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Physical Review A

Harmonic generation: Quantum-electrodynamical theory of the harmonic photon-number spectrum

D. J. Diestler

Published Sep 10, 2008• 34 citations
Publisher

Abstract

Simulations of harmonic generation in the single-atom limit usually describe the harmonic radiation as proportional to the squared magnitude of the Fourier transform (FT) of the expectation value of either the dipole moment or the dipole acceleration. However, no derivation of an explicit single-atom representation of the typical experimental measurement (i.e., the number of harmonic photons produced versus the frequency of the harmonic) has been given. By means of the first principles of quantum electrodynamics a formula for this ``harmonic photon-number spectrum'' is derived, which is proportional to the double FT of the time-autocorrelation function of the dipole velocity of the whole system. Within the long-wavelength approximation the time-correlation function can be recast as the FT of the squared magnitude of the expectation value of the dipole velocity of a single representative atom.

DOI
10.1103/physreva.78.033814

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Simulations of harmonic generation in the single-atom limit usually describe the harmonic radiation as proportional to the squared magnitude of the Fourier transform (FT) of the expectation value of either the dipole moment or the dipole acceleration. However, no derivation of an explicit single-atom representation of the typical experimental measurement (i.e., the number of harmonic photons produced versus the frequency of the harmonic) has been given. By means of the first principles of quantum electrodynamics a formula for this ``harmonic photon-number spectrum'' is derived, which is proportional to the double FT of the time-autocorrelation function of the dipole velocity of the whole system. Within the long-wavelength approximation the time-correlation function can be recast as the FT of the squared magnitude of the expectation value of the dipole velocity of a single representative atom.
In quantum theory, the description of radiation by a system of charged particles in stationary and nonstationary cases requires different approaches. While radiative processes in stationary systems are covered in textbooks, the emission of radiation by nonstationary systems driven by an external time-dependent force has not received due attention. In this paper, we develop a quantum theory describing the spectrum of photons emitted by a generic nonstationary atomic system and show how to implement it in practical calculations. We also discuss the approximation in which the exact quantum formula for the spectrum reduces to the well-known classical formula with the classical dipole moment replaced by the expectation value of the dipole moment calculated quantum mechanically. This approximation underlies the classical ansatz commonly used in the theory of high-order harmonic generation (HHG). To illustrate the theory, we apply it to calculating HHG spectrum for a one-dimensional zero-range-potential model. The spectra obtained from the quantum formula and from the ansatz are different and the difference grows as the probability of ionization grows. This difference is an observable effect predicted by the present theory.
The interaction of electrons with strong laser fields is usually treated with semiclassical theory, where the laser is represented by an external field. There are analytic solutions for the free electron wave functions, which incorporate the interaction with the laser field exactly, but the joint effect of the atomic binding potential presents an obstacle for the analysis. Moreover, the radiation is a dynamical system, the number of photons changes during the interactions. Thus, it is legitimate to ask how can one treat the high order processes nonperturbatively, in such a way that the electron-atom interaction and the quantized nature of radiation be simultaneously taken into account? An analytic method is proposed to answer this question in the framework of nonrelativistic quantum electrodynamics. As an application, a quantum optical generalization of the strong-field Kramers-Heisenberg formula is derived for describing high-harmonic generation. Our formalism is suitable to analyse, among various quantal effects, the possible role of arbitrary photon statistics of the incoming field. The present paper is dedicated to the memory of Prof. Dr. Fritz Ehlotzky, who had significantly contributed to the theory of strong-field phenomena over many decades.
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.
It is well established, both experimentally and theoretically, that atoms exposed to a strong laser pulse emit high order harmonics of the driving field. Although this process has been intensively studied theoretically, the main effort has been focused so far on the study of the harmonic spectrum while no attempt has been made to analyse systematically its time evolution. We show that the time profile of each harmonic may be obtained through a time-frequency analysis of the acceleration of the atomic dipole. We show also that such an analysis, which is very sensitive to the details of the dynamics, provides valuable information about the competition between photon emission and ionization processes.
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)].
Numerical simulations of stationary fluorescence spectra of molecular systems usually rely on the relation between the photon emission rate and the system’s dipole–dipole correlation function. However, research papers usually take this relation for granted, and standard textbook expositions of the theory of fluorescence spectra also tend to leave out this important relation. In order to help researchers with less theoretical training gain a deeper understanding of the emission process, we perform a step-by-step derivation of the expression for the fluorescence spectrum, focusing on rigorous mathematical treatment and the underlying physical content. Right from the start, we employ quantum description of the electromagnetic field, which provides a clear picture of emission that goes beyond the phenomenological treatment in terms of the Einstein A coefficient. Having obtained the final expression, we discuss the relation of the latter to the present level of theory by studying a simple two-level system. From the technical perspective, the present work also aims at familiarizing the reader with the density matrix formalism and with the application of the double-sided Feynman diagrams.