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Physical Review Letters

Two-Photon Coherent Transient Measurements of Doppler-Free Linewidths with Broadband Excitation

P. F. Liao, Nicholas P. Economou, Richard R. Freeman

Published Dec 5, 1977• 68 citations
Publisher

Abstract

We report the first measurements of Doppler-free two-photon linewidths obtained with a simple coherent transient technique using a wide-bandwidth laser. Measurements of two-photon optical-free-induction decay are used to determine pressure-broadening coefficients for the $3S\ensuremath{-}4D$ transition of sodium for collision with helium, neon, and argon. Pressure-broadened linewidths of several tens of MHz are measured with laser linewidths of several GHz.

DOI
10.1103/physrevlett.39.1473

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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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Due to the phase-coherent relationship of intra-cavity pulse reflections leading to the narrow frequency-selectivity of the cavity, Cavity Ring-Down Laser Absorption Spectroscopy (CRLAS) is a promising method lo study Doppler-free two-photon absorption at resolutions at least two orders of magnitude better than the pulse bandwidth of even Fourier Transform Limited nsec pulsed lasers. The nonlinear absorption will lead to a nouexponential cavity decay with can be used to discriminate it from both linear absorption and intrinsic cavity loss. In this study, several issues have been examined in order to access the feasibility of obtaining the high-resolution two-photon absorption spectra of the Rydberg states of alkali dimers by this technique. Using atomic transition dipoles as an approximation, the laser intensities needed to elicit reasonable excitation were estimated, and found to be well within presently available levels. The importance of the various linewidth- limiting mechanism was also examined. The relative magnitudes of pressure broadening, AC Stark broadening, cavity stability, and time-of-flight broadening lead us to expect a resolution of $\\sim$1 MHz or better.