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Physical Review A

Temporary negative-ion states of Na, K, Rb, and Cs

A. R. Johnston, P. D. Burrow

Published Jan 1, 1995• 16 citations
Publisher

Abstract

Electron-transmission spectroscopy is used to observe structure in the electron-scattering cross section associated with the formation of temporary negative ions and channel-opening effects. A strong ``family'' resemblance is apparent among the resonances of the alkali metals. From published calculations and angular scattering studies, the lower-lying features are known with some confidence. Based on these, plausible assignments for some of the higher-lying resonances are put forth. We propose that the absence of resonances near the Cs 5 $^{2}$D and possibly the Na 4 $^{2}$P and 5 $^{2}$P thresholds is associated with the negative polarizabilities of these excited states.

DOI
10.1103/physreva.51.406

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Scientific Herald of Uzhhorod University Series Physics•Nov 25, 2013•0 citations
Electron-transmission spectroscopy is used to observe structure in the electron-scattering cross section associated with the formation of temporary negative ions and channel-opening effects. A strong ``family'' resemblance is apparent among the resonances of the alkali metals. From published calculations and angular scattering studies, the lower-lying features are known with some confidence. Based on these, plausible assignments for some of the higher-lying resonances are put forth. We propose that the absence of resonances near the Cs 5 2^{2}2D and possibly the Na 4 2^{2}2P and 5 2^{2}2P thresholds is associated with the negative polarizabilities of these excited states.
Two techniques have been used to study low energy electron scattering processes in the alkali metals. A transmission experiment was used to search for resonance structure in the total scattering cross section of sodium, potassium, rubidium, and cesium. A shape resonance was observed in sodium at 0.08 (+OR-) 0.03 eV. In rubidium, evidence was found for the existence of a shape resonance below 0.05 eV. No shape resonance structure was observed in potassium or cesium for energies above 0.1 eV. For energies near the first excited state to near the lowest ionization potential, a progression of Feshbach resonances was observed in each atom. The graphical analysis technique of Spence was used to group most of these resonances into seven families. An analysis is given of the mechanisms affecting the rejection of scattered electrons in the transmission spectrometer. A quantitative description of two modes of operation of the spectrometer is presented. The second portion of this dissertation concerns the measurement of the near-threshold excitation and ionization cross sections in sodium, potassium, and rubidium. A trapped-electron experiment was used to make a relative measurement of these cross sections. The shapes of the excitation cross sections are, in general, somewhat different from other experimental work but are in good agreement with the close-coupling calculations of Moores and Norcross. The shapes of the ionization cross sections are in reasonable agreement with previous work. The ratio of the excitation cross section at 2.5 eV in sodium, 2.0 eV in potassium, and 1.8 eV in rubidium to the respective ionization cross section at the first peak was measured and found to be 3.9 (+OR-) 13% in Na, 5.8 (+OR-) 10% in K, and 6.4 (+OR-) 13% in Rb. These ratios are generally larger than those derived from independent values of the individual cross sections. An analysis of several systematic effects associated with the measurement of the cross section ratio was made. Results from this analysis were used to correct the measured excitation cross section for effects of the elastically scattered electrons.
We analyze negative-ion resonances in elastic and inelastic total scattering cross sections for slow electron collisions with the heavy-alkali-metal atoms Rb, Cs, and Fr. Our calculations are based on the Dirac RRR-matrix method [Thumm and Norcross, Phys. Rev. A 45, 6349 (1992)]. For incident electrons of up to 2.8 eV kinetic energy, we compare a 3Po{}^{3}{P}^{o}3Po shape resonance and 3Pe,{}^{3}{P}^{e},3Pe, 1P1o,{}^{1}{P}_{1}^{o},1P1o​, and 1D2o{}^{1}{D}_{2}^{o}1D2o​ Feshbach resonances, located below the first excitation threshold of the atomic target in the low-lying spectra of the ${\mathrm{Rb}}^{\ensuremath{-}},$ ${\mathrm{Cs}}^{\ensuremath{-}},$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ negative ions, with available experimental data and other calculations. We provide the resonance parameters, partial and converged total elastic and inelastic scattering cross sections, and discuss the relative importance of relativistic effects for the three heavy-alkali-metal targets.
Our Dirac R-matrix calculations suggest that none of the heavy alkali-metal negative ions, Rb, Cs, and Fr, has an excited bound state. Their lowest excited state appears to be a multiplet of 3PJo{}^{3}{P}_{J}^{o}3PJo​-shape resonances, the J=1J=1J=1 component of which was recently observed in photodetachment experiments on ${\mathrm{Cs}}^{\ensuremath{-}}.$ We analyze these 3PJo{}^{3}{P}_{J}^{o}3PJo​ and the 3Se{}^{3}{S}^{e}3Se excited negative ion states in partial and converged total scattering cross sections for slow electrons with incident kinetic energies below 120 meV. Our results are in excellent agreement with available experimental data. We also propose a new value for the electron affinity of Fr, provide the scattering length for electronic collisions with Rb, Cs, and Fr, and discuss the nuclear charge dependence of relativistic effects in the resonance profiles.
Studies of electron transmission through Ca vapor reveal two prominent resonances in the range 0--4 eV. The energies and widths of these temporary anion states suggest that they may be assigned to the strongly mixed (4${s}^{2}3d3d3d{)}^{2}Dand(4s4D and (4s4Dand(4s4{p}^{2}$)2{)}^{2})2D states of ${\mathrm{Ca}}^{\mathrm{\ensuremath{-}}}$. This interpretation is supported by ab initio configuration-interaction calculations and is consistent with previously unassigned structure observed in the photodetachment cross section.
We have measured the relative optical-excitation functions and polarizations of the K, Rb, and Cs resonance lines, using crossed electron and atom beams, for electron energies from threshold to 1500 eV. The electron energy resolution was \ensuremath{\sim}0.25 eV for energies below 13 eV, and the atom beam was optically thin. The atomic resonance-level (n2P{n}^{2}Pn2P) excitation functions have been normalized to the Born theory in the high-energy limit. Comparisons are made with other measurements and calculations. The polarizations and total cross sections for H, Li, Na, K, Rb, and Cs are also compared with each other in reduced units to investigate systematic behavior.
In the work, the main results on excitation and decay processes of autoionizing states in alkali atoms are considered. As follows from the data on excitation dynamics of subvalence shells in an impact energy region from the lowest excitation threshold up to 600 eV, at threshold energies their electron excitation results exclusively from the formation of negative-ion resonances. At mean impact energies, the cascade population processes due to resonance excitation and subsequent radiative decay of the upper states play an essential role for the low-lying autoionizing states. By comparing with theoretical data, the absolute excitation cross sections for autoionizing states and negative-ion resonances were determined. The absolute autoionization cross sections as well as the autoionization contribution to the total single ionization cross section were also determined. Keywords: atom, ion, autoionization, resonances, ionization, effective cross section.