Femtosekunden-Spektroskopie biologischer Systeme mittels kohärenter Kontrolle

摘要: This doctoral thesis presents new approaches for the characterisation of ultrafast energy flow in complex systems, based on concepts coherent control. By initiating a photoreaction with femtosecond pulses whose temporal phase and amplitude are shaped such manner that specific molecular vibrations states addressed, can be steered at will. The comparison between ensuing patterns following unshaped excitation constitutes differential measurement function controlled within photoreaction. Coherent control as spectroscopic tool is first applied to biological specifically light harvesting LH2 from photosynthetic purple bacterium Rhodopseudomonas acidophila, isolated carotenoid donor same complex. pump-probe method using shown successful time controlling natural system, namely network LH2. means closed-loop optimisation parametrised excitations, bending mode identified being responsible steering flow. bu vibrational couples S2-S1 states; its frequency determined 160±25cm-1. Furthermore deactivation S2 state solution studied pump-deplete-probe spectroscopy. Here it there exists an alternative singlet S*T (1Bu-) involved process, though only Its precursor triplet population transfer characterised novel evolutionary target analysis conventional spectra. Secondly, technique another extremely this case material dominated by non-linear interactions instantaneous dynamics: Propagation optical fibres few micrometers diameter generate supercontinuum frequencies. pump succeed resolving sequential steps leading enormous spectral broadening. Open-loop variations precompression allows evolution fission solitons followed, while optimisations render observable coupling phase-matched visible frequencies. On atoms, finally, open-loop interfering pathways ground excited application strongly modulated spectra seeks establish direct link experiments theory. phenomenon Fresnel zone plate domain developed theory then successfully realised experiment.