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Journal of Modern Optics

Photo-excitation of a Structured Continuum: A Soluble Model

PAUL M. RADMORE, Sam Tarzi

Published Nov 1, 1987• 6 citations
Publisher

Abstract

The photoexcitation of a structured continuum of states from a single ground state is considered. We investigate an analytically soluble model in which the dipole matrix elements between the ground state and the continuum vary sinusoidally between zero and a maximum. The time-evolution of the ground-state population still exhibits the periodic disruption observed in the Bixon-Jortner model, although the disruption is much reduced. We allow the ground state to be resonant with an arbitrary place in the continuum; population trapping is observed in the case of resonance with a zero in the continuum. We compare and contrast the results obtained with this model with those of quasi-continuum excitation. Lastly, we examine the final-state spectrum.

DOI
10.1080/09500348714551331

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The photoexcitation of a structured continuum of states from a single ground state is considered. We investigate an analytically soluble model in which the dipole matrix elements between the ground state and the continuum vary sinusoidally between zero and a maximum. The time-evolution of the ground-state population still exhibits the periodic disruption observed in the Bixon-Jortner model, although the disruption is much reduced. We allow the ground state to be resonant with an arbitrary place in the continuum; population trapping is observed in the case of resonance with a zero in the continuum. We compare and contrast the results obtained with this model with those of quasi-continuum excitation. Lastly, we examine the final-state spectrum.
The photoexcitation of a quasicontinuum of atomic or molecular levels by a laser pulse with a fast rise-time is considered. We first generalize non-perturbative treatments of quasicontinuum excitation. A second general theoretical method is developed in which resonant states are considered non-perturbatively whereas background non-resonant states are included through a perturbative approximation. As a simple example we show how our method describes the photoexcitation of a quasicontinuum of equally spaced levels, exhibiting Rabi oscillations periodically perturbed by background states. We then examine the case of a Rydberg series of highly excited states coherently excited from a low-lying initial state. The time evolution of the coherent superposition of Rydberg levels is shown to be a perturbed Rabi oscillation, but without the periodic disruption of the equally spaced quasicontinuum. Finally, we include the effect of further excitation to a second continuum.
We present an analytical solution to a multilevel model of light-induced continuum structure, in which, instead of a single level, a quasicontinuum of excited levels is laser embedded into a previously structureless atomic continuum. The found solution is fully time dependent and is valid for probing strengths of the structured continuum from the ground level by another laser, which can vary from being much weaker than the embedding one to being as strong as the embedding one. For three different embeddings (weak, moderate, and strong), each one determined by a different relation between the ionization rate \ensuremath{\gamma} and the spacing \ensuremath{\Delta} of the quasicontinuum levels (\ensuremath{\Elzxh}\ensuremath{\gamma}/\ensuremath{\Delta}\ensuremath{\ll}1, \ensuremath{\Elzxh}\ensuremath{\gamma}/\ensuremath{\Delta}\ensuremath{\simeq}1, and \ensuremath{\Elzxh}\ensuremath{\gamma}/\ensuremath{\Delta}\ensuremath{\gg}1), we study the evolution of the ionization spectrum with increasing probing strength. We observe and interpret such strong-field effects in the spectra as (i) conversion of a Fano-like train of peaks into a train of dips; (ii) peak moving, narrowing, and lowering; and (iii) saturation, population trapping, and stabilization against ionization.
We study the coupling of an initially occupied single level to an N-level quasi-continuum (QC) using perturbation theory. The single-level amplitude is expressed as a sum of harmonically oscillating factors whose dephasings and rephasings give rise to decay and recurrences, respectively. In particular, we study the most common model of this coupling in which the QC is infinite, uniform, and flat. We derive simple approximate formulas for resonant and nonresonant excitation that display absorption-rate reversal and enhancement effects and periodic time evolution. We show how these properties can be connected to few-level dynamics. The limits of applicability of few-level approximations are investigated.
An exactly soluble model is used to describe transitions, induced by two strong laser beams, proceeding from the initial discrete state to the continuum via two channels. In the first channel the transition occurs via an intermediate, near-resonant discrete state located close to the continuum edge. In the second channel the intermediate state belongs to the continuum. Population trapping occurs due to an interference between the two channels. The model can be used to describe the photodetachment of electrons from negative ions or the photodissociation of molecules.
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.