We investigate the nonlinear absorption of C60-doped porous sol-gel glasses by single- and double-pulse pump–probe experiments. We find that the reverse saturable absorption (RSA) of these samples can be explained in the frame of a five level system as it is commonly used for C60 solutions. We observe a strong saturation of the RSA at high fluences, especially if the molecules are prepared in the triplet state. In a double-pulse pump–probe experiment we measure the triplet quantum yield for C60 solutions (0.8) and doped glasses (0.25) and the singlet and triplet absorption cross sections. In the first excited singlet state (S1) lifetimes of 1 ns and 65 ps are determined in solutions and glasses, respectively. We find that the dynamics of both depopulation processes, direct S1–S0 relaxation, and intersystem crossing is faster in glasses than in the case where C60 is in solution in a liquid aromatic solvent. We tentatively explain these findings by the absence of a stabilizing solvent and a perturbation of the molecular energy levels due to interaction with the solid glass matrix. We finally determine the lifetime of the triplet states in our glass samples to 2 μs.

We present measurements of induced absorption and its dynamics in C60-doped solid xerogel matrices. The measurements are performed in a pump-test geometry using picosecond pulses generated from a frequency doubled mode locked Nd:YAG laser at 532 nm. We observe an induced absorption leading to optical limiting. We find outstanding optical limiting qualities for single shot excitation but some degradation above a certain threshold intensity for repetitive pulses. Below this degradation threshold, the material is stable and its limiting dynamics is studied. A decrease of the initial laser-induced absorption with a time constant of 150 ps is observed, down to a very long-lived constant level. We attribute this dynamics of induced absorption to a transition from excited singlet to triplet electronic states in the C60 molecule.

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