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Journal of Experimental and Theoretical Physics

Collective generation of higher optical harmonics by dipole molecules

Viktor A Kovarskii, O. B. Prepelitsa

Published Jul 1, 2000• 0 citations
Publisher

Abstract

An analysis is made of the collective resonant generation of higher harmonics by a spatially extended system of two-level molecules possessing an intrinsic electron dipole moment in the excited state. Frequency and angular dependences of the scattered radiation are studied. It is shown that for moderately small numbers of harmonics their intensity depends comparatively weakly on the number (plateau) and the intensity of the emitted harmonics then falls sharply as the number increases. The angular distribution of the harmonics is strongly anisotropic. It is also shown that collective effects significantly change the time profile of the generated harmonic pulse. In addition, as a result of cooperative effects harmonics of a certain parity are suppressed in the low-frequency part of the radiation spectrum.

DOI
10.1134/1.1307236

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An analysis is made of the collective resonant generation of higher harmonics by a spatially extended system of two-level molecules possessing an intrinsic electron dipole moment in the excited state. Frequency and angular dependences of the scattered radiation are studied. It is shown that for moderately small numbers of harmonics their intensity depends comparatively weakly on the number (plateau) and the intensity of the emitted harmonics then falls sharply as the number increases. The angular distribution of the harmonics is strongly anisotropic. It is also shown that collective effects significantly change the time profile of the generated harmonic pulse. In addition, as a result of cooperative effects harmonics of a certain parity are suppressed in the low-frequency part of the radiation spectrum.
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.
The theory of coherent radiation emission in two-level quantum systems with permanent dipole moments at the multiphoton resonant excitation by moderately strong laser fields is presented. A simple analytic formula for the expectation value of a dipole moment operator is obtained. The spectrum corresponding to harmonic generation and low-frequency radiation on the generalized Rabi frequency is investigated both analytically and numerically. The effect of dynamic Stark shift on a dipole spectrum under direct multiphoton resonant excitation is considered.
The phase relationship between an induced atomic dipole moment and a driving laser field is an essential aspect of high harmonic generation (HHG) in a dense medium. A ``phase-matching'' criterion must be fulfilled to obtain coherent amplification of harmonic radiation, which is critical for practical HHG. We have performed numerical calculations on model atoms to survey the intensity dependence of the phase in the case of strong one- or two-frequency laser fields. The calculations show that multiphoton resonances significantly affect the yield of harmonic generation and that in the ``plateau'' regime, the phases exhibit only weak dependence upon the intensity of the driving field. \textcopyright{}1996 The American Physical Society.
The effect of a double structure of saturated absorption resonance in the field of counterpropagating light waves interacting with an atomic gas is studied. The experimental observation of this effect was first reported in 2011 in a work by our colleagues at the P.N. Lebedev Physical Institute of the Russian Academy of Sciences (Laboratory of Frequency Standards). The essence of the effect lies in the fact that, on exciting an open dipole transition, another, narrower, resonance of an opposite sign can be observed at the center of the ordinary saturated absorption resonance. A theoretical analysis of this effect has also been performed in this work in terms of a simple spectroscopic model of an atom with two nondegenerate energy levels without taking into account higher spatial harmonics of atomic polarization and polarizations of light waves (scalar model). The present work is devoted to the development of a theory of the formation of a central narrow resonance for the example of a real F g = 1 → F e = 1 atomic transition and to the study of its main characteristics (amplitude, width, contrast, and amplitude-to-width ratio). In addition, the theoretical results obtained without taking into account the influence of higher spatial harmonics and with inclusion of the influence of first higher harmonics are compared. This comparison shows that their influence on the parameters of the new nonlinear resonance is strong even in moderately intense light fields (R ~ γ, where R is the Rabi frequency). The results of this study can be of interest for quantum metrology, as well as for many experiments in which the laser-radiation frequency is stabilized by the saturated absorption resonance on open dipole transitions in atoms and molecules.