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Canadian Journal of Physics

Infrared saturable absorbers. Part I: Five-level rate-equation analysis

Tuan-Kay Lim, Jerald R. Izatt, George F. Caudle

Published Feb 1, 1977• 0 citations
Publisher

Abstract

The saturation behavior of molecular absorbers characterized by absorption coefficients expressible as the ratio of two polynomials in the intensity is analyzed. Two cases are considered in detail. In the first, the absorption coefficient is the ratio of a linear equation in I to a quadratic equation in I. In the second, the highest order of the intensity occurring in both numerator and denominator is increased by two. The absorption coefficients are derived from two specific five-level models which are pertinent to the interpretation of the absorption of CO2 laser radiation at 937 cm−1 by SF6, but the analysis of the saturation curves is independent of the models from which they are derived. The saturation curves display as many as three extrema and provide considerable flexibility for fitting complicated experimental data. Both five-level models include excited-state absorption with the terminal level of the ground-state absorption distinct from the initial level of the excited-state absorption. Each of the five levels can be considered as a composite of many rotational states which interact in a like manner with the incident radiation. In one of the models the ratio of the excited-state and ground-state absorption cross sections is taken to be intensity dependent.

DOI
10.1139/p77-035

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The saturation behavior of molecular absorbers characterized by absorption coefficients expressible as the ratio of two polynomials in the intensity is analyzed. Two cases are considered in detail. In the first, the absorption coefficient is the ratio of a linear equation in I to a quadratic equation in I. In the second, the highest order of the intensity occurring in both numerator and denominator is increased by two. The absorption coefficients are derived from two specific five-level models which are pertinent to the interpretation of the absorption of CO2 laser radiation at 937 cm−1 by SF6, but the analysis of the saturation curves is independent of the models from which they are derived. The saturation curves display as many as three extrema and provide considerable flexibility for fitting complicated experimental data. Both five-level models include excited-state absorption with the terminal level of the ground-state absorption distinct from the initial level of the excited-state absorption. Each of the five levels can be considered as a composite of many rotational states which interact in a like manner with the incident radiation. In one of the models the ratio of the excited-state and ground-state absorption cross sections is taken to be intensity dependent.
We develop an analytical approach to the dynamics of band populations of reverse saturable absorbers modeled by the three-level approximation of the five-level rate equations. We find high-accuracy approximate solutions to these rate equations, taking into account the temporal shape of the incident laser pulse for different regimes of excitation. The results obtained are confirmed by direct numerical integration of the rate equations and are verified by solution of the full system of the rate and the propagation equations. The validity ranges of the approximations are determined. We also prove that for input pulses that are much longer than the lifetime of the first excited state the ground-state depletion obeys the same functional dependence on the input fluence as in the case of rectangular input pulses. The dynamics of the excited states, however, explicitly depends on the pulse shape. We quantitatively estimate the effect of various parameters on the nonlinear absorption coefficient and discuss implementation of the approach by a beam propagation method to reduce the computational time.
As a high-intensity monochromatic light pulse passes through a material containing two-level systems, saturable absorption or amplification of the radiation may occur. The resultant ``shaping'' of the intensity-vs-time curve as a function of distance into the sample is the subject of this paper. A theory is developed based on the Einstein rate equations, and pulse-shape functions are derived which depend on the absorption and loss coefficients of the material, the relaxation time of the systems, the input-pulse intensity and width, the initial ``state-of-pump'', and number density of absorbers in the sample.
We model the response of a molecular medium to an intense pulse of light. We begin by reducing the Maxwell-Bloch equations for a multilevel molecular model system to a set of simplified propagation equations. We thereby obtain expressions for the frequency, temperature, and field intensity dependence of the ground and excited electronic state absorption cross sections, and the emission cross section, as well as the temperature dependence of the decay rate of the excited state. The phenomena of saturation, excited-state absorption, optically induced dichroism and birefringence, vibronic energy transfer, induced molecular alignment, decay of the matter-field interaction energy, and rotational diffusion are considered within the general formalism for describing the propagation of an intense pulse of light in the molecular medium. We find that the cross section for absorption (emission) of a photon is not identical to the cross section for molecular excitation (deexcitation) via the matter-field interaction. This is explained in terms of an energy balance between the matter, radiation, the matter-radiation interaction, and the bath responsible for the broadening of the molecular transitions. The inequality of these cross sections determines whether the system supplies or draws energy from the thermal bath. The rise in the vibrational temperature of molecules subjected to an intense short pulse is shown to significantly affect propagation of the pulse. The alignment of the molecular system resulting from saturation of the ground-state transition by a polarized laser pulse and the effects of the orientational dependence of the matter-field interaction including effects of rotational diffusion are determined. As an example of the formalism we consider pulse propagation in a Rhodamine 6G solution. We fit the parameters of the model to determine the frequency dependence of the ground- and excited-state absorption cross sections and the emission cross section and compare with experimentally determined cross sections. We describe the propagation of a pulse whose temporal width is comparable to the rotational diffusion time of the molecules in the dye solution and calculate polarization pulse probe signals.
Phase conjugation by degenerate four-wave mixing in a saturable absorbing medium with a relatively long-lived excited state is analyzed; the analytical results are compared with experimental results. We propose a four-level model and take into account the effects of both excited-state absorption and pump propagation to explain the experimental results, which could not be explained by the models proposed previously. The numerical result predicts that the value of the phase-conjugate reflectivity as a function of the pump intensity is maximum at a certain absorbance (as absorbance increases) that is dependent on the cross section of the excited-state absorption. The present analysis explains most observations in the experiment, which was performed with a saturable-dye-doped polymer film as the saturable absorbing medium.
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.
A saturable absorber (SF(6)) is irradiated by a step of radiation from a CO(2) laser, and the step response of the medium is observed. Since the characteristic times of rotational, vibrational, and thermal excitation are different, it is possible to observe each process separately. A set of rate equations is developed for a simplified model of two energy levels. This set includes only one differential equation and qualitatively describes the effects of rotational hole burning and vibrational relaxation. Heat effects are accounted for separately.