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Physical Review A

Microwave forced autoionization of Na2 Rydberg states

Christopher R. Mahon, Chung Yi Lee, Thomas F. Gallagher

Published Sep 1, 1993• 1 citation
Publisher

Abstract

We have examined the ionization of ${\mathrm{Na}}_{2}$ Rydberg states of principal quantum number n=11--16 converging to rotational-vibrational, v=3--6 and R10, states of ${\mathrm{Na}}_{2}^{+}$ by 8-GHz microwave fields. Rydberg states lying below the lowest, v=0, R=0 (v and R are the vibrational and rotational quantum numbers of the molecular ion), ion limit of ${\mathrm{Na}}_{2}^{+}$ are observed to ionize at approximately E=1/3${\mathit{n}}_{0}^{5}$, where ${\mathit{n}}_{0}$ is the effective quantum number relative to the v=R=0 limit. The agreement with this dependence is not nearly as good as in an atom, and the possible reasons for the deviations are discussed.

DOI
10.1103/physreva.48.2270

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We have examined the ionization of Na2{\mathrm{Na}}_{2}Na2​ Rydberg states of principal quantum number n=11--16 converging to rotational-vibrational, v=3--6 and R10, states of Na2+{\mathrm{Na}}_{2}^{+}Na2+​ by 8-GHz microwave fields. Rydberg states lying below the lowest, v=0, R=0 (v and R are the vibrational and rotational quantum numbers of the molecular ion), ion limit of Na2+{\mathrm{Na}}_{2}^{+}Na2+​ are observed to ionize at approximately E=1/3n05{\mathit{n}}_{0}^{5}n05​, where n0{\mathit{n}}_{0}n0​ is the effective quantum number relative to the v=R=0 limit. The agreement with this dependence is not nearly as good as in an atom, and the possible reasons for the deviations are discussed.
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.
Bound Li2{\mathrm{Li}}_{2}Li2​ states of principal quantum number n=12--14 converging to v=2 and 3 levels of the ground state of Li2{\mathrm{Li}}_{2}Li2​+{\mathrm{}}^{+}+ can be ionized by fields of \ensuremath{\sim}200 V/cm, 2 orders of magnitude less than expected for direct field ionization of these levels. The result is shown to be due to forced autoionization. The field depresses the ionization limit of the series converging to the lowest rotational-vibrational Li2{\mathrm{Li}}_{2}Li2​+{\mathrm{}}^{+}+ levels, and the n=12--14 levels in question autoionize to the Stark-induced continuum.
The authors have observed the ionization of Na Rydberg states by strong microwave fields and have found that the field required for ionization is 1(3.7n5)\frac{1}{(3.7{n}^{5})}(3.7n5)1​ (in atomic units) for $n=20\ensuremath{-}37$. This field is close to the field 1(3n5)\frac{1}{(3{n}^{5})}(3n5)1​ at which the Stark manifolds of principal quantum numbers nnn and n+1n+1n+1 intersect. The ionization can be shown to arise from transitions occurring near these intersections.
In circularly polarized microwave fields of frequencies in the vicinity of 10 GHz ionization of Na Rydberg atoms occurs at a field E=1/16n4, up to principal quantum number n=50. This field is equal to the classical field for ionization and the static field required to ionize a Na atom. On the other hand, this field is far below the linearly polarized 10 GHz field required to ionize Na atoms, E=1/3n5. If the problem is transformed to a frame rotating with the microwave field, the field becomes a static field. In this case it is straightforward to calculate the ionization field classically. However, it is far lower than the experimentally observed field, a discrepancy which may be due to an angular momentum barrier.
\n \nWe have investigated the electric field ionization of highly excited (ns)\nand (nd) Rydberg states of the barium ion by microwave fields. For states\nwith a principal quantum number nleq40n\\leq 40nleq40 the observed microwave ionization\nthreshold fields show the Z3/3n5Z^3/3n^5Z3/3n5 dependence expected on the basis of\npreviously observed ionization of neutral Rydberg states with Z=1. We show\nthat for states in this n regime microwave ionization is a state selective\ndetection technique. Threshold fields for states with n> 40, however,\ndepart from the expected behaviour, the thresholds become broader and shift\nto higher fields. For a total of 58 states we present the field strengths\nwhere 90% , 50% and 10% ionization occur.\n\n\n
We report microwave ionization experiments with Rydberg states of Na using several microwave frequencies near 80 GHz. We observe substantial ionization of states as low as n=26n=26n=26 with microwave pulses of 170-V/cm amplitude. Unlike experiments at 38 and 17 GHz, microwave ionization is not always accompanied by the production of the extremely high-lying states just below the limit. It only occurs when the initial Rydberg state is in multiphoton resonance with the high-lying states. The resonance condition is apparent at 80 GHz because the ponderomotive energy shift of the limit, and of the high-lying states, is small compared to the microwave frequency, even at fields strong enough to produce ionization. At the lower microwave frequencies, the ponderomotive shift exceeds the microwave frequency, ensuring that the resonance condition is met and obscuring its importance. The same is true of many laser experiments.