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Laser Physics

Femtosecond photon echo and four-wave mixing in dye-doped polymer films, semiconductors and heterostructures

В. В. Самарцев, Vladimir S. Lobkov, Tatiana G. Mitrofanova

Published Aug 15, 2014• 1 citation
Publisher

Abstract

A review of femtosecond experiments on photon echo (PE) and four-wave mixing (FWM) performed at room temperature is presented. The Weiner–Ippen technique of FWM spectroscopy is demonstrated in dye-doped polymer films (such as polyvinilbutural doped with phthalocyanine), semiconductors (CdS) and heterostructures (GaAs/AlGaAs). The experimental setup used in these experiments is described. The dephasing times are estimated and the relaxation mechanisms are discussed.

DOI
10.1088/1054-660x/24/9/094013

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A review of femtosecond experiments on photon echo (PE) and four-wave mixing (FWM) performed at room temperature is presented. The Weiner–Ippen technique of FWM spectroscopy is demonstrated in dye-doped polymer films (such as polyvinilbutural doped with phthalocyanine), semiconductors (CdS) and heterostructures (GaAs/AlGaAs). The experimental setup used in these experiments is described. The dephasing times are estimated and the relaxation mechanisms are discussed.
The signals of primary and stimulated femtosecond photon echo in polymer films doped with dye (phthalocyanine) molecules have been experimentally investigated at room temperature. A femtosecond echo spectrometer for these echo experiments is described. The decay curves of echo signals with increasing time intervals between excitation femtosecond pulses are obtained and blue shifts of the spectra of femtosecond echo signals with respect to the spectrum of excitation pulses are revealed. The possibilities of using the studied doped polymer films as recording media for high-temperature echo processors and coolants in optical refrigerators are analyzed.
We report femtosecond photon echo and four-wave mixing measurements performed on GaAs/AlGaAs heterostructure at room temperature. In femtosecond photon echo experiment the dephasing time was obtained, found to vary between 40 and 55 fs depending on carrier density. The dependence showed a power-law behavior T 2 ∝ N -0.22 , which indicates that major phase coherence loss is due to screened Coulomb electron-electron interaction. Transient grating experiments yielded the electron diffusion coefficient value of 200 cm 2 /s and electron relaxation time equal to 3 ns.
Some results of femtosecond echo experiments on polyvinylbutyral polymer films doped with phtalocyanine molecules at high (up to room) temperatures are reported. Special attention is paid to the stimulated femtosecond photon echo (SFPE), which was observed in a solid-state medium at room temperature for the first time. A decay curve of the SFPE signal has been obtained and theoretically analyzed. The results of the analysis indicate that the random interaction between impurity molecules and quasi-localized low-frequency vibration modes in an amorphous matrix plays the dominant role in the character of optical dephasing at high temperatures.
The signals of both primary and stimulated femtosecond photon echoes are observed and investigated in a dye-doped polymer film at room temperature using a modernized femtosecond echo-spectrometer. It should be noted that stimulated photon echo in the solid-state sample is observed for the first time at such a high temperature. Experimentally obtained decay curves of these signals have a nonexponential character. The spectra of these echo signals are also measured. It is found that the spectrum of the primary photon echo is short-wave shifted with respect to the spectrum of excitation. This can be used for the coherent laser cooling of a sample. The spectrum of the stimulated photon echo is also shifted to the short-wave range relative to the spectrum of excitation, but its shift is much less than that of the primary photon echo. The experiment shows that the femtosecond echo signals at room temperature are excited via the phonon-side band of the absorption line.
It is reported about the first observation (in a solid-state sample) and detailed investigation of the stimulated femtosecond photon echo (SFPE) signals at room temperature in a polyvinylbutural film doped with molecules of phthalocyanine of HW 1009 type at the wavelength of 788 nm. A dependence of relative intensity of these echo-signals on time intervals between the second and the third exciting pulses was studied and the SFPE spectrum was investigated with respect to the spectra of both exciting pulses and signals of self-diffraction. It was found that the linear electron-phonon coupling is weak and the influence of the phonon-side band of the absorption line on the SFPE signals is less significantly than on the signals of primary photon echo.
The signals of primary and stimulated femtosecond photon echoes are investigated in a dye-doped polymer film at room temperature. The homogeneous S 0 → S 1 spectral line width, which is due to the interaction between the impurity molecules and the quasi-local low-frequency modes, is estimated (≈5 × 1012 Hz). Special attention is paid to the study of spectra of femtosecond echo signals. The short-wave shifts of these spectra, with respect to the spectrum of femtosecond exciting pulses, are observed. These shifts indicate that the anti-Stokes regime of femtosecond pulse emission is realized. Therefore, the coherent regime of laser cooling of solids appears to be possible. The prospects of using of this new cooling regime in the function of a solid-state optical refrigerator are discussed.