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Journal of the Optical Society of America B

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

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

Published Jan 1, 1991• 10 citations
Publisher

Abstract

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.

DOI
10.1364/josab.8.000037

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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.

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

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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
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.
A quantum theory of nondegenerate multiwave mixing in a two-level atomic medium is formulated, with emphasis on traveling-wave interaction geometries. Two equivalent alternative methods are developed to treat, with some rigor, the spatial propagation of the interacting multimode traveling-wave field. The theory is applied to the case of a single beam propagating through the medium to obtain the spectrum of squeezing. The effects of spontaneous emission, propagation loss, atomic collisions, and pump-probe phase mismatch are comprehensively taken into account for the first time.
We have generated squeezed states of light with a single pump beam propagating through Doppler broadened sodium vapor via forward four-wave mixing (FWM) with spatially degenerate pump and probe modes. The two probe-mode inputs are vacuum states at nondegenerate frequencies, which are transformed to squeezed vacuum by the FWM interaction. Compared with previous FWM configurations,1 this single-pass single-pump-beam configuration ensures maximal overlap of the four interacting beams, thus maximizing the squeezing nonlinearity and improving the overall efficiency. The transmitted pump has the wrong phase to act as the local oscillator for detecting the squeezed spectrum.1 Therefore, a cavity is used to filter out most of the transmitted pump intensity, and the squeezed vacuum is detected with another local oscillator using the standard dual-detector scheme. The residual pump beam provides a reference to monitor the phase between the pump and squeezed vacuum. The observed 0.8-dB reduction in the shot noise corresponds to an inferred 50% squeezing of the light at the exit of the vapor medium, which is in reasonable agreement with the theory given by Ho et al. 2 A linearly polarized pump is found to give less squeezing than a circularly polarized pump, possibly due to optical pumping.
A quantum theory of degenerate four-wave mixing is presented in which the atomic medium consists of stationary four-level atoms, each with three degenerate excited states, and the interacting light beams are allowed to be in different states of polarization. This vector-field theory differs from the scalar-field theory of Reid and Walls [Phys. Rev. A 31, 1622 (1985)] in that there are new atomic variables in the Langevin equations which are related to the induced coherence between the upper atomic states. It is found, for the assumed set of atomic levels, that this seemingly different mechanism of four-wave-mixing gain does not circumvent the degrading effect of spontaneous emission on squeezing obtainable via degenerate four-wave mixing. The theory is applied to both forward and backward degenerate four-wave mixing with nearly collinear geometry, and specialized to the case in which the polarization states of the two pump modes are mutually orthogonal. It is found that for both forward and backward configurations, the range of pump intensity for which squeezing can be achieved in the vector-field case is larger than that in the scalar-field case, and the maximum amount of squeezing obtainable at a particular pump detuning is comparable in both cases.
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.
In this first paper of a series on the quantum theory of nondegenerate multiwave mixing applicable to traveling-wave interaction geometries, we describe our problem formulation. We consider the explicit dynamics of a subset of the field quantization modes interacting with a system of stationary two-level atoms contained in a volume much smaller than the field quantization volume. Because we make the realistic assumption of leaving the remaining infinite set of field modes as a common thermal-field reservoir, the resulting Langevin equations contain extra decay terms due to collective spontaneous emission or super-radiance. We show that all but one of these super-radiance terms are negligible in the following two limits: (a) when the number of atoms in a diffraction volume is small; (b) when the atoms are pumped far off resonance. There is, however, an anomalous decay term which does not appear in a classical model of super-radiance based upon coherently phased atomic dipoles. The magnitude of this anomalous term is neither dependent upon the number of atoms nor on the pump-frequency detuning and may not be negligible at a low pump intensity. Neglecting the super-radiance terms, we then present a general Fourier-expansion solution technique for obtaining the atomic polarization in the presence of any number of field modes. The expansion is shown to be convergent in a commonly occurring situation in which all the strong pump modes are frequency degenerate and the remaining nondegenerate modes are all weak compared to the atomic saturation intensity. In subsequent papers of this series, we will present methods to treat, with some rigor, the spatial propagation of an interacting multimode quantum field and apply these methods to traveling-wave squeezed-state generation experiments.
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.