Advanced spectra analysis to determine complex structure and chirality

This thesis describes the measurement, computation, method development and analysis of several spectroscopic techniques that probe the structure of molecules and supramolecular complexes using their vibrational fingerprints. The technique that is primarily used for that purpose is vibrational circular dichroism (VCD) spectroscopy which has many positive features but also several issues that still need to be solved. The studies reported demonstrate the wealth of information that vibrational fingerprints of molecules are able to provide. Several challenges that so far have been restricting the use of circular dichroism have been taken up and met. First, methodologies have been developed to understand the very fundamentals of how VCD intensity is generated. Second, the molecular flexibility was explored, both from a structural as conformational point of view. Third, the ability to go beyond ‘small’ molecular systems was investigated. Fourth, molecules with many chiral sources have been studied. And last, several spectroscopic techniques were used to trace the behaviour of molecules in time. Overall, the studies reported in this thesis have contributed to bring VCD to a new level. A level at which it does no longer need to be considered as a scientific curiosity, but as a mature and powerful means to perform research and analysis in a large range of fundamental and applied areas.