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Annual Meeting Optical Society of America

Theory of two-photon multiwave mixing

Shlomo Ovadia, Murray Sargent, Mao Hong Lu

Published Jan 1, 1985• 0 citations
Publisher

Abstract

Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.

DOI
10.1364/oam.1985.we2

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TWO-PHOTON MULTIWAVE MIXING (DOPPLER-FREE SPECTROSCOPY).

Barbara A. Capron

This dissertation examines aspects of the interaction of multiple coherent light fields for the two-photon two-level model. In this model the interacting energy levels are not connected by an atomic dipole and a two-photon transition between them is necessary. We employ the density matrix formalism allowing easy comparison between the one- and two-photon two-level models. Significant differences are found due to dynamic Stark shifts and conjugate scattering off the pump-induced two-photon coherence. Averages over Doppler broadening are performed and the new upper-level relaxation mechanisms of decay to an intermediate nonresonant level and ionization from the upper state are included. The new relaxation mechanisms, introduced to the theory to better model experiments, are similar except that ionization is intensity dependent. They cause the resulting probe absorption spectra to become more complex and in general asymmetric. Doppler broadening is also important in experiments using gases. We analytically average over a Lorentzian velocity distribution for both co- and counterpropagating pump and probe beams. For copropagating fields the results are similar to those for the one-photon case averaged over inhomogeneous broadening, whereas counterpropagating pump and probe fields yield the so-called Doppler-free configuration that is normally only modelled to third order in the pump amplitude. We consider the pump field amplitude to all orders and find that as long as the width of the Doppler velocity distribution is significantly larger than the two-photon Rabi frequency the results are Doppler-free. The final part of the dissertation treats the question of two-photon squeezed states. This requires quantized sidemodes. Squeezed states are minimum uncertainty states with unequal variances in the two quadratures of the electromagnetic field amplitude. One way to generate these states is via multiwave mixing and we present here the first calculation for nondegenerate two-photon multiwave mixing as it applies to squeezed states. We find that in general two-photon squeezed states require lower intensities and detuning than those predicted by the one-photon model.

•Jan 1, 1986•0 citations
Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.
Steady-state interactions of one, two, and three waves with two-photon two-level media are treated semiclassically. Dynamic Stark shifts as well as dynamic Stark splittings are included in the theory. The intermediate levels are assumed to be nonresonant, and one wave is allowed to have arbitrarily large intensity. The theory parallels the one-photon theory of multiwave mixing couched in terms of population pulsations. We find the one-, two-, and three-wave two-photon absorption coefficients and the three-wave coupling coefficients. We find similarities and significant differences between the one- and two-photon polarizations of the medium. The work treats two-photon saturation spectroscopy, laser- and optical-bistability instabilities, and phase conjugation with a unified formalism.
Multiphoton transitions are of great interest in laser spectroscopy because they permit the study of new physical phenomena and because of their potential applications. Malcuit et al.1 studied two-photon transitions in atomic sodium and showed that for appropriate phase-matching four-wave mixing can overcome the usual spontaneous decay processes. We have recently developed a quantum theory2 to treat such multiwave mixing processes in two-photon media. Because of the greater complexity of two-photon transitions, many effects arise that are absent in the one-photon case, some of which have important consequences in the generation of squeezed states. For the two-photon two-level model, the field modes have frequencies approximately one-half the frequency difference between the levels. We find that our coefficients differ from the corresponding one-photon theory in that dynamic Stark shifts have a major effect and that the pump-induced coherence between the two levels has a new term in the conjugate coupling terms, which leads to improved squeezing.
Our semiclassical theory of two-photon multiwave mixing1 is a generalization of the degenerate four-wave mixing case2 to treat nondegenerate pump/signal/conjugate frequencies. We apply that theory to four-wave mixing in two-photon media. We present explicit formulas for the nondegenerate signal/conjugate absorption and coupling coefficients for cases for which the two-photon Stark shifts are sufficiently small compared to the homogeneous linewidths. More general cases require that the spatial hole burning averages be performed numerically. We find intricate dependencies of the transmission and reflection spectra on the pump intensity and on dynamic Stark shifts. In particular, the reflection coefficients do not necessarily bleach to zero as the pump intensity is increased indefinitely, and interferences occur between pure index and mixed absorption/index contributions
The theory of degenerate four-wave mixing using two-photon transitions is formulated. Two kinds of mechanisms compete in generating conjugate waves leading to two phenomena that do not occur in two-level media: (1) a double-peaked reflection spectrum and (2) coupled-mode oscillation in absorbing media. In addition, because of the dynamic Stark-shifted line center, the reflection coefficient approaches a constant value at large intensities, unlike the two-level coefficient, which bleaches to zero.
In a recent paper,1 we considered the stability of single-mode operation in two-photon lasers and two-photon optical bistability.2 The models assumed that two photons of equal or nearly equal frequencies span the atomic two-photon transition, with no resonant intermediate levels. The paper neglects possible Stark shifts of the two levels due to virtual transitions to nonresonant levels and back. For one-photon processes, these virtual transitions can be neglected because they have one nonresonant denominator. They cannot in general be neglected for the two-photon case, however, since all transition probabilities have at least one nonresonant denominator. In this paper we give formulas and illustrations for the two-photon two-level absorption and coupling coefficients including Stark shifts. For vanishing shifts, the coefficients have symmetric spectra that look very similar to their one-photon counterparts, but for nonzero shifts, they have asymmetric spectra with exaggerated resonances. These resonances appear to increase the likelihood of instabilities for certain combinations of pump detuning and Stark shifts.
This dissertation examines aspects of the interaction of multiple coherent light fields for the two-photon two-level model. In this model the interacting energy levels are not connected by an atomic dipole and a two-photon transition between them is necessary. We employ the density matrix formalism allowing easy comparison between the one- and two-photon two-level models. Significant differences are found due to dynamic Stark shifts and conjugate scattering off the pump-induced two-photon coherence. Averages over Doppler broadening are performed and the new upper-level relaxation mechanisms of decay to an intermediate nonresonant level and ionization from the upper state are included. The new relaxation mechanisms, introduced to the theory to better model experiments, are similar except that ionization is intensity dependent. They cause the resulting probe absorption spectra to become more complex and in general asymmetric. Doppler broadening is also important in experiments using gases. We analytically average over a Lorentzian velocity distribution for both co- and counterpropagating pump and probe beams. For copropagating fields the results are similar to those for the one-photon case averaged over inhomogeneous broadening, whereas counterpropagating pump and probe fields yield the so-called Doppler-free configuration that is normally only modelled to third order in the pump amplitude. We consider the pump field amplitude to all orders and find that as long as the width of the Doppler velocity distribution is significantly larger than the two-photon Rabi frequency the results are Doppler-free. The final part of the dissertation treats the question of two-photon squeezed states. This requires quantized sidemodes. Squeezed states are minimum uncertainty states with unequal variances in the two quadratures of the electromagnetic field amplitude. One way to generate these states is via multiwave mixing and we present here the first calculation for nondegenerate two-photon multiwave mixing as it applies to squeezed states. We find that in general two-photon squeezed states require lower intensities and detuning than those predicted by the one-photon model.