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arXiv:quant-ph/0005094 · Journal of Experimental and Theoretical Physics

Nonlinear interference effects in emission, absorption, and generation spectra

T. Ya. Popova, A. K. Popov, Sergey G. Rautian, R. I. Sokolovskiǐ

Published May 23, 2000• 4 citations
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Abstract

Nonlinear effects in emission and absorption spectra of gaseous systems are considered. It is shown that level splitting can be detected spectroscopically even if it is below the Doppler width. Conditions for distinguishing interference effects from those due to nonequilibrium velocity distribution are determined. In the case of large Doppler broadening the correction for atomic motion is equivalent to the substitution of an "effective immobile atom" for the moving atom ensemble. The spectral manifestation of nonlinear effects is analyzed in detail. The influence of nonlinear interference effects on the generation characteristics in the presence of external field is investigated.

DOI
10.48550/arxiv.quant-ph/0005094

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Nonlinear effects in emission and absorption spectra of gaseous systems are considered. It is shown that level splitting can be detected spectroscopically even if it is below the Doppler width. Conditions for distinguishing interference effects from those due to nonequilibrium velocity distribution are determined. In the case of large Doppler broadening the correction for atomic motion is equivalent to the substitution of an "effective immobile atom" for the moving atom ensemble. The spectral manifestation of nonlinear effects is analyzed in detail. The influence of nonlinear interference effects on the generation characteristics in the presence of external field is investigated.
The review systematizes the experimental material and reports the fundamental theoretical results on the study of nonlinear resonance effects in spectra of atomic systems situated in the radiation field of lasers. The theoretical part explains the topics of greatest importance and significance for understanding of the experimental studies: the Stark effect in an optical field; the nonequilibrium velocity distribution of the atoms; the shape of the spectral line for a transition adjacent to a transition combining with a strong field; the simultaneous manifestation of the Stark effect and of Doppler broadening in the form of a very sharp structure on the line contour; a brief mention of the influence of collisions, recoil, and other factors on the sharp structure in spectra. The experimental part reports the results of experiments on the observation of the Stark effect in the optical region of the spectrum, the fine structure of the profile of a Doppler-broadened line and its properties, namely the dependence on the observation direction, the anisotropy in the field of a standing wave, the polarization properties, etc. in spectra of spontaneous or stimulated emission, absorption, and generation.
Nonlinear effects of sublevel coherence on resonant backward-degenerate four-wave mixing are analyzed in the saturation regime of an inhomogeneously broadened and optically thin gas medium, composed of \ensuremath{\Lambda}-type three-level atoms. No limitations are set to the pump-field intensities, and an analytical approach is presented in the Doppler limit and efficient transverse-optical-pumping regime. It is shown that coherent population trapping due to strong pump-field coupling has a negligible incidence in phase conjugation, while interference of two imbalanced coherent-population-injection channels determines the mixing process. Level-crossing emission resonances are found to exhibit particular line-shape characteristics: (1) an insensitivity to power shifts, (2) strong power-broadening accompanied by incomplete line splitting, or (3) field-induced line-broadening inhibition. The conditions under which these effects should be observable are identified, and their dependence on pump imbalance is remarked.
SummaryWe have found new effects nonlinear in the atomic density caused by the free motion of atoms, considering the self-consistent solution of the Maxwell-Bloch equations in the mean-field approximation and for one-atomic density matrix in a gas of two-level atoms. These effects distort the Doppler lineshape (shift, asymmetry, broadening), but are not associated with an atom-atom interaction. In particular, in the case of dominating Doppler broadening of the linewidth (in respect with collisional broadening), founded atomic-motion-induced effects significantly exceed the well-known influence of the dipole-dipole interatomic interaction (e.g., Lorentz-Lorenz shift) by more than one order of magnitude.
The interatomic dipole–dipole interaction is commonly thought to be the main physical reason for spectroscopic effects, which are nonlinear in atomic density. However, we have found that the free motion of atoms can lead to other effects that are nonlinear in atomic density n , using a previously unknown self-consistent solution of the Maxwell–Bloch equations in the mean-field approximation for a gas of two-level atoms with an optical transition at unperturbed frequency ω 0 . These effects distort the Doppler lineshape (shift, asymmetry, broadening), but are not associated with an atom–atom interaction. In particular, in the case of n k 0 − 3 < 1 (where k 0 = ω 0 / c ) and significant Doppler broadening (with respect to collisional broadening), atomic-motion-induced nonlinear effects significantly exceed the well-known influence of the dipole–dipole interatomic interaction (e.g., Lorentz–Lorenz shift) by more than one order of magnitude. Moreover, under some conditions, a frequency interval appears in which a non-trivial self-consistent solution of the Maxwell–Bloch equations is absent due to atomic motion effects. Thus, the existing physical picture of spectroscopic effects that are nonlinear in atomic density in a gas medium should be substantially revised.
We study the effect of nonlinear interference processes on quantum transitions in intense resonant electromagnetic fields with allowance for changes in level populations, relaxation processes, incoherent excitation, and Doppler broadening of the transitions, on the absorption, amplification, and refraction of the interacting fields. The theory is generalized to the case of nonlinear interference interaction of two intense fields in open and closed three-level quantum systems. Using the density matrix, we derive general expressions in the case of stationary interaction that make it possible to analyze the optical characteristics for various configurations of the interfering transitions by a simple substitution of parameters. The possibility of amplifying light without saturated population inversion in a resonant transition is discussed. We formulate the conditions for such amplification and use examples to show that under appropriate changes in the initial level populations and the intensity of the auxiliary light, the inversionless amplification coefficient does not decrease with increasing intensity of the amplified radiation. We also show that allowance for these accompanying processes greatly affects the choice of optimal conditions for interference in optical transitions. As an illustration we list the results of a numerical analysis of possible experiments.
The influence of nonlinear interference processes and of changes in populations in strong electromagnetic fields, and also of the Doppler broadening on resonant four-wave frequency mixing is investigated for a system of Raman-type transitions. The case in which a quantum system interacts with one weak field and two strong fields is considered. Each of the energy levels is assumed to be perturbed by just one strong field. It is shown that the Doppler broadening alters drastically the contributions of the populations of the various levels to the investigated process and that this can alter by several orders of magnitude and nonlinear susceptibilities averaged over the velocities and influence significantly the selection of optimal configurations of the transitions and of the experimental conditions for effective resonant four-wave conversion of the radiation frequencies. A numerical analysis of the derived expressions is used to account for the experimentally observed considerable differences between the spectral dependences of the output power and the conclusions drawn from perturbation theory.