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AIP conference proceedings

A new technique to study Rydberg states by multiphoton ionization spectroscopy

R. D. Verma, Alak Chanda

Published Jan 1, 1988• 0 citations
Publisher

Abstract

A new technique to study the Rydberg states of the Ba atom has been developed. In this technique a Multiphoton Ionization signal is detected by selective excitation of the ground state ion (6s) to an excited state (6p), which results in a collimated Amplified Spontaneous Emission (ASE) signal at the 6p→5d transition of Ba+. Discrete Rydberg states, 6snl (l=0,2), as well as autoionizing Rydberg states, 5dnl (l=0,2) and 6pnl (l=0,2) are observed by this novel but very simple method.

DOI
10.1063/1.37327

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A new technique to study the Rydberg states of the Ba atom has been developed. In this technique a Multiphoton Ionization signal is detected by selective excitation of the ground state ion (6s) to an excited state (6p), which results in a collimated Amplified Spontaneous Emission (ASE) signal at the 6p→5d transition of Ba+. Discrete Rydberg states, 6snl (l=0,2), as well as autoionizing Rydberg states, 5dnl (l=0,2) and 6pnl (l=0,2) are observed by this novel but very simple method.
The authors have measured the population in each of the 5d 3/2 (m j ) ion states following autoionization of the (6p 3/2 nd) J=MJ=3 state by using a circularly polarized laser to excite the Ba + 5d 3/2 to 6p 1 2/ transition, and observing the polarized fluorescence of the Ba + 6p 1/2 to 6s 1/2 transition. The branching ratios for autoionization into each of the 5d 3/2 in l j channels can be related to these ion populations by using angular momentum algebra. The fractions of ions found in the m j =+3/2, +1/2, -1/2 and -3.2 state of the 5d 3/2 ion states were 5.9(+or-2.6)%, 4.5(+or-1.9)%, 3.2(+or-1.3)% and 1.9(+or-0.6)% respectively. This method can easily be generalized to measure the branching ratio for autoonization into other ion states.
We have studied multiphoton ionization of Ba 6snl Rydberg states by intense ps pulses and have shown that the duration of the laser pulse compared to the orbit time of the Rydberg electron determines the laser-atom interaction. For high-n states with a long orbit time, the loosely bound Rydberg electron is not affected by the intense laser pulse. Instead the inner electron is ejected by absorption of five photons, leaving the Ba+{\mathrm{Ba}}^{+}Ba+ ion in a Rydberg state. For low-n states the outer electron is ejected and the residual Ba+{\mathrm{Ba}}^{+}Ba+ ion can subsequently be multiphoton ionized to Ba++{\mathrm{Ba}}^{++}Ba++.
The authors have studied double ionization of Ba 6snl Rydberg states through resonant two-photon excitation of 8snl double-Rydberg states with n=13 and 14 and different l. The laser intensity dependence of Ba 2+ yield measured for l>or=8, when the electrons suffer long-range dipole interaction, shows a decrease from four-photon for l=8 to less than three for l=11. The four-photon dependence is due to autoionization decay populating the Ba + (7p) levels which gives an indirect signature to the Ba 2+ production. By increasing l this decay vanishes and the data show evidence of a direct double-ionization process via planetary-electron states for l>or=10. Additional intensity measurements performed for low l=6 states strongly mixed with 5fn'l' ones by short-range multipole interaction, reveal indirect Ba 2+ production and an individual case of partial stabilization due to destructive interference leading to direct double ionization.
We have studied the nununu=1 Rydberg states of BaF in the energy region E=38800-39100 wn (n*=15-25) via optical-optical double resonance spectroscopy. Rydberg states excited above the first ionization potential spontaneously autoionize and 138^{138}138Ba19^{19}19F+^{+}+ ions are detected by TOF-MS. In addition, BaF possesses a particularly low ionization potential, which allows for the study of autoionization dynamics in the absence of predissociative decay. This work extends the assignments of core-penetrating Rydberg states of BaF (Jakubek and Field, 2000) for applications to state-selective ion production schemes. Polarization and Stark spectroscopy techniques will be discussed in the context of accurate and efficient assignment of spectra.