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Physical Review Letters

Observation of Circular-Metastable Doubly Excited States of Barium

F. Roussel, M. Chéret, L. Chen, T. Bolzinger, G. Spiess, Jean Hare, M. Groß

Published Dec 17, 1990• 20 citations
Publisher

Abstract

Using the adiabatic crossed-field method we have prepared for the first time doubly excited barium atoms with one valence electron in an oriented circular Rydberg state (n=21, l=m=20, denoted 21c) and the other electron in a ${6\mathrm{p}}_{\mathrm{j}}$ state. In a fraction of these atoms the inner electron decays radiatively to a ${5\mathrm{d}}_{\mathrm{j}\ensuremath{'}}$ metastable level. The obtained circular-metastable doubly excited atoms are very stable. For the (${5\mathrm{d}}_{3/2>}$21c) state the autoionization lifetime \ensuremath{\tau} is longer than 400 \ensuremath{\mu}s; for the (${5\mathrm{d}}_{5/2}$21c) state, \ensuremath{\tau}=1\ifmmode\pm\else\textpm\fi{}0.2 \ensuremath{\mu}s. the specific role of the 5d electron is demonstrated. \textcopyright{} 1990 The American Physical Society

DOI
10.1103/physrevlett.65.3112

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We report the observation of unusual doubly excited states of barium: Ba (5dj, 21c). One of the valence electrons of Ba is prepared in an oriented circular Rydberg state (n = 21, l = m = 20, denoted 21c) by the adiabatic crossed-fields method. The other electron is excited to a 6pj state which decays radiatively to a 5dj metastable level. The measured autoionization lifetime of Ba (5d5/2, 21c) is T ~ 1 μ s , whereas for Ba (5d3/2, 21c), τ is estimated to be longer than 400 μs. This very large difference of lifetimes between the fine-structure states of the inner electron has been analysed.
Circular Rydberg states with n=70n=70n=70 have been prepared in helium using a modified version of the crossed-fields method. This approach to the preparation of high-nnn circular Rydberg states overcomes limitations of the standard crossed-fields method which arise at this, and higher, values of nnn. The experiments were performed with atoms traveling in pulsed supersonic beams that were initially laser photoexcited from the metastable 1s2s3S11s2s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s2s3S1​ level to the 1s73s3S11s73s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s73s3S1​ level by resonance-enhanced two-color two-photon excitation in a magnetic field of 16.154 G. These excited atoms were then polarized using a perpendicular electric field of 0.844 V/cm, and transferred by a pulse of microwave radiation to the state that, when adiabatically depolarized, evolves into the n=70n=70n=70 circular state in zero electric field. The excited atoms were detected by state-selective electric field ionization. Each step of the circular state preparation process was validated by comparison with the calculated atomic energy-level structure in the perpendicular electric and magnetic fields used. Of the atoms initially excited to the 1s73s3S11s73s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s73s3S1​ level, $\ensuremath{\sim}80%$ were transferred to the n=70n=70n=70 circular state. At these high values of $n, \mathrm{\ensuremath{\Delta}}n=1$ circular-to-circular Rydberg state transitions occur at frequencies below 20 GHz. Consequently, atoms in these states, and the circular state preparation process presented here, are well suited to hybrid cavity QED experiments with Rydberg atoms and superconducting microwave circuits.
Helium atoms have been prepared in the circular $|n=55,\ensuremath{\ell}=54,{m}_{\ensuremath{\ell}}=+54\ensuremath{\rangle}$ Rydberg state using the crossed electric and magnetic fields method. The atoms, initially traveling in pulsed supersonic beams, were photoexcited from the metastable 1s2s3S11s2s\phantom{\rule{0.16em}{0ex}}^{3}S_{1}1s2s3S1​ level to the outermost, ${m}_{\ensuremath{\ell}}=0$ Rydberg-Stark state with n=55n=55n=55 in the presence of a strong electric field and weak perpendicular magnetic field. Following excitation, the electric field was adiabatically switched off causing the atoms to evolve into the circular state with ${m}_{\ensuremath{\ell}}=+54$ defined with respect to the magnetic-field quantization axis. The circular states were detected by ramped electric-field ionization along the magnetic-field axis. The dependence of the circular state production efficiency on the strength of the excitation electric field, and the electric-field switch-off time was studied, and microwave spectroscopy of the circular-to-circular $|55,54,+54\ensuremath{\rangle}\ensuremath{\rightarrow}|56,55,+55\ensuremath{\rangle}$ transition at $\ensuremath{\sim}38.5$ GHz was performed.
We report the first observation of hyperfine structure and isotope shift in autoionizing states. This structure was investigated in the $5{d}_{\frac{3}{2}}\mathrm{nf} J=4,5(n=36\ensuremath{-}40)$ barium Rydberg series, excited from the recently localized metastable $5{d}^{2}^{1}G_{4}$ level. An isotope-selective detection method was used in a cw laser spectroscopic experiment on a collimated atomic beam. The experimental data provide valuable additional information for the analyses of these doubly excited series.
The authors propose to prepare oriented circular Rydberg states in atoms (i.e. states where one valence electron has spherical quantum numbers: m=l=n-1>>1) by combining the specific advantages of the adiabatic crossed-field method, recently tested in alkali and alkaline earth atoms, and of the adiabatic RF field method whose principle was described in 1986. The formal equivalence of the two methods is pointed out. Their association is made possible by considering the dynamical symmetry of the Coulomb potential. In order to illustrate the new process, calculations have been performed for the manifold n=5 of hydrogen.