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Physical Review A

Negative-ion resonances in cross sections for slow-electron–heavy-alkali-metal-atom scattering

Cristian Bahrim, Uwe Thumm, I. I. Fabrikant

Published Mar 19, 2001• 36 citations
Publisher

Abstract

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 $R$-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 ${}^{3}{P}^{o}$ shape resonance and ${}^{3}{P}^{e},$ ${}^{1}{P}_{1}^{o},$ and ${}^{1}{D}_{2}^{o}$ 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.

DOI
10.1103/physreva.63.042710

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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 Rb\ensuremath−,{\mathrm{Rb}}^{\ensuremath{-}},Rb\ensuremath−, Cs\ensuremath−,{\mathrm{Cs}}^{\ensuremath{-}},Cs\ensuremath−, and Fr\ensuremath−{\mathrm{Fr}}^{\ensuremath{-}}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.
Based on the relativistic Dirac R-matrix method, we calculate angle-dependent and momentum-transfer cross sections for electron scattering by Rb, Cs, and Fr atoms at impact energies below 3 eV. Our results for momentum transfer for ${e}^{\ensuremath{-}}+\mathrm{Rb}$ and Cs collisions are compared with available data from swarm experiments. We find clear evidence for a ${\mathrm{Cs}}^{\ensuremath{-}}{(}^{3}{F}^{o})$ shape resonance at 1.528 eV, in excellent agreement with angle-dependent electron-scattering measurements. We analyze and compare the 3Fo{}^{3}{F}^{o}3Fo shape resonance in ${e}^{\ensuremath{-}}+\mathrm{Rb},$ Cs, and Fr elastic collisions.
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 calculate near-threshold photodetachment cross sections for ${\mathrm{Rb}}^{\ensuremath{-}},$ ${\mathrm{Cs}}^{\ensuremath{-}},$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ using the Pauli equation method with a model potential describing the effective electron-atom interaction. Parameters of the model potential are fitted to reproduce ab initio scattering phase shifts obtained from Dirac R-matrix calculations. Special care is taken to formulate the boundary conditions near the atomic nucleus for solving the Pauli equation, based on the analytic solution of the Dirac equation for a Coulomb potential. We find a 3P1o{}^{3}{P}_{1}^{o}3P1o​ resonance contribution to the photodetachment cross section of ${\mathrm{Rb}}^{\ensuremath{-}},$ ${\mathrm{Cs}}^{\ensuremath{-}},$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ ions. Our calculated total photodetachment cross sections for Cs agree with experiments after tuning the resonance position by 2.4 meV. For ${\mathrm{Rb}}^{\ensuremath{-}}$ and ${\mathrm{Fr}}^{\ensuremath{-}}$ the resonance contribution is much smaller than for Cs. We therefore also provide angle-differential cross sections and asymmetry parameters which are much more sensitive to the resonant contribution than total cross sections.
In a joint experimental and theoretical effort, we carried out a detailed study of electron scattering from Kr atoms in the energy range of the low-lying Feshbach resonances. Absolute angle-differential cross sections for elastic electron scattering were measured over the energy range 9.3–10.3 eV with an energy width of about 13 meV at scattering angles between 10° and 180°. Using several sets of elastic scattering phase shifts, a detailed analysis of the sharp resonance was carried out, resulting in a resonance width of Γ 3/2 = 3.6(2) meV. By direct comparison with the position of the resonance, the energy for the resonance was determined as E 3/2 = 9.489(3) eV. A Fano-type fit of the higher lying resonance yielded the resonance parameters Γ 1/2 = 33(5) meV and E 1/2 = 10.126(4) eV. In order to obtain additional insights, B -spline R -matrix calculations were performed for both the elastic and the inelastic cross sections above the threshold for excitation. They provide the total and angle-differential cross sections for excitation of long-lived and short-lived levels of the configuration in Kr and branching ratios for the decay of the resonance into the three available exit channels. The results are compared with selected experimental data.
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.