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Journal of the Optical Society of America

Degenerate four-wave mixing in p-type germanium: an absorbing medium

David E. Watkins, Claude Phipps

Published May 1, 1983• 5 citations
Publisher

Abstract

We present the results of degenerate four-wave mixing (DFWM) studies in three samples of p-type Ge with a wide range of absorptive properties. Three mechanisms for DFWM are observed in this material. A model, which includes the mechanisms of the inhomogeneously broadened saturable absorption of p-type Ge and the optical Kerr effect that is due to bound electrons in Ge but not the mechanism of bulk plasma formation that occurs only at extremely high pump intensities, is developed and compared with the experimental results. Pump-beam attenuation by the medium is shown to be an important effect in modeling DFWM. The model, which has no free parameters, fits the experimental data well for samples with small-signal transmission of greater than 20%.

DOI
10.1364/josa.73.000624

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We present the results of degenerate four-wave mixing (DFWM) studies in three samples of p-type Ge with a wide range of absorptive properties. Three mechanisms for DFWM are observed in this material. A model, which includes the mechanisms of the inhomogeneously broadened saturable absorption of p-type Ge and the optical Kerr effect that is due to bound electrons in Ge but not the mechanism of bulk plasma formation that occurs only at extremely high pump intensities, is developed and compared with the experimental results. Pump-beam attenuation by the medium is shown to be an important effect in modeling DFWM. The model, which has no free parameters, fits the experimental data well for samples with small-signal transmission of greater than 20%.
Detailed measurements have been made of degenerate four-wave mixing (DFWM) in a resonant homogeneously broadened gas. The measurements were performed in SF6{\mathrm{F}}_{6}F6​ using a pulsed CO2{\mathrm{O}}_{2}O2​ laser operated on the 10.4-\ensuremath{\mu} m branch. A pulse width of 1.2 nsec was used to reduce effects of collisional relaxation. Data are also presented for pulse widths of 140 nsec. At high-energy fluences (\ensuremath{\sim}0.1 J/cm2{\mathrm{cm}}^{2}cm2) pulse breakup is observed and is believed to arise from multiple-photon effects. The data obtained with the short pulse width are compared to a four-level saturable-absorber model where excellent agreement is obtained when pump absorption is included. The qualitative behavior of DFWM due to dispersion is also demonstrated in the wings of the SF6{\mathrm{F}}_{6}F6​ absorption spectrum. Peak reflectivities of 38% were readily obtained. In addition contributions due to a coherent three-level nonlinearity are presented showing a contribution equal to the measured saturable contribution.
The transient behavior of degenerate four-wave mixing (DFWM) in a three-level saturable absorber is analyzed and verified experimentally. A sharp peak of phase-conjugated reflectivity is predicted and observed at high pump intensities for pulsed beams. The influence of the time-dependent behavior of the conjugate wave signal on results of pulsed-beam experiments is studied. It is shown that transient effects could account for discrepancies between previous experimental results and steady-state theory.
We have investigated degenerate four-wave mixing (DFWM) in a strongly absorbing molecular gas. A theory taking into account saturable absorption of the interacting beams is used to explain the dependence of the DFWM reflectivity on laser intensity and on the molecular number density. These parameters have a great influence on the observed spectra, owing to linear absorption that suppresses the DFWM signal in the line center of the molecular transitions. The great sensitivity of the spectra to the experimental conditions limits the applicability of DFWM for spectroscopic studies in absorbing media.
Saturation effects in gas-phase degenerate four-wave mixing (DFWM) are investigated for conditions of interest for diagnostic applications in flames and plasmas. In particular, the case in which Doppler and collisional broadening are comparable, as is often the case for flame species such as NO and OH, is investigated. DFWM line shapes and signal intensities are calculated nonperturbatively and compared with high-resolution laser measurements. In the nonperturbative calculations the time-dependent density-matrix equations for a two-level system interacting with three laser fields are integrated directly on a grid of spatial locations along the phase-matching axis. The electric-field amplitude for the DFWM signal is determined by multiplying the time-varying, laser-induced polarization at each grid point by the appropriate phase factor and then by summing over all grid points. The calculations are in excellent agreement with measurements of DFWM line shapes and signal intensities for NO in a buffer gas of He over a wide range of He pressure. Under saturation conditions the pressure dependence of the DFWM signal is reduced greatly compared with the unsaturated case. The signal level is still dependent on the ratio of pure dephasing to quenching collisions, even for saturation conditions. From the standpoint of minimal dependence on collisional processes it appears that operation with pump-laser intensities approximately equal to the saturation intensity is optimal. The dependence of the DFWM line shape and signal intensity on the ratio of probe to pump-laser intensity is also investigated.
A model of degenerate four-wave mixing (DFWM) in Cr4+:YAG saturable absorbers is given in the transient regime. Because of the presence of absorbing dipoles oriented along specific directions, the DFWM process exhibits an anisotropic behavior. The effects of pump beam fluences, relative polarization of the beams, crystal orientation, absorbance, excited-state absorption, and nonresonant losses are analyzed. The theoretical results are supported by DFWM experiments in Cr4+:YAG performed at 1.06 µm with nanosecond pulses.
Nowadays degenerate four wave mixing (DFWM) with forward geometry (FDFWM) has found increasing usage, for example, in the gas phase detection. In the fields of theoretical development of DFWM, most of the studies have been concentrated on the understanding of phase-conjugated DFWM. However, few theories have dealt with FDFWM. These models calculated the signal directly from the off-diagonal element of the density matrix by assuming optically thin medium. In the paper we obtain a theoretical model for FDFWM in Doppler broadened two-level absorbers including propagation effect and discuss the Doppler effect on the signal intensity and lineshape. Assuming that probe and signal field amplitudes are small compared with those of the pump fields and pump field amplitudes are constant in the interaction volume, we obtain the following coupled equations from the Maxwell equation using the slowly varying envelope approximation and the paraxial approximation.