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Journal of Applied Physics

The effects of intersystem and reverse intersystem crossing on the optical limiting properties of C60

Mohadeseh Veisi, Seyedeh Hamideh Kazemi, Mohammad Mahmoudi

Published Mar 10, 2020• 4 citations
Publisher

Abstract

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.

DOI
10.1063/1.5143286

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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 present a convenient way to obtain an optical power limiting behavior in a quantum dot molecule system, induced by an interdot tunneling. Also, the effect of system parameters on the limiting performance is investigated; interestingly, the tunneling rate can affect the limiting performance of the system so that the threshold of the limiting behavior can be a function of the input voltage, allowing the optimization of the limiting action. Furthermore, by investigating the absorption of the probe field, it is demonstrated that the optical limiting is due to a reverse saturable absorption mechanism; indeed, analytical results show that this mechanism is based on a cross-Kerr optical nonlinearity induced by the tunneling. Additionally, the limiting properties of the system are studied by using a Z-scan technique.
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 study the generation and control of the microwave (MW)-induced reverse saturable absorption (RSA) and optical limiting (OL) in a three-level pump-probe V-type quantum system. It is shown that the saturable absorption switches to the RSA by applying the MW field to the transition between two upper levels. Moreover, it is demonstrated that the RSA and the induced OL threshold are controlled by either the intensity or detuning of the MW field. In addition, the effect of the coupling field on the induced optical limiting is studied, and it is obtained that the cross-Kerr nonlinearity has a major role in establishing efficient optical power limiting. In addition, we demonstrate that an increase in the atomic density and length of the medium makes the optical limiter more powerful. Finally, the theoretical Z-scan technique is presented to confirm the obtained results of the microwave-induced OL. The proposed scheme can be used to prepare a controllable optical limiter with various thresholds, which can protect the optical devices with different sensitivities.
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.
We investigate the reverse saturable absorption (RSA) and optical limiting (OL) in a three-level V-type quantum system considering the effect of the spontaneously generated coherence (SGC). It is shown that in the absence of the SGC effect, the saturable absorption (SA) is dominant in the system. By taking into account the SGC effect, we prove that the SA dramatically switches to the RSA. Moreover, it is demonstrated that the OL threshold and OL efficiency can be controlled by the SGC effect. In addition, we show that the applied field properties such as detuning can modify the SGC-induced optical limiter efficiency. It is also shown an increase in the atomic density and length of the medium makes the optical limiter more efficient. The analytical calculation shows that the Kerr nonlinearity caused by the SGC effect is the main mechanism of the system evolution. Finally, the theoretical Z-scan experiment is presented to confirm the obtained results. Our proposed scheme can be useful to design controllable atomic optical limiters for optical devices with different sensitivities.