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Physical Review A

Optical triple resonance

Samuel J. Petuchowski, J. D. Oberstar, Thomas A. DeTemple

Published Aug 1, 1979• 33 citations
Publisher

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 $t\ensuremath{\gg}{T}_{2}$, 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.

DOI
10.1103/physreva.20.529

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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\ensuremath≫T2t\ensuremath{\gg}{T}_{2}t\ensuremath≫T2​, 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.
A semiclassical density matrix treatment is developed for the parallel near-resonant interaction of three waves in a four-level atomic or molecular system. Explicit solutions are developed and contain implicit AC Stark-shift and splitting information. The role of splitting and AC Stark-shifts is discussed for a system of two competing emitted waves starting from a common optically pumped level; a situation encountered in many optically pumped lasers. Application of the results to a Raman-Raman competition situation in ammonia is illustrated.
The extraction of ac Stark shifts and splittings from a semiclassical treatment of multiple wave-atom interactions is considered. Within the rotating-wave and quasistatic approximations, we show that the information can be extracted from the complex Beer's coefficient sensed by a weak tunable probe wave, whose lower level is fully populated and unconnected to the strong fields. This situation leads to a great simplification of the density-matrix equations of motion, from which algorithms are derived for the algebraic construction of the Beer's coefficients appropriate to other cases not treated. Both level-shifted resonance and line-strength information are contained in the Beer's coefficient, many examples of which are given, some for the first time. Generalized sum rules for the transitions are derived along with a connection of this approach to other approaches including dressing transformations.
The density-matrix approach, in the quasistatic or adiabatic limit, is applied to the case of resonant four-wave interactions in four-level systems resulting in explicit analytical expressions for the nonlinear optical parametric and nonparametric polarizations, including ac Stark effects. The results are applicable to any closed-linkage diagram of this type but are applied only to the specific case of resonant frequency tripling. The results revealed the presence of up to six Stark-shifted nonparametric resonances and the presence of saturation and interference effects on the parametric susceptibility. In particular, the third-order susceptibility is shown to saturate to a very small value under high-field conditions which restricts the range of useful pump intensities. Under near-resonant to resonant conditions, these imply that because of either nonparametric loss present at the pump or harmonic frequencies or power-dependent dispersive and saturation effects, conversion efficiencies higher than 25% may be difficult to realize in practice.
The parametric resonances and the quasi-level structure of an atom strongly driven by a near-resonant amplitude-modulated optical field are studied theoretically. An approximate analytical solution of the density-matrix equations of motion is obtained for two-level and three-level atoms. Based on this solution the quasi-level shifts are analyzed, and the conditions for the quasi-levels to cross each other are derived. Expressions are given for the probe-wave absorption/gain spectrum near the parametric resonance and far from it. It is pointed out that the parametric resonances appear when the pumping field sidebands are tuned to resonance with some transitions among the quasi-levels.
A nonperturbative semiclassical theory is presented for the treatment of four-wave mixing (FWM) in a four-level system. This treatment is based on a transformation to a generalized rotating frame followed by a numerical diagonalization of the resulting time-independent Hamiltonian. For strong fields, all resonant frequencies are shifted from the atomic (molecular) frequencies. Lines are split up in a way similar to the ac Stark effect for a two-level system, and for even stronger fields, the effect of stirring is observed for the first time in four-wave mixing. In addition, a new extra resonance appears which is induced by the saturating field. This field-induced resonance is the new member in the family of extra resonances (pressure induced, or stochastic fluctuation induced), and it should be observed whenever saturating fields interact with a multilevel atomic or molecular system.
We present a theory of Stark splitting in doubly resonant three-photon ionization (three-level system) with nonmonochromatic fields. The asymmetry of the peaks of the resonance curve due to Stark splitting is shown to be reversed when the laser bandwidth is larger than the width of the atomic transitions of the resonant states. It is further shown that ionization as well as the probe field have a significant effect on the features of the splitting. Similar effects are found with monochromatic fields in the presence of an additional level near the initial level (four-level system). The results of the analysis are in general qualitative agreement with existing observations.