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Journal of Physics B Atomic and Molecular Physics

High-n1Stark-state production by sudden electric-field reversal in Rydberg sodium

R G Rolfes, D. B. Smith, Keith B. MacAdam

Published Sep 28, 1983• 25 citations
Publisher

Abstract

By applying bipolar electric-field pulses of about 10 V cm-1, dE/dt approximately=109V cm-1s-1, the authors have demonstrated the conversion of laser-excited Na(nd) Rydberg states (n=30-38) to high-n1Stark states that lie at the top of the n manifold. These states correspond in zero field to orbits of the highest allowed angular momentum l. This transition phenomenon is believed to play an important role in the microwave electric-field ionisation of non-hydrogenic atoms.

DOI
10.1088/0022-3700/16/18/001

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Physical Review A•Aug 1, 1991•33 citations
By applying bipolar electric-field pulses of about 10 V cm-1, dE/dt approximately=109V cm-1s-1, the authors have demonstrated the conversion of laser-excited Na(nd) Rydberg states (n=30-38) to high-n1Stark states that lie at the top of the n manifold. These states correspond in zero field to orbits of the highest allowed angular momentum l. This transition phenomenon is believed to play an important role in the microwave electric-field ionisation of non-hydrogenic atoms.
The authors describe the details of an experiment using a sodium atomic beam and two dye lasers. By stepwise excitation they have selectively populated highly excited ns, nd and, using Stark mixing, np states fron n=20-50. The excited atoms were detected by field ionisation. The results obtained for the ionisation threshold fields for these states are presented and compared with the theoretical classical law F c =(2n*) -4 . A suitable field shape and detection technique allows the observation of multiple thresholds with high sensitivity. Multiple thresholds for nd states have been observed, as expected. Some ns singlet states also show multiple thresholds. Using suitably polarised laser beams the mod m L mod dependence of the ionisation threshold fields for the 20d state has been observed. The approach proposed recently by Gallagher for predicting the threshold fields is generally confirmed.
We have measured the microwave ionization threshold electric fields for ns-state Na Rydberg atoms from n=24--33 as a function of the duration of the ionizing microwave pulse. Pulses as short as 2.8 ns were used, containing fewer than 25 cycles of 8.55-GHz radiation. While the fields required to produce the onset of ionization were independent of pulse duration and exhibited the ${\mathit{n}}^{\mathrm{\ensuremath{-}}5}$ scaling characteristic of ionization by diffusion through higher-energy states, the fields required to produce nearly complete ionization increased dramatically as the pulse was shortened. Additional measurements of the populations of bound states after the shortest microwave pulses showed that up to \ensuremath{\sim}10% of the atoms were excited to states above the initially populated ns state and the adjacent (n-1) manifold of higher angular momentum states, while most either ionized or remained in these states. From this observation we conclude that the rate-limiting process for ionization is the transition from the initially populated ns states or the adjacent manifold to the next higher manifold, not the diffusion through higher-lying states.
Electric field ionization of excited Na atoms by microwave fields between 12 and 15 GHz exhibits several interesting phenomena. The ∣m∣=0and1|m|=0 \mathrm{and} 1∣m∣=0and1 states may be ionized with a very low microwave field, $\ensuremath{\sim}\frac{1}{{3n}^{5}}$, corresponding to the point at which the nnn and n+1n+1n+1 Stark manifolds of principal quantum numbers nnn and n+1n+1n+1 intersect. The ionization occurs by an atom's making a succession of Landau-Zener transitions to higher-lying states, finally reaching the classical ionization limit. The ∣m∣=2|m|=2∣m∣=2 states, on the other hand, ionize at a very high microwave field, $\ensuremath{\sim}\frac{1}{{9n}^{4}}$. Both these observations and the more familiar static or low-frequency result of ionization by a field of $\ensuremath{\sim}\frac{1}{{16n}^{4}}$ are all consistent with ionization in a completely classical fashion. The apparent differences are due to the dynamics of passing from zero field to a high ionizing field.
