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Journal of the Optical Society of America B

Dynamics of reverse saturable absorption and all-optical switching in C_60

Chunfei Li, Lei Zhang, Ruibo Wang, Yinling Song, Yuxiao Wang

Published Aug 1, 1994• 118 citations
Publisher

Abstract

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.

DOI
10.1364/josab.11.001356

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Physical Review A•Jan 1, 1995•45 citations
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.
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 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 dynamics of all-optical switching in C60 has been theoretically analyzed based on the principle of nonlinear intensity-induced excited-state absorption to achieve high contrast and fast switching. The transmission of a cw probe laser beam at 885 nm corresponding to the peak absorption of the S1 state through C60 in toluene is switched by a pulsed pump laser beam at 532 nm that excites molecules from the ground state. Switching characteristics are shown to be sensitive to the variation of pump pulse width, peak pumping intensity, thickness of the medium, intersystem crossing time between the S1 and T1 states and the absorption cross section of the S1 state at a probe wavelength, and their effect are analyzed in detail. It is shown that the transmission of the probe beam can be completely switched off (100% modulation) by the pump beam at a pump intensity of 100 MW/cm2 and a pulse width 1.5 ns, with switch on and off times of 2.5 and 7.5 ns, respectively. The results are used to design all-optical NOT and the universal NOR and NAND logic gates with multiple pump laser pulses, which are the basic building blocks of computing circuits.
The dynamic and steady-state processes of the reverse saturable absorption (RSA) and the related optical limiting (OL) and optical bistability (OB) in metallophthalocyanine have been studied in detail using rate equations and the light-propagation equation. The experiments for demonstrating RSA, OL, and OB in a copper phthalocyanine (CuPc) solution with a Q-switched, frequency-doubled neodymium-doped yttrium-aluminum-garnet (Nd:YAG) laser were accomplished. The experimental results were consistent with the dynamic theoretical simulations, also approximately in accordance with the expression of RSA derived from the same equations at the steady-state condition.
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 C60{\mathrm{C}}_{60}C60​ 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.