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The Study of Transient Species and Precursors of Biomolecules using Spectroscopic Techniques
Ferus, Martin ; Civiš, Svatopluk (advisor) ; Šponerová, Judit E. (referee) ; Wild, Jan (referee)
The presented thesis is focused on a spectroscopic study of unstable radicals, ions and molecules in a positive column glow discharge and laser plasma. The research of these fragments is supplemented by a study of biomolecules formation from these species and influence of catalysts. Molecular dynamics of radicals, ions and unstable molecules has been studied using a time resolved Fourier transform infrared spectroscopy. Time resolved spectra of CH4, HCONH2, BrCN, CH3CN, CF3Br, (CF3)2CHBr positive column glow discharges have been measured and simulated using a kinetic model including molecular dynamics, collisions and chemical and radiation transfer processes. The model has been compared with our experimental results and time resolved spectra were described in details. Fit to a complex reaction mechanism has been used to estimate a rate constant of a HCN conversion to HNC by a collision with H radical. The study of precursors of biomolecules was focused on chemical consequences of a laser induced dielectric breakdown in formamide vapor and gaseous carbon monooxide with 18 O labeled water. Dissociation products have been detected using the Fourier transform absorption spectroscopy. The experimental results have been explained by a help of a chemical laser spark dynamics model. Additionally, our the...
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Formation of nucleobases from formamide initiated by high-power density energy events
Michalčíková, Regina ; Civiš, Svatopluk (advisor) ; Šponerová, Judit E. (referee)
This Master's thesis deals with determination of nucleobases in formamide samples (pure or catalyzed form) after their initiation by high-power density energy events. The theoretical part states the reader to the problems of prebiotic chemistry and acquaints him with the various theories of the origin of the nucleobases. The experimental part deals with the analysis of the samples initiated by Laser System PALS, which was used for the simulation high-power density energy events. For the identification and determination of the final products of laser plasma initiated chemical reactions in the gaseous phase of the samples was used the Fourier Transform Infrared Spectroscopy. The liquid part of the samples and the nucleobases in this part were analyzed by the gas chromatography with the mass detection.
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Formation of organics molecules initiated by high-power density energy events in planetary atmospheres
Kamas, Michal ; Civiš, Svatopluk (advisor) ; Zelinger, Zdeněk (referee)
The focused laser beam delivered by the high-power laser system PALS was used for laboratory simulation of high-energy-density events in a planetary atmosphere. Several model gas mixtures were prepared to mimic the mildly reducing early Earth's atmosphere (CO-N2-H2O) as well as the atmosphere of Saturn's moon Titan and the strongly reducing early Earth's atmosphere (CH4-N2-H2O). In situ investigation of transient species generated by the laser-induced dielectric breakdown in the gaseous mixtures was performed by optical emission spectroscopy (OES). Final products of laser-plasma initiated chemical reactions were identified and determined by advanced mass-spectrometry (SIFT-MS) and absorption FT-IR spectroscopy. High-power laser system SOFIA was utilized to simulate in our laboratory a high-velocity impact into the icy satellites of the outer planets of the Solar system. OES was engaged in probing the plasmas produced by the SOFIA beam focused on ice surfaces (water, methanol, formamide), while final products were analyzed by means of gas chromatography (GC/MS) and mass-spectrometry (SIFT-MS).
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Catalytic and photocatalytic processes on 18O-labeled TiO2
Kavan, Ladislav ; Zukalová, Markéta ; Ferus, Martin ; Kürti, J. ; Koltai, J. ; Civiš, Svatopluk
18O-isotope labelled titania (anatase, rutile) was synthesized. The products were characterized by Raman spectra together with their quantum chemical modelling. The interaction with carbon dioxide was investigated using high-resolution FTIR spectroscopy, in dark and upon UV-excitation. The oxygen isotope exchange at the Ti18O2/C16O2 interface was elucidated. The C18O2 was formed as the dominating final product with a minor content of C16O18O. The rate of oxygen-isotope exchange is highly sensitive to the conditions of the titania pretreatment. The vacuum-annealed Ti18O2 at 450 C exhibited a very high spontaneous oxygen exchange activity with gaseous C16O2. A mechanism for the 18O/16O exchange process is discussed at the molecular level. The photocatalytic formation of methane, acetylene and C16O released from the Ti18O2 surface was triggered by an XeCl excimer laser irradiation.
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