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Journal of Physics Conference Series

Theory of three-step absorption of three light pulses

Inna Rebane

Published May 19, 2017• 0 citations
Publisher

Abstract

The theory of the absorption of three light pulses with an arbitrary duration in four-level systems is proposed. The pulses are in resonance with the corresponding transitions. By using the time-dependent perturbation theory the probability that the fourth level is excited at the moment t is found. The possible absorption lines and parameters on which their widths depend on are analysed.

DOI
10.1088/1742-6596/833/1/012023

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The theory of the absorption of three light pulses with an arbitrary duration in four-level systems is proposed. The pulses are in resonance with the corresponding transitions. By using the time-dependent perturbation theory the probability that the fourth level is excited at the moment t is found. The possible absorption lines and parameters on which their widths depend on are analysed.
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The time-dependent theory of the three-step absorption of three different light pulses in the electronic four-level systems is considered using the time-dependent perturbation theory. The first, the second, and the third pulse are in resonance with transitions from level 0 to level 1, from level 1 to level 2, and from level 2 to level 3, respectively. The spectral and temporal behaviour of the probability that the fourth level is excited at the moment of time t depends on the energy relaxation constants of the excited electronic levels, the frequencies of the maxima, the spectral widths (and so the durations) of the light pulses, and the time delays between the pulses. To conclude, there are 12 parameters that affect the spectra in the simple model used. We calculate and analyse the case where the frequencies of the maxima of the first and the second pulse are fixed and the frequency of the maximum of the third pulse varies. On the whole, three lines may exist, one of which corresponds to the coherent contribution and the others do not.
We report a theoretical investigation of effective four-photon absorption (4PA) process and propose a two-step 4PA model of three-photon- induced excited-state absorption (ESA). Based on three-level rate-equation theory, we find an analytical result for the effective 4PA coefficient that depends on the three-photon absorption (3PA) cross-section, excited-state photophysical properties, and laser pulse duration. We present the analytical theory of the z-dependent nonlinear transmission for straightforwardly yet unambiguously evaluating the 3PA and effective 4PA coefficients simultaneously.
Based on five-level rate-equation theory, we develop the laser-pulse-duration dependence of two-photon-absorption-induced singlet and triplet excited-state absorptions (ESAs). We present analytical expressions for the effective three-photon absorption coefficients caused by both singlet and triplet ESAs under the pulsed excitation on time scales from femtoseconds to microseconds. We demonstrate that the triplet ESA is predominant with longer laser pulses (microseconds to tens of nanoseconds) and that the resultant nonlinear absorption (NLA) can be adequately interpreted by a simplified four-level model. Under the excitation of picosecond laser pulses, generally speaking, the competition between singlet and triplet ESAs is observable. In this instance, the photodynamics of the system can be understood by a five-level model. In the femtosecond regime, however, a three-level model is validated in the prediction of NLA, because the triplet ESA becomes negligible.