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Physical Review

Theory of Optical Frequency Mixing Using Resonant Phenomena

Ali Javan, A. Szöke

Published Jan 18, 1965• 15 citations
Publisher

Abstract

The nonlinear interaction of two intense optical waves with three energy levels of an atomic system is analyzed theoretically. The frequencies of the applied fields are assumed to be on or near two of the resonances involving the three levels. Particular attention is given to the generation of power at the difference frequency of the two applied fields where their frequency separation lies in the far-infrared range of the spectrum. In the limit of large input fields where atomic transitions are driven to saturation, the generated difference-frequency power is no longer proportional to the product of the two input powers. It is shown that, in this limit, the total rate of emission of photons at the difference frequency may, in principle, approach a value given by $\frac{\mathrm{rN}}{T}$, where $N$ is the total number of atoms, $T$ is the average time of coherent interaction of atoms and the radiation field, and $r$ is a factor which in favorable cases approaches unity at low temperatures. Also, a number of additional effects are encountered due to coherent double-quantum transitions among various levels which may be ignored only for weak input powers. These effects are highly dependent on the modes of relaxations of atomic levels and the details of the line shape. The results are applied to several cases, in which the resonance condition yields large efficiency in nonlinear frequency mixing.

DOI
10.1103/physrev.137.a536

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Physical Review•Oct 7, 1966•185 citations
The nonlinear interaction of two intense optical waves with three energy levels of an atomic system is analyzed theoretically. The frequencies of the applied fields are assumed to be on or near two of the resonances involving the three levels. Particular attention is given to the generation of power at the difference frequency of the two applied fields where their frequency separation lies in the far-infrared range of the spectrum. In the limit of large input fields where atomic transitions are driven to saturation, the generated difference-frequency power is no longer proportional to the product of the two input powers. It is shown that, in this limit, the total rate of emission of photons at the difference frequency may, in principle, approach a value given by rNT\frac{\mathrm{rN}}{T}TrN​, where NNN is the total number of atoms, TTT is the average time of coherent interaction of atoms and the radiation field, and rrr is a factor which in favorable cases approaches unity at low temperatures. Also, a number of additional effects are encountered due to coherent double-quantum transitions among various levels which may be ignored only for weak input powers. These effects are highly dependent on the modes of relaxations of atomic levels and the details of the line shape. The results are applied to several cases, in which the resonance condition yields large efficiency in nonlinear frequency mixing.
The influence of nonlinear interference processes and of changes in populations in strong electromagnetic fields, and also of the Doppler broadening on resonant four-wave frequency mixing is investigated for a system of Raman-type transitions. The case in which a quantum system interacts with one weak field and two strong fields is considered. Each of the energy levels is assumed to be perturbed by just one strong field. It is shown that the Doppler broadening alters drastically the contributions of the populations of the various levels to the investigated process and that this can alter by several orders of magnitude and nonlinear susceptibilities averaged over the velocities and influence significantly the selection of optimal configurations of the transitions and of the experimental conditions for effective resonant four-wave conversion of the radiation frequencies. A numerical analysis of the derived expressions is used to account for the experimentally observed considerable differences between the spectral dependences of the output power and the conclusions drawn from perturbation theory.
A very large number of physical phenomena in the resonant interaction of atomic-molecular systems with the radiation fields can be studied by treating the atomic system as a two level system and by examining its response to the applied fields. Various perturbative results are well known. A number of recent experimental works require the knowledge of the nonperturbative response functions, when both the applied fields are strong. These include a variety of experiments on instabilities(1) in lasers involving the switching from a single mode to for example two mode operation. Similarly recent nonlinear mixing experiments, where not only four wave mixing but also higher mixing in saturating fields has been studied. Pump probe experiments have also been repeated with probes whose intensity could be large. The purpose of this paper is to formulate the general theory and use it to understand the experiments. The formulation we present is also well suited for studying the effect of collisions. Details of various collisional induced coherences in fourwave and six wave mixing etc. can be studied.
