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Physical Review A

Static electric-field effects in the photodetachment of Cs− at the 3P resonance region

A.A. Khuskivadze, I. I. Fabrikant, Uwe Thumm

Published Dec 10, 2003• 4 citations
Publisher

Abstract

We calculated near-threshold photodetachment cross sections for ${\mathrm{Cs}}^{\ensuremath{-}}$ in the presence of a dc electric field using three different approaches: the frame-transformation method with and without rescattering effects and the Kirchhoff-integral approach. Radial wave functions for the electronic motion were obtained using the Pauli equation method with a model potential describing the effective electron-atom interaction. Our results demonstrate the inadequacy of the frame-transformation method in the ${}^{3}P$ resonance region even for weak fields $(E<10\mathrm{k}\mathrm{V}/\mathrm{c}\mathrm{m}).$ We show that the triplet and singlet contributions to the total cross section can be manipulated by varying the external electric field. This can enhance spin-orbit effects in the photodetachment process and create more favorable conditions in the experiment for the observation of the lowest ${}^{3}P$ resonance in ${\mathrm{Cs}}^{\ensuremath{-}}.$

DOI
10.1103/physreva.68.063405

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We calculated near-threshold photodetachment cross sections for Cs\ensuremath−{\mathrm{Cs}}^{\ensuremath{-}}Cs\ensuremath− in the presence of a dc electric field using three different approaches: the frame-transformation method with and without rescattering effects and the Kirchhoff-integral approach. Radial wave functions for the electronic motion were obtained using the Pauli equation method with a model potential describing the effective electron-atom interaction. Our results demonstrate the inadequacy of the frame-transformation method in the 3P{}^{3}P3P resonance region even for weak fields (E<10kV/cm).(E<10\mathrm{k}\mathrm{V}/\mathrm{c}\mathrm{m}).(E<10kV/cm). We show that the triplet and singlet contributions to the total cross section can be manipulated by varying the external electric field. This can enhance spin-orbit effects in the photodetachment process and create more favorable conditions in the experiment for the observation of the lowest 3P{}^{3}P3P resonance in Cs\ensuremath−.{\mathrm{Cs}}^{\ensuremath{-}}.Cs\ensuremath−.
We 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 then integrate the Pauli equation using an effective potential that is adjusted to reproduce Dirac R-matrix scattering phase shifts, and find the (3)P(o)(1) resonance contribution to the photodetachment cross section of Cs-. Our photodetachment cross sections agree with recent experiments by Scheer et al. [Phys. Rev. Lett. 80, 684 (1998)] after tuning the resonance position by 2.4 meV. We also provide angle-differential photodetachment cross sections and the corresponding asymmetry parameter beta near the Cs(6s) threshold.
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.
Photodetachment from negative ions in a static electric field has been studied using ${\mathrm{Cl}}^{\mathrm{\ensuremath{-}}}$ and ${\mathrm{S}}^{\mathrm{\ensuremath{-}}}$. These experiments were done with greater precision than previous studies and allow a quantitative comparison of data with theory. A 10-keV ion beam was sent through a region with fields of up to 1.5 kV/cm applied parallel to the beam velocity. A pulsed dye-laser beam, perpendicular to the ion beam, photoneutralized the ions. The relative cross sections were measured by detecting the resulting fast neutral atoms. Detachment below threshold and oscillations on the cross section above threshold were observed near the ${\mathrm{S}}^{\mathrm{\ensuremath{-}}}$ threshold at 16 269.5 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ and near the ${\mathrm{Cl}}^{\mathrm{\ensuremath{-}}}$ threshold at 29 138.3 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. The phase of the oscillations in the data is in good agreement with predictions for s-wave photodetachment in a static electric field, but the amplitude of the oscillations is found to be slightly reduced.
A multichannel study of the photodetachment of a negative ion such as ${\mathrm{S}}^{\mathrm{\ensuremath{-}}}$ in the presence of a constant electric field is presented. The analysis is carried out as a series of frame transformations for the outgoing photoelectron. An earlier analysis in the absence of the external field is now augmented by the further transformations from spherical to cylindrical symmetry that are required. The interplay between the various thresholds due to fine structure in the negative ion and residual atom and the effects of the external field are analytically treated. The net effect is to eliminate the thresholds, to induce modulations in the detachment cross section, and to introduce field-assisted-tunneling contributions to the photodetachment. Numerical illustrations are provided. Our treatment closely parallels similar treatments of photoionization of neutral atoms in an electric field and of photodetachment in a magnetic field.
We have implemented an integrable method with B-spline basis which allows us to calculate photodetachment cross sections of the ion in the presence of a constant electric field. The behaviour of the Feshbach resonances lying below the N = 2 and N = 3 thresholds is analysed in detail. Further insight on the relative importance of autoionization and tunnelling is provided by using a stabilization procedure. Our results permit us to explain most of the experimental findings and show the existence of resonance structures previously unobserved.
An analytic momentum-space wave function for an electron in both laser and static uniform electric fields is presented. It is used to obtain analytic multiphoton detachment cross sections in a static, uniform electric field which include effects of static-field-induced electron-photon interactions. These general results are not restricted to weak laser intensities or to weak static-field strengths and depend only on (a) the electric dipole approximation and (b) the approximation that final-state electron-atom interactions are ignored. Four specific predictions of our general formulas for the most interesting case of linearly polarized light polarized along the static-field direction are presented for weakly bound electrons initially in an s state. First, the effects of a weak static electric field on N-photon detachment cross sections near threshold are shown to be described by two modulation factors, one for odd N and one for even N, which depend only on a scaled energy. Second, for photodetachment in a static electric field, effects of static-field-induced electron-photon interactions are demonstrated. Third, the lifetime against field ionization is presented. Fourth, the cross section for electric-field-induced stimulated emission is presented. Numerical results for the latter three effects are presented for the ${\mathrm{H}}^{\mathrm{\ensuremath{-}}}$ ion. The simpler case of circularly polarized light directed along the static-electric-field direction is treated briefly. In particular, we show for this case that the static- and laser-field effects are uncoupled and that the near-threshold, weak static-electric-field modulation factors for the N-photon detachment cross sections are dependent on N.