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Reports on Progress in Physics

Doppler-free multiphotonic spectroscopy

G. Grynberg, Bernard Cagnac

Published Jul 1, 1977• 201 citations
Publisher

Abstract

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.

DOI
10.1088/0034-4885/40/7/002

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Doppler-free many-photon spectroscopy

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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.

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Two-photon spectroscopy. II. Effects of residual Doppler broadening

Rainer Salomaa, Stig Stenholm

For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.

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Two-photon spectroscopy: effects of a resonant intermediate state

Rainer Salomaa, Stig Stenholm

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.

Journal of Physics B Atomic and Molecular Physics•Aug 1, 1975•53 citations

Three-Photon Doppler-Free Spectroscopy: Experimental Evidence

G. Grynberg, F. Biraben, M. Bassini +1 more

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.

Physical Review Letters•Aug 2, 1976•61 citations

Two-photon absorption yields Doppler-free spectroscopy

Gloria B. Lubkin

In one of those events so typical of research, three groups have independently and almost simultaneously demonstrated two-photon absorption in sodium vapor without blurring from Doppler broadening. The technique appears to open up a new way of achieving high-resolution spectroscopy with tunable lasers. And it can be applied, for example, to induce photochemical reactions selectively, to separate isotopes, or to provide more precise values for the Rydberg constant and Lamb shifts.

Physics Today•Jul 1, 1974•1 citation
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.
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.
For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.
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.