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中国科学通报：英文版

INTERFERENCE-BEAT MODULATION IN TIME-DELAY FOUR-WAVE MIXING WITH INCOHERENT LIGHT IN ABSORPTION BAND OF RUBY AT 20K

张瑞华, 周海天, 米辛, 王长顺, 姜谦, 叶佩弦

Published Jan 1, 1991• 0 citations
OpenAlex

Abstract

Ⅰ. INTRODUCTIONTime-delay four-wave mixing with incoherent light(TDFWM-IL)is a new nonlinearoptical time-domain technique developed in recent years for studying ultrafast relaxation processes by employing nanosecond pulses or even CW laser sources. Theoretically, two-

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Annual Meeting Optical Society of America•Jan 1, 1988•0 citations
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.
A multilevel model, including homogeneous and inhomogeneous broadening, is proposed for the study of time-delay four-wave mixing with incoherent light (TDFWM-IL) in absorption bands consisting of a series of vibrational transitions. A theory of TDFWM-IL is developed for this model, and a general formula for the delay-time dependence of the signal intensity Is(τ), considering both the homogeneous and inhomogeneous broadening of the transitions, is deduced. Special analyses are given to the homogeneous and inhomogeneous limits. The differences between Is(τ) derived from multilevel theory and from two-level theory, are pointed out. When the homogeneous broadening of individual transitions is much smaller than the frequency interval of adjacent transitions, Is(τ) in the multilevel theory is modulated periodically and the envelope is close to that in the two-level theory for both the homogeneous and inhomogeneous limits. When the individual transitions are homogeneously broadened enough so that an unresolved continuous band is formed, an effective two-level model can still be used approximately for the studies of TDFWM-IL in this continuous band, with both homogeneous and inhomogeneous broadening. However, the dephasing time [Formula: see text] in the formula of Is(τ) in this effective two-level model is not the real dephasing time of an individual transition of the band, but the effective one which reflects the behavior of the whole band.
Time-delayed four-wave mixing using incoherent light has been proposed as a new method to measure the ultrafast population relaxation time T1. Assuming three input beams of incoherent light with much longer duration than T1, the theoretical calculation has shown that the decay curve by T1 appears in the signal profile and that the time resolution is determined by the correlation time of the light. The decay time to be observed is twice that of the transient four-wave mixing with short pulses. We have experimentally confirmed the prediction by observing picosecond population relaxations of organic dye solutions, using nanosecond pulses from a normal broadband dye laser. An advantage of the present method over the pump-probe method using incoherent light is also discussed.
Photon-echo modulation spectroscopy is extended into a new regime to study coherences between states that are widely separated in frequency compared with the bandwidth of the exciting laser pulses. Time-delayed four-wave mixing (TDFWM) is observed on the Na DDD doublet by use of 7-nsec pulses of light spectrally peaked at each of the DDD-line transitions. As the two double-frequency, 7-nsec light pulses are delayed with respect to each other a 1.9-psec beating of the integrated TDFWM signal is observed, even for delays greater than the excitation pulse width.
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.
Two transient time-delayed four-wave mixing experiments have been performed on the Na D doublet and modulations of 1.9 ps and 980 as have been observed. These periods correspond to the difference and sum frequencies of the two Na D lines. Both experiments were performed using 7-ns pulses of light with frequency components at each of the D-line transitions. The effects of superimposition-state modulations are observed in the integrated TDFWM signal as a function of the time delay. As the time delay is varied, the lowest diffraction order mixing signal is modulated. Higher diffraction order mixing signals contain modulation components at integral multiples of the beat frequency.