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Physical Review A

Absorption of a Gaussian laser mode in a molecular beam

Udo Hübner, G. Kramer

Published Jan 1, 1987• 3 citations
Publisher

Abstract

This paper presents a calculation of the depth of the saturation dip observed when laser radiation of a Gaussian ${\mathrm{TEM}}_{00}$ mode is absorbed in a thermal molecular beam or in a very-low-pressure gas. Transit-time broadening is assumed to be the only broadening mechanism, with neglect of collisions and other relaxations. There is no restriction to small saturation parameters. The absorption experienced by one molecule has been calculated via the optical Bloch equations. Averaging over all relevant parameters of the molecular trajectory and the laser field followed. To get a reference for the saturation, from which to measure the dip depth, simply twice the absorption from a running-wave field has been taken, which therefore also had to be calculated in addition to the calculation of the absorption in a standing wave. Preliminary experiments have been carried out for comparison, and the data agree very well with the calculated shape of the curve and the absolute values of the calculated dip depth. From the laser-power scaling factor, necessary to fit the experimental data to the universal theoretical curve, the dipole moment can be derived without having to know such hard-to-determine quantities as absorber density, partition function, collision relaxation rate, or even the diameter of the laser beam.

DOI
10.1103/physreva.35.733

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Physical Review A•Jun 1, 1977•17 citations
This paper presents a calculation of the depth of the saturation dip observed when laser radiation of a Gaussian TEM00{\mathrm{TEM}}_{00}TEM00​ mode is absorbed in a thermal molecular beam or in a very-low-pressure gas. Transit-time broadening is assumed to be the only broadening mechanism, with neglect of collisions and other relaxations. There is no restriction to small saturation parameters. The absorption experienced by one molecule has been calculated via the optical Bloch equations. Averaging over all relevant parameters of the molecular trajectory and the laser field followed. To get a reference for the saturation, from which to measure the dip depth, simply twice the absorption from a running-wave field has been taken, which therefore also had to be calculated in addition to the calculation of the absorption in a standing wave. Preliminary experiments have been carried out for comparison, and the data agree very well with the calculated shape of the curve and the absolute values of the calculated dip depth. From the laser-power scaling factor, necessary to fit the experimental data to the universal theoretical curve, the dipole moment can be derived without having to know such hard-to-determine quantities as absorber density, partition function, collision relaxation rate, or even the diameter of the laser beam.
A theoretical analysis is made of the interaction of a spatially bounded plane standing optical wave with a molecular gas at a very low pressure. This theory applies to weak and strong (saturating) fields. Calculations are made of the profile, amplitude, and width of a Lamp dip as a function of the intensity of the saturating field and of the dimensions of the light beam. The role of slow molecules in the formation of the dip is identified. It is shown that in weak saturating fields the width of the resonance is governed by the average thermal velocity of molecules in a gas and by the transverse size of the light beam.
An exact expression of the gain constant of two-level molecules (or atoms) in a standing-wave optical field is obtained for a special case where the optical frequency is in exact resonance with the molecular transition and the longitudinal and transverse relaxations have equal decay constants. Secondly, an exact form of gain constant as a function of frequency detuning which decribes the shape of Lamb dip or saturated absorption is shown for another case where the transverse relaxation is much faster than the longitudinal relaxation. A flat velocity distribution of molecules at Doppler limit is assumed in either case.
A three-dimensional theory for the resonant interaction of electromagnetic waves with a gas of two-level atoms is formulated in terms of macroscopic variables. The theory is utilized to find the steady-state attenuation of a plane wave in the presence of another plane wave running in the opposite direction with different amplitude. Contributions are included from the reflection of the oppositely running wave by an induced standing-wave inhomogeneity in the population inversion of the medium. The resulting attenuation and reflection coefficients are expressed as velocity integrals of continued fractions. Correspondence is made with existing gas-laser theories, yielding the formulation of a high-intensity ring-laser theory. Analytic approximations for the coefficients are presented for the Doppler-limit cases of both waves weak, one wave weak, and negligible reflection (rate-equation approximation). More-general cases have been calculated numerically. The attenuation coefficients exhibit a Lamb-dip feature. The relative depth of the dip increases rapidly with power at low saturation levels, slowly at high saturation, and is greater in the attenuation of the weaker wave. The width of the dip is nonlinearly power broadened. The shape of the dip is very nearly Lorentzian, except for one special case at high power in which the line splits. The propagation equations for the two waves are integrated over long absorption paths. A large resulting attenuation increases the relative size of the dip while decreasing the power broadening.
We consider in this paper the Doppler-broadened absorption by two-level molecules of a gas from a weak traveling electromagnetic plane wave in the presence of an oppositely traveling strong plane wave at the same frequency. Here the absorption spectrum exhibits a dip that broadens and deepens as the gas is increasingly saturated by the strong wave. This saturation effect has been employed in the recent experiments on the fine structure of atomic hydrogen performed by H\"ansch, Shahin, and Schawlow (HSS). The form, linewidth, and strength of saturation dips in the fine-structure lines are studied for experimental parameters appropriate to the hydrogen experiment. In addition, saturation line-shape curves are calculated for experimental situations in which the strengths of the stronger field give rise to stronger or weaker saturation of the gas medium and varying degrees of Doppler broadening exist. The calculation of shape of the saturation dip and absorption curves for a Doppler-broadened gas of two-level atoms is made exactly; in effect, the strong field is treated as arbitrarily strong by avoiding a perturbation-theory treatment in favor of the exact solutions for a driven two-level system. The general behavior found is in accord with intuition and experimental observations by HSS. There is an optimum saturation power which gives a prominent dip and beyond which the dip suffers "power broadening."
A density-matrix calculation of the line shape for a Doppler-broadened two-level system subjected to a plane-standing-wave laser field with a Gaussian intensity profile is presented to fifth order in perturbation theory. The primary new result is that, for fixed pressure and intensity, the power-broadening contribution to the linewidth is at a minimum when the beam radius is approximately equal to the mean free path. In addition, an analytic solution for the linewidth in the collision-dominated regime is presented for general collision parameters.