Derives the equations of motion for the density matrix of a two-level molecule interacting with two oppositely propagating semiclassical waves. The equations are shown to correctly reproduce earlier results by Kol'chenko et al. (1969) for one travelling wave, and their perturbation treatment for a standing wave. The saturated absorber experiment is treated in the case when one travelling wave is weak enough to allow a perturbation expansion in its amplitude. The velocity dependent absorption function is investigated in detail, and the effect of recoil on the processes: Raman scattering, Rayleigh scattering and dynamic Stark splitting is obtained and discussed. These have been treated without recoil by Haroche and Hartmann (1972) and a detailed comparison with their work is included. Finally there is a brief discussion of the importance of recoil for different situations in quantum electronics.
Derives the equations of motion for the density matrix of a two-level molecule interacting with two oppositely propagating semiclassical waves. The equations are shown to correctly reproduce earlier results by Kol'chenko et al. (1969) for one travelling wave, and their perturbation treatment for a standing wave. The saturated absorber experiment is treated in the case when one travelling wave is weak enough to allow a perturbation expansion in its amplitude. The velocity dependent absorption function is investigated in detail, and the effect of recoil on the processes: Raman scattering, Rayleigh scattering and dynamic Stark splitting is obtained and discussed. These have been treated without recoil by Haroche and Hartmann (1972) and a detailed comparison with their work is included. Finally there is a brief discussion of the importance of recoil for different situations in quantum electronics.
The problem of saturated absorption by a gas of two-level molecules, including recoil effects, is formulated in a new quantum representation for the molecular motion. The relationship to other representations is clarified in a simple chart. The new formulation requires the solution of simultaneous linear differential equations with mixed boundary conditions, instead of linear difference equations in two variables followed by an integration over velocity. Analytic solutions are presented for one running wave with Doppler line broadening, and for a weak probe beam in the Doppler limit. The latter lineshape is analysed to show when power broadening obscures the recoil splitting.
Previously derived equations describing recoil effects in saturated absorption by a gas of two-level atoms or molecules are solved numerically for the case of standing plane-wave excitation and large Doppler broadening. The numerical techniques and accuracy estimates are discussed briefly. The lineshapes obtained are well approximated by the superposition of two Lorentzian functions whose width, heights, and separation parametrise the lineshape. The dependence of these parameters on saturation, recoil splitting, and relaxation rates is described and compared with corresponding results in the rate equation approximation and in the weak-probe-beam approximation. Saturation broadening depends strongly on these latter approximations, but very little on recoil splitting. When multiphoton processes are retained in the equations, increasing saturation causes a slight decrease in the fitted separation of the peaks. The ratio of the heights of the two Lorentzians is closely related to the ratio of relaxation rates for the level populations.
For pt.I see ibid., vol.7, p.1235 (1974). Uses the results of an earlier work to consider recoil effects on spectroscopic features observed with a saturable absorber. Systematic approximation schemes are presented, both the straightforward perturbation expansion in the field amplitudes and a non-perturbative approach, which neglects pulsations in the populations. This method generalizes the REA of recoil-free strong-signal theory and is expected to give good results for velocity-averaged observables. Its validity is discussed and the consequences are compared with those of other calculations. The results of numerical evaluations of spectra are shown, in particular the limit of poorly resolved recoil features is explored. Parameter regions where recoil-induced splittings and asymmetries occur are presented.
A class of molecular two-photon processes, occurring under transient or steady-state conditions, is analyzed exactly for certain cases using a density-matrix formalism. Our results are relevant to the recently observed phenomena of transient coherent Raman beats and steady-state two-photon absorption of oppositely directed laser beams. Lowest-order perturbation theories have shown that these processes are insensitive to the Doppler effect, and consequently the linewidth is unaffected by Doppler broadening and by elastic collisions that change molecular velocity. The solutions presented here are of the same form for the Raman and two-photon problems and reveal significant power-dependent frequency shifts and line broadening that correct the ideal Doppler-free solutions. For the transient case, we assume a molecular three-level quantum structure that can be switched in or out of optical resonance with cw laser radiation by means of a pulsed dc Stark field, but the solutions also apply when resonant optical pulses are introduced. During the resonant condition when the Stark pulse is on, the three levels are prepared in coherent superposition, and during the nonresonant condition following the Stark pulse, the laser field(s) stimulates the coherently prepared sample in a transient two-photon process. One of these processes, the Ramanbeat effect, has been observed in forward scattering, but the second one, transient two-photon emission, should be observable in backward scattering. Bloch-like equations are derived for this three-level problem that facilitate an exact pulse solution for state preparation. Following the pulse, transient decay is well-approximated by a perturbation calculation. For the steady-state case, an exact solution is also obtained and is of interest for continuous-wave spectroscopy or for transient experiments requiring an initial preparation of quantum states, prior to Stark switching. These solutions exhibit a power-dependent line broadening and a frequency shift of magnitude $\ensuremath{\sim}\frac{\ensuremath{\Delta}({\ensuremath{\alpha}}^{2}\ensuremath{-}{\ensuremath{\beta}}^{2})}{({\ensuremath{\Delta}}^{2}+\frac{1}{{T}_{2}^{2}})}$, in agreement with our earlier estimate, where $\ensuremath{\alpha}$ and $\ensuremath{\beta}$ are the Rabi flopping frequencies for the two intermediate transitions and $\ensuremath{\Delta}$ is the off-resonance tuning behavior for one of them.
The effect of correlations between an absorber atom and perturbers in the binary-collision approximation are applied to degenerate atomic systems. A generalized absorption profile which specifies the final state of the atom after an absorption event is related to the total intensities of Rayleigh scattering and fluorescence from the atom. It is suggested that additional dynamical information to that obtainable from ordinary absorption experiments is required in order to describe redistributed atomic radiation. The scattering of monochromatic radiation by a degenerate atom is computed in a binary-collision approximation; an equation of motion is derived for the correlation function which is valid outside the quantum-regression regime. Solutions are given for the weak-field conditions in terms of generalized absorption and emission profiles that depend on the indices of the atomic multipoles.
Using semiclassical radiation theory, a formalism similar to that used by Lamb in his Theory of an Optical Maser is developed for studying the amplification of vector traveling waves in a laser-type medium. The effect of the medium on the waves is given in terms of space (or time) dependent field amplitudes and phases and a nonlinear index of refraction. With particular emphasis on typical gaseous media, the effects of Doppler broadening are treated in detail for arbitrary ratios of natural to Doppler linewidths. Polarization and propagation vectors in various directions are considered, and the nonlinear effects are found to make an isotropic medium effectively anisotropic.
Lowest order nonlinear effects (due to a polarization cubic in the field amplitudes) are studied extensively, and the frequency dependence of several of these processes is presented in graphical form. In particular, the introduction of fields at new frequencies and polarization effects are considered. The characteristics of these nonlinear processes peculiar to Doppler broadened lines are discussed, and the processes are interpreted in terms of saturation and coherent modulation of the population inversion density.
Strong nonlinear effects are considered in a more approximate way and are found to consist of saturation of the various linear and nonlinear processes previously considered. These strong nonlinear effects should occur at low enough intensities to be easily observed in practice on a CW basis. With the present formalism, the analytical results of Gordon, White and Rigden regarding gain saturation in laser amplifiers are obtained, and the extension is made to include frequencies away from line center and the effects of multiple spectral components. Again, the introduction of fields at new frequencies is considered in detail. These results are also discussed in terms of saturation and coherent modulation of the populations and hole burning.