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Journal of Modern Optics

High-order Harmonic Generation in a Two-level Atom

Luis Plaja, L. Roso

Published May 1, 1993• 50 citations
Publisher

Abstract

Coherent high-order harmonic generation by an isolated two-level system is studied. A perturbative theory, for the adiabatic regime, is presented that describes the plateau structure experimentally found in noble gases. Numerical results, out of the rotating wave approximation, are used to check the analytical predictions. A dressed atom picture is introduced that shows the role of multiphoton resonances, tuned due to the light shift, to enhance high-order harmonic generation.

DOI
10.1080/09500349314550831

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•Aug 1, 1987•0 citations
Coherent high-order harmonic generation by an isolated two-level system is studied. A perturbative theory, for the adiabatic regime, is presented that describes the plateau structure experimentally found in noble gases. Numerical results, out of the rotating wave approximation, are used to check the analytical predictions. A dressed atom picture is introduced that shows the role of multiphoton resonances, tuned due to the light shift, to enhance high-order harmonic generation.
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.
The coherent scattering spectrum of a three-level atom driven by an intense laser field with multiphoton resonant excitation is considered. The spectrum corresponding to harmonic generation is investigated both analytically and numerically for different initial atomic states. The analytical calculations are based on the generalized rotating wave approximation, which allows one to explain obtained spectra containing in general both even and odd harmonics. The results applied to the hydrogen atom show that one can achieve efficient generation of moderately high harmonics using multiphoton resonant excitation by appropriate laser pulses.
This work examines the use of higher order multiphoton resonances in higher harmonic generation together with judicious exploitation of coherent interaction properties to achieve efficient harmonic generation. A detailed experimental study on third harmonic generation in two photon resonant coherent interaction and a theoretical study on four photon resonant coherent interaction have been conducted. Two photon resonant coheren propagation in lithium vapor (2S-4S and 2S-3D interaction) has been studied in detail as a function of phase and delay of the interacting pulse sequence. Under coherent lossless propagation of 90 phase shifted pulse pair, third harmonic generation is enhanced. A maximum energy conversion efficiency of 1% was measured experimentally. This experiment shows that phase correlated pulse sequence can be used to control multiphoton coherent resonant effects. A larger two photon resonant enhancement does not result in more efficient harmonic generation, in agreement with the theoretical prediction. An accurate (to at least 0.5 A°) measurement of intensity dependent Stark shift has been done with the newly developed "interferometric wavemeter." Stark shifts as big as several pulse bandwidths (of picosecond pulses) result in a poor tuning of multiphoton resonance and become a limiting factor of resonant harmonic generation. A complete theory has been developed for harmonic generation in a four photon resonant coherent interaction. A numerical application of the theory to the Hg atom successfully interprets the experimental observations in terms of the phase dependent stimulated Raman scattering. With the intensity required for four photon resonant transition, the calculation predicts a dramatic Stark shift effect which completely destroys the resonance condition. This model provides a basis for the development of future schemes for efficient higher order coherent upconversion.