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The Journal of Chemical Physics

Reverse saturable absorption in C60-doped porous glasses studied by single- and double-pulse pump–probe experiments

Jochen Schell, D. Ohlmann, Dirk Brinkmann, R. Lévy, Marguerite Joucla, Jean‐Luc Rehspringer, B. Hönerlage

Published Oct 1, 1999• 28 citations

Abstract

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.

DOI: 10.1063/1.479888

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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.

The dynamic processes of reverse saturable absorption (RSA) in a solution of C60 are studied in detail by use of rate equations and the light-propagation equation for a five-energy-level model. The RSA experimental results for C60 in toluene solution with a nanosecond–picosecond Nd:YAG laser at 532 nm are consistent with the theoretical simulations. Effects of sample concentration and thickness on RSA and contributions of the singlet and triplet excited states to RSA for various laser-pulse widths and wavelengths are also analyzed. Finally, an all-optical switch based on excited-state nonlinear absorption and the pump-probe technique is implemented.

Transition dynamics from optical saturable absorption (SA) to reverse saturable absorption (RSA) in multi-walled carbon nanotube (MWCNT)-doped fast sol-gel hybrid organic/inorganic glasses was studied by optical transmission of 532 nm laser pulses. Exposure to 6 ns long, temporally isolated single pulses of energies between 10−3 and 2×10−2 J/cm2 exhibited SA. Exposure to 1.5 ns long, 11 kHz repetitive pulses of energies between 2×10−2 and 1 J/cm2 exhibited a gradual development of RSA at a rate that increases with the pulse energy. SA results were analyzed by the slow saturable absorber theory, yielding a ground-state absorption cross section σgs=(1.5±0.1)×10−14 cm2 for a (2.0±0.13)×1015 cm−3 density of states. The first excited state absorption cross section was σes1=(9.3±0.6)×10−16 cm2 for a much higher, (2.3±0.15)×1016 cm−3, density of states. The SA/RSA transition temporal evolution effects were modeled by a five-level energy scheme. The numerical simulation yielded light-intensity dependent parameters: ground-state densities decreasing from (9±0.5)×1022 to (2±0.1)×1021 cm−3; ground-state absorption cross sections increasing from (2±0.1)×10−22 to (9.0±0.5)×10−21 cm2; and excited state absorption cross sections increasing from (7.8±0.4)×10−22 to (3.3±0.15)×10−20 cm2. The occurrence of such huge state densities is consistent with observation by others on the formation of ionized carbon-black particles as plasma states under illumination.

Three typical excited-state nonlinear absorption effects in molecular systems with weak ground-state absorption (at 532 nm) are experimentally demonstrated: (a) reverse saturable absorption (RSA) caused by strong triplet first-to-second excited-state absorption in a copper phthalocyanine solution with 15-ns laser pulses; (b) RSA caused by strong singlet first-to-second excited-state absorption in a

{\mathrm{C}}_{60}

solution with 21-ps laser pulses; (c) the RSA-SA turnover caused by strong singlet first-to-second excited-state absorption and weak singlet second-to-third excited-state absorption in a metallo-porphyrin-like solution with 21-ps laser pulses. To simulate these excited-state nonlinear absorption behaviors we propose a general ten-level density-matrix model and its simplified models for the three cases. All simulations are in good agreement with the experimental results.

By presenting a theoretical steady-state rate equation analysis, we demonstrate an efficient optical power limiting in a fullerene system, which can be attributed to a reverse saturable absorption mechanism. The limiting behavior, characterized by means of the sample’s transmittance, is explained via the population redistribution among singlet and triplet levels. In addition, the effects of intersystem crossing and reverse intersystem crossing rates on the limiting behavior are investigated. Our numerical results show how these rates alter the optical limiting performance; indeed, the intersystem crossing has a constructive role in decreasing the optical limiting threshold. In addition, a theoretical investigation of the z-scan technique is employed to further characterize the power limiting properties.

We theoretically and experimentally study absorption of picosecond laser pulses in materials described by a four-level system that exhibit reverse saturable absorption (RSA). Using an approximate solution to the rate equations, we derive, analyze, and verify, numerically and experimentally, a single dynamical equation for the spatial evolution of the pulse fluence that includes both the rate equations and the propagation equation. This analytical approach considerably simplifies the study of optical limiting with picosecond pulses and helps to predict the behavior of the nonlinear transmittance, the level of output signal clamping, and a possible turnover from RSA to saturable absorption that restricts the performance of optical limiters based on RSA. The results obtained can also be used to characterize RSA materials by the pump–probe technique.

The nonlinear absorption properties of organic materials in nanosecond (ns), picoseond (ps) and femtosecond (fs) regime were theoretically investigated by rate equations based on multilevel organic molecular system respectively. The results show that the reverse saturable absorption (RSA) phnomenon is mainly due to the absorption contribution of the triplet first excited state in the ns regime, and that of the singlet first excited state in the ps regime, both of which are a third-order nonlinear phenomena. The RSA phnomenon in fs regime is mainly due to the excited state absorption (ESA) induced by two-photon absorption (TPA), which is a fifth-order nonlinear phenomenon.