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Shortwavelength: Physics with Intense Laser Pulses

Transient Effects in Four-Wave Mixing

W. M. Schreiber, N. Chencinski

Published Jan 1, 1993• 0 citations
Publisher

Abstract

A formalism for four-wave mixing in the transient region, applicable to strong fields of short pulse duration, is developed. It is shown that transient effects can broaden resonance peaks and contribute to the appearance of extra resonances.
DOI
10.1364/swv.1993.fp100

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We show that extra resonances, such as those caused in frequency-domain nonlinear wave mixing by pure dephasing or laser fluctuations, can also be induced by operation in the time domain. These pulse-length-induced extra resonances arise in transient-grating experiments when the laser pulses are short enough that a steady state cannot be achieved during the excitation process. We show theoretically that these resonances increase in strength with decreasing excitation pulse length until the pulse length becomes shorter than the dephasing time of the medium and quote an experimental example to support this interpretation.
The general formalism of transient four-wave mixing is developed using the diagrammatic technique of Yee and Gustafson, and applied systematically to two-, three-, and four-level systems. The results predict all possible photon-echo phenomena including free-induction decay in the low-intensity limit. Connections to transient saturation spectroscopy and other coherent transient effects can also be made. The treatment can be readily extended to the more general problem of coherent transient optical effects with nnn waves.
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 use of picosecond lasers for degenerate four-wave mixing (DFWM) diagnostics of atmospheric pressure flames has been suggested as a means of overcoming the complicated collision-rate dependence of the DFWM signal in the nanosecond-laser pulse-length regime. In this paper DFWM spectroscopy in the regime in which the laser pulse length (τL) is less than the characteristic collisional time (τC) is investigated theoretically. DFWM signal levels for the phase-conjugate geometry (counterpropagating pump beams) are calculated by integration of the time-dependent density-matrix equations at numerous grid points along the phase-matching axis and by summing of the polarization contribution from each of these grid points. Both purely homogeneously broadened resonances and resonances that are both collision broadened and Doppler broadened are considered. DFWM signal generation for these two types of resonances in the fully transient regime (τL≪τC) is strikingly different. For a homogeneously broadened resonance, the DFWM signal persists long after the laser beam has passed through the medium. The decay rate of the DFWM signal is determined by the collision rate in the medium, and the integrated DFWM signal is still dependent on the collision rate even in this fully transient regime. However, when the Doppler broadening of the resonance is much greater than the collisional broadening, the DFWM signal decays with a fall time close to that of the laser pulse. For τL≪τC, we find that it is the laser spectral width, rather than the collisional width, that dictates the range of velocity groups with which the pulses effectively interact. The signal decays with a fall time close to that of the laser pulse because the excited velocity groups radiate out of phase with one another. In a medium in which the Doppler width is much greater than the collisional width, the DFWM reflectivity is independent of collision rate for τL≪τC, but the signal level is dependent on the Doppler width. Finally, we investigate the effect of different laser pulse lengths on reflectivity saturation curves for resonances with different levels of Doppler broadening.