Abstract
Light-induced spectral diffusion was detected in polymethylmethacrylate samples doped with a high concentration $(c=2.4\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}2}$ mol/L) of ${\mathrm{H}}_{2}\ensuremath{-}$tetraphenylporphine in the subkelvin temperature regime. Two interesting effects were observed in the measurements of spectral diffusion (SD) in optical hole burning experiments. The first observation is that of irreversible spectral hole broadening which occurs upon irradiation of the sample. This effect is explained in terms of a chromophore-chromophore interaction. The second observation involves an increase of the SD rate in highly concentrated samples. This is connected with additional two-level-system excitations by high-energy phonons emitted from closely spaced chromophore molecules by relaxation processes from optically excited states.
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