The method of Doppler – free comb – spectroscopy for dipole transitions was proposed. The numerical calculations for susceptibility spectrum for two-level system driving by strong counter propagating combs were made. The narrow peaks with homogeneous width arise on the background of Doppler counter. The contrast of these peaks is large for largest amplitudes of comb-components. Power broadening is increasing with increasing of field amplitudes. The amplitudes of peaks depend on the phase difference between carrier frequencies of combs. The spectral range of absorption spectrum is determined by the spectral range of comb generator and all homogeneous lines arise simultaneously. The spectral resolution is determined by the width of homogeneously –broadening lines. The physical nature of narrow peaks is in the existing of multi-photon transitions between manifolds of quasi-energy levels arising for different groups of atoms moving with velocities that satisfy to the resonant conditions 2kv= (n+l)Ω⁄j, where n, l, j-are integers and Ω - frequency difference between comb teeth.
The method of Doppler – free comb – spectroscopy for dipole transitions was proposed. The numerical calculations for susceptibility spectrum for two-level system driving by strong counter propagating combs were made. The narrow peaks with homogeneous width arise on the background of Doppler counter. The contrast of these peaks is large for largest amplitudes of comb-components. Power broadening is increasing with increasing of field amplitudes. The amplitudes of peaks depend on the phase difference between carrier frequencies of combs. The spectral range of absorption spectrum is determined by the spectral range of comb generator and all homogeneous lines arise simultaneously. The spectral resolution is determined by the width of homogeneously –broadening lines. The physical nature of narrow peaks is in the existing of multi-photon transitions between manifolds of quasi-energy levels arising for different groups of atoms moving with velocities that satisfy to the resonant conditions 2kv= (n+l)Ω⁄j, where n, l, j-are integers and Ω - frequency difference between comb teeth.
The method of Doppler - free comb - spectroscopy for dipole transitions was proposed. The calculations for susceptibility spectrum for moving two-level atoms driving by strong counter propagating combs have been done. The used theoretical method based on the Fourier expansion of the components of density matrix on two rows on kv (v-velocity of group of atoms, k-projection of wave vector) and Ω (frequency between comb components). For testing of validity of this method the direct numerical integration was done. The narrow peaks with homogeneous width arise on the background of Doppler counter. The contrast of these peaks is large for largest amplitudes of comb-components. Power broadening is increasing with increase of field amplitudes. The spectral range of absorption spectrum is determined by the spectral range of comb generator and all homogeneous lines arise simultaneously.
The two-photon transition of 87Rb ($5{S}_{1/2}\ensuremath{-}4{D}_{3/2}$, $5{S}_{1/2}\ensuremath{-}4{D}_{5/2}$) in a vapor cell is investigated with direct frequency-comb spectroscopy. When strong chirp is imposed on a frequency comb, it is found that the Doppler-free signal amplitude barely degrades despite a significant reduction in peak intensity. In addition, it is found that the Doppler-broadened signal is strongly dependent on the applied chirp. We present a simple model that explains this counterintuitive behavior based on the elongated spatial extent of chirped pulses. Keeping Doppler-free signals almost constant, Doppler-broadened background signals can be strongly suppressed with chirped-pulse excitations. Consequently, in the case of uniformly distributed target atoms, chirped-pulse direct frequency-comb spectroscopy can be a useful method to improve the signal-to-noise ratio in two-photon direct frequency-comb spectroscopy.
For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.
In this article, we analyse a new sensitive spectroscopic technique in which a sample cell is irradiated by a two-frequency pump beam (ω + Δ ± δ/2) and a counter-propagating probe beam (ω). The phase-conjugate fields re-emitted at frequencies ω ± δ, via four-wave mixing processes, are detected through their heterodyne beating with the probe field. The properties of the heterodyne beat signal are studied by means of a perturbation calculation of the nonlinear response of the medium, carried out to the third order in the incident fields. In resonant gas media, the emission lineshape exhibits a Doppler-free doublet structure [frequency splitting 3 δ/2 for single-photon resonances, and δ/2 for two-photon transitions]. By using a phase-sensitive detection of the beat signal, one can separately analyse real (dispersion) or imaginary parts (absorption) of the nonlinear susceptibility. For single-photon transitions, the signal phase shift is related to the atomic levels lifetime and allows one to study the relaxation dynamics in gas phase (like quenching collisions, velocity diffusion, etc...). This is particularly interesting for cross-over resonances, in which only the common level contributes. In three-level systems, one also predicts a selective resonant enhancement of the phase-conjugate emission through Raman-type two-photon processes. Most of these predictions have been experimentally verified.
We have studied the excitation spectrum arising from the optical mixing of the frequencies of a strong bichromatic field interacting with a three-level atom, where the two initially populated modes ωa and ωb are equal to the two atomic transition frequencies, respectively. In the limit of high photon densities, the excitation spectrum near the frequency ω = ωa – 2ωb has been calculated as a function of the parameter η = Ωa2/Ωb2, where Ωa and Ωb are the Rabi frequencies of the two laser fields, respectively. For [Formula: see text] and for weak fields for which [Formula: see text], the spectral function describes a Lorentzian line peaked at the frequency ω = ωa – 2ωb and has a width of the order of γ0, where γ0/2 is the natural width for a two-level atom. When Ωb2 > γ02 and [Formula: see text], the band at ω = ωa – 2ωb splits into two bands described by two Lorentzian lines peaked at ω = ωa – 2ωb ± Ωb/√2 and have spectral widths of the order of 3γ0/4. The ratio of the height of the band ω = ωa – 2ωb to the height ω = ωa – 2ωb ± Ωb/2 is 3:2. The probability amplitudes for both bands take large negative values indicating that optical amplification of the signal field may be expected to occur at these frequencies. When Ωa = Ωb = Ω, η = 1, and for Ω2 < γ02, the spectral function describes a single band at ω = ωa – 2ωb while for Ω2 > γ02, the single band splits into five pairs of bands which are separated from the frequency ω = ωa – 2ωb by frequency shifts which are equal to: ± Ω/√2, [Formula: see text], ± Ω, ± Ω√2, and ± Ω√3, respectively, and have spectral widths of the order of 3γ0/4. For [Formula: see text] and for laser fields for which Ωa2 > γ02 and Ωb2 > γ02, the spectral function consists of three pairs of bands. The probability amplitudes for these bands vary linearly with η and may take large values for [Formula: see text]. A complete discussion of the excitation spectrum as well as a graphical representation of the derived results has been given.
The polarization and power spectra of radiation of two-level atoms moving in a field of biharmonic and monochromatic counterpropagating waves are computer simulated. It is shown that, as the frequencies of the counterpropagating waves are scanned with respect to the central frequency of the Doppler contour in the intensity distribution of groups of atoms moving at velocities that satisfy the resonance conditions for multiphoton transitions between quasi-energy levels, apart from well-known sub-Doppler resonances, narrow peaks appear. Such resonances should also occur for the stimulated light pressure force.