Abstract
A repetitive low-power laser-pulse apparatus has been developped which allows both absorption relaxation and light-induced grating experiments without changing geometry or components. The influence of pulse width and coherence time on the diffracted intensity correlation function is discussed for a weak amplitude grating in terms of a simplified theory. From the corresponding absorption relaxation signals including the coherent coupling contribution some easy ways for detecting vibronic-relaxation, intersystem-crossing and orientational-relaxation times are deduced. The advantage of the “in-situ” measurement of the amplitude grating autocorrelation function leads to a precise zero-delay calibration of the transient absorption equipment. Furthermore one gets the response function for the absorption experiments from the grating experiments, if stable mode-locking operation of the argon laser is reached. This condition can be controlled either by the time course of the absorption or grating signals. A surprisingly short coherence length is detected for the cavity-dumped laser beam. A reliable check of the coherent-coupling theory confirms the theoretical assumptions incorporated into the fast-relaxation signal analysis. Experiments on dye molecules show high triplet yield of heavy-atom substituted dyes and fast rotational diffusion of oblong molecular rotors.
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von Jena, A. A combination of laser-induced grating and transient-absorption experiments for investigation of laser pulse properties and fast molecular relaxation processes. Appl. Phys. B 26, 1–17 (1981). https://doi.org/10.1007/BF00702680
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DOI: https://doi.org/10.1007/BF00702680