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Physical Review A

Investigation of fine-structure quantum beats in sodium Rydberg atoms by field ionization

THOMAS H. JEYS, K. A. Smith, F. B. Dunning, R. F. Stebbings

Published Jun 1, 1981• 31 citations
Publisher

Abstract

Pulsed dye lasers are used to excite sodium atoms into a coherent superposition of high Rydberg $\mathrm{nd} (^{2}\mathrm{D}_{\frac{3}{2}},^{2}D_{\frac{5}{2}})$ 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 $n=32, 34, 35, 36, 38, \mathrm{and} 40$.

DOI
10.1103/physreva.23.3065

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The outer electron of a Rydberg atom is so weakly bound to the atomic core that a relatively small electric field may cause the electron to be stripped from the atom. The field strength at which this ionization happens is strongly dependent on the state of the Rydberg atom. Pulsed electric field ionization serves, therefore, not only as a means by which a Rydberg atom may be efficiently detected, but also a means by which the state of the Rydberg atom may be analyzed.\nThe first observation of predominantly diabatic passage to field ionization of a non-hydrogenic Rydberg atom has resulted in an improved understanding of the adiabatic and diabatic ionization processes. The magnitudes of the various field ionization features have been measured and found to agree with theory, and by detailed analysis, it is now possible to label the various field ionization signal features with the appropriate (VBAR)m(,l)(VBAR) quantum numbers. A much better understanding of the laser excitation process, the Rydberg state production, and the response of the excited state to an increasing electric field has enabled measurement of some Rydberg fine-structure intervals, through observation of field ionization quantum beats.
We excite ultracold rubidium atoms in a magneto-optical trap to a coherent superposition of the three ∣mj∣|{m}_{j}|∣mj​∣ sublevels of the 37d5/237{d}_{5/2}37d5/2​ Rydberg state. After some delay, during which the relative phases of the superposition components can evolve, we apply an electric field pulse to ionize the Rydberg electron and send it to a detector. The electron traverses many avoided crossings in the Stark levels as it ionizes. The net effect of the transitions at these crossings is to mix the amplitudes of the initial superposition into the same final states at ionization. Similar to a Mach-Zehnder interferometer, the three initial superposition components have multiple paths by which they can arrive at ionization and, since the phases of those paths differ, we observe quantum beats as a function of the delay time between excitation and initiation of the ionization pulse. We present a fully quantum-mechanical calculation of the electron's path to ionization and the resulting interference pattern.
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.
We present a theory of quantum beats in photoionization from a coherent superposition of D32,5.2{D}_{\frac{3}{2},5.2}D23​,5.2​ levels in alkali-metal atoms. The semiclassical density-matrix formalism is used to describe both the excitation of the D32,52{D}_{\frac{3}{2},\frac{5}{2}}D23​,25​​ levels by a two-photon resonant pulse and the subsequent photoionization by a delayed probe pulse. Quantum beats occur in the ionization signal as a function of the delay of the probe pulse. The depth of modulation is determined for different light polarizations.
Rydberg states in sodium are excited using two identical broadband, dye laser pulses. Each 8 ns pulse has a bandwidth of approximately 45 cm -1 , and Rydberg states with several different principal quantum numbers are simultaneously excited. The number of Rydberg atoms created by each pulse pair is detected as a function of the delay between the two pulses. Strong modulations in the population in each Rydberg level and in the total Rydberg signal are observed. The oscillations are identical to those which would be expected if two transform-limited, 300 fs laser pulses had been used. We show explicitly, in the limit of weak pulses, that these 'bound-state interferograms' acquired using the time-domain, Ramsey separated-oscillatory fields method are only dependent on the excitation cross section and pulse frequency spectrum. Therefore, weak-field interferograms do not in themselves give information on the spatial-distribution of the electron wavefunction. In addition, the benefits of using strong or weak pulses for bound-state interferometry are discussed.