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Physical Review Letters

Direct Observation of Atomic Energy Level Shifts in Two-Photon Absorption

P. F. Liao, John E. Bjorkholm

Published Jan 6, 1975• 174 citations
Publisher

Abstract

We report direct observation of optically induced shifts of atomic energy levels in sodium vapor that occur in two-photon absorption. These shifts must be considered in high-resolution two-photon spectroscopy. Two cw dye laser beams of different frequencies and propagating in opposite directions are utilized to obtain high-resolution spectra. The intensity and frequency dependence of the level shifts are examined.

DOI
10.1103/physrevlett.34.1

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Physical Review A•Jan 4, 2000•78 citations
We report direct observation of optically induced shifts of atomic energy levels in sodium vapor that occur in two-photon absorption. These shifts must be considered in high-resolution two-photon spectroscopy. Two cw dye laser beams of different frequencies and propagating in opposite directions are utilized to obtain high-resolution spectra. The intensity and frequency dependence of the level shifts are examined.
Polarization rotation effects in atomic sodium vapor are studied both experimentally and theoretically. Two pulsed dye laser beams propagate collinearly through a cell containing sodium vapor. The direction of polarization of a linearly polarized dye laser beam of frequency ${\ensuremath{\omega}}_{1}$ is found to be rotated by a circularly polarized beam of frequency ${\ensuremath{\omega}}_{2}$. This rotation is due to the difference in refractive index at ${\ensuremath{\omega}}_{1}$ for right and left circularly polarized light which is produced by the circularly polarized beam. When ${\ensuremath{\omega}}_{1}+{\ensuremath{\omega}}_{2}$ is tuned near the $3S\ensuremath{-}5S$ two-photon transition of atomic sodium, this difference is primarily due to the dispersion associated with the two-photon transition. Other sources of polarization rotation which were identified include (i) real transfers of population to excited atomic levels due to collisionally induced transitions and (ii) optically induced atomic energy-level shifts. The theory includes both the effects of two-photon dispersion and optically induced energy shifts. The application of the two-photon polarization rotation effect as a fast, optically controlled shutter or modulator and as a sensitive detection technique for two-photon spectroscopy are briefly 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.
We have used two-photon absorption from counterpropagating laser beams of different frequencies to measure Stark shifts and splittings of the 62S6^{2}S62S, 72S7^{2}S72S, 82S8^{2}S82S, 52D5^{2}D52D, and 62D6^{2}D62D states in sodium. Beams from a fixed-frequency, single-mode Ar+{\mathrm{Ar}}^{+}Ar+ laser and a tunable, single-frequency cw dye laser were focussed into a coarse sodium atomic beam and the fluorescence was monitored. The collimation of the atomic beam reduced the residual Doppler width inherent in using two different frequencies. Using the two lasers allowed two-photon transitions to be observed at frequencies unattainable with the dye laser alone, and enhanced the transition rates due to the near resonance of the dye laser with the strong Na $3^{2}S\ensuremath{\rightarrow}3^{2}P$ transition. Our experimental results for the scalar and tensor polarizabilities, ${\ensuremath{\alpha}}_{0}$ and ${\ensuremath{\alpha}}_{2}$, agree with calculations in the Bates and Damgaard Coulomb approximation within 2% for ${\ensuremath{\alpha}}_{0}$ and 9% for ${\ensuremath{\alpha}}_{2}$. As a by-product the hyperfine-interaction constants aaa for the SSS states and the fine-structure intervals $\ensuremath{\delta}\ensuremath{\nu}=\frac{({E}_{\frac{3}{2}}\ensuremath{-}{E}_{\frac{5}{2}})}{h}$ for the DDD states were obtained.