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Physical Review A

Threshold effects and photoelectron spectra in model-system descriptions of photodetachment

Stanley L. Haan, P. A. Polstra, W. H. Schotanus, E. Van Timmeren

Published Nov 1, 1992• 2 citations
Publisher

Abstract

Near-threshold single-photon photodetachment processes are considered for simple model systems representing negative ions exposed to monochromatic radiation. The model systems considered feature an initial discrete state, the photoelectron continuum, and in some cases an excited or autodetaching discrete state. Population trapping through the formation of a bound dressed state and the photoelectron spectra are examined. Two photoelectron spectra are defined : a primary spectrum which results from decay while the laser interaction is on and a secondary spectrum which results from the destabilization of the bound dressed state if the interaction is turned off again. Careful attention is given to the passage of the poles of the Green's operator through the low-energy boundary of a continuum, and it is concluded that such poles move nonmonotonically through the boundary of an s-wave continuum, but monotonically through the boundary of a p-wave or higher-l-wave continuum. Two example systems, one featuring a single discrete state and an s-wave continuum and one featuring two discrete states and a p-wave continuum, are considered in detail.

DOI
10.1103/physreva.46.5600

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arXiv:2010.01122•Physical Review A•Oct 13, 2020•3 citations
Near-threshold single-photon photodetachment processes are considered for simple model systems representing negative ions exposed to monochromatic radiation. The model systems considered feature an initial discrete state, the photoelectron continuum, and in some cases an excited or autodetaching discrete state. Population trapping through the formation of a bound dressed state and the photoelectron spectra are examined. Two photoelectron spectra are defined : a primary spectrum which results from decay while the laser interaction is on and a secondary spectrum which results from the destabilization of the bound dressed state if the interaction is turned off again. Careful attention is given to the passage of the poles of the Green's operator through the low-energy boundary of a continuum, and it is concluded that such poles move nonmonotonically through the boundary of an s-wave continuum, but monotonically through the boundary of a p-wave or higher-l-wave continuum. Two example systems, one featuring a single discrete state and an s-wave continuum and one featuring two discrete states and a p-wave continuum, are considered in detail.
Complex dressed states and photoelectron spectra are considered for a model system containing two discrete states that are coupled by separate lasers to a continuum that supports a resonance such as an autoionizing state. Spontaneous radiative decay from the structured continuum has been included and its effects are examined. It is shown that population can be trapped within the model atom even when radiative decay is included provided (1) the two Fano q values which characterize the discrete-state--continuum interactions are equal, and (2) the two-photon resonance condition is satisfied.
The dynamics of the bound-state populations and the photoelectron spectra are calculated for model atomic systems irradiated by a pulse with a harmonically modulated frequency. For a system including a single bound state a model is adopted, which takes into account the threshold behavior typical of negative ions and admits continuum-continuum transitions. For a model one-dimensional atom the results are obtained through a numerical integration of the Schr\"odinger equation. The case of a resonant ionization is also considered. The modulation of the frequency results in changing the instantaneous rate of decay of the initial state, in inducing additional population oscillations for multilevel systems, and in additional peaks in the photoelectron spectra.
We examine the excitation of continuum-state resonances close to the threshold, paying particular attention to the breakdown of the Markov approximation and the consequences of this for initial-state time dependences and final-state spectra. Several theoretical dressed-state alternative descriptions are analyzed and compared: the nonperturbative coupling of a discrete state to a structured continuum with a threshold, the complete Fano diagonalization of the interacting system, and finally a partial diagonalization of the bound-state couplings to reveal the origin of dressed-state stabilization and partial decay suppression observed in this model.
The negative ion of lanthanum, La–\mathrm{L}{\mathrm{a}}^{\text{--}}La–, has one of the richest bound state spectra observed for an atomic negative ion and has been proposed as a promising candidate for laser-cooling applications. In the present experiments, La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– was investigated using tunable infrared photodetachment spectroscopy. The relative signal for neutral atom production was measured with a crossed ion-beam--laser-beam apparatus over the photon energy range 585--920 meV (2120--1350 nm) to probe the continuum region above the La neutral atom ground state. Eleven prominent peaks were observed in the La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– photodetachment cross section due to resonant excitation of quasibound transient negative ion states in the continuum, which subsequently autodetach. In addition, thresholds were observed for photodetachment from several bound states of La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– to both ground and excited states of La. The present results provide information on the excited state structure and dynamics of La–\mathrm{L}{\mathrm{a}}^{\text{--}}La– that depend crucially on multielectron correlation effects.