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Journal of the Optical Society of America B

Observation of the waveform of accumulated photon echoes in a dye-doped polymer film by use of an interferometer

Takuya Yoda, Takao Fuji, Toshiaki Hattori, Hiroki Nakatsuka

Published Oct 1, 1999• 2 citations
Publisher

Abstract

We used a Michelson-type interferometer to observe the waveform of the accumulated photon echoes in a 3,3′-diethylthiatricarbocyanine iodide–doped poly(vinyl alcohol) film. By Fourier analysis of the measured interferograms we obtained the shapes of the burned population grating and the phase grating in the sample. From the frequency distribution of the dye molecules, that is efficient for persistent spectral hole burning, we estimated the inhomogeneous frequency distribution of the 0–0 transition from S0 to S1 levels of the dye molecules in the poly(vinyl alcohol) film.

DOI
10.1364/josab.16.001768

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International Conference on Ultrafast Phenomena•Jan 1, 2002•2 citations
We used a Michelson-type interferometer to observe the waveform of the accumulated photon echoes in a 3,3′-diethylthiatricarbocyanine iodide–doped poly(vinyl alcohol) film. By Fourier analysis of the measured interferograms we obtained the shapes of the burned population grating and the phase grating in the sample. From the frequency distribution of the dye molecules, that is efficient for persistent spectral hole burning, we estimated the inhomogeneous frequency distribution of the 0–0 transition from S0 to S1 levels of the dye molecules in the poly(vinyl alcohol) film.
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.
Fourier-transform photon echo spectroscopy has been applied to the vibronic absorption band in dye molecule. The quantum beat between the vibronic lines has been observed in cresyl-violet and tetraphenyl-porphine doped in polymer films. The vibronic lines associated with the quantum beat have been identified with comparing the Fourier-transformed spectrum of the echo signal and the persistent hole-burning spectrum. The observed steep temperature dependence of the vibronic coherence has been discussed in comparison with the mild temperature dependence of vibrational coherence (sublevel coherence between vibronic states).
The stimulated photon echo memory using persistent hole-burning materials has been attracting much attention as a possible candidate for high-density data storage. Most studies have been related to the writing and reading processes and little attention has been paid for a partial erasing. We demonstrate for the first time that partial erasing of photon echo memory can be accomplished by simply employing a half-wave plate. In a photon echo memory, the write and data pulses with a time separation /spl tau/ excite a hole-burning material. These pulses create a periodic absorption modulation (periodic hole) with a frequency of l//spl tau/ in the absorption spectrum. When the read pulse excites the sample, a stimulated echo pulse is emitted at /spl tau/ after the read pulse, We note that a bit of data is stored as a periodic hole in the sample. A rotation of a half-wave plate inserted in the data pulse path (which induce a retardation of /spl lambda//2) creates two periodic holes that have the same frequency and opposite phase. Therefore, erasing a periodic hole can be done by rotating the wave plate. A dye (Sulforhodamin 640) doped polymer film (polyvinyl alcohol) cooled at 2 K was used as a persistent hole-burning material.
Optical dephasing of the zero-phonon line (ZPL) of organic dye molecules doped in polyvinyl alcohol (PVA) and several cross-linked PVA derivatives was studied by using the incoherent photon echoes and the photophysical persistent hole-burning. It was found in the incoherent photon echo measurements that optical dephasing time of the ZPL increases with increasing the length of a cross-linker introduced to the PVA backbone. The difference in the temperature dependence of the dephasing time was also observed between a dye doped in PVA with and without the cross-link. When a longer cross-linker was introduced, the phonon sideband component in the incoherent photon echo signal became dominant in contrast to that in PVA with a relatively short cross-linker, while the dephasing time of the ZPL was still longer than that in PVA without the cross-link. Hole-burning studies showed that the phonon sideband spectrum of a dye doped in the cross-linked PVAs is essentially similar to that in PVA. However, the depth of the zero-phonon hole burnt with the same burning power was found to depend on the PVA hosts with the cross-linkers. These our findings suggest that the introduced cross-link does not alter the electron–phonon coupling modes or pseudo-local mode, but it drastically reduces the effect of the two-level tunneling systems in PVA on the optical dephasing of a doped dye. As a result, the dephasing time of the dye in the cross-linked PVAs becomes longer than that in PVA without the cross-link. The decrease of the optical dephasing by introducing the cross-link can be interpreted by assuming a void space in PVA, which is created near to the cross-linker. In addition, absorption and fluorescence spectra in these systems were measured, which imply the occurrence of weak dye–dye interaction when the dye is doped in PVA with a much longer cross-linker.
Spatio-temporal holography using persistent spectral hole-burning in dye molecules embedded in plastic films is promising for applications such as femtosecond pulse shaping, data storage or phase conjugation. In addition to the common 2 spatial dimensions of classical holograms, each point in the sample plane can be used to store spectral informations such as the shape of a femtosecond pulse. On each point of the sample, spectral interferences between a reference pulse and an object pulse (for example chirped) are recorded via spectral hole-burning in the absorption band of the dye molecule. As early as 1983, photon echo and time-reversal experiments using persistent spectral hole-burning were performed in porphyrazine styrol solutions at 630 nm [1]. Then several developments, like the reconstruction of the polarization state of object pulses [2], time and space holography [3,4], image holograms using a single pair of femtosecond pulses [5] were demonstrated in different photosensitive media.