A Theory for the Temperature Dependence of Hole-Burned Spectra

A theory is presented for the temperature dependence of the absorption and hole-burned spectra of chromophores imbedded in solids characterized by structural heterogeneity. The theory is applicable for arbitrarily strong linear electron-phonon coupling and describes the overall hole profile which consists of the zero-phonon hole and its associated phonon sideband hole structure. A novel and convenient form for the thermally averaged Franck-Condon factors is employed. Illustrative calculations are presented which pertain to the temperature dependence of the absorption band of the primary electron donor of the photosynthetic bacterial reaction center and the design of high-temperature hole-burning materials for high-density frequency domain optical storage. 44 refs., 4 figs., 3 tabs.