Multiphoton processes in dense atomic vapors such as four-wave mixing or coherent blue light generation are typically viewed from single-atom perspective. Here we study the surprisingly important effect of phase matching near two-photon resonances that arises due to spatial extent of the atomic medium within which the multiphoton process occurs. The non-unit refractive index of the atomic vapor may inhibit generation of light in nonlinear processes, significantly shift the efficiency maxima in frequencies and redirect emitted beam. We present these effects on an example of four-wave mixing in dense rubidium vapors in a double-ladder configuration. By deriving a simple theory that takes into account essential spatial properties of the process, we give precise predictions and confirm their validity in the experiment. The model allows us to improve on the geometry of the experiment and engineer more efficient four-wave mixing.
The effect of stochastic laser phase fluctuations on nonlinear optical phenomena are investigated within the phase-diffusion model. Averaged equations of motion are derived in the limit of infinitely short correlation times and the results are applied to multiphoton absorption and to four-wave mixing. The effect of the stochastic phase fluctuations is shown to be equivalent to a
T2 dephasing process, and a procedure is described for the inclusion of this equivalence in many nonlinear-optical problems. When a given mode contributes n photons to a multiphoton absorption process, its contribution to the width of the multiphoton transition is
n2 times its own stochastic width. When correlated lasers are used as the excitation sources in four-wave-mixing experiments, (new) stochastic-fluctuation-induced extra resonances in four-wave mixing (SFIER4) will be observed, in complete analogy to the extra resonances induced by collisions [pressure-induced extra resonances in form-wave mixing (PIER4)].
The influence of nonlinear interference processes and of changes in populations in strong electromagnetic fields, and also of the Doppler broadening on resonant four-wave frequency mixing is investigated for a system of Raman-type transitions. The case in which a quantum system interacts with one weak field and two strong fields is considered. Each of the energy levels is assumed to be perturbed by just one strong field. It is shown that the Doppler broadening alters drastically the contributions of the populations of the various levels to the investigated process and that this can alter by several orders of magnitude and nonlinear susceptibilities averaged over the velocities and influence significantly the selection of optimal configurations of the transitions and of the experimental conditions for effective resonant four-wave conversion of the radiation frequencies. A numerical analysis of the derived expressions is used to account for the experimentally observed considerable differences between the spectral dependences of the output power and the conclusions drawn from perturbation theory.