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Intermolecular structure in a single component polymer glass



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Intermolecular structure in a single component high resolution measurements of the sidechain polymer glass Towards pair correlation function A H Marcusa and M D Fayer Department of Chemistry Stanford University Stanford California 94305 John G Curro Sandia National Laboratory Albuquerque New Mexico 87185 Received 10 January 1994 accepted 4 March 1994 Electronic excitation transport among interacting polymer molecules lightly tagged with chromophore substituents is theoretically examined as a function of tagged polymer concentration in the polymeric solid The results are compared to experimental data obtained in a previous study Macromolecules 26 3041 1993 The dependence of time resolved fluorescence observables on intermolecular polymer structure is of primary interest A theory is presented which describes excitation transport for both donor donor DD and donor trap DT systems For the case of DD transport the theory is based on a first order cumulant approximation to the transport master equation For DT transport the theory does not involve approximations and is an exact representation of the assumed model In both cases the model makes use of the Flory ideality postulate by depicting the intramolecular segmental distribution as a Gaussian with a second moment that scales linearly with chain size The only adjustable parameter in the treatment is the form of the intermolecular segmental pair distribution function g r The model is found to be extremely sensitive to the behavior of g r Comparisons to experimental data indicate that g r is primarily made up of hard core interactions between the chromophore sites The DT calculations display a higher sensitivity to the form of g r than the corresponding DD calculations For purposes of comparison the analysis is applied to a DT system in which every polymer chain has chromophore tags The sensitivity of the method for 100 tagged systems to g r is comparable to the analysis for systems with only some of the chains tagged 1



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