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Physical Review A

Harmonic generation for atoms in fields of varying ellipticity: Single-active-electron model with Hartree-Fock potential

Igor A. Ivanov, Anatoli S. Kheifets

Published May 15, 2009• 12 citations
Publisher

Abstract

We propose a theoretical procedure for calculating harmonics yield from atoms based on the solution of a three-dimensional time-dependent Schr\"odinger equation. The atomic system is described by means of the Hartree-Fock potential, including the exchange interaction. We present results for the harmonics generation in lithium and rubidium in situation when ellipticity of the driving laser changes with time. These results show that harmonics are formed primarily at the intervals of time when the driving laser field has nearly zero ellipticity. This can be used for generation of short (hundreds of attoseconds) bursts of radiation.

DOI
10.1103/physreva.79.053827

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We propose a theoretical procedure for calculating harmonics yield from atoms based on the solution of a three-dimensional time-dependent Schr"odinger equation. The atomic system is described by means of the Hartree-Fock potential, including the exchange interaction. We present results for the harmonics generation in lithium and rubidium in situation when ellipticity of the driving laser changes with time. These results show that harmonics are formed primarily at the intervals of time when the driving laser field has nearly zero ellipticity. This can be used for generation of short (hundreds of attoseconds) bursts of radiation.
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 extend our recently developed semiclassical strong-field Herman-Kluk propagator (SFHK) method to calculate high-order harmonic generation (HHG) for atoms in intense lasers. We show that our method, based on a combination of the Herman-Kluk propagator and the strong-field approximation, can provide highly accurate results for both HHG yield and phase, nearly identical to those from the exact numerical solutions of the time-dependent Schrödinger equation. We provide detailed analyses of our method and its applications to the HHG process, particularly the recombination time. The main computational task in this method is to solve the classical Newton equations for the active electron in the combined atomic potential and laser-electron interaction. The motion of the centers of the electron wave packets, modeled by coherent states, is governed by independent classical trajectories so that the computation can therefore be parallelized very efficiently.
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.
A simple, "exactly solvable" atomic model will be presented that helps to discuss some of the interesting features of multiphoton ionization of atoms. The electromagnetic field is treated non-perturbatively, it can be strong. The atomic electrons are assumed to be non-interacting (Hartree model). They are bound in a harmonic oscillator potential (one- or three-dimensional). At the ionization energy, the potential is cut off and the free electron has no Coulomb attraction. The Schrodinger equation has exact analytic solutions valid in the inner or outer regions. If the field is turned on adiabatically, the exact solution can be found by matching these solutions at the boundary; both of their value and the normal derivative at all times. Thus the machine calculation reduces to repeated application of fast Fourier transforms and to the solution of linear equations (unfortunately a lot of them).
The dependence on the ellipticity of the incident laser field of the harmonics generated by atoms of hydrogen in the multiphoton regime is examined for two fundamental wavelengths, 532 and 1064 nm. The single atom response is calculated nonperturbatively using the Floquet method in conjunction with basis sets of complex Sturmian functions. The results are compared with those obtained using lowest order perturbation theory. Nonperturbative effects modify the strength and polarization of the harmonics at the highest intensities investigated, particularly, for the threshold harmonics and in the vicinity of Stark-shift-induced resonances. No anomalous dependence of the rate of harmonic generation on the ellipticity of the fundamental field is found.
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].