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Journal of the Optical Society of America B

Broadband degenerate four-wave-mixing measurements

Stanislav G. Rozouvan

Published Aug 1, 2000• 2 citations
Publisher

Abstract

The nonlinear signal in a degenerate four-wave mixing experiment as a result of diffraction of a spatially distributed third-order nonlinearity is studied theoretically. The approach has been applied for the case of monochromatic and ultrashort pulses. As a consequence, the degenerate four-wave mixing signal is found to be independent of light-coherence parameters and cannot be explained as a product of diffraction on a dynamic grating. In this model only the fast component of the signal (the coherent artifact) is related directly to third-order nonlinear processes. The main features (the origins, temporal shapes, dependencies of pump intensity, and modulation effects) of the coherent artifact and a slow-decay component are discussed theoretically and experimentally.

DOI
10.1364/josab.17.001354

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The Journal of Chemical Physics•Sep 7, 2007•11 citations
The nonlinear signal in a degenerate four-wave mixing experiment as a result of diffraction of a spatially distributed third-order nonlinearity is studied theoretically. The approach has been applied for the case of monochromatic and ultrashort pulses. As a consequence, the degenerate four-wave mixing signal is found to be independent of light-coherence parameters and cannot be explained as a product of diffraction on a dynamic grating. In this model only the fast component of the signal (the coherent artifact) is related directly to third-order nonlinear processes. The main features (the origins, temporal shapes, dependencies of pump intensity, and modulation effects) of the coherent artifact and a slow-decay component are discussed theoretically and experimentally.
We present a time-resolved study of the diffracted pulse in degenerate four-wave mixing experiments with short-response-time materials. The first step is the validation of a theoretical model that takes into account the temporal characteristics of the energy level (relaxation time T1 and dephasing time T2) and of the incident pulse (duration and spectral phase) in a simple particular case. Two methods are used for characterizing the diffracted beam: the amplitude correlation with the reference pulse and the spectrum intensity measurements. We discuss the experimental results, which show good agreement with the theoretical model and evidence the strong influence of the incident pulse characteristics.
A systematic study of degenerate two-wave mixing in the stationary regime in thin nonlinear local-response media is presented. The model is based on the coherent interaction of four waves, the two incident beams, and the two main diffracted waves. Analytical results are obtained in all cases investigated under the assumption of weak-beam amplification. It is demonstrated that the energy transfer arises only from the forward degenerate four-wave mixing terms. In particular, the theoretical results show two new features: (1) the gain factor of the interaction is substantially reduced because of the phase change associated with the two-wave mixing terms and (2) a phase mismatch can compensate for this phase change, leading to an appreciable gain enhancement. Moreover, the general case is solved numerically. Particular attention is given to the influence of separate two-wave and forward degenerate four-wave mixing terms. Self-diffraction effects and the gain dependence versus the ratio of the pump-beam intensity to the signal-beam intensity are investigated.
In this work the different schemes of propagation and interaction of the light beams in nonlinear Fabry-Perot interferometer have been studied theoretically and experimentally. Degenerate and non-degenerate four-wave mixing have been realized in the cavity of Fabry-Perot type using Rhodamine-6G dye and polymethine dye 3274U solution as saturable absorber. The diffraction efficiency of intracavity dynamic grating has been studied in dependence on intensity of interacting beams and parameters of resonator. The theoretical model of the processes of intracavity degenerate and non-degenerate four-wave mixing has been developed and applied to the analysis of the efficiency of light beams conversion by mean of Bragg diffraction from intracavity dynamic gratings. For theoretical description of typical experimental situations we used the round-trip model of nonlinear interferometer adapted for the geometry of degenerate four-wave mixing, which can be realized in the scheme of symmetrical oblique incidence of pump, signal and probe beams to the front and back mirrors of cavity.
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.
We show that four-wave mixing in optically dense media is very different than in an optically thin medium. In time-resolved degenerate four-wave mixing we experimentally observe ``negative'' time delay response, fast decay rates at short delay times, and broad shoulders at long delays. The observations are explained very well in terms of pulse propagation effects, and a theoretical framework is presented for the analysis of the nonlinear interaction. We treat both the incident and generated fields self-consistently, and solve for the interaction of short pulses with a resonantly absorbing medium. The implications for the extraction of relaxation rates from four-wave-mixing experiments involving ultrashort pulses in optically dense matter are discussed.
A two-pulse degenerate four-wave mixing experiment is analyzed in the case where the medium under investigation can be modeled by two-level systems having unequal permanent dipole moments. By modeling the light pulses by double exponentials [exp(-Gamma/t/)], we give an analytical expression of the third-order nonlinear polarization of the medium. We apply this result to simulate the measured signal in such experiment. We show that in the case of a two-photon transition, a signal can be detected if the pump pulse interacts with the medium before the probe pulse contrary to what is observed for excitations in the resonance region. An attempt to explain this behavior is made and the detected signal is analyzed in terms of pure coherent processes. This effect appears as a signature of the presence of permanent dipole moments. To test this property on a more realistic system, we then have considered a one-dimensional frequency-selected infrared degenerate four-wave mixing experiment on a molecular anharmonic vibrational mode modeled by a Morse potential and coupled to a dissipative bath of harmonic oscillators. We show that the two-photon transitions allowed by the presence of permanent dipole moments enable to analyze the multilevel system dynamics as if they were the one of a two-level system. Our results can also be extended to the case of inhomogeneous broadening and are of interest to study the infrared photon-echo response of anharmonic vibrational modes.