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Cambridge University Press eBooks

Resonant nonlinearities

P N Butcher, David Cotter

Published Jul 27, 1990• 0 citations
Publisher

Abstract

In earlier chapters we have considered in detail the susceptibility formalism of nonlinear optics, which is perhaps the most familiar approach and has a wide range of application. Starting from the constitutive relations of Chapter 2, the susceptibility formalism is quite general. In many practical applications, a particular phenomenon can be described accurately by a single order of nonlinearity, and the susceptibility then provides a useful and convenient description. However, this is not always the case. Some of the most interesting phenomena in nonlinear optics involve close resonance with the transition frequencies of the medium, and perhaps also the use of very intense optical fields. As remarked in §4.5, in these circumstances the resonant susceptibilities display mathematical divergences which are clearly unphysical. Strictly, these divergences occur only because higher-order nonlinearities have been neglected. Successive orders of nonlinearity take into account such effects as saturation, power broadening and level shifts (optical Stark effect). For intense fields or very close resonance, the contributions from several orders of nonlinearity may be comparable in magnitude. Therefore, despite its generality, the susceptibility formalism does not necessarily provide the most practical approach for the description of resonant processes. This chapter is concerned with the problem of deriving alternative and more manageable descriptions of resonant nonlinear processes, illustrated by examples. For much of the chapter, the nonlinear medium is treated as a two-level system (described in §6.2).

