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Optics and Spectroscopy

Free polarization decay in media with a short-range dipole-dipole interatomic interaction

Oleg Kh Khasanov, Русецкий Григорий Александрович, Anatoly A. Afanas'ev, R. A. Vlasov, T. V. Smirnova, Olga M. Fedotova

Published Oct 1, 2003• 1 citation
Publisher

Abstract

The effect that may be exerted by an interatomic dipole-dipole interaction upon optical transient processes in dense resonance media, in particular, free polarization decay, is analyzed. The behavior of the macroscopic polarization after a single-pulse excitation of a dense ensemble of two-level atoms is considered. It is shown that the free polarization signal is of oscillatory nature, with the oscillation frequency varying in time and being dependent on the dipole-dipole interaction constant, the intensity and duration of the exciting pulse, and the detuning of its carrier frequency from the resonance. The free polarization signal decay, which depends on the magnitude and sign of the sum of the detuning of the exciting pulse carrier frequency from the resonance and the Lorentz frequency, may obey either a power or an exponential law. The signal decay rate is determined not only by the inhomogeneous broadening, but also by the ratio of the above parameters.

DOI
10.1134/1.1621450

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The effect that may be exerted by an interatomic dipole-dipole interaction upon optical transient processes in dense resonance media, in particular, free polarization decay, is analyzed. The behavior of the macroscopic polarization after a single-pulse excitation of a dense ensemble of two-level atoms is considered. It is shown that the free polarization signal is of oscillatory nature, with the oscillation frequency varying in time and being dependent on the dipole-dipole interaction constant, the intensity and duration of the exciting pulse, and the detuning of its carrier frequency from the resonance. The free polarization signal decay, which depends on the magnitude and sign of the sum of the detuning of the exciting pulse carrier frequency from the resonance and the Lorentz frequency, may obey either a power or an exponential law. The signal decay rate is determined not only by the inhomogeneous broadening, but also by the ratio of the above parameters.
The effect that may be exerted by an interatomic near dipole-dipole interaction upon optical transient processes in dense resonance media is analyzed. The behavior of the macroscopic polarization after a one-pulse excitation of a dense ensemble of two-level atoms is considered. It is shown that the free polarization signal is of oscillatory nature, with the oscillation frequency varying in time and being dependent on the dipole-dipole interaction constant, the intensity and duration of the exciting pulse, and the detuning of its carrier frequency from the resonance. The free polarization signal decay, which depends on the magnitude and sign of the sum of the detuning of the exciting pulse carrier frequency from the resonance and the Lorentz frequency, may obey either a power or an exponential law. The signal decay rate is determined not only by the inhomogeneous broadening, but also by the ratio of the above parameters. The peculiarities of echo-responses under one- or two-pulse excitation conditions are studied.
The near dipole-dipole interatomic interaction effect on transients in dense Yb vapors is considered. The influence of excitation-induced-dephasing as well as the frequency shift on signals of nonstationary nutation, free polarization decay and photon echo are taken into account. The conditions of intrinsic optical bistability occurrence in dense resonant media are discussed. The local field is shown to result in multiple single-pulse echo signals. Besides, in such media one can observe a lot of primary photon echo responses under various phase-matching conditions.
Abstract The optical effect of free polarization decay in an ultrathin gas cell the inner thickness of which is less than or of the order of the wavelength of the exciting monochromatic laser pulse transmitted orthogonally to plane-parallel walls of this cell is studied theoretically. A new mechanism of the studied effect is established; it is caused by the specificity of phase mismatch of light-induced atomic dipole moments due to transit-time relaxation of atoms in such a cell. As a result, the dynamics of free polarization decay in the considered situation radically differs from the known case in a usual (macroscopic) gas cell. Nontrivial oscillatory dependences of free polarization decay signals on the ratio of the thickness of such ultrathin cell to the radiation wavelength of the exciting pulse are revealed and analyzed.
The optical density of a resonant medium significantly affects the output signal in time resolved nonlinear optical interactions. The resonant interaction with a medium reshapes any propagating short pulse, and the mutual interaction of several such pulses, as in four-wave mixing, must be treated self-consistently. We present a theoretical framework for the proper handling of the propagation of all pulses, input as well as generated, in the small area limit. For optically thick resonant absorbers, negative time delay signals are observed, and the apparent decay rate of the induced polarization is faster than the rate observed for thin samples. We experimentally measure degenerate four-wave mixing in an atomic medium as an example, and demonstrate the quality of the theoretical model by the excellent fit to measured signals over several orders of magnitude. The improved understanding enables us to provide a simple, but surprisingly accurate, estimate for the apparent decay rate in homogeneously broadened optically thick media: If the absorption is given by \ensuremath{\alpha}, the propagation length is L, and the transverse relaxation time is T2{\mathit{T}}_{2}T2​, the apparent decay rate 2/Ta{\mathit{T}}_{\mathit{a}}Ta​ of a time resolved four-wave mixing signal is given by 2/Ta{\mathit{T}}_{\mathit{a}}Ta​=(2/T2{\mathit{T}}_{2}T2​)(1+\ensuremath{\alpha}L/2).