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Physical Review A

Studies of xenon atoms in high Rydberg states

R. F. Stebbings, Colin J. Latimer, W.P. West, F. B. Dunning, T. B. Cook

Published Oct 1, 1975• 155 citations
Publisher

Abstract

Thermal beams of xenon atoms in single high Rydberg states have been produced by photoexcitation of $\mathrm{Xe}(^{3}P_{0})$ metastable atoms. The highly excited states which were populated in this way were identified as $\mathrm{np}{[\frac{1}{2}]}_{1}$ with $11\ensuremath{\le}n\ensuremath{\le}16$ and $\mathrm{nf}{[\frac{3}{2}]}_{1}$ with $8\ensuremath{\le}n\ensuremath{\le}40$. The field ionization characteristics and radiative lifetimes of these atoms have been studied.

DOI
10.1103/physreva.12.1453

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Thermal beams of xenon atoms in single high Rydberg states have been produced by photoexcitation of Xe(3P0)\mathrm{Xe}(^{3}P_{0})Xe(3P0​) metastable atoms. The highly excited states which were populated in this way were identified as np[12]1\mathrm{np}{[\frac{1}{2}]}_{1}np[21​]1​ with 11\ensuremath≤n\ensuremath≤1611\ensuremath{\le}n\ensuremath{\le}1611\ensuremath≤n\ensuremath≤16 and nf[32]1\mathrm{nf}{[\frac{3}{2}]}_{1}nf[23​]1​ with 8\ensuremath≤n\ensuremath≤408\ensuremath{\le}n\ensuremath{\le}408\ensuremath≤n\ensuremath≤40. The field ionization characteristics and radiative lifetimes of these atoms have been studied.
We have excited helium atoms from their metastable 2 3S{}^{3}\phantom{\rule{-0.16em}{0ex}}S3S state to Rydberg states in the range 13<n<5013<n<5013<n<50 in a two-step process via the 3 3P{}^{3}\phantom{\rule{-0.16em}{0ex}}P3P state using light at $\ensuremath{\lambda}=389$ nm and 785--815 nm. Atoms in a thermal beam (100 K) cross partially overlapping laser beams of the appropriate frequencies in the counterintuitive order to exploit the high efficiency of stimulated rapid adiabatic passage. The interaction region is between two plates that can be used for Stark tuning in a few V/cm field or for field ionization. At fields much too low for field ionization, we observe signals attributed to ionization by blackbody radiation. Multiple tests confirm this attribution as the cause of ionization. For example, by heating the plates we observe the expected signal increases. Our experiments reinforce previous work where the interaction between Rydberg atoms and room temperature blackbody radiation is important for experiments.
Neutral Rydberg state excitation in strong UV laser fields of Xe atoms has been studied and compared with direct ionization. The yields of both strong-field excitation and ionization have been measured as a function of UV laser intensity and ellipticity. The underlying physical mechanism has been discussed based on the experimental results, indicating that the Rydberg states are populated via multi-photon resonance excitation in strong 400 nm laser fields. Finally, a comparative study of Xe and O2O_2O2​ with similar ionization potentials have been performed, showing the suppressed excitation of molecules in strong UV laser fields.
We have studied the Stark effect for the bound Rydberg states of xenon (2{(}^{2}(2P3/2{\mathrm{P}}_{3/2}P3/2​ core) in the vicinity of n=17. These are the first detailed measurements of Rydberg-state Stark structure in a heavy rare-gas atom. The experiment was performed by one-photon laser spectroscopy from the metastable 6s'[(1/2)]0{[(1/2)]}_{0}[(1/2)]0​ state in an atomic beam. Laser polarization can be chosen to excite pure M=0 or \ensuremath{\Vert}M\ensuremath{\Vert}=1 levels. Stark maps are presented for electric fields from 0 to 2000 V/cm. The major low-field features are a prominent linear manifold for states with l\ensuremath{\ge}3 and an isolated group of states arising from mixing within the overlapping p and d terms. A simple model of the p,d complex, showing strong mixing at fields as low as 200 V/cm, is used to correlate observed states with the zero-field states. The spectra become exceedingly complex for fields greater than 1000 V/cm because of mixing within the extensive fine structure of xenon.
The production of very-high-nnn ($n\ensuremath{\sim}300$--500) strontium Rydberg atoms is explored using a crossed-laser-atom-beam geometry. nnn1S0{}^{1}{S}_{0}1S0​ and nnn1D2{}^{1}{D}_{2}1D2​ states are created by two-photon excitation via the 5s5p5s5p5s5p 1P1{}^{1}{P}_{1}1P1​ intermediate state using radiation with wavelengths of $\ensuremath{\sim}$461 and $\ensuremath{\sim}$413 nm. Rydberg atom densities as high as $\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{5}$ cm${}^{\ensuremath{-}3}$ have been achieved, sufficient that Rydberg-Rydberg interactions can become important. The isotope shifts in the Rydberg series limits are determined by tuning the 461-nm light to preferentially excite the different strontium isotopes. Photoexcitation in the presence of an applied electric field is examined. The initially quadratic Stark shift of the nnn1P1{}^{1}{P}_{1}1P1​ and nnn1D2{}^{1}{D}_{2}1D2​ states becomes near-linear at higher fields and the possible use of n1D2n{}^{1}{D}_{2}n1D2​ states to create strongly polarized, quasi-one-dimensional electronic states in strontium is discussed. The data are analyzed with the aid of a two-active-electron (TAE) approximation. The two-electron Hamiltonian, within which the Sr2+{}^{2+}2+ core is represented by a semi-empirical potential, is numerically diagonalized allowing the calculation of the energies of high-nnn Rydberg states and their photoexcitation probabilities.
Rydberg states of atomic helium with principal quantum numbers ranging from n=20n=20n=20 to n=100n=100n=100 have been prepared by non-resonance-enhanced single-color two-photon excitation from the metastable 23S12\phantom{\rule{0.16em}{0ex}}{{}^{3}S}_{1}23S1​ state. Photoexcitation was carried out using linearly and circularly polarized pulsed laser radiation. In the case of excitation with circularly polarized radiation, Rydberg states with azimuthal quantum number $|{m}_{\ensuremath{\ell}}|=2$ were prepared in zero electric field and in homogeneous electric fields oriented parallel to the propagation axis of the laser radiation. In sufficiently strong electric fields, individual Rydberg--Stark states were resolved spectroscopically, highlighting the suitability of non-resonance-enhanced multiphoton excitation schemes for the preparation of long-lived high-$|{m}_{\ensuremath{\ell}}|$ hydrogenic Rydberg states for deceleration and trapping experiments. Applications of similar schemes for Doppler-free excitation of positronium atoms to Rydberg states are also discussed.