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Physical Review A

Theory of strongly saturated double-resonance line shapes in arbitrary angular momentum states of molecules

H. W. Galbraith, Martin Dubs, J. I. Steinfeld

Published Sep 1, 1982• 30 citations
Publisher

Abstract

We calculate the steady-state probe absorption line-shape function for a strongly driven, Zeeman-degenerate molecular system. The probe laser is treated to lowest order while the pump laser is dealt with to all orders. We obtain the probe line shape for the cases of parallel and perpendicular linear polarization of the two lasers. As expected, the effects of $M$ degeneracy, as well as differences due to the relative laser polarizations, are most pronounced when Doppler broadening is not important. However, even in the presence of large Doppler broadening we find a narrowing of the population hole by including the Zeeman degeneracy and a further narrowing if perpendicular laser polarizations are used.

DOI
10.1103/physreva.26.1528

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Pump-probe spectroscopy in degenerate two-level atoms with arbitrarily strong fields

T. Zigdon, A. D. Wilson‐Gordon, Harry Friedmann

We study the pump and probe absorption spectra, as a function of the probe detuning, in a degenerate two-level atomic system, for the case where the probe intensity is high enough to affect the pump absorption. The theory is valid for any ${F}_{g}\ensuremath{\rightarrow}{F}_{e}$ alkali-metal transition interacting with an arbitrarily intense pump and probe (with general Rabi frequencies ${\ensuremath{\Omega}}_{1,2}$) which are perpendicularly polarized with either ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ or $\ensuremath{\pi}$ polarization. We have constructed a computer program that can calculate the spectra without requiring one to write out the Bloch equations explicitly. We show that, when the pump is ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ polarized and the probe $\ensuremath{\pi}$ polarized, or vice versa, the pump and probe absorptions depend on the Zeeman coherences between the nearest-neighboring ground or excited Zeeman sublevels, whereas when the pump is ${\ensuremath{\sigma}}_{+}$ polarized and the probe ${\ensuremath{\sigma}}_{\ensuremath{-}}$ polarized, or vice versa, the Zeeman coherences that directly determine the absorption are between next-nearest neighbors. We report calculations of the pump and probe absorption spectra for the cycling ${F}_{g}=2\ensuremath{\rightarrow}{F}_{e}=3$ transition in the ${D}_{2}$ line of $^{87}\text{R}\text{b}$, interacting with a resonant ${\ensuremath{\sigma}}_{+}$-polarized pump and either a $\ensuremath{\pi}$- or a ${\ensuremath{\sigma}}_{\ensuremath{-}}$- polarized probe. The probe and pump absorption spectra are analyzed by considering the contributions that derive from the individual ${m}_{g}\ensuremath{\rightarrow}{m}_{e}$ transitions. We then show how these contributions depend on the ground- and excited-state populations and Zeeman coherences, and investigate the role played by transfer of coherence from the excited to the ground hyperfine state. We show that the pump and probe absorption spectra are mirror images of each other when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}>\ensuremath{\Gamma}$, and have the same behavior at line center and complementary behavior in the wings, when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}<\ensuremath{\Gamma}$ ($\ensuremath{\Gamma}$ is the rate of spontaneous decay from ${F}_{e}$ to ${F}_{g}$).

