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Chinese Physics Letters

Effects of Field-Correlation on Raman-Enhanced Nondegenerate Four-Wave Mixing Spectra

Xin Mi, Zuhe Yu, Jiang Qian, Li Xiaofeng, Panming Fu

Published Apr 1, 1997• 1 citation
Publisher

Abstract

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. An enhancement of the ratio between the resonant and nonresonant RENFWM signal intensities was found as the time delay was increased when the laser had broadband linewidth.

DOI
10.1088/0256-307x/14/4/011

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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. An enhancement of the ratio between the resonant and nonresonant RENFWM signal intensities was found as the time delay was increased when the laser had broadband linewidth.
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.
We report an experiment of the time-delayed Raman-enhanced nondegenerate four-wave mixing (RENFWM) with a broadband laser in carbon disulfide (CS2{\mathrm{CS}}_{2}CS2​). We studied the RENFWM signal intensity as a function of the relative time delay \ensuremath{\tau} between two beams which originate from a single broadband laser source. Our results indicate that the temporal behavior of the RENFWM is asymmetric with the maximum of the signal shifted from \ensuremath{\tau}=0. Furthermore, unlike the corresponding coherent Stokes Raman scattering (CSRS) no coherent spike appears at \ensuremath{\tau}=0. From our experimental results the relaxation time of the Raman mode can be extracted directly. We present a second-order coherence function theory to elucidate the physics of the basic features of the time-delayed RENFWM. We also discuss the difference between the RENFWM and the CSRS from a physical viewpoint.
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.