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Physical Review Letters

Observation of Fine-Structure Quantum Beats Following Stepwise Excitation in Sodium D States

S. Haroche, M. Groß, Mark P. Silverman

Published Oct 28, 1974• 89 citations
Publisher

Abstract

We report the observation of fine-structure and Zeeman quantum beats in highly excited sodium $D$ 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 $9D$ and $10D$ 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.

DOI
10.1103/physrevlett.33.1063

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Physical Review Letters•Oct 11, 1976•3 citations
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.
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.
Pulsed dye lasers are used to excite sodium atoms into a coherent superposition of high Rydberg nd(2D32,2D52)\mathrm{nd} (^{2}\mathrm{D}_{\frac{3}{2}},^{2}D_{\frac{5}{2}})nd(2D23​​,2D25​​) states. Analysis of the field ionization behavior of these atoms reveals the time evolution of the superposition state. Rapid application of a weak electric field projects different components of the superposition state onto states having identifiably different field ionization behavior. Analysis of the signal from subsequent field ionization as a function of the time of weak-field application reveals fine-structure quantum beats. These beats result from the time development of the original superposition state. Measurements of the fine-structure quantum beat frequency are presented for the principal quantum numbers n=32,34,35,36,38,and40n=32, 34, 35, 36, 38, \mathrm{and} 40n=32,34,35,36,38,and40.
We have observed spontaneous Raman processes in a sodium atomic beam. When one sodium 3p2P3p^{2}P3p2P fine-structure level is strongly excited by a dye laser, the other level, is weakly populated by spontaneous Raman emission and the absorption of another laser photon. This effect is detected by further stepwise excitation plus photoionization. The observed magnitude agrees well with theory. This technique is much more sensitive than methods involving direct observation of the Raman emission.