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Physical Review A

Spectroscopy of atoms and molecules in gases: Corrections to the Doppler-recoil shift

Mark P. Haugan, Frank V. Kowalski

Published Apr 1, 1982• 6 citations
Publisher

Abstract

We analyze the excitation by an electromagnetic wave of a two-level molecule (or atom) within a rarefied gas. This process differs from the excitation of an isolated molecule because there is significant interaction between the molecule and the surrounding gas particles as they are all polarized by the electromagnetic wave. These interactions lead to corrections to the recoil and Doppler shifts of the molecule's transition frequency. We propose an experiment using saturation spectroscopy to observe sodium molecular transitions near the atomic $D$ lines which could easily detect the correction to the first-order Doppler shift caused by the interaction between the sodium molecules and the surrounding atomic vapor.

DOI
10.1103/physreva.25.2102

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Physical Review A•Jan 1, 1977•10 citations
We analyze the excitation by an electromagnetic wave of a two-level molecule (or atom) within a rarefied gas. This process differs from the excitation of an isolated molecule because there is significant interaction between the molecule and the surrounding gas particles as they are all polarized by the electromagnetic wave. These interactions lead to corrections to the recoil and Doppler shifts of the molecule's transition frequency. We propose an experiment using saturation spectroscopy to observe sodium molecular transitions near the atomic DDD lines which could easily detect the correction to the first-order Doppler shift caused by the interaction between the sodium molecules and the surrounding atomic vapor.
We develop a field-nonlinear theory of sub-Doppler spectroscopy in a gas of two-level atoms, based on a self-consistent solution of the Maxwell-Bloch equations in the mean field and single-atom density matrix approximations. This makes it possible to correctly take into account the effects caused by the free motion of atoms in a gas, which lead to a nonlinear dependence of the spectroscopic signal on the atomic density even in the absent of a direct interatomic interaction (e.g., dipole-dipole interaction). Within the framework of this approach, analytical expressions for the light field were obtained for an arbitrary number of resonant waves and arbitrary optical thickness of a gas medium. Sub-Doppler spectroscopy in the transmission signal for two counterpropagating and co-propagating waves has been studied in detail. A previously unknown red shift of a narrow sub-Doppler resonance is predicted in a counterpropagating waves scheme, when the frequency of one wave is fixed and the frequency of the other wave is varied. The magnitude of this shift depends on the atomic density and can be more than an order of magnitude greater than the known shift from the interatomic dipole-dipole interaction (Lorentz-Lorenz shift). The found effects, caused by the free motion of atoms, require a significant revision of the existing picture of spectroscopic effects depending on the density of atoms in a gas. Apart of fundamental aspect, obtained results are important for precision laser spectroscopy and optical atomic clocks.
We develop a field-nonlinear theory of sub-Doppler spectroscopy in a gas of two-level atoms, based on a self-consistent solution of the Maxwell-Bloch equations in the mean-field and single-atom density-matrix approximations. This makes it possible to correctly take into account the effects caused by the free motion of atoms in a gas, which lead to a nonlinear dependence of the spectroscopic signal on the atomic density even in the absence of a direct interatomic interaction (e.g., dipole-dipole interaction). Within the framework of this approach, analytical expressions for the light field were obtained for an arbitrary number of resonant waves and arbitrary optical thickness of a gas medium. Sub-Doppler spectroscopy in the transmission signal for two counterpropagating and copropagating waves has been studied in detail. A previously unknown redshift of a narrow sub-Doppler resonance is predicted in a counterpropagating waves scheme, when the frequency of one wave is fixed and the frequency of the other wave is varied. The magnitude of this shift depends on the atomic density and can be more than an order of magnitude greater than the known shift from the interatomic dipole-dipole interaction (Lorentz-Lorenz shift). The found effects, caused by the free motion of atoms, require a significant revision of the existing picture of spectroscopic effects depending on the density of atoms in a gas. Apart from the fundamental aspect, obtained results are important for precision laser spectroscopy and optical atomic clocks.
The purpose of this work was to investigate coherence effects in the interaction of two counterpropagating electromagnetic waves with the atoms of a gas, in the case in which one of the waves is weak and frequency modulated, while the other is sufficiently intense to cause saturation. Solving the equations for the density matrix in first-order perturbation theory, the authors obtained in analytic form the real part of the susceptibility integrated over the atom's velocity, expressed in terms of the rate equation model (REM) predictions plus the coherence corrections. The relaxation constants of the levels involved in the transition were kept different in order to allow a wider range of applications of the results. Calculated line shapes related either to the frequency-modulated (FM) sideband or to the ordinary dispersion techniques are presented. The REM approximation and the coherence corrections are shown in detail for an optical line which is of interest for frequency standard investigations.
Up to now, Doppler-free nonlinear spectroscopy has been applied to atoms inside a gas medium (volume spectroscopy). We have extended these methods to atoms in the vicinity of a surface. The basic principle consists of monitoring reflectivity changes produced when a laser beam, incident on a glass–vapor interface, is brought into resonance with an atomic transition. For Doppler-free spectroscopy, two counterpropagating beams are used to operate velocity selection. If these two beams are under normal incidence in the glass—velocity selection perpendicular to the surface—one observes saturated dispersion (selective reflection sensitive to the real index). For incidence angles in the glass (prism) larger than the critical angle (total internal reflection), a standing evanescent wave is produced in the gas (velocity selection along the surface), and saturated absorption is detected. Experimental demonstration was performed on the Na resonance line; high sensitivity (10−4 relative reflectivity change) and spectral resolution as good as 20 MHz were obtained. The main limitation to better resolution comes from the short atomic transit time in the evanescent wave (typical extension ~λ). Relevant applications of these techniques should also concern the diagnostics of optically thick media, as analysis of interaction between gas-phase atoms and the surface, notably atom–wall collisions, and modification of the spontaneous emission characteristics.
The authors consider the Doppler-broadened index of refraction of a two-level molecule of a gas for a weak travelling electromagnetic plane wave in the presence of a strong plane wave travelling in the opposite direction at the same frequency. The authors use the FVH vector model for a two-level system to calculate the real part of the non-linear susceptibility of the gas. The optical dispersion curve exhibits a wiggle at the centre line, that broadens and deepens as the gas is increasingly saturated by the strong incident wave.
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."