We observe dephasing‐induced third‐and higher‐order wave‐mixing spectra of Zeeman and hyperfine coherences in a sodium‐seeded flame in a magnetic field. As the perturbation parameter approaches unity, we compare our experimental spectra with theoretical higher‐order selection rules.
Dephasieg-induced phenomena are a novel class of effects that are ordinarily forbidden because the two or more relevant quantum-mechanical amplitudes add coherently and cancel out.1 When dephasing is present, however, these amplitudes no longer cancel, and previously unseen effects can be observed. Indeed, a number of novel dephasing-induced phenomena have been seen.2-5 Of particular interest, both for fundamental reasons and for diagnostic purposes, are (third-order) dephasing-induced resonances between equally populated levels of a ground electronic state,6,7 specifically, Zeeman and hyperfine coherences. Working with a sodium-seeded flame, we8 have observed these latter effects and, at higher intensities, subharmonics of them.
Using diagrammatic perturbation theory, we calculate the higher-order susceptibility for the n-wave process, omega(0) = (n/2 - 1)(omega(1) - omega(2)) + omega(1), in a phase-matched n-wave-mixing geometry. We include the 16 Zeeman and hyperfine levels of the sodium ground (3S((1/2))) and excited (3P((1/2))) states, finding resonances at subharmonics [+/-(1/2), +/-?, ..., +/-1(n/2 - 1)] of the ground-level transition frequencies. The computed spectrum for eight-wave mixing is in satisfactory agreement with experiment. In addition, a theoretical twelve-wave-mixing spectrum predicts a new higher-order selection rule.
The theoretical formulation of the nonlinear optical activity is utilized to describe the signal intensity in forward scattering. For cases in which the ratio of the Rabi frequency of an isolated transition to its relaxation rate is less than one, a perturbation procedure in this parameter is presented. The successive terms in the resulting series are interpreted as higher-order coherences or induced multipole moments. Application is made to the hyperfine components of the sodium D transitions where experimental data is described by a third-order calculation. Good agreement is obtained without invoking an induced hexadecapole moment as was proposed originally.
Near-resonant four-wave light mixing in Na vapor with inert buffer gases reveals collision-induced coherences when the difference frequency between two incident light beams equals the hyperfine splitting or the Zeeman splitting between two states of the 32S ground-state manifold. The Doppler broadening of the corresponding resonances decreases with increasing buffer-gas pressure. The width of the resonances becomes significantly narrower than the spontaneous linewidth of the near-resonant intermediate state and is determined by spin-exchange collisions between ground-state atoms. The dependence of the intensity of these collision-induced resonances on buffer-gas pressure and detuning from one-photon resonances is measured. Selection rules for various polarizations of the incident light fields and directions of an externally applied magnetic field are established.