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Optical hole burning and -free induction decay of molecular mixed crystals

Harmen de Vries

Published Jan 1, 2008• 1 citation
OpenAlex

Abstract

The main theme in the research of which this thesis forms a part, is the dephasing after electronic (vibronic) excitation of organic guest molecules in suitable host crystals ("mo1ecular mixed crystals") at 1ow temperature. ... Zie: Summary

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The Journal of Chemical Physics•Mar 15, 1990•12 citations
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
Permanent and transient hole-burning experiments carried out on various types of amorphous systems at temperatures between 0.3 and 20 K are presented. Optical dephasing on organic molecules in glasses and polymers measured on different time scales are discussed in relation to spectral diffusion processes and compared to the literature. The pure dephasing time appears to be proportional to the excited state lifetime of the guest. Organic molecules adsorbed on the surface of porous silica glass show that their homogeneous linewidth is an order of magnitude larger than in polymers and glasses in the bulk, but follows the same temperature dependence. Hole-burning results on bacteriochlorophyll in various disordered hosts are compared to those on a isolated light-harvesting photosynthetic pigment-protein complex (B800–850). From the holewidth in the latter the energy transfer rate between aggregated bacteriochlorophyll pigments is determined and compared to time-resolved spectroscopy results in the literature.
The temperature-dependent optical dephasing of anthracene, 9-methylanthracene, and 2-methylanthracene monomers in phenanthrene host crystals has been measured using photon echo experiments. Despite large linear electron–acoustic phonon coupling, all three systems dephase because of coupling to pseudolocal modes (local motions of the guest molecule). Computer simulations of the three systems calculate the pseudolocal mode eigenvalues and eigenvectors. In contrast to previous discussions in the literature which describe pseudolocal modes as librations, the predicted eigenvalues are in reasonable agreement with the measured pseudolocal mode energies. The predicted eigenvectors are combinations of translational motion along the long molecular axis and rotational motion about the out-of-plane axis of the guest. Differences in site energies for various locations and orientations of the methyl group are calculated.