Two-photon resonant and near-resonant four-wave difference-frequency mixing in gases in the interaction regime when laser pulse durations are comparable to or shorter than the medium polarization relaxation time ${T}_{2}^{\ensuremath{'}}$ is investigated. The results of experimental studies of the process in Ar and Kr using pump pulses from the ArF-excimer laser are presented demonstrating a generation of tunable short pulse radiation in the range 102--124 nm. The results are discussed in terms of a theoretical model based on a self-consistent solution of the Bloch equations for the atomic transitions and the Maxwell equations for the fields. This enables one to interpret specific nonstationary resonant and quasiresonant phenomena involved in the frequency conversion process. It is shown that the femtosecond-pulse four-wave frequency-mixing technique with probe pulses significantly shorter than the pump pulses makes it possible to study the coherent dynamics of an atomic transition exposed to an intense field. Using atomic Kr as the nonlinear medium, coherent Rabi oscillations and the subsequent phase relaxation of excitation were observed under the condition of two-photon interaction of Kr with femtosecond 193-nm laser pulses. The obtained information is important for controlling and optimizing processes of two-photon resonant frequency conversion and for time-resolved studies of Rydberg states in atoms and molecules.
An investigation is reported of resonant four-wave frequency mixing of the type ω 4 =ω 1 —ω 2 +ω 3 under coherent population trapping conditions. Such mixing may appear when radiations of frequencies ω 1,2 are strong and when ω 1 —ω 2 =ω 20 (ω 20 is the frequency of a dipole-forbidden transition). The density matrix method is used to calculate (taking quantum interference into account) the absorption coefficients, the refractive indices, and the nonlinear susceptibilities exactly for the strong fields and in the first order of perturbation theory for the weak fields. A study is made of the dependence of the power of nonlinear optical generation on various characteristics of the transitions and of the radiation, subject to the propagation effects. The cases of homogeneous and Doppler broadening of the resonant transitions are considered. The characteristics of transitions in the barium atom are used in numerical illustrations. It is shown that the efficiency of resonant nonlinear-optical conversion of radiation can be enhanced by utilising interference processes in quantum transitions, which represent coherent population trapping.
Multiphoton nonlinear frequency mixing effects on coherent electromagnetically induced absorption spectra of 85Rb^{85}\mathrm{Rb}85Rb atoms using two orthogonal linear polarizations of strong-coupling and weak probe beams are investigated theoretically and experimentally with respect to an applied longitudinal magnetic field and coupling powers. Herein, we confirm that at least five-photon interactions in solving density matrix equations for the ${F}_{g}=3\ensuremath{\rightarrow}{F}_{e}=4$ transition of 85Rb^{85}\mathrm{Rb}85Rb atoms are required to explain experimentally observed coherent electromagnetically induced absorption spectra when a quantum axis is selected as the propagation direction of co-propagating coupling and probe laser beams. Distinct calculated spectral differences owing to variations in the magnetic field and coupling power between three- and five-photon interactions are confirmed. The obtained asymmetrical spectral shapes match very well with those calculated from five-photon interactions considering the off-resonant ${F}_{g}=3\ensuremath{\rightarrow}{F}_{e}=2,3$ transitions. Genuine coherent spectral shapes are observed with a single laser combined with two acousto-optic modulators, wherein the spectral resolution is limited because of the decoherence rate between Zeeman sublevels in the ground state from transit-time relaxation.
The nonlinear absorption or gain characteristics of an optical-frequency, Doppler-broadened atomic resonance involving levels with closely spaced structure are analyzed. The level structures are assumed to be resolved with respect to their natural widths, but not necessarily with respect to the Doppler width at the optical transition. The radiation field consists of two closely spaced monochromatic frequencies lying within the Doppler width of the resonance. This type of radiation field may be obtained, for example, from a laser operating in two of its Fabry-Perot resonator modes. It is shown that, because of saturation of level populations and double-quantum Raman transitions between levels, appreciable nonlinear coupling takes place between the two fields. This coupling shows a resonance behavior when the frequency separation of the two applied fields becomes equal to the frequency splitting between two of the components which form either level structure. The width of this resonance is determined entirely by the natural widths of these two level components and not by the Doppler width of the optical transition or the natural width of other level components. When such a resonance occurs, the over-all gain or attenuation characteristics of the atomic resonance change drastically. In practice the frequency spacing of the fields may be kept constant while the level structures are tuned, e.g., magnetically. The effects are analyzed for cases of running-wave and standing-wave radiation fields. The use of this effect in precise determination of level structures as well as mode or transition coupling of a gas laser is discussed. Portions of the analysis are applicable to resonances with more general forms of inhomogeneous broadening.