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Molecular crystals and liquid crystals science technology. Section A, Molecular crystals and liquid crystals/Molecular crystals and liquid crystals science and technology. Section A, Molecular crystals and liquid crystals

Spectral and Time Domain Studies of Accumulated Photon Echo

Iosif Zeylikovich, G. Bai, A.A. Gorokhovsky, R. R. Alfano

Published Dec 1, 1996• 0 citations
Publisher

Abstract

Multishot or single-shot retrieval of femtosecond echo signal without substantial spectral distortion was experimentally demonstrated for a H2-octaethylporphine doped polystyrene sample. Upto 104 single-shot readout cycles using a femtosecond pulse were observed without substantial echo signal degradation. The echo decay time was determined for this sample to be (50 ± 15) ps.

DOI
10.1080/10587259608042757

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Multishot or single-shot retrieval of femtosecond echo signal without substantial spectral distortion was experimentally demonstrated for a H2-octaethylporphine doped polystyrene sample. Upto 104 single-shot readout cycles using a femtosecond pulse were observed without substantial echo signal degradation. The echo decay time was determined for this sample to be (50 ± 15) ps.
Summary form only given. Coherent optical transients such as photon echo are a versatile method far measurement of the homogeneous absorption spectrum of molecular systems in the presence of strong inhomogeneous broadening. Such experiments require measurement of the decay of the optical coherence, typically accomplished by gradually varying the time delay between the excitation pulses. Time-domain information is then Fourier transformed to frequency domain by a computer. In this paper we demonstrate a new method that yields the homogeneous spectrum in a single shot of femtosecond laser pulse illumination by performing Fourier transformation of coherent optical transient signal with a lens. We apply this method to measure the homogeneous spectrum of dye molecules in a polymer film in a broad range of temperatures.
Fourier-transform spectroscopy using the technique of femtosecond accumulated photon echo with incoherent light has been performed in dye-doped polymers. Several types of interference effect or quantum beat between the zero-phonon line and other spectral components including the phonon sideband, the vibronic lines, and the photoproduct state have been observed. Based on the density matrix incorporating the transition-frequency modulation, it is pointed out that the factorization approximation for the relaxation function holds rigorously in the accumulated photon echo. We also clarified that the Fourier cosine transform of the heterodyne-detected echo signal provides the hole-burning spectrum.
The first observation is reported of the primary femtosecond photon echo at a liquid nitrogen temperature in a dye-doped polymer film at a wavelength of 780 nm. Echo signals were generated by pulses with the duration of 130 fs. The echo signal decay can not be described by a simple exponential function. There is a fast decay region below 250-300 fs and a slow decay region at longer time intervals. There were also detected signals of the self-diffraction of exciting pulses on a nonequilibrium population difference grating, induced in resonant medium by these pulses.