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Journal of Physics B Atomic Molecular and Optical Physics

Polarization effects in two-colour photodetachment of negative ions

Wilhelm Becker, Li-E Li, John K. McIver

Published Nov 28, 1990• 10 citations
Publisher

Abstract

Two-colour photodetachment of a negative ion modelled by a three-dimensional delta-function potential is theoretically investigated. The high-frequency low-intensity field is closely tuned to the detachment energy of the ion, the low-frequency high intensity field creates a ponderomotive potential of 2.6% of the detachment energy and at the same time sidebands. The two fields are circularly polarized with either equal or opposite polarizations. In accordance with the Wigner threshold law, for equal and opposite polarizations, the sideband-induced thresholds are above or below the one-photon detachment threshold, respectively. The one-photon threshold is markedly visible for opposite polarizations at the position shifted by the full ponderomotive potential. For equal polarizations and low frequencies it is not noticeable at all.

DOI
10.1088/0953-4075/23/22/004

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Physical Review A•Apr 1, 1988•59 citations
Two-colour photodetachment of a negative ion modelled by a three-dimensional delta-function potential is theoretically investigated. The high-frequency low-intensity field is closely tuned to the detachment energy of the ion, the low-frequency high intensity field creates a ponderomotive potential of 2.6% of the detachment energy and at the same time sidebands. The two fields are circularly polarized with either equal or opposite polarizations. In accordance with the Wigner threshold law, for equal and opposite polarizations, the sideband-induced thresholds are above or below the one-photon detachment threshold, respectively. The one-photon threshold is markedly visible for opposite polarizations at the position shifted by the full ponderomotive potential. For equal polarizations and low frequencies it is not noticeable at all.
A polarization dependence of a two-colour two-photon detachment cross section has been observed and calculated for the first time. In a Penning ion trap, electrons were detached from Cl - by an intense infrared laser beam at 1064 nm and a weak ultraviolet laser beam at 343 nm. Both beams were circularly polarized. The ratio of the two-colour two-photon cross section for photons with the same circular polarization to that for photons with opposite circular polarization was measured to be 1.085 +0.012 -0.007 . Also presented is a simple calculation of the ratio, the result of which is consistent with the observation.
The behavior of near-threshold cross sections for dissociation of a target into a pair of particles, as described by Wigner's threshold law, can depend sensitively on the angular momentum of the particles. In this Letter, we investigate the near-threshold nonresonant two-photon detachment process in the negative ion of gold. The expected s-wave threshold behavior is observed with linearly polarized light. Closure of the s-wave channel is realized by using circular polarization, allowing the first observation of a d-wave threshold. Practical applications are discussed, including extensions which could prove valuable for investigations of negative ions with near-threshold structure.
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.
We show that by using the approximation method of Bivona et al , two-colour photodetachment cross sections are obtained that behave according to the Wigner threshold law even if the dressing effect of the low-frequency radiation field on the bound state is ignored. Within the range of the low frequency and intensity of the radiation field considered, it is found that the values of the cross sections calculated by using the field-free bound state are not significantly modified when the corrections to the wavefunction of the bound state due to the driving action of the low-frequency field are accounted for.
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.