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ELECTRIC FIELD IONIZATION OF HIGHLY EXCITED RUBIDIUM ATOMS (COLLISIONS, RYDBERG)

G. B. McMillian

Published Jan 1, 1985• 0 citations
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Abstract

A frequency stabilized ring dye laser, with a linewidth of (TURN)250 kHz, has been utilized to selectively excite Rb(N('2)S, N('2)D) states in the range N = 20 - 100 by a two photon process. The highly excited atoms were detected by the technique of electric field ionization. Excited states with (VBAR)M(,L)(VBAR) < 3 have been observed to ionize along predominantly adiabatic paths and states with (VBAR)M(,L)(VBAR) (GREATERTHEQ) 3 have been observed to ionize along predominantly diabatic paths for the range of N investigated. The electric field dependence of the ionization threshold has been determined to be in good agreement with that calculated from a simple model based on the energies and ionization rates of hydrogen.\nCollisions between highly excited rubidium atoms and neutral xenon atoms, which result in a change in the N and L of the excited state of the rubidium atom, have been investigated. The N of the final state has been shown to be limited to those states which lie closest in energy to the initial state, in good agreement with theory. The distribution of L of the final states has been shown to be completely statistical or biased towards production of high L. The distribution of final L is definitely not biased toward production of states with low values of L.

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•Jan 1, 1982•0 citations
A frequency stabilized ring dye laser, with a linewidth of (TURN)250 kHz, has been utilized to selectively excite Rb(N('2)S, N('2)D) states in the range N = 20 - 100 by a two photon process. The highly excited atoms were detected by the technique of electric field ionization. Excited states with (VBAR)M(,L)(VBAR) < 3 have been observed to ionize along predominantly adiabatic paths and states with (VBAR)M(,L)(VBAR) (GREATERTHEQ) 3 have been observed to ionize along predominantly diabatic paths for the range of N investigated. The electric field dependence of the ionization threshold has been determined to be in good agreement with that calculated from a simple model based on the energies and ionization rates of hydrogen.\nCollisions between highly excited rubidium atoms and neutral xenon atoms, which result in a change in the N and L of the excited state of the rubidium atom, have been investigated. The N of the final state has been shown to be limited to those states which lie closest in energy to the initial state, in good agreement with theory. The distribution of L of the final states has been shown to be completely statistical or biased towards production of high L. The distribution of final L is definitely not biased toward production of states with low values of L.
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.
This paper summarizes a long series of experiments that have been done on Rydberg states of Rb. The basic experimental technique that has been used is atomic-beam laser spectroscopy which allows both low-resolution and high-resolution studies. Excitation of Rydberg states is provided by single-photon absorption from a suitably frequency-doubled rhodamine 6G6G6G tunable laser. Detection is done by field ionization and ion counting. These techniques have allowed us to study the critical ionizing field, which has been found to follow classical, hydrogenic behavior closely. Rydberg states of Rb have been observed from n=28n=28n=28 up to n>100n>100n>100. High-resolution spectroscopic studies have led to measurement of the fine structure for np\mathrm{np}np levels located between n=28n=28n=28 and n=60n=60n=60, as well as the isotope shift of the ground state, $\ensuremath{\delta}\ensuremath{\nu}=(172\ifmmode\pm\else\textpm\fi{}15)$ MHz. Anomalies in the intensity ratio of the doublet $5s\ensuremath{-}np$ transitions have been observed and interpreted as relativistic effects. Perturbations by weak and strong dc electric field are reported. In the case of weak electric fields it is possible to evaluate the polarizability. In the case of strong dc electric fields, new phenomena have been observed and analyzed. We also find experimental evidence of selective photoionization in the presence of an appropriate dc electric field, which could have some applications in laser isotope separation. Finally, we give the preliminary results of an experiment on the effect of a strong nonresonant electromagnetic field on high-lying Rydberg states.
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.
Multiphoton ionization (MPI) of rubidium atoms at both low (atomic beam) and high (heat pipe) densities is studied using a tunable OPO laser. At high Rb densities ionization of the laser excited ns, np, and nd states occurs both through photoionization and collisional ionization. Excitation of the np states is found to be induced by the external electric field at both low and high densities. In addition, np signal is also seen at very low (E→0) fields in the heat pipe, providing evidence for collision mixing as well as field mixing. At low densities, signal for the high np states initially increases with applied field, but soon saturates (i.e. becomes field independent) while the signal for high nd states decreases with increasing field. At low Rb densities strong resonance features are observed in the energy region between the zero field limit (IP) and the field ionization limit. These features, as well as the field ionization threshold, are found to be dependent upon the angle between the laser polarization and the direction of the applied dc field. Evidence for tunneling through the barrier created by the −e2/r−eEr potential is also presented for ns and nd states.
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.
Utilizing the technique of high resolution selective field ionization it is possible to observe ionization structure as narrow as 2 V/cm for Na(nS,nD) atoms. Field ionization structure this narrow is characteristic of atoms evolving predominantly adiabatically in a rapidly increasing electric field. By increasing the slew rate of the applied field it is possible to induce departures from the adiabatic path at specific avoided level crossings. These departures result in multiple ionization thresholds which may be explained by arguments based on a simple quantum mechanical model of adiabatic field ionization.