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Physical Review A

Temporal effects in multiphoton ionization of lithium

J. G. Story, Thomas F. Gallagher

Published Jun 1, 1993• 10 citations
Publisher

Abstract

The temporal effects of multiphoton ionization are investigated using a two-color method which determines both the time and intensity at which the process occurs. We show that the total ionization efficiency depends strongly on the time at which an atom makes a transition to an excited state during an intense laser pulse. This result clearly shows that the ac-Stark-shifted bound-state resonances not only enhance the cross section for photoionization, but that the excited bound states provide temporary storage states for the atomic population during the photoionization process.

DOI
10.1103/physreva.47.5037

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The temporal effects of multiphoton ionization are investigated using a two-color method which determines both the time and intensity at which the process occurs. We show that the total ionization efficiency depends strongly on the time at which an atom makes a transition to an excited state during an intense laser pulse. This result clearly shows that the ac-Stark-shifted bound-state resonances not only enhance the cross section for photoionization, but that the excited bound states provide temporary storage states for the atomic population during the photoionization process.
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It has been widely believed that short-pulse multiphoton ionization is dominated by a resonance process: excited states of the atom are shifted by the radiation field into multiphoton resonance with the ground state, are populated, and then rapidly ionized. A recent experiment, shows significant population remaining in excited states at the end of the laser pulse, and this result has been interpreted as indicating that ionization proceeds slowly out of these states. We investigate this issue in the framework of Floquet theory, supplemented by direct numerical solution of the time-dependent Schrodinger equation. In this framework, the standard picture is portrayed as an adiabatic transition between Floquet eigenstates, which occurs as the amplitude of the laser field is ramped through the resonance value (i.e. through an avoided crossing of Floquet quasienergies). Thus it follows that the same type of transition must occur as the field is turned off. This mechanism can yield significant populations of excited states that do not suffer appreciable ionization. We exhibit this effect by numerical studies of a model atom with two bound states and two continua.
We present results from a time-dependent two-level-plus-continuum model of multiphoton ionization in order to better understand the short-pulse photoelectron spectrum resulting from multiphoton ionization and the role of intermediate states. Both resonant and nonresonant population transfer to the upper state are found to play an important role in the multiphonon ionization process. The dynamic modeling reveals the potential for broadening and shifting peaks in the photoelectron spectrum. However, we conclude that despite the complex dynamics of the excitation, short-pulse photoelectron spectra can be used to measure ac Stark shifts of both ponderomotively and nonponderomotively shifted states in strong laser fields.
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The most important results of study of multiphoton ionization of atoms are reviewed. Discussions are presented of specific features of the process, theoretical methods of description of ionization of atoms in a strong light field, the basic principles of design of experiments in which intense laser radiation is used, results of investigation of direct and resonance processes of multiphoton ionization, and the mutual relation between multiphoton processes (multiphoton excitation and ionization) and various phenomena leading to perturbation of the spectrum of bound states of an electron in an atom under the influence of a strong light field.