Physical Review A•Mar 19, 2008•18 citations
We calculate the steady-state probe absorption line-shape function for a strongly driven, Zeeman-degenerate molecular system. The probe laser is treated to lowest order while the pump laser is dealt with to all orders. We obtain the probe line shape for the cases of parallel and perpendicular linear polarization of the two lasers. As expected, the effects of MMM degeneracy, as well as differences due to the relative laser polarizations, are most pronounced when Doppler broadening is not important. However, even in the presence of large Doppler broadening we find a narrowing of the population hole by including the Zeeman degeneracy and a further narrowing if perpendicular laser polarizations are used.
The physics of the degenerate four-wave mixing process for resonant transitions between two degenerate energy levels is investigated by direct numerical integration of the time-dependent density matrix equations. The Zeeman structure of the upper and lower energy levels is included in a multistate formulation of the density matrix equations. The inclusion of the Zeeman structure enables the investigation of the degenerate four-wave mixing process for different polarization configurations of the forward pump, backward pump, and probe beams. Saturation curves and lineshapes are calculated for different polarization configurations and for numerous low-J transitions. At low laser intensity, the results of our calculations are in excellent agreement with perturbation theory in terms of the relative intensities of the degenerate four-wave mixing signal for linear polarization configurations. As the laser intensity increases and the resonance starts to saturate, we find in general that the relative degenerate four-wave mixing reflectivity increases for the crossed polarization configurations compared to the parallel polarization configuration because the saturation intensity is higher. However, for some resonance transitions, some of the crossed polarization configurations saturate at lower laser intensities than the parallel polarization configuration, even though the reflectivity for these crossed polarization configurations is much lower than for the parallel polarization configuration in the perturbative intensity limit. This result is explained in terms of the coupling of the various Zeeman states during the degenerate four-wave mixing interaction for specific polarization configurations. The effect of saturation on the resonance line shapes for the different polarization configurations is also investigated. Finally, a limited number of calculations are performed for resonances that are Doppler broadened as well as collision broadened. The effect of saturation on the reflectivity of the crossed polarization configurations compared to the parallel polarization configuration is even more significant for resonances with comparable Doppler and collisional broadening.
An analytical expression for the degenerate four-wave mixing signal produced in a medium composed of two-level atoms by pump and probe lasers of arbitrary intensities and parallel linear polarization, suffering negligible absorption and depletion, has been derived. The Abrams–Lind approach [Opt. Lett.2, 94 and 3, 205 (1978)] for deriving the phase-matched polarization has been extended to find all the other higher-order polarization terms contributing to the signal. The signal field amplitude is expressed as an infinite series whose convergence rate depends on the intensity of the input fields and their detuning from resonance. The solution is successfully verified by comparison with a full numerical nonperturbative calculation and is found to be equivalent to the Abrams–Lind result in the limit of weak probe intensity. The result is used to calculate the saturation effects on spectral line shape that are relevant to simulation of molecular spectra obtained by degenerate four-wave mixing with saturating pump and probe fields. The result is extended to treat atomic motion in the case of forward geometry of the input beams.
This paper presents a theory of lineshapes for molecular Optical-Optical Double Resonance (DR) Spectroscopy with arbitrary strength for both pump and probe fields using the steady-state solutions for the 3-level density matrix. When Doppler broadening can be neglected, the results are analytical, and the probe spectrum is a pair of Lorentzian lines that display Autler-Townes splitting, each with an angular frequency half-width half maximum equal to the relaxation rates, which are assumed to be equal. When Doppler broadening is introduced, one must resort to numerical integration except for the limit of weak pump and probe fields. When the Doppler width is assumed to be much larger than the pump and probe Rabi frequencies and the probe frequency is higher than that of the pump, the calculated DR lineshapes are found to be Lorentzian with a strong pump field limit width that is proportional to the pump Rabi frequency, which is commonly known as power broadening. However, the width does not equal that Rabi frequency and is different for co- and counter-propagating pump and probe fields. Furthermore, that broadening is largely inhomogeneous, despite the Lorentzian shape. The saturation power is found to be about 4 times higher than for the bare probe transition with the same relaxation rate, dramatically lower than that expected if the width is interpreted as homogeneous.
