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Physical Review Letters

Three-Photon Doppler-Free Spectroscopy: Experimental Evidence

G. Grynberg, F. Biraben, M. Bassini, Bernard Cagnac

Published Aug 2, 1976• 61 citations
Publisher

Abstract

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.

DOI
10.1103/physrevlett.37.283

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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 3S12\ensuremath−3P123{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}3S21​​\ensuremath−3P21​​ transition with absorption of two photons and induced emission of one.
Three-photon laser excitation of Rydberg states by three different laser beams can be arranged in a starlike geometry that simultaneously eliminates the recoil effect and Doppler broadening. Our analytical and numerical calculations for a particular laser excitation scheme $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}6{S}_{1/2}\ensuremath{\rightarrow}nP$ in Rb atoms have shown that, compared to the one- and two-photon laser excitation, this approach provides much narrower linewidth and longer coherence time for both cold atom samples and hot vapors, if the intermediate one-photon resonances of the three-photon transition are detuned by more than respective single-photon Doppler widths. This method can be used to improve fidelity of Rydberg quantum gates and precision of spectroscopic measurements in Rydberg atoms.
We demonstrate coherent Doppler-free three-photon excitation of the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ optical clock transition and the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ intercombination transition in free-space thermal clouds of 88Sr^{88}\mathrm{Sr}88Sr atoms. By appropriate orientation of the wave vectors of three lasers incident on the atoms, the first-order Doppler shift can be eliminated for all velocity classes. Three-photon excitation of the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ transition enables high-contrast Ramsey spectroscopy with interrogation times comparable to the $21\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ natural lifetime using a single near-resonant laser source. Three-photon spectroscopy on the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ clock transition, using only laser frequencies nearly resonant with the $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{0}$ and $^{1}S_{0}\phantom{\rule{0.16em}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{0.16em}{0ex}}^{3}P_{1}$ transitions, enables a reduction in Doppler broadening by two orders of magnitude and a corresponding $\ensuremath{\sim}470\phantom{\rule{0.16em}{0ex}}\mathrm{Hz}$ linewidth without a confining potential.
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 $3S\ensuremath{-}5S$ 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.