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Journal of Physics B Atomic Molecular and Optical Physics

QED theory of harmonic emission by a strongly driven atom

G. Compagno, Klaus Dietz, Franco Persico

Published Oct 14, 1994• 20 citations
Publisher

Abstract

We present a theory of harmonic generation by a strongly driven atom within the framework of non-relativistic QED. The atom is assumed to possess a finite number N of levels and ionization is neglected. This atom is dressed by the driving field using a unitary time-dependent transformation. Within the quasistatic approximation this transformation is shown to lead from the bare to the Floquet atom. The interaction of the Floquet atom with the vacuum modes is derived and it is shown to give rise both to the high-order harmonic and to the hyper-Raman spectrum. In the case N=2 the spectrum of the light scattered into the vacuum modes can be evaluated analytically and it is shown to consist of two parts. Neglecting interference between these two parts, the first of them is the high-order harmonic spectrum displaying peaks at the odd harmonics of the driving field. The second part is the hyper-Raman spectrum which has finite bandwidth and which displays peaks at the even harmonics of the laser frequency, centred at the Stark-shifted natural atomic frequency. These two spectra partially overlap and they are discussed in various ranges of intensity of the driving field, both in the minimal coupling and in the multipolar scheme. The results support recent suggestions that the presence of the plateau is related to interference between the two spectra. The dependence of the high-order harmonic spectrum from the driving field intensity is found to be related to that of the hyper-Raman spectrum in such a way that when the former increases the latter decreases and vice versa. It is argued that this might help to explain the non-visibility of the hyper-Raman lines when the high-order harmonics are visible.

DOI
10.1088/0953-4075/27/19/031

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Physical Review A•May 29, 2001•30 citations
We present a theory of harmonic generation by a strongly driven atom within the framework of non-relativistic QED. The atom is assumed to possess a finite number N of levels and ionization is neglected. This atom is dressed by the driving field using a unitary time-dependent transformation. Within the quasistatic approximation this transformation is shown to lead from the bare to the Floquet atom. The interaction of the Floquet atom with the vacuum modes is derived and it is shown to give rise both to the high-order harmonic and to the hyper-Raman spectrum. In the case N=2 the spectrum of the light scattered into the vacuum modes can be evaluated analytically and it is shown to consist of two parts. Neglecting interference between these two parts, the first of them is the high-order harmonic spectrum displaying peaks at the odd harmonics of the driving field. The second part is the hyper-Raman spectrum which has finite bandwidth and which displays peaks at the even harmonics of the laser frequency, centred at the Stark-shifted natural atomic frequency. These two spectra partially overlap and they are discussed in various ranges of intensity of the driving field, both in the minimal coupling and in the multipolar scheme. The results support recent suggestions that the presence of the plateau is related to interference between the two spectra. The dependence of the high-order harmonic spectrum from the driving field intensity is found to be related to that of the hyper-Raman spectrum in such a way that when the former increases the latter decreases and vice versa. It is argued that this might help to explain the non-visibility of the hyper-Raman lines when the high-order harmonics are visible.
Numerical results are presented on the spectrum of the light scattered into the vacuum modes by a two-level atom driven by a strong ramped field of frequency smaller than the natural atomic frequency. The attention is focused on the role of the hyper-Raman part of the spectrum, which is shown to decrease dramatically with increasing ramp time. It is suggested that this may explain lack of experimental observation of the hyper-Raman lines. For zero ramp time, the numerical intensity of both high-order harmonics and hyper-Raman peaks is shown to agree satisfactorily with previous analytical predictions except in the region of overlap of the two series of peaks. This lends support for the suggestion that the plateau in the spectrum is related to quantum-mechanical interference between high-order harmonics and hyper-Raman processes. There is also good agreement between the numerical amplitude of the plateau and previous analytical predictions. A physical mechanism for the cut-off frequency which terminates the plateau, based on approximate energy conservation in hyper-Raman transitions, is presented and is shown to be in agreement with present numerical and previous analytical results.
We present the most prominent features in two-colour coherent control of high-order harmonic generation using a strongly driven two-level atom model, which are known to generate high harmonics as well as hyper-Raman lines with a plateau and a cut-off. Furthermore, for one laser field case, we find, when the hyper-Raman lines are located at the position of the high harmonics, that the high harmonics are strongly enhanced due to the interference effect between the high harmonics and the hyper-Raman lines. Within these conditions, by combining the laser field with another much weaker laser field, we show plentiful and strong high harmonics in the light spectrum of the driven atomic system.
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 investigate a two-level atom in the field of a strong laser pulse. The resulting time-dependent polarization is the source of a radiation the frequency components of which are essentially harmonics of the driving field's carrier frequency. The time evolution of this secondary radiation is analyzed in terms of the expectation values of the photon-number operators for a large number of electromagnetic modes that are initially in the vacuum state. Our method is based on a multimode version of the Jaynes-Cummings-Paul model and can be generalized to different radiating systems as well. We show that, after the exciting pulse, the final distribution of the photon numbers is close to the conventional (Fourier-transform-based) power spectrum of the secondary radiation. The details of the high-order-harmonic spectra (HHG spectra) are also analyzed; for many-cycle excitations a clear physical interpretation is given in terms of the Floquet quasienergies. A first step towards the determination of the photon statistics of the high-order-harmonic modes reveals states with slightly super-Poissonian distribution.