Abstract

A theory is developed for exciton—phonon interactions in ionic molecular crystals showing triplet-exciton magnetic resonance. By using a simple model for the phonon Hamiltonian it is shown that the triplet excitons tend to be localized, or ``self-trapped,'' and to move in a diffusional manner. The activation energy for diffusion is found to be essentially ½Λ, where Λ is the ``self-energy'' of the triplet exciton due to exciton—phonon interaction. It is suggested that the anomalous excess activation energy for exciton—exciton spin-exchange line broadening is ½Λ rather than the phonon-coupled exciton—exciton repulsion suggested previously. It is also shown that exciton creation and annihilation with the absorption and emission of phonons has no significant effect on the exciton magnetic resonance linewidths at low temperatures.

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