A theory of saturation spectroscopy is developed which accounts for effects of level degeneracy. The theory can be applied to those situations in which a pump laser field of arbitrary strength and polarization acts between two manifolds of degenerate or nearly degenerate atomic levels, while a probe laser field of arbitrary strength and polarization acts between a coupled manifold of levels. As such, this theory of "three-level" systems could, in principle, include effects arising from level degeneracy, optical pumping, atomic motion, transient laser fields, different polarizations and strengths for pump and probe fields, and atomic transit across the laser fields. The present calculation, however, is limited to a study of optical pumping and field polarization effects for pump fields of arbitrary strength and weak probe fields interacting with a single velocity subclass of atoms. Probe absorption line shapes clearly display the effects of pump-field strength (Rabi splittings), pump-field polarization (positions and number of Rabi-split resonance peaks), pump-field detuning (positions of resonance peaks), and optical pumping (relative strengths of the resonance peaks). The calculation is carried out with the use of an irreducible tensor basis for the atomic density matrix although a standard (mmm-basis) calculation is included in an appendix.
A theory of line shape for a Doppler broadened probe in the presence of a strong infrared pump is presented. The optical analog of Bloch equations has been developed; the T1, T2 relaxations are introduced phenomenologically in these equations. Doppler broadening of both the pump and signal transitions are taken into account to obtain the absorption coefficient for the signal. This leads to a Doppler broadened Gaussian function weighted by a pump induced Lorentzian function whose position and linewidth are controlled by the detuning and power respectively of the pump radiation. The absorption coefficient is further modulated by a Lorentzian function containing the fourth power of the radiation. The off-resonance pumping leads to two symmetrically located ‘‘Lamb dips’’ or ‘‘peaks’’ around the Gaussian pedestal for co- and counter propagating laser radiations. A calculation of the line shape of the central sub-Doppler feature for the on-resonance pumping is in good agreement with the observed variation of linewidth with pressure. Numerical results are presented graphically to demonstrate the pump and signal power dependence of the central hole or peak for the bent and cascade-type double resonances. The results obtained confirm the expected behavior based on level populations.
We study the pump and probe absorption spectra, as a function of the probe detuning, in a degenerate two-level atomic system, for the case where the probe intensity is high enough to affect the pump absorption. The theory is valid for any ${F}_{g}\ensuremath{\rightarrow}{F}_{e}$ alkali-metal transition interacting with an arbitrarily intense pump and probe (with general Rabi frequencies ${\ensuremath{\Omega}}_{1,2}$) which are perpendicularly polarized with either ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ or $\ensuremath{\pi}$ polarization. We have constructed a computer program that can calculate the spectra without requiring one to write out the Bloch equations explicitly. We show that, when the pump is ${\ensuremath{\sigma}}_{\ifmmode\pm\else\textpm\fi{}}$ polarized and the probe $\ensuremath{\pi}$ polarized, or vice versa, the pump and probe absorptions depend on the Zeeman coherences between the nearest-neighboring ground or excited Zeeman sublevels, whereas when the pump is ${\ensuremath{\sigma}}_{+}$ polarized and the probe ${\ensuremath{\sigma}}_{\ensuremath{-}}$ polarized, or vice versa, the Zeeman coherences that directly determine the absorption are between next-nearest neighbors. We report calculations of the pump and probe absorption spectra for the cycling ${F}_{g}=2\ensuremath{\rightarrow}{F}_{e}=3$ transition in the D2{D}_{2}D2​ line of 87Rb^{87}\text{R}\text{b}87Rb, interacting with a resonant ${\ensuremath{\sigma}}_{+}$-polarized pump and either a $\ensuremath{\pi}$- or a ${\ensuremath{\sigma}}_{\ensuremath{-}}$- polarized probe. The probe and pump absorption spectra are analyzed by considering the contributions that derive from the individual ${m}_{g}\ensuremath{\rightarrow}{m}_{e}$ transitions. We then show how these contributions depend on the ground- and excited-state populations and Zeeman coherences, and investigate the role played by transfer of coherence from the excited to the ground hyperfine state. We show that the pump and probe absorption spectra are mirror images of each other when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}>\ensuremath{\Gamma}$, and have the same behavior at line center and complementary behavior in the wings, when ${\ensuremath{\Omega}}_{1}\ensuremath{\ge}{\ensuremath{\Omega}}_{2}<\ensuremath{\Gamma}$ ($\ensuremath{\Gamma}$ is the rate of spontaneous decay from Fe{F}_{e}Fe​ to Fg{F}_{g}Fg​).