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Journal of Physics B Atomic Molecular and Optical Physics

High-lying long-lived doubly excited states near ionization thresholds of helium

Emma J. Sokell, A A Wills, P. R. Hammond, Michael A. MacDonald, M. K. Odling-Smee

Published Dec 28, 1996• 27 citations
Publisher

Abstract

Long-lived, excited neutral particles, arising from the interaction of monochromatic synchrotron radiation with ground state He atoms, have been observed at photon energies close to the (N = 1,2,3 and 4) ionization thresholds. The measurements have been made using an unconventional experimental arrangement in which charged particles, responsible for the dominant signal in conventional photon impact studies, are prevented from reaching the detector. For , it appears that the formation, via photoexcitation, of relatively long-lived, doubly excited Rydberg states is a necessary step in the production of the observed signal. Four processes that might account for the production of the excited neutral particles are considered. The simplest, that atoms in the initial doubly excited Rydberg states are themselves directly observable, is considered unlikely. However, the lifetimes of the photoexcited double Rydberg states may be increased through the effects of electric fields present in the apparatus. Transitions from these double Rydberg states, occurring either as a result of collisions or by fluorescence, could result in metastable, singly excited neutral particles. The presence of signal related to the existence of long-lived doubly excited states could be significant in the interpretation of other photon impact measurements.

