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Shortwavelength: Physics with Intense Laser Pulses

Super-Dressed Two-Level Atom: Very High Harmonic Generation and Multi-Resonances

A. E. Kaplan, P. L. Shkolnikov

Published Jan 1, 1993• 1 citation
Publisher

Abstract

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].

DOI
10.1364/swv.1993.h156

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Intensity dependence of the phase of harmonics in one- and two-frequency laser fields

W.-C. Liu, Charles W. Clark

The phase relationship between an induced atomic dipole moment and a driving laser field is an essential aspect of high harmonic generation (HHG) in a dense medium. A ``phase-matching'' criterion must be fulfilled to obtain coherent amplification of harmonic radiation, which is critical for practical HHG. We have performed numerical calculations on model atoms to survey the intensity dependence of the phase in the case of strong one- or two-frequency laser fields. The calculations show that multiphoton resonances significantly affect the yield of harmonic generation and that in the ``plateau'' regime, the phases exhibit only weak dependence upon the intensity of the driving field. \textcopyright{}1996 The American Physical Society.

Physical Review A•May 1, 1996•5 citations
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].
Harmonic generation is studied in an idealized model medium in which the laser field essentially interacts only with a single atomic transition and where ionization can be neglected. Such two-level models are known to generate high harmonics with a plateau and a cutoff. We put forward a quantitative rule for the cutoff frequency in the harmonic spectrum in this model which we relate to the ``IP{\mathrm{I}}_{\mathrm{P}}IP​+3UP{3\mathrm{U}}_{\mathrm{P}}3UP​ rule'' in real systems with ionization. We examine the phase properties of the emitted harmonics and show that their coherence and thus phase matching is more favorable in the cutoff regime than in the plateau of the harmonic spectrum. This behavior is known to occur in realistic models of neon, and that this occurs also for the simple idealized two-level model strongly suggests that the sudden change of phase coherence from the cutoff to the plateau regime is as intrinsic a property of nonlinear systems as are the plateau and the cutoff.
Two-electron processes can generate high harmonics beyond the conventional single-active-electron cutoff. Motivated by recent experimental evidence of an extended secondary plateau in the helium high-harmonic spectrum [S. Wang et al, Optica, (2023); S. Wang et al, In Print in Nature Photon., (2026)], we present a two-electron generalisation of the strong-field approximation. We analyse the resulting expressions using the saddle-point method and determine the extended cutoff. We find good agreement with classical predictions of cutoff scalings of 4.74.74.7 and 5.55.55.5 times the ponderomotive energy, which significantly exceed the established single-electron scaling of 3.17. We calculate high-harmonic spectra generated via a two-electron process in helium atoms driven by an intense few-cycle infrared laser pulse. Our results demonstrate that the harmonic spectrum extends far beyond the water window, reaching photon energies up to ≈1.2 keV\approx 1.2\,\mathrm{keV}≈1.2keV in the soft x-ray region. The large spectral bandwidth can support the generation of sub-attosecond soft x-ray pulses, which are of particular interest for probing ultrafast dynamics across matter, including applications in core-level spectroscopy and biological imaging.
The phase relationship between an induced atomic dipole moment and a driving laser field is an essential aspect of high harmonic generation (HHG) in a dense medium. A ``phase-matching'' criterion must be fulfilled to obtain coherent amplification of harmonic radiation, which is critical for practical HHG. We have performed numerical calculations on model atoms to survey the intensity dependence of the phase in the case of strong one- or two-frequency laser fields. The calculations show that multiphoton resonances significantly affect the yield of harmonic generation and that in the ``plateau'' regime, the phases exhibit only weak dependence upon the intensity of the driving field. \textcopyright{}1996 The American Physical Society.