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

Barbara A. Capron

Published Jan 1, 1986• 0 citations
OpenAlex

Abstract

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.

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Theory of multiwave mixing in two- and three-level media.

Sunghyuck An

This dissertation presents theories of multiwave mixing in two- and three-level media. The first part of the dissertation treats the semiclassical theories in two-level media. Chapter 2 gives the simple semiclassical theory of four-wave mixing when the two pump frequences differ by more than the reciprocal of the population-difference lifetime. This difference washes out the pump spatial holes as well as one of the two reflection gratings. We compare the results to the degenerate treatment of Abrams and Lind and find significant differences in the reflection coefficient spectra. Chapter 3 presents the semiclassical theory of multiwave in a squeezed vacuum characterized by unequal in-phase and in-quadrature dipole decay times. For a highly squeezed vacuum, we find sharp resonances in both probe absorption and reflection coefficients, which provide sensitive ways to measure the amount of squeezing in the vacuum. The second part of the dissertation treats the quantum theories in two- and three-level media. Chapter 4 develops the fourth-order quantum theory of multiwave mixing to describe the effects of sidemode saturation in two-level media. We derive explicit formulas for the fourth-order quantum coefficients and show that the fourth-order quantum theory reproduces the third-order semiclassical coefficient obtained by truncating a continued fraction. We apply the results to cavity problems and find significant differences in the sideband spectra given by the second- and fourth-order treatments, particularly as the sidemode approaches the laser threshold. The final chapter presents a quantum theory of multiwave mixing in three-level cascades with a two-photon pump. The explicit formulas for the resonance fluorescence spectrum and the quantum combination-tone source term are derived. The theory is applied to the generation of squeezed states of light. We find almost perfect squeezing for some strong pump intensities and good broad-band squeezing for low pump intensities.

•Jan 1, 1988•0 citations

Quantum theory of multiwave mixing. IX. Squeezed states in two-photon media

Barbara A. Capron, David A. Holm, Murray Sargent

We apply our quantum theory of multiwave mixing for the two-photon two-level model to the generation of squeezed states of light. Because of the two-photon transition, a larger number of interaction potentials are present compared to one-photon models, leading to effects absent in the one-photon case. The two most significant of these are the appearance of dynamic Stark shifts and conjugate scattering off the pump induced two-photon coherence. We show that this can lead to almost perfect squeezing, even for low pump intensities and low detunings from the two-photon resonance.

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Squeezing in nondegenerate two-photon two-level media

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We recently1 calculated the amount of squeezing predicted by our quantum theory of multiwave mixing for a one-photon two-level model. Here we use the corresponding theory for the two-photon two-level model,2 which allows for nonsaturating nondegenerate pump and probe waves and includes dynamic Stark shifts. We simplify the more complicated general model using a fourthorder perturbation limit and find very simple expressions that show even for very weak pumps with no Stark shifts or atomic detuning significant squeezing can be achieved. Much of this squeezing is due to scattering of the conjugate field off the pump-induced two-photon coherence, which does not arise in the one-photon case. In general, Stark shifts induce large regions of significant gain, resulting in instabilities. We also show results for high intensity pumps that require larger atomic detunings to obtain a large amount of squeezing. The low intensities required in the two-photon case should make squeezing easier to observe than in the one-photon case.

Annual Meeting Optical Society of America•Jan 1, 1986•0 citations

Theory of two-photon multiwave mixing

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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.

Annual Meeting Optical Society of America•Jan 1, 1985•0 citations

Quantum theory of nondegenerate multiwave mixing III Application to single-beam squeezed-state generation

Seng‐Tiong Ho, Prem Kumar, Jeffrey H. Shapiro

We apply our quantum theory of nondegenerate multiwave mixing [ Phys. Rev. A37, 2017 ( 1988)] to squeezed-state generation experiments with two-level atoms. Our main interest is to predict the amount of squeezing achievable with a Doppler-broadened two-level medium. We are particularly interested in the single-beam configuration, in which all four interacting beams are spatially degenerate. We analytically solve the coupled-mode quantum Langevin equations for nondegenerate four-wave mixing. The solutions are used to compute the amount of squeezing. In the computation the effects of pump–probe phase mismatch, collisions, Doppler broadening, and Gaussian-intensity variation are comprehensively taken into account for the first time to our knowledge. Simple rules of thumb as to where one can see squeezing in both degenerate- and nondegenerate-frequency cases are derived by examining the limit of a short medium. We then present the case of an infinitely long medium, in which maximum squeezing is achieved when there is no pump–probe phase mismatch. With the inclusion of pump–probe phase mismatch, however, the maximum amount of squeezing is obtained with a finite-length medium instead. This prompts us to investigate in detail the finite-length medium case. Our results show that the effects of Doppler broadening and Gaussian-intensity variation can be largely circumvented by detuning the pump frequency more than three Doppler half-widths from resonance and that good broadband squeezing can be achieved even with a Doppler-broadened medium that has a moderate amount of collision broadening. Under these circumstances it is found that the effect of pump self-focusing or defocusing will be the major factor that limits the amount of achievable squeezing. In particular, the spatially varying nonlinear refractive indices seen by the pump and the probe modes are quite different, which causes the former to become spatially mismatched with the latter in the region in which strong squeezing is otherwise expected.

