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arXiv:physics/0211110 · Physical Review A

Harmonic generation by atoms in circularly polarized two-color laser fields with coplanar polarizations and commensurate frequencies

F. Ceccherini, D. Bauer, F. Cornolti

Published Nov 4, 2003• 21 citations
arXivHTMLPDF

Abstract

The generation of harmonics by atoms or ions in a two-color, coplanar field configuration with commensurate frequencies is investigated through both an analytical calculation based on the Lewenstein model and the numerical ab initio solution of the time-dependent Schr\"odinger equation of a two-dimensional model ion. Through the analytical model, selection rules for the harmonic orders in this field configuration, a generalized cutoff for the harmonic spectra, and an integral expression for the harmonic dipole strength are provided. The numerical results are employed to test the predictions of the analytical model. The scaling of the cutoff as a function of both one of the laser intensities and frequency ratio $\ensuremath{\eta}$ as well as entire spectra for different $\ensuremath{\eta}$ and laser intensities are presented and analyzed. The theoretical cutoff is found to be an upper limit for the numerical results. Other discrepancies between analytical model and numerical results are clarified by taking into account the probabilities of the absorption processes involved.

DOI
10.1103/physreva.68.053402

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The generation of harmonics by atoms or ions in a two-color, coplanar field configuration with commensurate frequencies is investigated through both an analytical calculation based on the Lewenstein model and the numerical ab initio solution of the time-dependent Schr"odinger equation of a two-dimensional model ion. Through the analytical model, selection rules for the harmonic orders in this field configuration, a generalized cutoff for the harmonic spectra, and an integral expression for the harmonic dipole strength are provided. The numerical results are employed to test the predictions of the analytical model. The scaling of the cutoff as a function of both one of the laser intensities and frequency ratio \ensuremathη\ensuremath{\eta}\ensuremathη as well as entire spectra for different \ensuremathη\ensuremath{\eta}\ensuremathη and laser intensities are presented and analyzed. The theoretical cutoff is found to be an upper limit for the numerical results. Other discrepancies between analytical model and numerical results are clarified by taking into account the probabilities of the absorption processes involved.
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.
We study harmonic generation by a single atom exposed to two short perpendicularly polarized laser pulses. The two perpendicular electric fields oscillate at two different frequencies ${\ensuremath{\omega}}_{1}$ and ${\ensuremath{\omega}}_{2}$. Hence, the resultant field has a polarization which depends on time. Since harmonics are emitted when the resultant oscillating field is linearly polarized, it is expected that a short pulse of harmonics may be emitted if the external field is linearly polarized during a short period of time. We show that, indeed, the atom may emit an ultrashort pulse of a given harmonic. This result has been obtained by time-frequency analyzing the acceleration of the induced dipole moment with a filter whose frequency bandwidth is smaller than twice the frequency of the external field. Our calculation of the dipole acceleration is based on the numerical solution of the time-dependent Schr\"odinger equation. We then address the question of how far it is possible to reduce the duration of the emitted pulse of one given harmonic by adjusting both ${\ensuremath{\omega}}_{1}$ and ${\ensuremath{\omega}}_{2}$ and keeping the amplitude of this pulse significant. In order to answer to this question, we used the quantum version of the two-step model [M. Lewenstein et al., Phys. Rev. A 49, 2117 (1994)].
We show that the parity of the order of the harmonics generated by a bichromatic field with commensurate frequencies may be related to the invariance properties of the time-dependent Hamiltonian with respect to some suitable transformations. To simplify the mathematical treatment, we have used a simple model atom to perform calculations that show the effects of the relative phase of the driving fields. Harmonic generation has been described as a two-step process that involves replicas of the Stark levels. In agreement with other previous treatments in which other model atoms were used, we have found that a small contamination of the fundamental harmonic can produce significant modifications of the emission spectra.
We show that a simple nonperturbative two-level model of an atom driven by a very strong periodic field, results in a rich picture of very high harmonic generation and related phenomena. It reproduces experimentally observed plateau, yields for the first time simple analytic formulas for the plateau cutoff frequency, critical driving intensity, and saturation, and predicts intensity-induced multi-resonances. One of the most fascinating phenomenon discovered recently in nonlinear interaction of light with atoms and ions, is very high-order (up to 135) odd harmonic generation (HHG) by intense (∼ 1013 W/cm2 and higher) optical laser radiation in rare gasses and some ions [1], The spectra of generated harmonics drasticly deviate from the perturbation theory predictions [2], In particular, intensity of harmonics, falling monotonically with their orders only up to a certain point, levels off forming a so-called “plateau", and falls monotonically again beyond it. Generally, harmonte generation depends on phase-matching conditions and nonlinear response of individual atoms. It has recently become clear however [3,4] that the major features of HHG, in particular the plateau, result mainly from general properties of atomic nonlinear response. The most direct and apparently successful way so far to approach the problem theoretically has been numerical simulation of the Schrödinger [2,5-7] (including an empiric rule [6]) for many-electron atoms using Hartry-Slater approximation. This approach requires, however, tremendous amount of calculations and involves many processes, making it difficult to gain simple insights. An interesting simplified model [8] based on 3-D delta-potential with a single (ground) level [9] produces results in integration form. The idea of retaining a single energy scale (ionization energy) brings one close to an even simpler system: a two-level model atom. A two-level model of HHG [10], however, due to various complications introduced into it, failed to generate simple results, whereas an analytic solution [11] holds for a virtually degenerate two-level model only (see below) which is unapplicable to the experimental conditions [1-4,7,9]; besides, no relaxation was considered in [10,11].
We consider harmonics generation and wave mixing by two-color multiphoton resonant excitation of three-level atoms and molecules in strong laser fields. The coherent part of the spectra corresponding to multicolor harmonics generation is investigated. The obtained analytical results on the basis of a generalized rotating wave approximation are in a good agreement with numerical calculations. The results applied to the hydrogen atoms and homonuclear diatomic molecular ions show that one can achieve efficient generation of moderately high multicolor harmonics via multiphoton resonant excitation by appropriate laser pulses.
We investigate the third order harmonic generation for model atoms interacting with intense short laser pulses. We focus on the cases where the ponderomotive energy is not big enough to generate high-order harmonics, and where resonant transitions between bound states are also as important as multi-photon ionization and low-order harmonic generation. We find that the third order harmonic intensity from a model hydrogen atom can decrease as the laser frequency draws near a resonance between bound states. We explain this result by looking into the ionization and Rabi oscillation from the numerical calculation of the time-dependent 1-D Schrödinger equation. In order to support our explanation we also investigate the populations of bound states that play an important role in this atomic process.