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The time-dependent optical properties of molecular systems are investigatedby step-scan Fourier-transform spectroscopy in order to explore the dynamics atphase transitions and molecular orientation in the milli- and microsecondrange. The electrical switching of liquid crystals traced by vibrationalspectroscopy reveals a rotation of the molecules with a relaxation time of 2ms. The photo-induced neutral-ionic transition in TTF-CA takes place by asuppression of the dimerization in the ionic phase and creation of neutraldomains. The time-dependent infrared spectra depend on temperature and laserpulse intensity; the relaxation of the spectra follows a stretched-exponentialdecay with relaxation times in the microsecond range strongly dependent ontemperature and laser intensity. We present all details of the experimentalsetups and thoroughly discuss the technical challenges.

Molecular Dynamics at Electrical- and Optical-Driven Phase Transitions Time-Resolved Infrared Studies Using Fourier-Transform Spectrometers