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Physical Review Letters

Rayleigh-Type Nondegenerate Four-Wave Mixing: Ultrafast Measurement and Field Correlation

Panming Fu, Qiang Jiang, Xin Mi, Zuhe Yu

Published Mar 5, 2002• 25 citations
Publisher

Abstract

We report on an ultrafast longitudinal time measurement by a nonresonant Rayleigh-type nondegenerate four-wave mixing (NFWM). We investigated the field-correlation effects on Rayleigh-type NFWM by examining the time-delayed dependence of the NFWM spectra. Based on the field-correlation effects, a time-delayed method is proposed to suppress the thermal effect, and ultrafast relaxation time can be measured even in an absorbing medium.

DOI
10.1103/physrevlett.88.113902

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Physical Review A•Jul 18, 2005•19 citations
We report on an ultrafast longitudinal time measurement by a nonresonant Rayleigh-type nondegenerate four-wave mixing (NFWM). We investigated the field-correlation effects on Rayleigh-type NFWM by examining the time-delayed dependence of the NFWM spectra. Based on the field-correlation effects, a time-delayed method is proposed to suppress the thermal effect, and ultrafast relaxation time can be measured even in an absorbing medium.
The effects of field correlation on Raman-enhanced nondegenerate four-wave mixing (RENFWM) have been investigated by examining the RENFWM spectra as a function of time delay between two beams. We present a theory in which the underlying physics is emphasized. The field correlation has little influence on the RENFWM spectra when the laser has narrow bandwidth. In contrast, the ratio between the resonant and nonresonant RENFWM signal intensities increases as time delay is increased when the laser has broadband linewidth. Experiments with CS2{\mathrm{CS}}_{2}CS2​ as sample have been performed to demonstrate the field-correlation effects on the RENFWM spectra.
We have employed phase-diffusion model to study the effects of laser field correlation on the Raman-enhanced nondegenerate four-wave mixing (RENFWM). The different roles of the field fluctuations have been pointed out. A time-delayed method has been proposed to suppress the thermal background. An enhancement of the ratio between the resonant and nonresonant RENFWM signal intensities was found as the time delay is increased when the laser has broadband linewidth. When the lasers have Gaussian line shape, we also present a second-order coherence function theory to elucidate the temporal asymmetry behavior of the RENFWM.
Based on color-locking noisy field correlation, a time-delayed method is proposed to suppress the thermal effect, and the ultrafast longitudinal relaxation time can be measured even in an absorbing medium. One interesting feature in field-correlation effects is that Rayleigh-enhanced four-wave mixing (RFWM) with color-locking noisy light exhibits spectral symmetry and temporal asymmetry with no coherence spike at $\ensuremath{\tau}=0$. Due to the interference between the Rayleigh-resonant signal and the nonresonant background, RFWM exhibits hybrid radiation-matter detuning with terahertz damping oscillations. The subtle Markovian high-order correlation effects have been investigated in the homodyne- or heterodyne-detected Rayleigh-enhanced attosecond sum-frequency polarization beats (RASPBs). Analytic closed forms of fourth-order Markovian stochastic correlations are characterized for homodyne (quadratic) and heterodyne (linear) detection, respectively. Based on the polarization interference between two four-wave mixing processes, the phase-sensitive detection of RASPBs has also been used to obtain the real and imaginary parts of the Rayleigh resonance.