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Optics and Spectroscopy

Resonance-parametric mechanism of optical rectification and high harmonic generation

С. В. Сазонов, N. V. Ustinov

Published Mar 1, 2009• 8 citations
Publisher

Abstract

The generation of zero and high-order harmonics in the spectrum of a laser pulse propagating through a medium containing quantum particles whose constant resonance transition dipole moment is nonzero is studied theoretically. The consideration is performed in the approximation of slowly varying envelopes modified for the case of the medium with the nonzero permanent dipole moment. It is shown that this modification requires consideration of antiresonance terms, in particular, the Bloch-Siegert shift in equations. The conditions are revealed for the efficient optical rectification and excitation of the second harmonic at a quasi-monochromatic signal applied to the medium.

DOI
10.1134/s0030400x09030175

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Journal of Physics B Atomic Molecular and Optical Physics•Apr 7, 2000•12 citations
The generation of zero and high-order harmonics in the spectrum of a laser pulse propagating through a medium containing quantum particles whose constant resonance transition dipole moment is nonzero is studied theoretically. The consideration is performed in the approximation of slowly varying envelopes modified for the case of the medium with the nonzero permanent dipole moment. It is shown that this modification requires consideration of antiresonance terms, in particular, the Bloch-Siegert shift in equations. The conditions are revealed for the efficient optical rectification and excitation of the second harmonic at a quasi-monochromatic signal applied to the medium.
The propagation of a two-component laser pulse in an optically uniaxial medium is investigated under the conditions of the Zakharov-Benney resonance (viz., resonance of long and short waves). The short-wave ordinary component of the pulse, which is in resonance with the atomic subsystem, effectively generates a video pulse of the extraordinary wave (long-wave component). The latter dynamically detunes the ordinary pulse from the resonance and causes its phase modulation due to nonzero diagonal matrix elements of the dipole moment. An approximate operator approach is proposed for solving constitutive equations for the density matrix, which is equivalent to the asymptotic WKB method and makes it possible to reduce the analysis to solving a system of nonlinear wave equations for both components of the pulse. The possibility an extraordinary wave video pulse being generated with the help of a quasimonochromatic ordinary pulse with a longer wave-length. It is shown that, when the ordinary component dominates, the self-induced transparency mode is realized; in the opposite limit, the effect known as extraordinary transparency takes place. Solitary pulses corresponding to the latter case experience a decrease in the velocity of propagation, which is similar to that observed for self-induced transparency and practically do not change the population of quantum levels. Physical situations reducing the initial system of constituent and wave equations to familiar integrable models are analyzed.
A theoretical investigation is made of collinear propagation of high-power optical pulses through a medium under conditions of two-photon resonance ω 0 ± ω s ≈ ω 21 ( ω 0 and ω s are the pulse frequencies, ω 21 is the frequency of an atomic transition in the medium). It is assumed that the condition for coherent interaction τ 0 , τ s < T 2 is satisfied ( τ 0 and τ s are the pulse durations at the entrance, T 2 is the phase relaxation time of the medium). By means of numerical integration of equations for the fields and the medium, it is shown that efficient generation of the harmonics ω 1 = 2 ω 0 ± ω s , ω 2 = 2 ω s ± ω 0 is possible under short and ultrashort pulse conditions.
Echo responses of a three-level medium formed by the λ-scheme of quantum transitions under exposure to optical pulses consisting of an arbitrary number of oscillations have been studied theoretically. The cases of pulses consisting of few optical oscillations (for which the concept of an envelope cannot be used) and combinations of such pulses and quasi-monochromatic resonance signals have been considered. The approach used can be reduced to the renormalization of dipole moments of allowed quantum transitions through their multiplication by coefficients depending on the shape and duration of pump pulses and having absolute values in the range from zero (for nonresonance pulses) to unity (for resonance quasi-monochromatic pulses and broadband pulses consisting of few oscillations, whose spectrum covers the quantum transitions). A general equation has been proposed for the pulse area. In the limit of a large number of oscillations, it transforms into the well-known definition of the area of a quasi-monochromatic signal. The characteristics of primary and longlived photon echoes have been analyzed in detail. It has been shown that, when a medium is exposed to only pulses consisting of a few oscillations, three echo responses of both types can be principally generated at each frequency of the λ-scheme. Introduction of quasi-monochromatic pulses in pump pulse series decreases the number of echoes, and their qualitative character has a non-commutative property with respect to pulse permutation in a series. The extension of the proposed approach to more complex schemes of quantum transitions with the large number of quantum levels faces no principal difficulties.
This paper presents an analytical study of high-order harmonic generation (HHG) by quantum systems possessing permanent dipole moments (PDMs), such as atoms/molecules placed in a static electric field or polar molecules. HHG by conventional, non-PDM systems typically demonstrated a plateau in the envelope of harmonics followed by a steep fall in harmonic intensities when the harmonic number exceeds a certain threshold. This paper shows that the HHG by PDM systems results in a significant extension of the plateau to higher frequencies and a slower decline of intensities at frequencies higher than the end of the plateau . Moreover, there occurs a substantial growth of the total, summed intensity of all components of the scattering spectrum . Other physically interesting distinctive features of the HHG by PDM systems are: the presence of both odd and even harmonics of the laser frequency in the scattering spectrum; a triplet structure of both odd and even harmonics; and the appearance of a component at the doubled Rabi frequency (i.e. at a frequency much lower than the laser frequency). The results are obtained by using the adiabatic basis for the analysis of a multi-quantum resonance in a two-level system possessing PDMs.