A report is given of the first quantitative study of the spontaneous and stimulated electronic Raman scattering by a resonance doublet of the sodium atom excited resonantly at the D 1 and D 2 lines by a tunable dye laser. Theoretical and experimental analyses of the differential scattering cross section and polarization properties at the Stokes and anti-Stokes frequencies show that the observed scattering is due to a nearly resonant process involving the ground state 3 S 1/2 as the dominant intermediate state. The stimulated Stokes and anti-Stokes scattering lines, which are shifted from the D 1 and D 2 lines by an amount corresponding to the frequency separation between lowest-lying excited doublets 3 P 1/2 and 3 P 3/2 , are observed by exciting a sodium vapor cell with a passively mode-locked dye laser.
We have used two-photon absorption from counterpropagating laser beams of different frequencies to measure Stark shifts and splittings of the
62S,
72S,
82S,
52D, and
62D states in sodium. Beams from a fixed-frequency, single-mode
Ar+ laser and a tunable, single-frequency cw dye laser were focussed into a coarse sodium atomic beam and the fluorescence was monitored. The collimation of the atomic beam reduced the residual Doppler width inherent in using two different frequencies. Using the two lasers allowed two-photon transitions to be observed at frequencies unattainable with the dye laser alone, and enhanced the transition rates due to the near resonance of the dye laser with the strong Na $3^{2}S\ensuremath{\rightarrow}3^{2}P$ transition. Our experimental results for the scalar and tensor polarizabilities, ${\ensuremath{\alpha}}_{0}$ and ${\ensuremath{\alpha}}_{2}$, agree with calculations in the Bates and Damgaard Coulomb approximation within 2% for ${\ensuremath{\alpha}}_{0}$ and 9% for ${\ensuremath{\alpha}}_{2}$. As a by-product the hyperfine-interaction constants
a for the
S states and the fine-structure intervals $\ensuremath{\delta}\ensuremath{\nu}=\frac{({E}_{\frac{3}{2}}\ensuremath{-}{E}_{\frac{5}{2}})}{h}$ for the
D states were obtained.
The atoms at autoionization state can be excited to higher continuum state, as well as transit to bond states by spontaneous emission a photon in laser induced autoionization. The effect of these processes on the laser induced autoionization process has been investigated by means of using the reaction matrix. The effect of spontaneous emission process is small in general case, but its spectrum shows that the emission is contributed mainly from the spontaneous Raman scattering enhanced by the cutoioni-zation state, and the Dressed atom picture was shown clearly. The multiphoton process makes the photoelectron spectra and laser induced autoionization process very complicated. For example, the photoelectron spectra of one and two-photon process have multi-maxium structure.
Two independently tunable, linearly polarized dye lasers are counterpropagated through a heat pipe containing sodium vapor. The frequency of the first laser ${\ensuremath{\omega}}_{1}$ is incremented through both 3
p2P1/2,3/2 fine-structure levels while the second laser ${\ensuremath{\omega}}_{2}$ is scanned through the energy increment necessary to reach ns
2S1/2 and
nd2D3/2,5/2 levels (n=5--35). Following excitation, ionization occurs through chemi-ionizing collisions. The polarization (defined as the ionization intensity measured when the two planes of polarization of the laser beams are parallel minus the intensity when perpendicular divided by the sum of the intensities) P=(
I?-${I}_{\ensuremath{\perp}}$)/(
I?+${I}_{\ensuremath{\perp}}$) goes from +1 to -1 as ${\ensuremath{\omega}}_{1}$ is tuned between the 3
p2P1/2,3/2 fine-structure levels. This novel polarization effect is shown to be due to an interference between the two pathways to the ns
2S1/2 levels. Upon exciting the unresolved nd
2D3/2,5/2 levels, the polarization is very close to zero when ${\ensuremath{\omega}}_{1}$ is at or near the 3p
2P3/2,1/2 levels. A simple few-level atom theory reproduces the experimental observations except for the case when both lasers are in resonance.
Laser excitation and ionization processes in dense (1–10 Torr) sodium vapor have been studied for laser wavelengths near the two-photon allowed nd 2D(n=3, 4, 5) and ns 2S(n=4, 5, 6) states. In particular, the 1 3Σ+g→1 3Σ+u excimer emission in Na2, predicted in 1980 by Konowalow and Julienne and observed recently by Dinev et al, was studied here in greater detail. Strong excimer emission (∼830 nm) was observed for two-photon pumping to both sides of the unresolved 4D states, and weak excimer emission was seen when pumping near the 5D levels. The excimer emission exhibits a complicated pump laser profile with a pronounced ‘‘dip’’ at the 4d 2D two-photon resonance. Similarly, [2+1] photon ionization via the 3d 2D and 4d 2D states shows a dramatic decrease as the sodium density increases. These results can be attributed either to depleted 3d 2D or 4d 2D population due to stimulated electronic Raman scattering (SERS) or to the interference effects recently reported by Malcuit et al. and Krasnikov et al. and treated theoretically by Manykin and Afanas’ev and by Agarwal. It is argued that both mechanisms are operative. Strong ionization and SERS signals were observed at the hybrid resonances corresponding to 3p 2P3/2, 1/2 →4d 2D transitions; however, no excimer lasing at 830 nm was detected. No excimer emission was detected upon two-photon pumping near or at the 3d 2D or ns 2S(n=4, 5, 6) states. Based on these and other observations, the 1 3Σ+g→1 3Σ+u excimer emission is attributed to a molecular Raman process involving stimulated emission or six-wave mixing via a pathway of the type 1 3Σ+u→2hν 3Δu→ j 3Πg→(k 3Πu, l 3Σ +u)→1 3Σ+g→1 3Σ +u .
The multiphoton excitation of rubidium has been investigated over the 4600-6500-\AA{} wavelength region with a tunable dye-laser source having a linewidth better than 0.1 \AA{} and a space-charge ionization detector sensitive to a few ions per second. Multiphoton transitions have been observed to occur both through intermediate atomic states and through intermediate continuum states of the rubidium molecule. In the former case two-photon transitions have been observed from the
52S ground state of atomic rubidium to higher-lying
n2D levels for values of
n ranging from 9 to 34 and to
n2S levels for values of
n from 11 through 20. The fine-structure intervals of the
n2D levels for
n=9toc13 were measured together with the line-strength ratios and were found to be in good agreement with the predictions of a simple theoretical model. At the shorter wavelengths hybrid two-photon resonances were observed to be excited through resonant intermediate continuum states of
Rb2. As a result the dispersion curve for two-photon absorption in rubidium showed what appears to be resonant intermediate $p\ensuremath{\pi}(^{3}\ensuremath{\Sigma}_{u1})$ and
0g+ terms dissociating to give a
5P23 atom and resulting in the strong development of features corresponding to the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}D_{\frac{3}{2},\frac{5}{2}}$ part of the diffuse series, for $n\ensuremath{\le}50$ in absorption and the $5^{2}P_{\frac{3}{2}}\ensuremath{\rightarrow}n^{2}S_{\frac{1}{2}}$ part of the sharp series. Components to
322D and
302S were recorded to a precision of 0.3 ${\mathrm{cm}}^{\ensuremath{-}1}$ and quantum defects for these previously unobserved terms were derived. The corresponding hybrid two-photon resonances involving intermediate states dissociating to give a
52P21 atom were not observed in the wavelength interval available in this experiment.