DOI
10.1017/cbo9781139167994.007

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In earlier chapters we have considered in detail the susceptibility formalism of nonlinear optics, which is perhaps the most familiar approach and has a wide range of application. Starting from the constitutive relations of Chapter 2, the susceptibility formalism is quite general. In many practical applications, a particular phenomenon can be described accurately by a single order of nonlinearity, and the susceptibility then provides a useful and convenient description. However, this is not always the case. Some of the most interesting phenomena in nonlinear optics involve close resonance with the transition frequencies of the medium, and perhaps also the use of very intense optical fields. As remarked in §4.5, in these circumstances the resonant susceptibilities display mathematical divergences which are clearly unphysical. Strictly, these divergences occur only because higher-order nonlinearities have been neglected. Successive orders of nonlinearity take into account such effects as saturation, power broadening and level shifts (optical Stark effect). For intense fields or very close resonance, the contributions from several orders of nonlinearity may be comparable in magnitude. Therefore, despite its generality, the susceptibility formalism does not necessarily provide the most practical approach for the description of resonant processes. This chapter is concerned with the problem of deriving alternative and more manageable descriptions of resonant nonlinear processes, illustrated by examples. For much of the chapter, the nonlinear medium is treated as a two-level system (described in §6.2).
In the previous chapter we examined nonlinear propagation in a two-level medium, which leads to amplification or absorption of the radiation field. As we will see further on in this volume, when the medium is placed in an optical cavity one realizes a laser in the case of amplification or an optically bistable system in the absorptive configuration. On the other hand, the nonlinear response of the atomic polarization to the electric field leads to further fascinating scenarios [29, 51–60]. For example, a field with central ω 0 can generate harmonic components with central frequencies 2 ω 0 , 3 ω 0 etc., processes that are called second-harmonic generation, third-harmonic generation etc. Furthermore, the interaction of two fields with central frequencies ω 1 and ω 2 , with ω 1 > ω 2 , can generate components with central frequency ω 1 + ω 2 (sum-frequency generation) and ω 1 − ω 2 (difference-frequency generation). Such phenomena have not yet appeared in this volume because we have assumed that the electric field corresponds to a narrow frequency band around a central frequency ω 0 only, whereas to describe them it is necessary to assume that the electric field is the superposition of a number of frequency bands. In this chapter we will provide a description of the basic elements which are necessary to describe these phenomena and we will discuss a small number of them for the case of materials with a quadratic nonlinearity, referring to textbooks in nonlinear optics for the description of other phenomena. The following chapter is devoted, instead, to the case of materials with cubic nonlinearities. The starting point of nonlinear optics is the expansion of the atomic polarization in powers of the electric field, when the electric field is not too intense. In our treatment in Chapter 5 we saw that the expansion of the nonlinear susceptibility contains only even powers of the electric field (see Eq. (5.27)), and therefore the expansion of the polarization includes only odd powers.
Abstract The book so far is almost entirely concerned with linear optical processes, where the response of a material to incident light is described by its linear susceptibility and the rates of optical processes are proportional to the incident intensity. However, examples of nonlinear behaviour occur in the saturation of atomic transitions, discussed in §1.7, and in the power-broadened susceptibility, derived in eqn (2.8.6). Atomic saturation is also an important component in the laser theory of§§t.10 and 7.3. The expressions derived in these examples contain the electromagnetic energy density or photon number in denominators whose expansions include terms proportional to all positive powers of the optical energy. The higherorder, or nonlinear, terms are normally much smaller than the linear term for conventional light sources but their influence is often significant in experiments that use laser sources. The present chapter treats the effects of the nonlinear terms in modifying the properties of incident light beams.
The density-matrix approach, in the quasistatic or adiabatic limit, is applied to the case of resonant four-wave interactions in four-level systems resulting in explicit analytical expressions for the nonlinear optical parametric and nonparametric polarizations, including ac Stark effects. The results are applicable to any closed-linkage diagram of this type but are applied only to the specific case of resonant frequency tripling. The results revealed the presence of up to six Stark-shifted nonparametric resonances and the presence of saturation and interference effects on the parametric susceptibility. In particular, the third-order susceptibility is shown to saturate to a very small value under high-field conditions which restricts the range of useful pump intensities. Under near-resonant to resonant conditions, these imply that because of either nonparametric loss present at the pump or harmonic frequencies or power-dependent dispersive and saturation effects, conversion efficiencies higher than 25% may be difficult to realize in practice.
A nonlinear response theory of a quantum-mechanical system undergoing arbitrary relaxation and interacting with fields, some of which may be strong enough to saturate optical transitions, is developed. Explicit expressions for second-order and third-order susceptibilities are obtained. If the fields are weak, then these expressions show the existence of additional resonant contributions to ${\ensuremath{\chi}}^{(n)}$ which arise due to inelastic collisions. Various applications of these ${\ensuremath{\chi}}^{(n)}$'s to modulation spectroscopy, four-wave mixing, and pump-probe experiments are discussed. The general structure suggests how the additional resonances can be used to determine inelastic rates in a Doppler-broadened medium. For saturating fields, ${\ensuremath{\chi}}^{(n)}$'s become dependent on the intensity of such fields and can be formally obtained from weak-field ${\ensuremath{\chi}}^{(n)}$'s, provided proper identification of unperturbed eigenfunctions, eigenvalues, and relaxation times is made. Such intensity-dependent ${\ensuremath{\chi}}^{(n)}$'s have resonant denominators which lead to resonances at Rabi frequencies and submultiples of these frequencies, the widths of which are also dependent on the strength of the field. In the special cases intensity-dependent ${\ensuremath{\chi}}^{(1)}$ agrees with the work of Cohen-Tannoudji and co-workers.
Frequency-dependent and nonlinear susceptibilities are common in nonlinear optics, but they are scarcely used in coherent resonant pulse propagation because of their complexity. Early studies1 include the frequency quadratic susceptibilities, but none was proportional to the spectral pulse strength other than in the time-dependent case.2 We consider the propagation of short duration pulses through a medium described by an ensemble of resonant two-level atoms embedded in a nonresonant but nonlinear host medium. The nonlinear susceptibility is given by monomial terms of the spectral pulse strength.
The amplification of noise in a laser amplifier is treated theoretically. The model for the active medium and its description using density-matrix techniques, are taken from the theory of laser operation. The fundamental concern of this investigation is the spectral behavior of the radiation in the nonlinear regime; hence, the formalism is written from the onset in the frequency domain. The statistics of the light are gradually modified by the nonlinear amplification process, and expressions are derived for the rate of change of fluctuations in intensity as a measure of statistical changes. These expressions should be easily susceptible to detailed experimental observations. In addition, the range of validity of Litvak's Gaussian-statistics approximation is discussed with some detail. In the homogeneous-broadening case, the evolution of initially broadband Gaussian radiation toward quasimonochromatic oscillations with laserlike statistics is extensively explored in several numerical examples. The connections of this study with the time-domain work of Risken and Nummedal, on self-pulsing in a ring-laser configuration, are clearly established. Finally, spectral-narrowing and -rebroadening effects in Doppler-broadened media are discussed both analytically and with numerical examples. These examples show the distinct contribution of pulsations in the population ("Raman-type terms"), and saturation phenomena. The predicted narrowing-rebroadening rate is compared with expressions found in previous literature.