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Physical Review A

Theory of optical near-resonant cone emission in atomic vapor

B. D. Paul, J. Cooper, Alan Gallagher, Michael G. Raymer

Published Dec 31, 2002• 8 citations
Publisher

Abstract

A time-dependent theory for conical emission during near-resonant propagation of laser light in an atomic vapor, which includes full propagation for the laser and frequency sidebands in a nonlinear two-level medium is presented. The density-matrix equations for the dipole moment and population are solved in the dressed atomic frame. The polarization source terms are accurate to order \ensuremath{\gamma}/R, where \ensuremath{\gamma} is a damping constant and R is the generalized Rabi frequency. Analytical plane-wave solutions and numerical, cylindrically symmetric propagation simulations including diffraction are presented. It is shown that the calculations with cylindrically symmetric fields and atomic excitation profiles are incapable of accounting for the high levels of optical gain that are responsible for the intense conical emission observed in experiments. This result is at first surprising, since the model accounts rigorously for all of the physical phenomena that have been previously proposed as being responsible for generating large gains, and the calculation matches the symmetry of the observations. The lack of large calculated gain seems to imply the existence of higher-order $(m>0)$ radial modes in the field for the experimental conditions that give rise to cone emission. In the simulations, however, the cylindrically symmetric fields do produce weak red-detuned cones with angular-frequency distributions similar to those seen in experiments.

DOI
10.1103/physreva.66.063816

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Conical emission by 2-ps excitation of potassium vapor

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Conical emission, redshifted from the atomic resonance, is observed when a ∼2-ps laser beam, blueshifted from resonance, propagates through potassium vapor. In contrast, no cone is visible when a 150-fs pulse is used. The 2-ps-pulse-induced cone has a unique, small, angular spread of Δθ/θ≈0.1, compared with Δθ/θ≈0.3 from other pulsed experiments, which used 25-ps–5-ns-excitation pulses. In addition, the fraction of the 2-ps-pulse power emitted in the cone reached 7.5%, far exceeding this fraction from the longer-pulse experiments. An additional, unexpected result is that the spectral width of the laser pulse is narrower, without significant intensity loss, after propagation through the vapor. The vapor densities and laser detunings that yield cones in the present experiment are similar to those from the longer-pulse experiments. Although the 2-ps-pulse spectrum partially overlaps the resonance, the cone spectrum and cone angles versus density and laser detuning are similar to those previously reported for nanosecond pulses. The fourth (blue-detuned) wave required for satisfying four-wave mixing is absent, again equivalent to what is observed in the nanosecond experiments. The physical origin of cone emission by pulsed excitation of atomic vapors is still largely unknown, and this high efficiency and narrow angular spread of a spectrally broad cone further contradicts existing models, perhaps ultimately providing a clue to a correct explanation.

