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Acta Physica Sinica

Thermal background suppression in Rayleigh-type nondegenerate four-wave mixing based on field-correlation effects

孙江 Sun Jiang, Jiang Qian, Xin Mi, Zuhe Yu, Panming Fu, 中国科学院物理研究所光物理实验室,北京 100080

Published Jan 1, 2004• 0 citations
Publisher

Abstract

We apply the principle of field-correlation to the thermal background suppression of the Rayleigh-type nondegenerate four-wave mixing spectra,which have been employed for the measurement of ultrafast longitudinal time in the frequency-domain recently. Conditions,under which contributions from the thermal grating can be neglected,are given and numerical results that illustrate the validity of this method are presented.

DOI
10.7498/aps.53.450

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We apply the principle of field-correlation to the thermal background suppression of the Rayleigh-type nondegenerate four-wave mixing spectra,which have been employed for the measurement of ultrafast longitudinal time in the frequency-domain recently. Conditions,under which contributions from the thermal grating can be neglected,are given and numerical results that illustrate the validity of this method are presented.
We have studied theoretically the dependence of the Raman-enhanced nondegenerate four-wave-mixing (RENFWM) spectrum on the relative time delay between two pump beams \ensuremath{\tau} when a thermal effect exists in the sample. Using the chaotic model for the incident laser beams, we give the conditions that the thermal background can be eliminated completely when the relative time delay is much longer than the laser coherence time. In this limit, the theoretical RENFWM spectra show the normal asymmetry due to the interference between the Raman-resonant term and the nonresonant background originating solely from the molecular-reorientational grating. We then turn our attention to the dependence of the RENFWM signal intensity on the relative time delay when the laser frequencies are fixed. Our results indicate that RENFWM is asymmetric about \ensuremath{\tau}=0 and the maximum of the RENFWM signal does not occur at \ensuremath{\tau}=0. When the beating frequency between the pump beam and the probe beam is off resonant from the Raman mode, the RENFWM signal exhibits damping oscillation as the time delay increases. We also show that the temporal behavior of the RENFWM signal is drastically different if the laser sources are described by a phase-diffusion model. The different roles of the phase fluctuation and the amplitude fluctuation can be understood in the time domain.
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.
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.