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Optics Letters

Observation of quantum beats in forward scattering after stepwise excitation: the 3 ^2P ↔ 4 ^2D sodium transition

J. Koperski, K. Szymaniec, T. Dohnalik

Published Jul 1, 1993• 2 citations
Publisher

Abstract

We describe quantum beats in forward scattering for the 3 2p ↔ 4 2D transition in sodium. For the excitation of the 4 2D3/2,5/2 states, the pulsed-stepwise method, through the 3 2P1/2 or 3 2P3/2 intermediate level, was used. We observed changes in the quantum-beats pattern that are due to the probe laser detuning, similar to these observed previously for the sodium D2 line.

DOI
10.1364/ol.18.001086

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We describe quantum beats in forward scattering for the 3 2p ↔ 4 2D transition in sodium. For the excitation of the 4 2D3/2,5/2 states, the pulsed-stepwise method, through the 3 2P1/2 or 3 2P3/2 intermediate level, was used. We observed changes in the quantum-beats pattern that are due to the probe laser detuning, similar to these observed previously for the sodium D2 line.
levels of atomic sodium using ultrashort laser pulses in a stepwise excitation scheme. Two broadband femtosecond laser pulses are used to excite the 6S level from the 3S ground level in sodium vapor. The first one is simultaneously resonant with the D1 and D2 lines of the 3S→3P transition, and the second one with the 3P→6S transition. The delay between the two pulses is scanned in order to probe the dephasing between the two excited intermediate levels. Quantum beating is observed by monitoring the fluorescence signals at 330 nm and 515 nm, namely transition 4P→3S and 6S→3P, respectively. Signals are compared to a semi-classical model that reproduces the oscillations with a very good agreement.
We report the observation of fine-structure and Zeeman quantum beats in highly excited sodium DDD states prepared, for the first time in a quantum-beat experiment, by stepwise excitation using two synchronously pulsed dye lasers. We have used this new technique to measure the previously unknown fine-structure intervals of levels 9D9D9D and 10D10D10D of sodium, the values being, respectively, 124.5\ifmmode\pm\else\textpm\fi{}1.5 and 91.5\ifmmode\pm\else\textpm\fi{}1 MHz.
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 .
Intensity modulations have been observed in the superradiant signals on the 4 2 P 1/2 -4 2 S 1/2 transitions obtained by pulsed dye laser beam excitation of the 4 2 P 1/2 level in Na vapour. The modulations were interpreted as beats among the frequencies of the electric dipole transitions resulting from the different HFS levels. The HFS splitting both of the upper and the lower levels must be taken into consideration in explaining the observed signals. Preliminary results of the study are reported, in particular the characteristics of the time development and polarisation of the superradiance.