Journal of the Optical Society of America B•Feb 1, 2001•11 citations
A time-dependent theory for conical emission during near-resonant propagation of laser light in an atomic vapor, which includes full propagation for the laser and frequency sidebands in a nonlinear two-level medium is presented. The density-matrix equations for the dipole moment and population are solved in the dressed atomic frame. The polarization source terms are accurate to order \ensuremath{\gamma}/R, where \ensuremath{\gamma} is a damping constant and R is the generalized Rabi frequency. Analytical plane-wave solutions and numerical, cylindrically symmetric propagation simulations including diffraction are presented. It is shown that the calculations with cylindrically symmetric fields and atomic excitation profiles are incapable of accounting for the high levels of optical gain that are responsible for the intense conical emission observed in experiments. This result is at first surprising, since the model accounts rigorously for all of the physical phenomena that have been previously proposed as being responsible for generating large gains, and the calculation matches the symmetry of the observations. The lack of large calculated gain seems to imply the existence of higher-order (m>0)(m>0)(m>0) radial modes in the field for the experimental conditions that give rise to cone emission. In the simulations, however, the cylindrically symmetric fields do produce weak red-detuned cones with angular-frequency distributions similar to those seen in experiments.
Computational results show that the conical emission and Rabi sidebands observed when a nearly resonant laser pulse propagates through an atomic vapor are the result of the breakup of the pulse into solitary waves. For an incident pulse with a transverse as well as a temporal profile, the crests and troughs of the 2-D solitary waves are curved in a time-radius plane. The temporal modulation associated with pulse breakup appears as Rabi sidebands in the spectrum, while the curvature of the solitary waves in the time-radius plane results in a transverse spatial modulation, resulting in conical emission in the far field. These results were obtained by performing detailed numerical calculations of the time-dependent paraxial propagation of a cylindrically symmetric laser pulse through a vapor of two-level atoms. Our results can be interpreted readily in terms of optical nutation on the Bloch sphere and in terms of noncollinear phase matching through the curvature of the solitary waves rather than through additional parametrically generated waves. The cone opening angle depends on the initial transverse profile of the pulse and the process of beam breakup as well as self-focusing.
We report computational results that show that the conical emission observed when a nearly resonant laser pulse propagates through an atomic vapor is the result of the breakup of the pulse into solitary waves. For an incident pulse with a radial as well as a temporal profile, the crests and troughs of the two-dimensional solitary waves are curved in a time-radius plane. The temporal modulation associated with pulse breakup appears as Rabi sidebands in the spectrum, while the curvature of the solitary waves in the time-radius plane results in a transverse spatial modulation that leads to conical emission in the far field. These results were obtained by performing detailed numerical calculations of the time-dependent paraxial propagation of a cylindrically symmetric laser pulse through a vapor of two-level atoms under the rotating-wave and slowly-varying-envelope approximations in the limit of no collisional damping or Doppler broadening. Our results can be interpreted readily in terms of optical nutation on the Bloch sphere and in terms of noncollinear phase matching through the curvature of the solitary waves rather than through additional parametrically generated waves. We find that self-focusing is not required for the generation of conical emission, although it would be difficult to separate these effects experimentally.
It is now known that conical emission in a two-level atomic system is a fundamental propagation effect brought about by the breakup of the exciting laser pulse into solitary waves.1 This report presents a semiclassical numerical calculation that extends this previous work by solving the optical Bloch and Maxwell equations for a three-level atomic vapor excited by laser fields of two different frequencies. The applied fields satisfy a two-photon resonance condition between the ground and final states and are slightly detuned from the intermediate state to enhance the nonlinear polarization.2 As the fields propagate, oscillations in the nonlinear polarization of the pump beam dominate the interaction and lead to the pump's breakup into solitary waves. The Stokes polarization, depending on the pump radiation, also experiences these oscillations. Because of the intensity-dependence of the refractive index, the solitary waves experience a curvature in the time-radius plane. This curvature manifests itself in the spectrum as a radial component of the wave vector at the Rabi frequency. The Stokes field, experiencing parametric breakup, displays a similar curvature. Spectral analysis reveals a radial component of the Stokes wave vector as well. This frequency-shifted off-axis radiation is identified as conical emission in the Stokes field.
The cone emission obtained from pumped two-level atoms is related, by a perturbation theory, to time-dependent terms in the macroscopic Bloch equations. It is described as a cooperative superfluorescence radiation from collections of spatially distributed atoms, including in the theory the far-zone dipole-dipole interactions, in the presence of the strong monochromatic field. The distribution of the cone emission as a function of frequencies and cone angles is analyzed. A phase-matching condition is obtained for the wave vectors of the pump and conical beams that is similar to the Cherenkov condition. The frequency shift for the maximum of the cone light is found to be equal to the generalized Rabi frequency. The broadening of the cone emission is related to inhomogeneity in Rabi frequencies and decoherence effects. An approximate result is obtained for the ratio of intensities of the blue-shifted cone relative to the red-shifted cone so that the blue-shifted cone can appear only for extremely strong laser intensities.
Conical light emission is observed when an intense quasiresonant laser beam propagates in an atomic vapor.1-4 A parametric four-wave mixing process was suggested to explain this effect.1 However, this model is inconsistent with experiments both quantitatively in the value of the predicted cone angle and qualitatively due to the absence of the obligatory blue counterpart to the red-shifted cone photon.2-4 A model of Cherenkov radiation by a laser-induced moving polarization was proposed to account for the origin and angular/spectral dependencies of the conical emission.3
Conical emission, redshifted from the atomic resonance, is observed when a ∼2-ps laser beam, blueshifted from resonance, propagates through potassium vapor. In contrast, no cone is visible when a 150-fs pulse is used. The 2-ps-pulse-induced cone has a unique, small, angular spread of Δθ/θ≈0.1, compared with Δθ/θ≈0.3 from other pulsed experiments, which used 25-ps–5-ns-excitation pulses. In addition, the fraction of the 2-ps-pulse power emitted in the cone reached 7.5%, far exceeding this fraction from the longer-pulse experiments. An additional, unexpected result is that the spectral width of the laser pulse is narrower, without significant intensity loss, after propagation through the vapor. The vapor densities and laser detunings that yield cones in the present experiment are similar to those from the longer-pulse experiments. Although the 2-ps-pulse spectrum partially overlaps the resonance, the cone spectrum and cone angles versus density and laser detuning are similar to those previously reported for nanosecond pulses. The fourth (blue-detuned) wave required for satisfying four-wave mixing is absent, again equivalent to what is observed in the nanosecond experiments. The physical origin of cone emission by pulsed excitation of atomic vapors is still largely unknown, and this high efficiency and narrow angular spread of a spectrally broad cone further contradicts existing models, perhaps ultimately providing a clue to a correct explanation.