We present results of an experimental survey of the n=15n=15n=15 state of Na in electric fields from 0 to 4 kV/cm. Both linear and higher-order Stark effects play important roles. States with low ∣m∣|m|∣m∣ show marked differences from hydrogenic behavior, particularly in the vicinity of level crossings. Computed values for the energy levels are in good agreement with the data. The experimental method provides a simple technique for populating selected Stark or angular momentum levels of a Rydberg state.
The authors have studied phenomena related to the ionisation of indium Rydberg atoms by an external electric field. The indium atoms are excited in an atomic beam apparatus by pulsed dye laser light. The high-lying states are populated in one step from the ground state by an ultraviolet, frequency-doubled dye laser or by stepwise excitation using two dye lasers in the visible region. Shortly after the excitation, an electric field is applied in the interaction region which causes ionisation of the highly excited atoms. The authors have investigated (i) the lowest adiabatic ionisation threshold over a wide range of n values and compared the results with model predictions, (ii) the structure in the adiabatic part of the ionisation spectrum, and (iii) the transition from adiabatic to diabatic ionisation as a function of the slew rate of the ionising field pulse and the quantum defect and quantum numbers of the atomic state concerned. The ionisation signal is demonstrated to shift considerably towards higher field strengths with increasing slew rate. A qualitative explanation is presented and consequences for the detection efficiency are mentioned. Differences in the field ionisation behaviour between nearly degenerate excited states are demonstrated and exploited to achieve selective detection of fine-structure and even hyperfine-structure states.
We have studied the ionization of Na ns and nd Rydberg atoms by \ensuremath{\sim}1-\ensuremath{\mu}s pulses of 10-MHz, 670-MHz, 2-GHz, and 4-GHz fields, bridging the gap between the previous measurements of ionization by \ensuremath{\sim}1-\ensuremath{\mu}s rise-time pulses and 8- and 15-GHz microwave fields. We have also studied the ionization of Li ns and nd Rydberg atoms by 4-, 8-, and 15-GHz fields, which, due to the smaller Li quantum defects, represents the high-frequency limit of nonhydrogenic microwave ionization. The Na measurements show that ionization at 10 MHz occurs without change in n at fields of 1/16n4{\mathit{n}}^{4}n4 and 1/9n4{\mathit{n}}^{4}n4. At 670 MHz \ensuremath{\Vert}m\ensuremath{\Vert}=0, 1, and 2 states are all ionized at fields between 1/3n5{\mathit{n}}^{5}n5 and 1/9n4{\mathit{n}}^{4}n4, indicating that transitions to higher-n states are occurring. As the frequency is raised further, to 2 and 4 GHz, the \ensuremath{\Vert}m\ensuremath{\Vert}=0 and 1 states exhibit an increasingly sharp threshold for ionization at E=1/3n5{\mathit{n}}^{5}n5, but the \ensuremath{\Vert}m\ensuremath{\Vert}=2 states are unlikely to ionize at this field, with ionization occurring mostly at higher fields, 1/3n5{\mathit{n}}^{5}n5E1/9n4{\mathit{n}}^{4}n4, approaching the 15-GHz behavior of ionization at E=1/9n4{\mathit{n}}^{4}n4. At 4 GHz, Li n=20 \ensuremath{\Vert}m\ensuremath{\Vert}=0 and 1 states ionize at E=1/3n5{\mathit{n}}^{5}n5, but at n\ensuremath{\simeq}45, \ensuremath{\Vert}m\ensuremath{\Vert}=1 states ionize at E=1/9n4{\mathit{n}}^{4}n4, and the \ensuremath{\Vert}m\ensuremath{\Vert}=0 states ionize at E>1/3n5{\mathit{n}}^{5}n5. The \ensuremath{\Vert}m\ensuremath{\Vert}=2 states appear to ionize at E=1/9n4{\mathit{n}}^{4}n4. As the frequency is raised to 8 and then to 15 GHz, the transition of \ensuremath{\Vert}m\ensuremath{\Vert}=0 and 1 states to ionization at E=1/9n4{\mathit{n}}^{4}n4 occurs at lower n. When a small static field is applied, the Li ionization threshold fields drop from 1/9n4{\mathit{n}}^{4}n4 to fields somewhat above 1/3n5{\mathit{n}}^{5}n5. Together the Na and Li measurements show that microwave ionization depends on a rate-limiting step, which is a resonant multiphoton transition.