DOI
10.1088/0953-4075/29/24/002

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Bulletin of the American Physical Society•Jan 1, 2000•0 citations
Long-lived, excited neutral particles, arising from the interaction of monochromatic synchrotron radiation with ground state He atoms, have been observed at photon energies close to the (N = 1,2,3 and 4) ionization thresholds. The measurements have been made using an unconventional experimental arrangement in which charged particles, responsible for the dominant signal in conventional photon impact studies, are prevented from reaching the detector. For , it appears that the formation, via photoexcitation, of relatively long-lived, doubly excited Rydberg states is a necessary step in the production of the observed signal. Four processes that might account for the production of the excited neutral particles are considered. The simplest, that atoms in the initial doubly excited Rydberg states are themselves directly observable, is considered unlikely. However, the lifetimes of the photoexcited double Rydberg states may be increased through the effects of electric fields present in the apparatus. Transitions from these double Rydberg states, occurring either as a result of collisions or by fluorescence, could result in metastable, singly excited neutral particles. The presence of signal related to the existence of long-lived doubly excited states could be significant in the interpretation of other photon impact measurements.
Doubly excited states below the N=2N=2N=2 ionization threshold are populated by exciting helium atoms in a supersonic beam with monochromatized synchrotron radiation. The fluorescence decay of these states triggers a radiative cascade back to the ground state with large probability to populate long lived singlet and triplet helium metastable states. The yield of metastables is measured using a multichannel plate detector after the beam has passed a singlet-quenching discharge lamp. The variation of the yield observed with the lamp switched on or off is related to the triplet-singlet mixing of the doubly excited states.
Rydberg atoms are increasingly being used as a means of introducing long-range, tunable interactions into atomic systems through their strong dipole-dipole interactions. When creating such interactions, however, there are a variety of potential effects that can occur, such as state (n and/or L) changing or Penning ionization, which can complicate the dynamics of the system. In the following work, such interactions are investigated for Rydberg-Rydberg collisions using very high-n, n ~300, strontium Rydberg atoms in an atomic beam configuration. By exploiting Rydberg blockade and the inherent distribution of atomic velocities present in an atomic beam, it is possible to create a 1D array of moving Rydberg atoms which will naturally overtake each other over time. Measurements of both Penning ionization and state changing for such collisions are made and compared with classical trajectory Monte-Carlo (CTMC) simulations, with both indicating large collisional cross sections on the order of 1 x 10-6 cm2 for Penning ionization and nearly 8 x 10-5 cm2 for state changing interactions. In a second series of experiments, previous work involving doubly-excited Rydberg states is expanded upon by investigating autoionization with high-n, L > 3, Rydberg states. Past research involving autoionization has shown that the effect is strongly L-dependent, with high-L states having significantly smaller autoionizing rates. To create well-defined, L > 3 states, the use of microwave fields to drive various high-n, n ~ 150, n1F3 → (n+1)1G4, (n+2)1H5 transitions is investigated, with spectroscopic measurements of these transitions providing quantum defect values for n1G4 and n1H5 states. These measurements provide a basis for future studies into the L-dependence of high-n, n ~ 300, autoionizing Rydberg atoms, with the eventual goal of creating a long-lived, doubly-excited “planetary” Rydberg state.
The asymmetry parameter β for fluorescence photons emitted during the radiative decay of the sp2, n +( 1 P o ), sp2, n −( 1 P o ), 2p n d( 1 P o ) and 2p n d( 3 D o ) series of helium doubly excited states, formed by the absorption of linearly polarized synchrotron radiation, has been measured. The results are compared with recent theoretical calculations (Žitnik et al 2002 Phys. Rev. A 65 032520). At high n the β parameter is shown to increase and oscillate due to the excitation of triplet states, optically accessible from the helium ground state due to spin–orbit effects.
Highly excited (Rydberg) atoms are produced and can exist for significant periods of time in various plasma environments. It is necessary to know cross sections for the various collision processes involving these atoms if a complete understanding of the physics of these environments is to be attained.\nThe experimental investigation of collisional phenomena between high Rydberg sodium atoms and electrons is described in this thesis. A fraction of the atoms in a ground state sodium beam is optically excited (using lasers) to well-defined, high Rydberg states (principal quantum numbers chosen around 40). Subsequent to their production the Rydberg atoms are allowed to interact with 25 eV electrons for a specified time interval following which the collision products are detected. The electrons are produced in a beam which is crossed at right angles with the sodium beam. Important collision processes are (1) electron impact ionization of the Rydberg atom, and (2) electron-Rydberg atom interactions in which the quantum state of the atom is changed (state changing collisions).\nResults are presented for an observed state changing process which is identified as angular momentum state changing only (no change in the value of the principal quantum number). Cross sections for this process are measured to be 10('-10) to 10('-9) cm('2). Problems encountered during the work which prevented the measurement of electron impact ionization cross sections are discussed. In the course of the work two other topics required study: (1) the process of electric field ionization of Rydberg atoms (used to detect the atoms), and (2) the effects of background (300 K) radiation (from the chamber walls, for example) on Rydberg atoms. Results of these studies are also presented.
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.
There is considerable interest in the dynamics of ultracold plasmas and ultracold Rydberg gases. Ultracold plasmas are typically formed by photo-excitation of ultracold atoms to an energy region near (both above and below) an ionization threshold. Excitation to bound, highly-excited Rydberg states can lead to formation of a plasma via several processes, including collisions between Rydberg atoms. Three-body recombination in an ultracold plasma can also result in the production of ultracold Rydberg atoms. Understanding the dynamics of ultracold Rydberg gases is therefore important for understanding the dynamics of ultracold plasmas. In this dissertation, we have investigated the formation and survival of a particular class of Rydberg atoms. These atoms are known as ZEKE state Rydberg atoms, where the term ZEKE is derived from "Zero Kinetic Energy." ZEKE Rydberg states are high angular momentum and high angular momentum projection excited states which can be formed by laser excitation in the presence of electric fields. Without the electric fields, these states would be optically dark. We have investigated ZEKE Rydberg states in ultracold argon in an energy region just below the second ionization threshold of the atoms in our magneto-optical trap. Here, low angular momentum states decay very quickly (< 1 ns) by auto-ionization through a core spin flip due to the Rydberg electron-core interaction. This interaction has been significantly reduced due to the dilution of low l and m states as a result of l and m mixing during excitation. Hence, ZEKE Rydberg states live orders of magnitude longer than low angular momentum states. We are reporting on our experimental investigation of these states in the ultracold regime and prospects for future studies in which external control of these states may be used to control ultracold plasma dynamics.