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Physical Review A

Accumulated photon echoes generated by synchrotron radiation

Hiroshi Itoh, Shunsuke Nakanishi, Masaya Kawase, Hitoshi Fukuda, Hiroki Nakatsuka, M. Kamada

Published Oct 1, 1994• 7 citations
Publisher

Abstract

We demonstrate that accumulated photon echoes can be generated by synchrotron radiation. This is an experiment of a nonlinear optical effect carried out by using the radiation from an electron storage ring. A dye-doped polymer film was excited by the visible light from the storage ring, and the accumulated photon echoes from the sample were observed by employing a phase-modulation technique. The use of synchrotron radiation facilitates the extension of the spectral range where we can observe photon echoes with ultrahigh time resolution.

DOI
10.1103/physreva.50.3312

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Accumulated photon echoes have been observed by use of a light-emitting diode. This is to our knowledge the first observation of photon echoes that are excited by a nonlaser light source. In the incoherent-light photon echo, the time resolution is equal to the inverse of the overall spectral width of the excitation light. Therefore we can easily get a high time resolution by using nonlaser light with a broad spectrum. Moreover the use of nonlaser light in the photon-echo experiment will extend the technique into wavelength regions where lasers are not currently available.

Optics Letters•May 15, 1993•15 citations
We demonstrate that accumulated photon echoes can be generated by synchrotron radiation. This is an experiment of a nonlinear optical effect carried out by using the radiation from an electron storage ring. A dye-doped polymer film was excited by the visible light from the storage ring, and the accumulated photon echoes from the sample were observed by employing a phase-modulation technique. The use of synchrotron radiation facilitates the extension of the spectral range where we can observe photon echoes with ultrahigh time resolution.
Synchrotron radiation (SR) can be applied as an excitation source of the accumulated photon echoes. The accumulated photon echoes of sulforhodamine 640 ( SRh 640) doped in polyvinyl alcohol film (PVA) was successfully observed by exciting the sample with the SR and employing the phase modulation method. When we used SR passed through a bandpass filter with bandwidth of about 13 nm, the photon echo decay curve was obtained with a time resolution of 133 fs. In addition, when the bandpass filter was removed, the field autocorrelation time of the SR beam decreased to about 3 fs.>
We study theoretically and experimentally the influence of a homogeneous static electric field on a photochemically accumulated stimulated photon echo in dye-doped polymers. The dependence of the time profile of the echo signal on the strength of the electric field is evaluated in the case of a linear Stark effect. Experiments using polymers doped with organic dye molecules are carried out at low temperature, and our new technique is applied to determine the difference of the permanent dipole moment in the ground and the first excited singlet electronic state of the impurity molecules.
We demonstrated partial erasing of temporal optical data on a picosecond time scale by use of accumulated photon echoes. In a photon-echo memory the temporal data at time tau are stored as a frequency grating of period 1/tau in the absorption spectrum of a material. Partial erasing of the temporal data is achieved by irradiation of the material with a pulse pair at time separation tau , but the phase of one of the pulses is shifted 180 degrees . This process does not produce a frequency grating, and no echo is emitted. The experiment was performed with a dye-doped polymer film. The 180 degrees phase shift was obtained by use of a half-wave plate.
This talk presents a review of our recent experimental results on femtosecond accumulated photon echo in dye-doped polymers. The aim of this research is to clarify the parameter that is most important in affecting seriously the linear electron-phonon coupling in these samples, and to find the materials which have extremely weak linear electron-phonon coupling. The latter research is needed for the improvement of the PHB memory materials. We have so far demonstrated experimentally that Fourier-transform spectroscopy [1] based on the femtosecond accumulated photon echo is most useful for these studies. Furthermore, the detection sensitivity for the accumulated photon echoes has been improved significantly with the use of the phase modulation technique [2].
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.
Accumulated photon echoes have been observed by use of a light-emitting diode. This is to our knowledge the first observation of photon echoes that are excited by a nonlaser light source. In the incoherent-light photon echo, the time resolution is equal to the inverse of the overall spectral width of the excitation light. Therefore we can easily get a high time resolution by using nonlaser light with a broad spectrum. Moreover the use of nonlaser light in the photon-echo experiment will extend the technique into wavelength regions where lasers are not currently available.