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Chemical Physics Letters

Pitfalls in the determination of optical homogeneous linewidths in amorphous systems by hole-burning. Influences of the structure of the host

H.P.H. Thijssen, Silvia Volker

Published Nov 1, 1985• 2 citations
Publisher
DOI
10.1016/0009-2614(85)85504-4

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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.

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Picosecond photon echo experiments on pentacene in polymethylmethacrylate (PMMA) show that the homogeneous width exhibits a T1.3 temperature dependence. This behavior is ascribed to coupling of the pentacene transition to randomly distributed low-frequency excitations in the amorphous host. A calculation of the resulting homogeneous width is presented which uses optical Redfield theory as a starting point. From the results of this calculation we conclude that the coupling between the pentacene molecule and the host low frequency excitations is of static dipolar nature and that the density of states of these excitations varies as ω0.3. Results of nonphotochemical hole-burning experiments on the same system are also reported. Comparison of these results with the ones obtained by the photon echo method indicates, that in the hole-burning experiments, the hole width and its temperature-induced broadening are dominated by spectral diffusion.
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.