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Physical Review A

Bandwidth-induced reversal of asymmetry in optical-double-resonance amplitudes

D. E. Nitz, A. V. Smith, M. D. Levenson, Stephen J. Smith

Published Jul 1, 1981• 33 citations
Publisher

Abstract

Optical-double-resonance measurements using ionization detection have been carried out in the $3{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}\ensuremath{-}4D$ atomic-sodium system. Asymmetries observed in production of $4D$ atoms from the two components of the Stark-split $3{P}_{\frac{1}{2}}$ state are found to be controlled by the far, very weak wings of the 17-MHz full-width-at-half-maximum laser line which is used to drive the $3{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}$ transition at detunings in the range 0-70 GHz. Suppression of the wings with a Fabry-Perot filter causes a pronounced reversal of the asymmetry.

DOI
10.1103/physreva.24.288

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Optical-double-resonance measurements using ionization detection have been carried out in the 3S12\ensuremath−3P12\ensuremath−4D3{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}\ensuremath{-}4D3S21​​\ensuremath−3P21​​\ensuremath−4D atomic-sodium system. Asymmetries observed in production of 4D4D4D atoms from the two components of the Stark-split 3P123{P}_{\frac{1}{2}}3P21​​ state are found to be controlled by the far, very weak wings of the 17-MHz full-width-at-half-maximum laser line which is used to drive the 3S12\ensuremath−3P123{S}_{\frac{1}{2}}\ensuremath{-}3{P}_{\frac{1}{2}}3S21​​\ensuremath−3P21​​ transition at detunings in the range 0-70 GHz. Suppression of the wings with a Fabry-Perot filter causes a pronounced reversal of the asymmetry.
An intense laser and a probe laser in near resonance with the sodium $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ and $3{P}_{\frac{1}{2}}\ensuremath{\rightarrow}4{D}_{\frac{3}{2}}$ transitions, respectively, produce a three-photon ionization current used to study the broadening and Rabi splitting of the 3P123{P}_{\frac{1}{2}}3P21​​ intermediate state as a function of probe-laser tuning. We find a narrow, intense-laser detuning region where the peak-heights ratio of the Rabi-split 3P123{P}_{\frac{1}{2}}3P21​​ doublet is reversed from that predicted for a monochromatic laser field. This is attributed to the finite (\ensuremath{\sim} GHz) laser linewidth.
The dependence of the optical Autler-Townes effect on laser field phase fluctuations describable by a two-dimensional Markovian process (phase-diffusion model with a non-Lorentzian line shape) is investigated experimentally in atomic sodium. An intense cw laser tuned to near resonance with the 3S1/2{3\mathrm{S}}_{1/2}3S1/2​(F=2,MF{\mathrm{M}}_{\mathrm{F}}MF​=2)\ensuremath{\rightarrow}3P3/2{3\mathrm{P}}_{3/2}3P3/2​(F=3,MF{\mathrm{M}}_{\mathrm{F}}MF​=3) transition was frequency modulated to generate phase fluctuations with the desired characteristics. A weak probe laser coupling to the 4D5/2{D}_{5/2}D5/2​(F=4, MF{M}_{F}MF​=4) state was used to obtain the double-peaked optical Autler-Townes absorption profiles in order to investigate their dependencies on band shape, bandwidth, intensity, and detuning of the intense fluctuating laser field. Reversals of the peak-height asymmetry and reversion to normal asymmetry with increased detuning were observed and measured. Quantitative studies of the spectral widths and splittings of the peaks are also reported. Measured absorption profiles are in excellent agreement with calculations based on previous theoretical work.
Sodium vapor, in the density range 1013{10}^{13}1013 to 5 \ifmmode\times\else\texttimes\fi{} 1014{10}^{14}1014 ${\mathrm{cm}}^{\ensuremath{-}3}$, was excited by a cw dye laser, tuned 20-150 GHz from either the D1{D}_{1}D1​ or D2{D}_{2}D2​ resonance line. We observed a three-peak scattered spectrum, consisting of the Rayleigh component at the laser frequency, and the two fluorescence components (direct and sensitized) at the atomic resonance-line frequencies. Corrections to the Rayleigh signals for anisotropy and polarization effects, and to the fluorescence signals for radiation trapping, were made in order to obtain the ratio of the sum of the total intensities of the two fluorescence components to that of the Rayleigh component. This ratio combined with a measurement of the line-wing absorption coefficient yields the sodium density and the DDD-line self-broadening rate coefficients [${k}_{\mathrm{br}}=4.67\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ cm3{\mathrm{cm}}^{3}cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the D2{D}_{2}D2​ line and ${k}_{\mathrm{br}}=3.07\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ cm3{\mathrm{cm}}^{3}cm3${\mathrm{s}}^{\ensuremath{-}1}$ (\ifmmode\pm\else\textpm\fi{}15%) for the D1{D}_{1}D1​ line]. Asymmetry in the self-broadened line wings due to fine-structure recoupling was observed. The measured intensity ratio of the DDD lines, combined with pulsed measurements of the effective radiative decay rates in the presence of radiation trapping, yields the fine-structure collisional-mixing cross section [$\ensuremath{\sigma}(3{P}_{\frac{3}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}})=172$A˚2{\mathrm{\AA{}}}^{2}A˚2(\ifmmode\pm\else\textpm\fi{}18%)] at $T\ensuremath{\cong}300\ifmmode^\circ\else\textdegree\fi{}$ C. Our results are compared to other experiments and to theory.
The authors examine the theory of optical double resonance using two lasers whose finite linewidths are produced by the process of phase-diffusion. Their lineshapes, which are nonLorentzian, are characterised by a bandwidth B and a cut off C. The authors are concerned with obtaining an analytic theory; they achieve this by assuming the ratio B/C to be small and work to first order in B/C (although the method can be extended to higher order in B/C). They obtain analytic expressions for the optical double resonance spectrum and discuss the results of recent experiments by Hogan et al. (1978) and Nitz et al. (1981) in which it was found that the asymmetry of the peaks in the optical double resonance spectrum changed with detuning. It is found that a qualitative understanding can be achieved but that a full quantitative comparison is not yet possible.
We present a theory of Stark splitting in doubly resonant three-photon ionization (three-level system) with nonmonochromatic fields. The asymmetry of the peaks of the resonance curve due to Stark splitting is shown to be reversed when the laser bandwidth is larger than the width of the atomic transitions of the resonant states. It is further shown that ionization as well as the probe field have a significant effect on the features of the splitting. Similar effects are found with monochromatic fields in the presence of an additional level near the initial level (four-level system). The results of the analysis are in general qualitative agreement with existing observations.