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Soviet Journal of Quantum Electronics

Doppler-free many-photon spectroscopy

Bernard Cagnac

Published Aug 31, 1978• 0 citations

Abstract

A description is given of the apparatus which represents realization of the well-known principle of cancellation of the Doppler effect in two-photon transitions. A brief review is given of the applications of the Doppler-free two-photon spectroscopy in the measurements of the fine and hyperfme structure of highly excited states, isotopic shifts, etc. Collisional broadening and spectral shift in sodium vapor mixed with various buffer gases is considered. A detailed discussion is given of the application of the Doppler-free two-photon spectroscopy to studies of transient optical processes. The method is extended to the case of many-photon transitions. A description is given of the apparatus suitable for the observation of Doppler-free three-photon transitions. Advantages and shortcomings of the new and existing methods are discussed.

DOI: 10.1070/qe1978v008n08abeh010619

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A description is given of the apparatus which represents realization of the well-known principle of cancellation of the Doppler effect in two-photon transitions. A brief review is given of the applications of the Doppler-free two-photon spectroscopy in the measurements of the fine and hyperfme structure of highly excited states, isotopic shifts, etc. Collisional broadening and spectral shift in sodium vapor mixed with various buffer gases is considered. A detailed discussion is given of the application of the Doppler-free two-photon spectroscopy to studies of transient optical processes. The method is extended to the case of many-photon transitions. A description is given of the apparatus suitable for the observation of Doppler-free three-photon transitions. Advantages and shortcomings of the new and existing methods are discussed.

The review describes atomic transitions where two or more photons are simultaneously absorbed by an atom or a molecule (without any intermediate resonant level). The authors show theoretically and experimentally the possibilities of these transitions for numerous high-resolution spectroscopic studies. The Doppler broadening is suppressed in two-photon transitions if the atoms are irradiated by two laser waves travelling in opposite directions, because the Doppler shift in one wave cancels that in the other. A generalization is made for multiphotonic transitions. A typical experimental set-up with a CW dye laser is described in detail, but the possibilities of other light sources are also discussed.

Doppler-free two-photon transitions between the

3s

,

J=2

metastable state and the subconfiguration $7{d}^{\ensuremath{'}}$ of neon are studied with a pulsed-dye-laser oscillator-amplifier system which was synchronized with a chopped rf discharge in neon vapor. The isotopic shifts for these transitions are measured, and based on these measurements we have made a systematic study of Ne-Ne and Ne-He collisional broadening and shift of these very narrow Doppler-free two-photon resonances.

Discusses the theory of Doppler-free two-photon transitions. The theory is worked out for the case of one arbitrarily strong field and one weak field. The Doppler limit is assumed. These simplifications allow the authors to discuss the experimental manifestations of various parameters. They consider power shifts and broadening the number of resonant peaks and their positions. The general case of an off-resonant intermediate state and the single-frequency case with a resonant intermediate state are discussed. The former is found to lead to a power shift, whereas the latter is unshifted in a certain region. In addition the resonant case gives an enhancement without an appreciable increase in width.

We report here the first experimental demonstration of Doppler-free three-photon spectroscopy. The Doppler broadening is eliminated by insuring that the sum of the momenta of the three photons simultaneously exchanged between the atom and the laser beams is equal to 0. This is accomplished by making a proper choice of the angles between the three exciting beams. The observation has been made on the sodium $3{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}$ transition with absorption of two photons and induced emission of one.

Doppler-free two-photon absorption spectroscopy was applied to study highly-excited D states of Rb atoms. Using a cw dye laser as an excitation source, transitions from the ground 5S state to nd 2D states (n=11-32) were observed, the ionization energy of the highest state being only 117cm-1. These D doublets are not inverted. The fine structure splittings of these states do not vary as (neff) -3, nor as n-3. The isotope shift of the 85Rb, 87Rb ground states is found to be 160±12MHz. No pressure broadening was observed for these transitions within the instrumental resolution of 15 MHz.