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Soviet Journal of Quantum Electronics

Influence of the laser radiation field on the absorption of pump radiation in a three-level system

V Yu Baranov, Dmitrii D. Malyuta, A P Strel'tsov, С. В. Хоменко

Published Apr 30, 1987• 0 citations
Publisher

Abstract

A reduction in the absorption of the pump radiation under the influence of the laser radiation field was observed for a pulsed CF4 laser. The effect was due to two-photon processes and appeared for a small detuning of the radiation frequencies from a resonance. The results of a calculation carried out on the basis of a steady-state three-level model agreed well with the experimental data.

DOI
10.1070/qe1987v017n04abeh008600

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A reduction in the absorption of the pump radiation under the influence of the laser radiation field was observed for a pulsed CF4 laser. The effect was due to two-photon processes and appeared for a small detuning of the radiation frequencies from a resonance. The results of a calculation carried out on the basis of a steady-state three-level model agreed well with the experimental data.
A theoretical study is made of the influence of changes in the relaxation of a three-level system in a resonance field on the dispersion, absorption, and difference between the populations of levels activated by noncoherent pumping. This change in the relaxation is due to a tendency of a thermal reservoir to create an additional difference between the populations of quasienergy states that appear under the influence of the resonance field. It is shown that as a consequence there is a considerable change in the nature of the interaction with the radiation field in laser crystals with three-level active centers when the pump power is close to the threshold. The lasing conditions are found subject to such changes. It is shown that the threshold pump power can be reduced in this case to a value at which the difference between the populations of the active levels vanishes and lasing appears because of an inversion of the populations in a system of quasienergy levels. Under transient conditions the lasing frequency near the threshold should then depend on the pump
In this paper we report on the effects of recoil on the steady state response of a three level atomic system in two photon absorption. The strength of the fields and their respective frequencies are arbitrary. The expression we derive reduces to that derived earlier, when recoil is neglected. From numerical calculations we conclude that the inclusion of recoil introduces shifts and asymmetries in the response vs. the detuning. We found how the magnitude of the shift depends on the ratio of the probe frequency to the pumping frequency.
The rate of absorption and emission of radiation is calculated for two laser fields interacting with a homogeneously broadened, three-level molecular system. The time-dependent Schrödinger equation is used in the density matrix formalism and the laser fields are treated classically. The laser fields, at frequencies ωpand ωs, are off resonance by δpand δs, respectively, such that|\delta_{p}|, |\delta_{s}| \ll \omega_{p}, \omega_{s}. Analytic expressions are derived for the imaginary part of the electric susceptibility,\chi"(\omega_{p})and\chi"(\omega_{s}). The present work differs from previous calculations in that the laser fields may have arbitrary values of field strength and each field may be on or off resonance. A discussion is presented of the properties of the solutions for\chi"(\omega_{p})and\chi"(\omega_{s}), for both strong and weak laser fields, based on computer evaluation of the general analytic expressions. It is shown that the solutions may be divided into single-photon and two-photon, or Raman, contributions. Conditions for optimizingdI(\omega_{s})/dzand the photon conversion efficiency are derived. These results may be applied to analyzing the pulsed, optically pumped submillimeter laser and to studying two-photon absorption in a gas.
The physics of the two-photon absorption process is investigated for a three-state system. The density-matrix equations for the two-photon interaction are solved in the steady-state limit assuming that the pump laser radiation is monochromatic. Collisional broadening, saturation, and Stark shifting of the two-photon resonance are investigated in detail by numerical solution of the steady-state density-matrix equations. Analytical expressions for the saturation intensity and the Stark shift are derived for the case where the single-photon transitions between the intermediate state and the initial and final states are far from resonance with the pump laser. For this case, it is found that the direction of the Stark shift is dependent on the relative magnitudes of the dipole-moment matrix elements for the single-photon transitions that couple the intermediate state with the initial and final states. Saturation and Stark shifting are also investigated for the case where the single-photon transitions between the intermediate state and the initial and final states are close to resonance with the pump laser.
The effect of radiative decay and collisional damping on the delayed-field population transfer in the three-level system is investigated. The simple analytical steady-state solution of the three-level system, interacting with two intense delayed laser pulses in the dressed-state frame, is obtained and analyzed. The radiative relaxation transfers the system to the ``trapped state,'' which is shown to be stable relative to both radiative decay and collisional damping. The effect of an additional level \ensuremath{\Vert}m〉, situated close to the final level \ensuremath{\Vert}3〉, on the population-transfer process is considered. The field-induced relaxation rate from intermediate level \ensuremath{\Vert}2〉 to level \ensuremath{\Vert}3〉 is shown to be a very easily controllable parameter of the field intensities and their relative delay. This result leads to selective population transfer to the desired level and may prevent leaking out of the three-level system. Theoretical analysis corresponds entirely to recent experimental data [U. Gaubatz et al., J. Chem. Phys. 92, 1 (1990); 92, 5363 (1990)].
A three-level system which radiates at both intermediate transition frequencies is considered to be coherently pumped at a frequency near the two-photon resonance frequency. A sharply resonant rise in the second- and third-level population is found for slight detuning of the pump from two-photon resonance. Population inversion in either transition is shown to be possible, depending on the pertinent parameters. This effect furnishes a novel method of population inversion at a frequency higher than the pump frequency. Keywords include: Laser, Laser-type devices, Coherent pumping, Three-level systems, and Quantum electronics.