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Journal of the Optical Society of America B

Two-color coherent control of atomic multiphoton ionization with high-order harmonics: time-dependent Schrödinger equation treatment

Richard Taïeb, Valérie Vëniard, A. Maquet

Published Feb 1, 1996• 25 citations
Publisher

Abstract

We present a theoretical study of the main characteristics of two-color photoionization spectra obtained when atoms are subjected to an intense radiation pulse containing the fundamental of an infrared laser and one of its higher harmonics. The frequency of the latter is chosen to be high enough that the atom can be ionized by a single photon. The calculation is performed by numerical integration of the time-dependent Schrödinger equation for a (three-dimensional) hydrogen atom. We present the general properties of the spectra and angular distributions as well as the possible occurrence of interferences between the laser-assisted process and above-threshold ionization. Our results indicate that such interference effects, which can lead to partial coherent control of the photoionization process, can be observed at moderate laser intensities within the reach of currently operated laser and harmonic sources.

DOI
10.1364/josab.13.000363

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We discuss, via a numerical calculation, the main properties of atomic photoelectron spectra, as they would be obtained by using a radiation pulse containing higher harmonics together with the laser which has been used to generate them. We address more precisely the physically relevant situation in which the harmonics have much weaker intensities than the one of the laser. In such multicolor photoionization processes, the atom can simultaneously absorb harmonic UV photons and exchange, i.e. absorb and/or emit (via stimulated emission) laser IR photons. An interesting outcome of our study is to show that such new effects should be observable with currently developed harmonic sources.
Ultrafast high harmonic beams provide new opportunities for coherently controlling excitation and ionization processes in atoms, molecules, and materials on attosecond time scales by employing multiphoton two-pathway electron-wave-packet quantum interferences. Here we use spectrally tailored and frequency tuned vacuum and extreme ultraviolet harmonic combs, together with two phase-locked infrared laser fields, to show how the total single and double photoionization yields of argon can be coherently modulated by controlling the relative phases of both optical and electronic-wave-packet quantum interferences. This Letter is the first to apply quantum control techniques to double photoionization, which is a fundamental process where a single, high-energy photon ionizes two electrons simultaneously from an atom.
We theoretically investigate strong-field ionization of hydrogen atoms by orthogonally polarized two-color (OTC) laser pulses consisting of a fundamental field that is resonant with the 1s - 2p transition and its second harmonic. Numerical simulations are performed by solving the two-dimensional time-dependent Schrödinger equation and recording the photoelectron momentum distribution. In this strong-field resonant ionization, the atom undergoes many Rabi cycles and the electron can be emitted within a completed Rabi-cycle leading to the splitting of the localized momentum distribution. Here, the splitting is attributed to dynamic Rabi-splitting as a result of the dynamic Stark effect. The employed OTC scheme is shown to be efficient for controlling the dynamic Rabi-splitting through the control of quantum-path interferences involved in one-photon and two-photon absorption processes. The control scheme is accomplished by varying the relative ratio intensity and optical phase between the two pulses, and its footprint is mapped in the momentum distribution. This is shown to lead to an asymmetric distribution and suppression of the ionization process. The obtained results suggest the OTC scheme as a tool for coherent control of dynamic Rabi-oscillations via the controlled quantum-path interferences, thus opening new directions towards designing quantum states via the control OTC scheme.
We present a quantitative theory with detailed calculations pertaining to multiphoton ionization of helium under moderately strong uv radiation of photon energy 13eV13\phantom{\rule{0.3em}{0ex}}\mathrm{eV}13eV. Employing both, the nonperturbative solution of the time-dependent Schr\"odinger equation, as well as perturbation theory, we obtain detailed results for all processes expected to be of quantitative relevance within the range of intensities and pulse durations in this work, which have been chosen so as to match the conditions of a recent experiment on exactly this problem [T. Laarman et al., Phys. Rev. A 72, 023409 (2005)]. The conclusion, in connection with the experimental data, which our results lead to is that, without the presence of the second harmonic of the fundamental in the radiation, it is impossible to reconcile the reported observations with fundamental features of the processes involved. A more general conclusion seems to be that the presence of these harmonics, even at intensities less than 1% of that of the fundamental, are apt to produce profound side effects that will mask multiphoton processes by the fundamental.
A nonperturbative method is used to study the two-color multiphoton ionization of atoms by solving the Schr\"odinger equation in momentum space, which facilitates the extraction of the rapidly varying part of the wave function. Our method generalizes the problem for cases where an arbitrary number of ionization photons are absorbed, and also takes into account the threshold shifts due to both the high- and low-frequency fields. The photoelectron energy spectra of the hydrogen atoms are calculated and the dependence on the laser field strengths and frequencies is discussed. \textcopyright{} 1996 The American Physical Society.