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Journal of Experimental and Theoretical Physics

Generation of undamped stokes radiation under resonant pumping of the dipole-forbidden transition in a Ξ-atom

Victor P. Kochanov

Published Dec 1, 2009• 2 citations
Publisher

Abstract

We have developed a theory of the nonlinear ring interaction of three intense fields in the scheme of resonant Raman scattering on the dipole-allowed transition from the ground state to the first excited state of a cascade three-level quantum system. We show that the backward Stokes radiation generated by a pump resonant to the dipole-forbidden transition can be used in remote laser sensing of metal vapors.

DOI
10.1134/s1063776109120024

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We have developed a theory of the nonlinear ring interaction of three intense fields in the scheme of resonant Raman scattering on the dipole-allowed transition from the ground state to the first excited state of a cascade three-level quantum system. We show that the backward Stokes radiation generated by a pump resonant to the dipole-forbidden transition can be used in remote laser sensing of metal vapors.
The theory of stimulated Raman and hyper-Raman scattering involving resonance transitions to the ground states of atoms is presented, where the atoms are modeled by the three-level cascade quantum system. The possibility of efficient inversionless generation of radiation is shown for all three transitions participating in the stimulated Raman scattering and for the two electric-dipole allowed transitions in the hyper-Raman scattering. The existence conditions for such generation are determined depending on intensities of the three waves participating in closed-loop wave mixing, their total phase, and pump frequency detuning from the frequency of the dipole-forbidden transition. A new method of remote sensing of atomic components of the atmosphere based on inversionless generation is proposed, which may have significantly higher detection sensitivity as compared to traditional fluorescence technique.
The main properties of infrared stimulated electronic Raman scattering (SERS) at the 6 2 S 1/2 -7 2 S 1/2, 3/2 transitions in cesium atoms are studied theoretically and experimentally as functions of the atomic concentration, which was varied from 10 11 to 10 16 cm −3 . It is found that the efficiency of generation of Stokes radiation strongly depends on one-photon absorption of the pump radiation tuned near frequencies of the 6 2 S 1/2 -7 2 P 1/2, 3/2 transitions. By using the equation for the density matrix, which describes the evolution of a three-level system, the theory of resonance excitation of IR radiation upon one-photon absorption at an adjacent transition is developed. The theory describes well the main features of IR SERS in alkali-metal vapors.
The influence of a strong field resonant to the Raman transition on the behavior of the Stokes harmonic in saturated two-wave stimulated Raman scattering is theoretically considered based on the description of a gas of three-level atoms by medium density matrix equations. The vibrational mode of energy redistribution between laser and scattered radiation, threshold with respect to the resonant field intensity, is predicted. The action of optical fields on the absorption and amplification of the resonant field in a Raman medium is described.
When a principal atomic transition (dipole allowed from the ground state) is driven by odd- multi-photon excitation or by stimulated hyper-Raman scattering, a nonlinear multi-wave mixing field is generated at the transition frequency. A number of dramatic effects on such odd-photon mediated processes can ensue as a result of the internally generated wave-mixing fields. Excellent agreement between theory and experimental studies in Xe and in metal vapors is illustrated for a number of predicted effects including: suppression and strong shifting of resonance lines and hyper-Raman emissions under single and multi-laser excitation. We illustrate the dependence of the interference-related effects on pressure, oscillator strength, wavelength combination and relative propagation directions of pump laser beams. Contrary to most other nonlinear effects, we show that none of the features (in the semi-classical regime) depends on the intensity of the driving laser field.
A model is developed for the description of stimulated Raman scattering. This model allows for changes in the level populations due to radiative transitions and it can be used also for an arbitrary detuning of the pump radiation from the center of a line of an atom in the active medium. A study is made of the conversion of wide-band laser radiation into a Stokes signal. It is shown that this conversion is quite efficient and the Stokes signal gain corresponds to coherent scattering. This result is related to the matching of the phases of the pump and Stokes signals. Numerical investigations carried out using this model under the experimental conditions described elsewhere give results in agreement with the experimental data.
The general method developed in a previous paper (see ibid., vol.10, p.345 (1977)) is applied to the problem of resonance Raman scattering in very intense laser fields. At very low intensities the spectrum consists of three monochromatic lines (Rayleigh, Raman Stokes and anti-Stokes) which split into a triplet and two doublets when the laser light, tuned on one of the two transitions connecting the upper state to the two lower sublevels, has a sufficiently high intensity to saturate this transition but not the second one. The Raman and Rayleigh lines are completely mixed when the intensity becomes so high that both transitions are saturated. The corresponding evolution of the spectrum is determined. Optical-pumping effects leading to asymmetries in the fluorescence spectrum are taken into account.