerBidermaneetal.2022, author = {Johansson, Fredrik O. L. and Leitner, Torsten and Bidermane, Ieva and Born, Artur and F{\"o}hlisch, Alexander and Svensson, Svante and M{\aa}rtensson, Nils and Lindblad, Andreas}, title = {Auger- and photoelectron coincidences of molecular O2 adsorbed on Ag(111)}, series = {Journal of electron spectroscopy and related phenomena : the international journal on theoretical and experimental aspects of electron spectroscopy}, volume = {256}, journal = {Journal of electron spectroscopy and related phenomena : the international journal on theoretical and experimental aspects of electron spectroscopy}, publisher = {Elsevier}, address = {New York, NY [u.a.]}, issn = {0368-2048}, doi = {10.1016/j.elspec.2022.147174}, pages = {6}, year = {2022}, abstract = {The oxygen on Ag(111) system has been investigated with Auger electron-photoelectron coincidence spectroscopy (APECS). The coincidence spectra between O 1s core level photoelectrons and O KLL Auger electrons have been studied together with Ag(3)d/AgM4,5NN coincidences. We also describe the electron-electron coincidence spectrometer setup, CoESCA, consisting of two angle resolved time-of-flight spectrometers at a synchrotron light source. Contributions from molecular oxygen and chemisorbed oxygen are assigned using the coincidence data, conclusions are drawn primarily from the O 1s/O KLL data. The data acquisition and treatment procedure are also outlined. The chemisorbed oxygen species observed are relevant for the catalytic ethylene oxidation.}, language = {en} }