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Physical Review A

Negative-ion photodetachment in an electric field

Hin-Yiu Wong, A. R. P. Rau, Chris H. Greene

Published Apr 1, 1988• 59 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.37.2393

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s-wave photodetachment in a static electric field

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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.

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Strong-Field Photodetachment of Negative Ions – Orbital Alignment Effects and Tomographic Imaging of Photoelectrons

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Photoelectron imaging techniques are used to experimentally investigate photodetachment of negative ions in a strong laser-field as well as the orbital alignment dynamics in the residual neutral.\n\nStrong-field photodetachment in a linearly polarized pulsed laser with 100 fs pulse length is used to create a wave packet in the neutral atoms of carbon, germanium and silicon. The negative ions of these three atomic species are isoelectronic with a half-filled $p$-shell. The photodetachment rate is highly dependent on the magnetic quantum number $m_\\ell$ with the orbital with $m_\\ell = 0$ having a detachment rate of an order of magnitude larger than orbitals with $m_\\ell$ non-zero, with the polarization axis acting as a quantization axis. The residual neutral is thus left in an aligned state after photodetachment. The aligned state constitutes of a coherent superposition of fine-structure states and the population in the different orbitals will accordingly display a time-dependent spatial oscillation. The created wave packet is subsequently probed through photoionization by a second strong-field laser pulse.\n\nSecondly, a tomographic method is implemented to observe the three-dimensional distribution of photoelectrons produced in strong-field photodetachment processes. The method makes no assumptions of the existence of any symmetry axes in the photoelectron distribution and is thus applicable to any laser polarization ellipticity. Traditional imaging methods are dependent on the photoelectron distribution to be cylindrically symmetric by using either linearly or circularly polarized light, a requirement which can be lifted by using a tomographic technique. The method is applied to multiphoton detachment of the negative ion of silver.\n\nFinally, strong-field photodetachment of homonuclear diatomic negative ions is performed. The possibility of the additional electron being ejected from either of the two atomic centers can significantly alter the photoelectron distribution compared to an atomic negative ion with the same detachment energy. Experiments are performed on C$_2^-$, Si$_2^-$ and Ag$_2^-$ and compared to theoretical models.

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

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

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 ${\mathrm{Cs}}^{\ensuremath{-}}.$

Physical Review A•Dec 10, 2003•4 citations
A multichannel study of the photodetachment of a negative ion such as S\ensuremath−{\mathrm{S}}^{\mathrm{\ensuremath{-}}}S\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.
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.
Photoelectron imaging techniques are used to experimentally investigate photodetachment of negative ions in a strong laser-field as well as the orbital alignment dynamics in the residual neutral.\n\nStrong-field photodetachment in a linearly polarized pulsed laser with 100 fs pulse length is used to create a wave packet in the neutral atoms of carbon, germanium and silicon. The negative ions of these three atomic species are isoelectronic with a half-filled ppp-shell. The photodetachment rate is highly dependent on the magnetic quantum number $m_\\ell$ with the orbital with $m_\\ell = 0$ having a detachment rate of an order of magnitude larger than orbitals with $m_\\ell$ non-zero, with the polarization axis acting as a quantization axis. The residual neutral is thus left in an aligned state after photodetachment. The aligned state constitutes of a coherent superposition of fine-structure states and the population in the different orbitals will accordingly display a time-dependent spatial oscillation. The created wave packet is subsequently probed through photoionization by a second strong-field laser pulse.\n\nSecondly, a tomographic method is implemented to observe the three-dimensional distribution of photoelectrons produced in strong-field photodetachment processes. The method makes no assumptions of the existence of any symmetry axes in the photoelectron distribution and is thus applicable to any laser polarization ellipticity. Traditional imaging methods are dependent on the photoelectron distribution to be cylindrically symmetric by using either linearly or circularly polarized light, a requirement which can be lifted by using a tomographic technique. The method is applied to multiphoton detachment of the negative ion of silver.\n\nFinally, strong-field photodetachment of homonuclear diatomic negative ions is performed. The possibility of the additional electron being ejected from either of the two atomic centers can significantly alter the photoelectron distribution compared to an atomic negative ion with the same detachment energy. Experiments are performed on C2−_2^-2−​, Si2−_2^-2−​ and Ag2−_2^-2−​ and compared to theoretical models.
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.
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.
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 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 ${\mathrm{Cs}}^{\ensuremath{-}}.$