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Chinese Physics

Raman-enhanced polarization beats with phase-conjugation geometry

Zhang Yan-peng, Xun Hou, Keqing Lu, WU Hong-cai

Published Dec 1, 2000• 2 citations
Publisher

Abstract

The Raman-enhanced polarization beats (REPB) with phase-conjugation geometry in carbon disulfide are investigated using chaotic and phase-diffusion models. The overall accuracy of using REPB to measure the resonant frequency of Raman-active vibrational mode is determined by the relaxation rates of the Raman mode and the molecular-reorientational grating. Different stochastic models of the laser field only affect the sixth- and fourth-order coherence function. The difference between the REPB and the fourth-order coherence on ultrafast modulation spectroscopy is discussed as well from a physical viewpoint.

DOI
10.1088/1009-1963/9/12/005

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The Raman-enhanced polarization beats (REPB) with phase-conjugation geometry in carbon disulfide are investigated using chaotic and phase-diffusion models. The overall accuracy of using REPB to measure the resonant frequency of Raman-active vibrational mode is determined by the relaxation rates of the Raman mode and the molecular-reorientational grating. Different stochastic models of the laser field only affect the sixth- and fourth-order coherence function. The difference between the REPB and the fourth-order coherence on ultrafast modulation spectroscopy is discussed as well from a physical viewpoint.
We have employed chaotic and phase-diffusion models to study the effects of laser fourth-order coherence on polarization beats with phase-conjugation geometry in a four-level system (PBFS). We found that the temporal behavior of the beat signal depends on the stochastic properties of the lasers and the transverse relaxation rate of the transition. The modulation terms of the beat signal depend on the second-order coherence function, which is determined by the laser line shape. Inasmuch as different stochastic models of the laser field affect only the fourth-order coherence function, they have little influence on the general temporal modulation behavior of the beat signal. The different roles of phase fluctuation and amplitude fluctuation are pointed out. The cases that pump beams have either narrow-band or broadband linewidth are considered, and it is found that for both cases a Doppler-free precision in the measurement of the energy-level difference between two states that are dipolar forbidden from the ground state can be achieved. We also discuss the difference between the PBFS and ultrafast modulation spectroscopy from a physical viewpoint.
The effect of fourth-order coherence on ultrafast modulation spectroscopy with phase-conjugation geometry (PCUMS) in a cascade three-level system is investigated using chaotic and phase-diffusion models. It has been found that the temporal behavior of the beat signal depends on the stochastic properties of the lasers and the transverse relaxation rate of the transitions, and the modulation terms of the beat signal depend on the second-order coherence function, which is determined by the laser line shape. Since different stochastic models of the laser field affect only the fourth-order coherence function, they have little influence on the general temporal modulation behavior of the beat signal. The different roles of the phase fluctuation and amplitude fluctuation can be investigated in the time domain. The cases where the pump beams have either a narrow or broad band linewidth are considered and it has been found that for both cases a Doppler-free precision in the measurement of the energy-level difference between two states can be achieved. The difference between the PCUMS and the DeBeer, UMS [D. DeBeer et al., Phys. Rev. Lett. 56, 1128 (1986)] is discussed as well from a physical viewpoint.
The correlation effects of fourth-order on polarization beats in a V-type three-level system (PBVTS) are investigated using chaotic and phase-diffusion models. It has been found that the temporal behaviour of the beat signal depends on the stochastic properties of the lasers and transverse relaxation rate of the transitions, and the modulation terms of the beat signal depend on the second-order coherence function, which is determined by the laser line shape. Since different stochastic models of the laser field affect only the fourth-order coherence function, they have little influence on the general temporal modulation behaviour of the beat signal. The different roles of the phase fluctuation and amplitude fluctuation have been pointed out in the time domain. The fourth-order coherence function theory of chaotic field is of vital importance in PBVTS. The cases where the pump beams have either narrow band or broadband linewidth are considered and it has been found that for both cases a Doppler-free precision in the measurement of the energy-level splitting between two states can be achieved. Finally, the difference between the PBVTS and DeBeer's ultrafast modulation spectroscopy is discussed as well from a physical viewpoint.
Based on three stochastic models, the subtle, Markovian field-correlation effects have been investigated in homodyne-detected attosecond sum-frequency Raman-enhanced polarization beating (REPB) and heterodyne-detected femtosecond difference-frequency REPB. The different roles of the amplitude fluctuations and the phase fluctuations have been pointed out in both time and frequency domains. Analytic closed forms of the sixth-order and fourth-order Markovian stochastic correlations are characterized for homodyne (quadratic) and heterodyne (linear) detection, respectively. The attosecond sum-frequency REPB signal shows resonant-nonresonant cross correlation, asymmetric temporal behavior, and drastic difference for three Markovian stochastic fields, and the autocorrelation of REPB exhibits hybrid-radiation-matter-detuning-terahertz damping oscillation. The phase-diffusion model predicts a damping oscillation of the signal around a constant value in the narrowband case. The heterodyne-detected signal of REPB potentially offers rich dynamic information about the homogeneous, broadening, material phase of the third-order nonlinear susceptibility.