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Optics and Spectroscopy

Modulation of the carrier frequencies (chirp) and spectra of waves in nonstationary four-photon parametric scattering

B. V. Kryshanovskii

Published Sep 1, 1990• 0 citations
OpenAlex

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Effects of nonlinear phase modulation on Bragg scattering in the low-conversion regime

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In this paper, we consider the effects of nonlinear phase modulation on frequency conversion by four-wave mixing (Bragg scattering) in the low-conversion regime. We derive the Green functions for this process using the time-domain collision method, for partial collisions, in which the four fields interact at the beginning or the end of the fiber, and complete collisions, in which the four fields interact at the midpoint of the fiber. If the Green function is separable, there is only one output Schmidt mode, which is free from temporal entanglement. We find that nonlinear phase modulation always chirps the input and output Schmidt modes and renders the Green function formally nonseparable. However, by pre-chirping the pumps, one can reduce the chirps of the Schmidt modes and enable approximate separability. Thus, even in the presence of nonlinear phase modulation, frequency conversion with arbitrary pulse reshaping is possible, as predicted previously [Opt. Express 20, 8367-8396 (2012)].

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Chirped four-wave mixing

Koos Duppen, Foppe de Haan, Erik T. J. Nibbering +1 more

We will demonstrate that four-wave mixing with linearly chirped (phase-modulated) pulses is a unique tool for obtaining information on the dynamics and level structure of a system. Especially, it will be shown that the transient-grating-scattering type of experiment with chirped pulses provides an immediate answer to the question of whether the dynamics of a system occurs on a fast and/or slow time scale. In addition, we present compelling evidence that chirped four-wave mixing in a molecular system is a viable method for measuring excited-state vibrational frequencies. Double-sided Feynman diagrams are used for a third-order perturbative calculation of two-level four-wave-mixing effects and chirped coherent Raman scattering. The diagrams provide a visual representation of the quantum-mechanical pathways that the system can take as a result of the different field interactions. The number of quantum-mechanical pathways that contribute to the signal is shown to depend on the chirp rate compared to the time scale(s) of the system dynamics. A stochastic model is used to describe the optical dynamics of the system. The resulting expressions for the third-order nonlinear polarization are so complex that numerical calculations are necessary to simulate the time dependence of the optical response. It will also be shown that our theoretical results in the appropriate limits converge to those obtained for impulsive or continuous-wave excitation.

Physical Review A•Jun 1, 1993•65 citations
In this paper, we consider the effects of nonlinear phase modulation on frequency conversion by four-wave mixing (Bragg scattering) in the low-conversion regime. We derive the Green functions for this process using the time-domain collision method, for partial collisions, in which the four fields interact at the beginning or the end of the fiber, and complete collisions, in which the four fields interact at the midpoint of the fiber. If the Green function is separable, there is only one output Schmidt mode, which is free from temporal entanglement. We find that nonlinear phase modulation always chirps the input and output Schmidt modes and renders the Green function formally nonseparable. However, by pre-chirping the pumps, one can reduce the chirps of the Schmidt modes and enable approximate separability. Thus, even in the presence of nonlinear phase modulation, frequency conversion with arbitrary pulse reshaping is possible, as predicted previously [Opt. Express 20, 8367-8396 (2012)].
An analysis was made of four-photon interaction processes under conditions of two-photon resonance excitation of the 3 D sodium level by two-frequency radiation from a single-pulse picosecond YAG:Nd laser with frequency doubling and a KDP optical parametric oscillator. The spatial and frequency spectra of the four-photon parametric scattering (FPPS) were recorded and studied experimentally at various sodium vapor densities (10 15 –10 17 cm −3 ) and also using collinear and noncollinear excitation. It was found that the observed conical structure of the FPPS radiation may be interpreted by an analysis of whether the frequency and spatial phase-matching conditions were satisfied. Dependences of the intensity of the FPPS radiation on the intensity of the exciting radiation, the sodium vapor density, and the detuning of the exciting radiation frequency from the two-photon resonance were obtained.
We will demonstrate that four-wave mixing with linearly chirped (phase-modulated) pulses is a unique tool for obtaining information on the dynamics and level structure of a system. Especially, it will be shown that the transient-grating-scattering type of experiment with chirped pulses provides an immediate answer to the question of whether the dynamics of a system occurs on a fast and/or slow time scale. In addition, we present compelling evidence that chirped four-wave mixing in a molecular system is a viable method for measuring excited-state vibrational frequencies. Double-sided Feynman diagrams are used for a third-order perturbative calculation of two-level four-wave-mixing effects and chirped coherent Raman scattering. The diagrams provide a visual representation of the quantum-mechanical pathways that the system can take as a result of the different field interactions. The number of quantum-mechanical pathways that contribute to the signal is shown to depend on the chirp rate compared to the time scale(s) of the system dynamics. A stochastic model is used to describe the optical dynamics of the system. The resulting expressions for the third-order nonlinear polarization are so complex that numerical calculations are necessary to simulate the time dependence of the optical response. It will also be shown that our theoretical results in the appropriate limits converge to those obtained for impulsive or continuous-wave excitation.