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Journal of Applied Physics

Theory of Pulse-Shaping by Saturable Optical Materials

James D. Macomber

Published Aug 1, 1967• 24 citations
Publisher

Abstract

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.

DOI
10.1063/1.1710165

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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.
Reverse-saturable absorbers are of considerable interest for optical limiting. Using the electric dipole perturbation, we derived the rate equation for a five-level system describing reverse-saturable absorbers. Traditional theories for the propagating laser beam in these materials are expressed in terms of the optical intensity. However, with the introduction of high-power short-pulsed lasers, the propagation of light in these materials may be subject to nonlinear phenomena such as self-focusing and self-phase modulation. Furthermore, conventional theories treat the laser light as a continuous wave or as a very broad temporal pulse in which dispersive effects are neglected. In order to incorporate these other nonlinear or dispersive effects, and therefore determine their influence in reverse-saturable absorbers, we derived an equation for the propagation of the electromagnetic field, rather than the intensity, coupled to the rate equations for a five-level system. We also coupled our theory to experimentally measurable parameters for these materials and detailed the various physical approximations used to obtain the rate equations.
The distortion of an intense light pulse by a saturable absorber is analysed on the basis of the dynamic transmission equation. The conclusions are in accord with an earlier numerical analysis for a particular pulse function, but are here proved for arbitrary pulse shape. Bounds are derived for maximum transmittance and energy loss, and the existence of stable periodic solutions is demonstrated. The region in which saturable absorption theory is valid is discussed and compared with that for self-induced transparency. The two phenomena are examples of completely incoherent and completely coherent absorption, respectively.
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.
A theoretical study has been made of the transmission of a monochromatic, well-collimated beam of radiation normally incident on idealized material containing only two energy levels. The nonlinear partial differential equations governing the variation of population and photon density in space and time have been solved exactly for arbitrary initial conditions under the assumption that spontaneous emission and thermal relaxation from the excited state can be neglected. These conditions are satisfied in practice when the radiation is in the form of a pulse whose duration is short compared with the characteristic times of these relaxation processes. Two cases are considered in detail: (a) when all atoms are in the ground state and the material absorbs; and (b) when there is a population inversion and the material amplifies. In case (a), the radiation, with a characteristic velocity, ``bores'' its way through an optically dense substance emerging delayed in time and leaving the material in a perfectly transparent or saturated state. In case (b), an incoming pulse is amplified and sharpened—to a degree determined by the gain of the medium. In addition to these cases, the dependence of the apparent spontaneous emission lifetime on the size and population distribution of the material is mentioned.
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.
A general theory of the saturated-absorption phenomenon in a two-level atomic system is developed, in which the phase relationships between the oscillating atomic dipoles as well as the population differences between energy levels are taken into account. The absorbing gaseous medium considered in this theory is subjected to irradiation by a quasi-running-wave composed of a strong pump field and a weak probe field propagating in opposite directions. Some new interesting results, not predicted by the so-called hole-burning or rate-equation model, are obtained. In particular, the probe-field-transmission peak line shape is found to be markedly different from what is expected according to the rate equations. For finite Doppler widths and a strong saturating pump field, absorption of the probe field can even change sign, and amplification of this field can actually occur. All these features are explained by a close inspection of the evolution of each atomic ensemble of given velocity. Detailed comparison with similar phenomena already observed in rf experiments is presented and permits us to clarify the new predicted effects.