Optical triple resonance

Abstract

A semiclassical treatment is given for the serial, near-resonant interaction of three waves in seven equivalent four-level atomic or molecular systems. Explicit equations are presented for the complex susceptibilties for the three waves, valid for $t\gg T_2$, which contain implicit ac Stark-shift and -splitting information, and can be separated into one-, two-, and three-photon contributions. For the case of a weak third or terminal wave, equations for the degree of ac Stark shifting and splitting are found and indicate that the three-photon or triple-resonance contribution is immune to the optical Stark effect if the remaining two waves are tuned to at least two-photon resonance conditions. The conditions for Doppler-free triple resonance are outlined, and it is shown that an equivalent ac Stark broadening may exist but may also be minimized by an appropriate choice of field intensities.