Journal of the Optical Society of America B•Jan 1, 1991•10 citations

Quantum theory of multiwave mixing in two-photon two-level media

David A. Holm, Murray Sargent

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.

Annual Meeting Optical Society of America•Jan 1, 1986•0 citations
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.
This dissertation presents theories of multiwave mixing in two- and three-level media. The first part of the dissertation treats the semiclassical theories in two-level media. Chapter 2 gives the simple semiclassical theory of four-wave mixing when the two pump frequences differ by more than the reciprocal of the population-difference lifetime. This difference washes out the pump spatial holes as well as one of the two reflection gratings. We compare the results to the degenerate treatment of Abrams and Lind and find significant differences in the reflection coefficient spectra. Chapter 3 presents the semiclassical theory of multiwave in a squeezed vacuum characterized by unequal in-phase and in-quadrature dipole decay times. For a highly squeezed vacuum, we find sharp resonances in both probe absorption and reflection coefficients, which provide sensitive ways to measure the amount of squeezing in the vacuum. The second part of the dissertation treats the quantum theories in two- and three-level media. Chapter 4 develops the fourth-order quantum theory of multiwave mixing to describe the effects of sidemode saturation in two-level media. We derive explicit formulas for the fourth-order quantum coefficients and show that the fourth-order quantum theory reproduces the third-order semiclassical coefficient obtained by truncating a continued fraction. We apply the results to cavity problems and find significant differences in the sideband spectra given by the second- and fourth-order treatments, particularly as the sidemode approaches the laser threshold. The final chapter presents a quantum theory of multiwave mixing in three-level cascades with a two-photon pump. The explicit formulas for the resonance fluorescence spectrum and the quantum combination-tone source term are derived. The theory is applied to the generation of squeezed states of light. We find almost perfect squeezing for some strong pump intensities and good broad-band squeezing for low pump intensities.
We apply our quantum theory of multiwave mixing for the two-photon two-level model to the generation of squeezed states of light. Because of the two-photon transition, a larger number of interaction potentials are present compared to one-photon models, leading to effects absent in the one-photon case. The two most significant of these are the appearance of dynamic Stark shifts and conjugate scattering off the pump induced two-photon coherence. We show that this can lead to almost perfect squeezing, even for low pump intensities and low detunings from the two-photon resonance.
We recently1 calculated the amount of squeezing predicted by our quantum theory of multiwave mixing for a one-photon two-level model. Here we use the corresponding theory for the two-photon two-level model,2 which allows for nonsaturating nondegenerate pump and probe waves and includes dynamic Stark shifts. We simplify the more complicated general model using a fourthorder perturbation limit and find very simple expressions that show even for very weak pumps with no Stark shifts or atomic detuning significant squeezing can be achieved. Much of this squeezing is due to scattering of the conjugate field off the pump-induced two-photon coherence, which does not arise in the one-photon case. In general, Stark shifts induce large regions of significant gain, resulting in instabilities. We also show results for high intensity pumps that require larger atomic detunings to obtain a large amount of squeezing. The low intensities required in the two-photon case should make squeezing easier to observe than in the one-photon case.
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.
We apply our quantum theory of nondegenerate multiwave mixing [ Phys. Rev. A37, 2017 ( 1988)] to squeezed-state generation experiments with two-level atoms. Our main interest is to predict the amount of squeezing achievable with a Doppler-broadened two-level medium. We are particularly interested in the single-beam configuration, in which all four interacting beams are spatially degenerate. We analytically solve the coupled-mode quantum Langevin equations for nondegenerate four-wave mixing. The solutions are used to compute the amount of squeezing. In the computation the effects of pump–probe phase mismatch, collisions, Doppler broadening, and Gaussian-intensity variation are comprehensively taken into account for the first time to our knowledge. Simple rules of thumb as to where one can see squeezing in both degenerate- and nondegenerate-frequency cases are derived by examining the limit of a short medium. We then present the case of an infinitely long medium, in which maximum squeezing is achieved when there is no pump–probe phase mismatch. With the inclusion of pump–probe phase mismatch, however, the maximum amount of squeezing is obtained with a finite-length medium instead. This prompts us to investigate in detail the finite-length medium case. Our results show that the effects of Doppler broadening and Gaussian-intensity variation can be largely circumvented by detuning the pump frequency more than three Doppler half-widths from resonance and that good broadband squeezing can be achieved even with a Doppler-broadened medium that has a moderate amount of collision broadening. Under these circumstances it is found that the effect of pump self-focusing or defocusing will be the major factor that limits the amount of achievable squeezing. In particular, the spatially varying nonlinear refractive indices seen by the pump and the probe modes are quite different, which causes the former to become spatially mismatched with the latter in the region in which strong squeezing is otherwise expected.
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.