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Europhysics Letters (EPL)

Threshold behaviour in photodetachment into a final state with large negative polarizability

Johan Rohlén, Anton O. Lindahl, Hannes Hultgren, Richard Thomas, D. J. Pegg, D. Hanstorp

Published May 30, 2014• 5 citations
Publisher

Abstract

In a recent experiment, Lindahl et al. ( Lindahl A. O. et al. , Phys. Rev. Lett. , 108 (2012) 033004) observed a new threshold behavior in the photodetachment of the potassium negative ion when the residual atom is left in the state. Unfortunately the resonance close to threshold made it more difficult to apply the semi-classical model that was developed to describe the threshold behavior. In this paper we present a study of the threshold behavior of the partial cross-section in the photodetachment of the sodium negative ion. The experiment was conducted using a collinear beams apparatus where the detection was performed using a resonance ionization scheme. We observe the same threshold behavior as in the previous experiment, but without any obfuscating resonance. The model derived in the previous paper is found to fit the observed cross-section up to 35 meV above threshold. The present experiment clearly demonstrates the threshold behaviour for the fundamental process of a free electron moving in the field of an atom with a large negative polarizability.

DOI
10.1209/0295-5075/106/53001

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In a recent experiment, Lindahl et al. ( Lindahl A. O. et al. , Phys. Rev. Lett. , 108 (2012) 033004) observed a new threshold behavior in the photodetachment of the potassium negative ion when the residual atom is left in the state. Unfortunately the resonance close to threshold made it more difficult to apply the semi-classical model that was developed to describe the threshold behavior. In this paper we present a study of the threshold behavior of the partial cross-section in the photodetachment of the sodium negative ion. The experiment was conducted using a collinear beams apparatus where the detection was performed using a resonance ionization scheme. We observe the same threshold behavior as in the previous experiment, but without any obfuscating resonance. The model derived in the previous paper is found to fit the observed cross-section up to 35 meV above threshold. The present experiment clearly demonstrates the threshold behaviour for the fundamental process of a free electron moving in the field of an atom with a large negative polarizability.
We report on the first experimental observation of a new threshold behavior observed in the 5(2)G partial channel in photodetachment of K(-). It arises from the repulsive polarization interaction between the detached electron and the residual K(5(2)G) atom, which has a large negative dipole polarizability. In order to account for the observation in the K(5(2)G) channel, we have developed a semiclassical model that predicts an exponential energy dependence for the cross section. The measurements were made with collinear laser-ion beams and a resonance ionization detection scheme.
The effect of final-state interactions on the photodetachment cross section of negative ions in a magnetic field is discussed. Experiments on the location of the 2P32^{2}P_{\frac{3}{2}}2P23​​ threshold in ${\mathbf{S}}^{\ensuremath{-}}$ as a function of magnetic field show clearly the effect of the zero-point energy of an electron in a magnetic field. The experiments also give a precise value for the electron affinity and provide information about the interaction between the atom and the detached electron.
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 collinear beam apparatus has been used to study photodetachment of Cs${}^{\ensuremath{-}}$. Partial cross sections were measured using state-selective detection based on a resonance ionization scheme. Several resonances were observed in the Cs(102S10{\phantom{\rule{0.16em}{0ex}}}^{2}S102S), Cs(62F6{\phantom{\rule{0.16em}{0ex}}}^{2}F62F), Cs(62G6{\phantom{\rule{0.16em}{0ex}}}^{2}G62G), and Cs(62H6{\phantom{\rule{0.16em}{0ex}}}^{2}H62H) final-state channels below the Cs(102P10{\phantom{\rule{0.16em}{0ex}}}^{2}P102P3/2{}_{3/2}3/2​) channel opening. A model was developed to account for the interference between overlapping resonances. This model is essentially a generalization of the Fano [U. Fano, Phys. Rev. 124, 1866 (1961)] and Shore [B. W. Shore, Phys. Rev. 171, 43 (1968)] parametrizations for single resonances. Resonance parameters were extracted by fitting the model to the data sets. The openings of the Cs(102S10{\phantom{\rule{0.16em}{0ex}}}^{2}S102S) and Cs(62F6{\phantom{\rule{0.16em}{0ex}}}^{2}F62F) channels, where the polarizabilities of the atomic states are large and positive, showed rapid onsets. In the case of the Cs(62G6{\phantom{\rule{0.16em}{0ex}}}^{2}G62G) and Cs(62H6{\phantom{\rule{0.16em}{0ex}}}^{2}H62H) channels, on the other hand, the photodetachment cross sections increased slowly with energy. For the Cs(62H6{\phantom{\rule{0.16em}{0ex}}}^{2}H62H) channel this is the expected behavior, since it is the result of a large and negative polarizability of the 62H6{\phantom{\rule{0.16em}{0ex}}}^{2}H62H state. In addition, the excitation of the Cs(62H6{\phantom{\rule{0.16em}{0ex}}}^{2}H62H) state with respect to the Cs ground state was found to be 28 356.3(2) ${\mathrm{cm}}^{\ensuremath{-}1}$, in agreement with a previous experiment.
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.