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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Nonlinear optics at maximum coherence

Alexei V. Sokolov, G. Y. Yin, Stephen E. Harris

Published Oct 21, 1998• 1 citation
Publisher

Abstract

We describe nonlinear optical processes in a medium with maximal coherence on a Raman transition. The nonlinear polarization of such a medium is of the same order of magnitude as the linear polarization. This allows efficient frequency conversion and generation of a wide spectrum of Raman sidebands. The phase of the coherence can be controlled through a small two-photon detuning from the Raman resonance. An appropriate choice of the phase improves nonlinear generation and propagation of sidebands through an inhomogeneous gaseous medium.

DOI
10.1117/12.328253

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We describe nonlinear optical processes in a medium with maximal coherence on a Raman transition. The nonlinear polarization of such a medium is of the same order of magnitude as the linear polarization. This allows efficient frequency conversion and generation of a wide spectrum of Raman sidebands. The phase of the coherence can be controlled through a small two-photon detuning from the Raman resonance. An appropriate choice of the phase improves nonlinear generation and propagation of sidebands through an inhomogeneous gaseous medium.
We describe a method for generating a wide spectrum and at the same time improving propagation through a model inhomogeneous gaseous medium. The method is based on using a small two-photon detuning from a Raman resonance to adiabatically establish an appropriate molecular superposition state. This state, in turn, generates a broad spectrum of sidebands whose refractive index, Rayleigh scatter, and accumulated phase delay are much less than those of a single spectral component, if propagating alone.
Recent experiments have shown that coherent molecular oscillations may generate a comb of coherent collinear sidebands with 50,000 cm/sup -1/ of spectral bandwidth. The essence of this technique is the use of a Raman transition with a sufficiently large coherence that the generation and phase slip length are of the same order. The coherence is established by driving the molecular transition with two single-mode laser fields slightly detuned from the Raman resonance, so as to excite a single molecular superposition state. This talk will summarize the characteristics of this light source and describe two recent experiments which show the mutual coherence of the generated sidebands.
We study the generation of subfemtosecond pulses with the molecular coherence control in stimulated Raman scattering. We show analytically that the antiphased state temporally advances the higher frequencies with respect to the lower frequencies during a beating cycle. After some propagation distance, due to the dispersion and the difference between the antiphased and phased states in advancing high or low frequencies, the coherence is highest on the negative side of the detuning, when the two-photon Rabi frequency is about equal to the detuning. This asymmetry of the coherence magnitude with respect to the negative and positive sides of the Raman detuning is reflected in the behavior of the tuning characteristics of the high-order frequency components. When the Raman detuning is small, although the process is nonadiabatic, the subfemtosecond pulse generation may occur for both negative and positive sides of the detuning.