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Optics Communications

Study of Time-Delayed Four-Wave Mixing with Incoherent Light in the absorption band of ruby

Ruihua Zhang, Xin Mi, Haitian Zhou, Peixian Ye

Published Aug 1, 1988• 9 citations
Publisher
DOI
10.1016/0030-4018(88)90218-0

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A series of experiments of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands of ruby and dye molecules at 300 K-20 K are reported, which demonstrate that two-level theory fails in the interpretation of the results, and that our multilevel theory of TDFWM-IL should be applied. The following experimental results are emphasized: the normalized delay-time dependences of the signal intensity IS (τ) are not dependent on the sample temperature from 80 K to 300 K for the pump-beam wavelengths not closed to the zero-phonon line or the absorption edge as the power spectrum S0(ω) of the incoherent light source kept invariable; at low temperature of 20 K, IS(τ) is modulated periodically with a period equal to the interval of two adjacent vibrational transitions in the absorption band 4T2 of ruby, as predicted by the multilevel theory. The experiments performed at the zero-phonon line of ruby and at the absorption edge of Cresyl Violet in PMMA demonstrate that the effective two-level model is suitable to approximately analyze not only the experimental results of TDFWM-IL in the unresolved continuous absorption bands with homogeneous broadening, but also the effects of inhomogeneous broadening on the behavior of TDFWM-IL in these bands. Additionally, some data of the subpicosecond dephasing processes of these materials are also obtained for the first time.

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In this paper, our multi-level theory of time-delay four wave mixing with incoherent light (TDFWM-IL) developed previously for the case of homogeneous broadening system has been extended to a generally inhomogeneous broadening case. From the present theory, a general expression of signal intensity for absorption band with both homogeneous and inhomogeneous broadening is given as a function of mutual time delay τ between two pump beams. Photon echo with incoherent light under the condition of extremely inhomogeneous broadening is discussed, and the difference of results obtained scperately from multi-level and two-level theory is pointed out. It has been demonstrated that the experiment of TDFWM-IL can also be analysed approximately by using an effective two-level model when a weak effect of inhomogeneous broadening of absorption band exists. Finally, our experimental results of TDFWM-IL obtained at zero-phonon line of ruby and absorption edge of cresyl violet film in PMMA are also presented and compared with the theory mentioned above.

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A series of experiments of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands of ruby and dye molecules at 300 K-20 K are reported, which demonstrate that two-level theory fails in the interpretation of the results, and that our multilevel theory of TDFWM-IL should be applied. The following experimental results are emphasized: the normalized delay-time dependences of the signal intensity IS (τ) are not dependent on the sample temperature from 80 K to 300 K for the pump-beam wavelengths not closed to the zero-phonon line or the absorption edge as the power spectrum S0(ω) of the incoherent light source kept invariable; at low temperature of 20 K, IS(τ) is modulated periodically with a period equal to the interval of two adjacent vibrational transitions in the absorption band 4T2 of ruby, as predicted by the multilevel theory. The experiments performed at the zero-phonon line of ruby and at the absorption edge of Cresyl Violet in PMMA demonstrate that the effective two-level model is suitable to approximately analyze not only the experimental results of TDFWM-IL in the unresolved continuous absorption bands with homogeneous broadening, but also the effects of inhomogeneous broadening on the behavior of TDFWM-IL in these bands. Additionally, some data of the subpicosecond dephasing processes of these materials are also obtained for the first time.
In this paper, our multi-level theory of time-delay four wave mixing with incoherent light (TDFWM-IL) developed previously for the case of homogeneous broadening system has been extended to a generally inhomogeneous broadening case. From the present theory, a general expression of signal intensity for absorption band with both homogeneous and inhomogeneous broadening is given as a function of mutual time delay τ between two pump beams. Photon echo with incoherent light under the condition of extremely inhomogeneous broadening is discussed, and the difference of results obtained scperately from multi-level and two-level theory is pointed out. It has been demonstrated that the experiment of TDFWM-IL can also be analysed approximately by using an effective two-level model when a weak effect of inhomogeneous broadening of absorption band exists. Finally, our experimental results of TDFWM-IL obtained at zero-phonon line of ruby and absorption edge of cresyl violet film in PMMA are also presented and compared with the theory mentioned above.