The initial goal of this thesis was to demonstrate chaos in an open two-mirror resonator. We have designed a bifocal mirror that forms a resonator with an unstable inner and a stable outer part. To... Show moreThe initial goal of this thesis was to demonstrate chaos in an open two-mirror resonator. We have designed a bifocal mirror that forms a resonator with an unstable inner and a stable outer part. To be able to distinguish phenomena unique for configuration from phenomena also present in conventional resonators, i.e., roughness-induced scattering and aberrations, the performance of a conventional stable resonator is investigated first. Roughness-induced scattering turns out to affect the cavity finesse as well as the average power throughput and produces mode coupling close to frequency-degenerate points. We demonstrate, furthermore, a method to accurately determine aberrations by measuring the Gouy phase of subsequent higher-order modes around frequency-degeneracy. The bifocal mirror is not fabricated by traditional grinding and polishing, but by diamond-machining. The eigenmodes of a resonator with one diamond-machined bifocal mirror turn out to be Laguerre-Gaussian. We demonstrate furthermore, the coupling of two resonators based on transmission spectra and patterns, and report on the ability of the configuration to fulfill the basic requirements to obtain chaos. Show less
The research in this thesis comprises two separate topics: single-molecule spectroscopy and resonant Raman spectroscopy. The first part concerns single-molecule (SM) spectroscopy on polyethylene ... Show moreThe research in this thesis comprises two separate topics: single-molecule spectroscopy and resonant Raman spectroscopy. The first part concerns single-molecule (SM) spectroscopy on polyethylene (PE) films. Ultra thin (200 nm) films of pure high density PE were produced by spincoating. By determining the position (accuracy 10 nm) and in-plane orientation (acc. 5 deg.) of single 2.3,8.9-dibenzanthanthrene (DBATT) guest molecules, by means of SM microscopy and spectroscopy respectively, we demonstrated that these thin PE films have a shish-kebab morphology, instead of the spherulitic morphology common in thicker PE films. We have also investigated the alignment process of individual quest chromophores by stretching thicker (50 um), low density PE films. Using SM spectroscopy, we have shown that individual guest chromophores are not better aligned along the stretch direction, as draw ratio increases. Instead alignment occurs suddenly, due to the destruction and (oriented) reformation of local crystalline regions and subsequent adsorption of chromophores. Each chromophore's orientation is determined by specific interactions with the oriented PE crystal surface. The second part of this thesis concerns a quantum-chemical analysis of the resonant Raman spectrum of the carotenoid spheroidene reconstituted in the photosynthetic reaction center (RC) of Rhodobacter sphaeroides. Our analysis demonstrates that spheroidene can adopt at least two cis forms in the RC. One of these has been conclusively shown to be the 15,15'-cis structure. Show less
