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Physical Review Letters

Experimental Evidence of Two-Photon Transition without Doppler Broadening

F. Biraben, Bernard Cagnac, G. Grynberg

Published Mar 25, 1974• 299 citations
Publisher

Abstract

Experiments on the $3S\ensuremath{-}5S$ two-photon transition in sodium give evidence that Doppler broadening is eliminated if the atom absorbs two photons propagating in opposite directions. The proof is given by the comparison of the two-photon absorption line shape in traveling and standing waves.

DOI
10.1103/physrevlett.32.643

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Experiments on the 3S\ensuremath−5S3S\ensuremath{-}5S3S\ensuremath−5S two-photon transition in sodium give evidence that Doppler broadening is eliminated if the atom absorbs two photons propagating in opposite directions. The proof is given by the comparison of the two-photon absorption line shape in traveling and standing waves.
The $3S\ensuremath{-}5S$ transition of Na atoms is induced by absorption of two photons, one each from two circularly polarized beams traveling in opposite directions through the vapor. The beams are derived from a tunable, narrow-band pulsed dye laser. Doppler broadening is absent and the hyperfine structure is resolved. The hyperfine interaction constant A5S{A}_{5S}A5S​ in the 5S5S5S state of the Na23{\mathrm{Na}}^{23}Na23 atom is determined to be 101\ifmmode\pm\else\textpm\fi{}15 MHz.
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.
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.
The two-photon spectrum of sodium atoms, excited by two counterpropagating evanescent waves, is investigated both experimentally and theoretically. Sub-Doppler linewidths are observed, which are quantitatively reproduced by a rigorous theoretical approach that takes into account optical pumping and transit time broadening due to the translational motion of the arriving and departing atoms through the evanescent-wave fields. The velocity distribution of the atoms desorbing from the surface is found to obey a cosine law, which has a significant influence on the observed line shapes.