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Physical Review A

Nonperturbative theory of harmonic generation in helium under a high-intensity laser field: The role of intermediate resonance and of the ion

Huale Xu, Xian Tang, P. Lambropoulos

Published Sep 1, 1992• 68 citations
Publisher

Abstract

The time-dependent Schr\"odinger equation for the helium atom with a model potential is solved on a numerical grid. The effects of intermediate-state resonance and of the ionization of the atom upon the harmonic generation are investigated. We also evaluate the contribution of the helium ion when the laser intensity is sufficiently high for most of the atoms to be ionized during the laser pulse. We find that the harmonics with order higher than 13 are due to the ion when the photon energy is 5.0 eV, while for photon energy 2.0 eV the atom produces up to about the 49th harmonic.

DOI
10.1103/physreva.46.r2225

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The time-dependent Schr"odinger equation for the helium atom with a model potential is solved on a numerical grid. The effects of intermediate-state resonance and of the ionization of the atom upon the harmonic generation are investigated. We also evaluate the contribution of the helium ion when the laser intensity is sufficiently high for most of the atoms to be ionized during the laser pulse. We find that the harmonics with order higher than 13 are due to the ion when the photon energy is 5.0 eV, while for photon energy 2.0 eV the atom produces up to about the 49th harmonic.
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.
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.
We theoretically study intensity-saturation effects in resonant harmonic generation and multiphoton ionization. A first laser excites a two-photon resonance which is coupled by a second laser to an autoionizing state. Starting from an effective Hamiltonian for the three resonant atomic states, we derive a set of equations for the density matrix of the gaseous medium and the electromagnetic field within a semiclassical framework. We present and discuss analytical and numerical solutions of these equations which show a variety of line profiles depending critically on the intensities of the incident laser pulses.
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].
When an atom is driven by a laser field with a photon energy that is nearly resonant with an atomic transition, it can undergo periodic population transfers between the ground and excited state, known as Rabi oscillations [1], [2]. The aim of this work is to study photoionization from atoms for parameters accessible to a free-electron laser (FEL) [3]. Using time dependent perturbation theory to model photoionization from a Rabi oscillating atom, we have shown that in addition to the expected pathway of ionization from the excited state, non-resonant two-photon ionization will have a comparable amplitude at intensities on the order of 1013W/cm2[3].