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Bulletin of the Russian Academy of Sciences Physics

Anti-Stokes femtosecond photon echo in dye-doped polymer films and the possibility of coherent optical cooling

A. Yu. Vorobyev, S. V. Petrushkin, В. В. Самарцев

Published Jan 1, 2008• 0 citations
Publisher

Abstract

An anti-Stokes model is proposed to explain the known experimental data on the femtosecond photon echo in dye-doped polymer films at room temperature. The possibility of implementing the anti-Stokes mode of coherent laser cooling of such films is analyzed.
DOI
10.3103/s1062873808010140

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Bulletin of the Russian Academy of Sciences Physics•Jul 1, 2008•1 citation
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.
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.
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.
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.