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Physical Review Letters

Electric Field Ionization of High Rydberg States of Ar with Sequences of Identical Pulses

Frédéric Merkt, R. J. Rednall, Stuart R. Mackenzie, T. P. Softley

Published May 6, 1996• 26 citations
Publisher

Abstract

Novel field-ionization behavior of very high Rydberg states of Ar ( $n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}50--250$) is observed using sequential pulsed electric fields. Fast autoionization acts as a filter against adiabatic field ionization near the ${}^{2}{P}_{1/2}$ threshold, whereas both diabatic and adiabatic field ionization occur near the ${}^{2}{P}_{3/2}$ threshold. Sequences of up to 9 equivalent pulses yield recurrent field ionization signals near the ${}^{2}{P}_{3/2}$ threshold, provided that the field returns close to zero between pulses, demonstrating a statistical redistribution of the Rydberg population amongst all states of a given Stark manifold near zero field.

DOI
10.1103/physrevlett.76.3526

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Novel field-ionization behavior of very high Rydberg states of Ar ( n=50−−250n\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}50--250n=50−−250) is observed using sequential pulsed electric fields. Fast autoionization acts as a filter against adiabatic field ionization near the 2P1/2{}^{2}{P}_{1/2}2P1/2​ threshold, whereas both diabatic and adiabatic field ionization occur near the 2P3/2{}^{2}{P}_{3/2}2P3/2​ threshold. Sequences of up to 9 equivalent pulses yield recurrent field ionization signals near the 2P3/2{}^{2}{P}_{3/2}2P3/2​ threshold, provided that the field returns close to zero between pulses, demonstrating a statistical redistribution of the Rydberg population amongst all states of a given Stark manifold near zero field.
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.
Field ionization of high Rydberg manifold states (n=112–137)(n=112\text{--}137)(n=112–137) of rubidium-85 under a rotating electric field has been investigated experimentally and theoretically. Applying a rapidly reversed electric field with a small static perpendicular field to rotate the total electric field around zero, we have observed substantial increase of the fraction of the tunneling field-ionization process and a profound broadening of its ionization peak over a wide range of field strengths with increasing transverse electric field. The observed tunneling field-ionization fraction is almost independent of the slew rate of the applied electric field, and also on the principal quantum number nnn over the range investigated. To compare with these experimental results, theoretical calculations have been performed with a successive two-step regime. As the first step we calculated the redistributions of magnetic quantum number ${m}_{\ensuremath{\ell}}$ and parabolic quantum number ${n}_{1}\ensuremath{-}{n}_{2}$ of the states under the rotating electric field. Then the following time evolution of the manifold states with $\ensuremath{\mid}{m}_{\ensuremath{\ell}}\ensuremath{\mid}\ensuremath{\leqslant}3$ was traced on the Stark map in a coherent as well as an incoherent model. The calculated results are generally in good agreement with the experimental ones. The increase of the tunneling field-ionization fraction under a rotating electric field plays an essential role in achieving the high efficiency in the recently proposed selective-field-ionization scheme for high Rydberg atoms.
We have observed the selective ionization of the degenerate ∣mj∣|{m}_{j}|∣mj​∣ levels of sss, ppp, and ddd states of sodium in the range of nnn from 15 to 20 and have shown that atoms produced in these low-field (\ensuremath{\sim} 10 V/cm) states pass adiabatically from low-field ∣mj∣|{m}_{j}|∣mj​∣ to intermediate-field ∣ml∣|{m}_{l}|∣ml​∣ states. Experiments on the Stark manifold states in intermediate fields (\ensuremath{\sim} 1 kV/cm) and high fields (\ensuremath{\sim} 4 kV/cm) show that the ∣ml∣=0and1|{m}_{l}|=0 \mathrm{and} 1∣ml​∣=0and1 states pass adiabatically from intermediate- to high-field states and that the passage of the ∣ml∣=2|{m}_{l}|=2∣ml​∣=2 states is very nearly adiabatic. These findings suggest a general approach for predicting the threshold fields for ionization of atomic Rydberg states.
Coherent time evolution of highly excited Rydberg states in Rb (98 n 150) under pulsed electric field in high slew rate regime was investigated with the field ionization detection. We observed for the first time a discrete transition of the threshold ionization field with slew rate, the behavior of which depends also on the position of the low l states relative to the adjacent manifold. The experimental results strongly suggest that the coherent interference effect plays decisive role for such transitional behavior, and bring us a new, quite effective scheme for the stringently selective field ionization.
The first detailed observation of the perturbations by an electric field of the Rydberg autoionizing resonances of a rare-gas atom is reported. The Stark spectroscopy of autoionizing Rydberg states converging to the second ionization limit $4{p}^{5}^{2}P_{\frac{1}{2}}^{o}$ in Kr I is performed in an atomic beam with the use of a two-step laser excitation from the 4p55s[32]204{p}^{5}5s{[\frac{3}{2}]}_{2}^{0}4p55s[23​]20​ metastable state. In addition to the verification of the ${({n}^{*})}^{\ensuremath{-}3}$ dependence of the zero-field width of two autoionizing series and of the linear dependence of the Stark-manifold splittings with the electric field, we have observed an (n)0.7{(n)}^{0.7}(n)0.7 law for the dependence of the Stark-manifold splitting along the series, an important narrowing and dissymmetrization of the $n{d}^{\ensuremath{'}}$ resonances, and a nonlinear-field behavior of Stark-manifold components in the vicinity of the first anticrossing. Discussions are carried out with the use of the recent work on Rydberg-Stark spectroscopy and on autoionizing states in two-electron atoms.
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.