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Journal de physique

Fourth-order coherence-function theory of laser-induced molecular reorientational grating and population grating

Panming Fu, Zuhe Yu, Xin Mi, Peixian Ye

Published Jan 1, 1987• 15 citations
Publisher

Abstract

We have employed fourth-order coherence-function theory to study the influence of the partial-coherence properties of pump beams on the laser-induced gratings. First, we examine the formation of molecular reorientational grating. The different roles of phase fluctuation and amplitude fluctuation have been pointed out. A time-delayed method has been proposed to distinguish molecular reorientational grating from thermal grating. We then apply the fourth-order theory to study the Bragg reflection from a population grating. We obtain an analytic solution which enables us to make an extensive investigation on the temporal behaviour of the Bragg reflection signal. This study is especially helpful for elucidating the generation mechanism of population grating.

DOI
10.1051/jphys:0198700480120208900

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We have employed fourth-order coherence-function theory to study the influence of the partial-coherence properties of pump beams on the laser-induced gratings. First, we examine the formation of molecular reorientational grating. The different roles of phase fluctuation and amplitude fluctuation have been pointed out. A time-delayed method has been proposed to distinguish molecular reorientational grating from thermal grating. We then apply the fourth-order theory to study the Bragg reflection from a population grating. We obtain an analytic solution which enables us to make an extensive investigation on the temporal behaviour of the Bragg reflection signal. This study is especially helpful for elucidating the generation mechanism of population grating.
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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.
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 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 present a theoretical study of the induced transient birefringence of a low density homogeneous molecular gas in a resonant pump–probe experiment. The molecular coherent state induced by the resonant pump field is described by second-order perturbation theory. The induced birefringence can be detected by a delayed probe pulse propagating through the molecular medium after illumination by the pump pulse. In the case of a nonresonant probe, the birefringence is linearly proportional to the mean value of the electronic polarizability of the molecular gas. The birefringence signal is composed of distinct components due to population change and those of rotational, vibrational, and mixed vibrational–rotational origins. This is demonstrated by numerical simulations on Li2 gas. Moreover, the quantum beats contained in the birefringence, as a function of the time delay between the pump and probe pulses, is dominated by the pure rotational motion. Finally, the birefringence is sensitive to the shape of the applied pump pulse and dependent on the spectral phase of the pump pulse.