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Physical Chemistry Chemical Physics

Purely electronic zero-phonon lines in optical data storage and processing

Karl K. Rebane

Published Jan 1, 2005• 2 citations
Publisher

Abstract

Spectroscopies of matrix isolated species and impurity activated solids are close relatives. Both are among the well developing chapters of solid state spectroscopy and optics. In this paper I am trying to give very brief overview what has been achieved in science and applications of impurity activated solids based on zero-phonon lines (ZPLs) in optical data storage and processing. I would like to show that the latter comprises via persistent spectral hole burning time-and-space domain holography in a certain meaning also the "stopping of light". ZPLs are beginning to play a role in the approaches to optical quantum computing.

DOI
10.1039/b417730b

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It is acknowledged that inhomogeneous absorption bands consisting of narrow homogeneous zero-phonon lines (ZPL) can be used for the purpose of optical data storage in the frequency dimension /1/. Persistent spectral hole-burning (PSHB) /2,3/ has made it feasible to preserve the recorded frequency domain information for a practically unlimited period of time. Via PSHB the inhomogeneous distribution function of the resonance frequencies of the impurity zero-phonon lines can be altered in an almost arbitrary fashion. This, in turn, makes it possible to manipulate the absorption coefficient and correlated to it index of refraction of the optical storage media. On this basis it has been proposed to use PSHB for the shaping of laser pulses via Fourier synthesis /4/. Holographic storage of time domain optical signals in PSHB media was proposed by Mossberg /5/. In the first experiments on the PSHB time domain holography the reproduction of various temporal shapes of picosecond pulses was demonstrated in dye doped polymers cooled to liquid helium temperature /6/. Earlier Zuikov et al. observed correlation between the temporal shapes of nanosecond excitation laser pulses and photon echo signals /7/. Since that time a variety of experiments on time domain holography in different resonant media have been reported (see /8/ and references therein).

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Spectroscopies of matrix isolated species and impurity activated solids are close relatives. Both are among the well developing chapters of solid state spectroscopy and optics. In this paper I am trying to give very brief overview what has been achieved in science and applications of impurity activated solids based on zero-phonon lines (ZPLs) in optical data storage and processing. I would like to show that the latter comprises via persistent spectral hole burning time-and-space domain holography in a certain meaning also the "stopping of light". ZPLs are beginning to play a role in the approaches to optical quantum computing.
A few examples of recent progress in the study and applications of purely electronic zero-phonon line (ZPL) and its offshoots are briefly considered: new experimental values of the narrowest ZPL; time-and-space-domain holography in the femtosecond domain, and the realization of a femtosecond Taffoli gate by it; single-impurity-molecule spectroscopy, its relation to single-photon interference and to the realization of quantum computing; the promises of quantum computing compared to what has already been done in holography.
Persistent spectral hole burning (PSHB) has remarkable applications in optical data storage and processing, including space-frequency and space-time domain holographies. Experiments have proven practically everything predicted and proposed by theory. The bottleneck between laboratory experiments and commercial applications is the need in low (liquid He) temperatures, as the main parameter of the data storage efficiency-the ratio between the inhomogeneous and homogeneous zero-phonon line (ZPL) widths α(T) = Γinh/Γhom(T)-- decreases owing to the rapid increase of Γhom(T) with temperature. A few optical and Mossbauer ZPLs are narrow even at RT, but they have usually also narrow Γinh. It is proposed to enlarge Γinh by making use of the Doppler effect. Two possible manifestations of the Doppler effect in the Universe are also discussed.
Persistent spectral hole-burning (PSHB) and its applications in data storage and processing are described. Purely electronic zero-phonon lines having very high peak values in the low temperature impurity spectra of solids are considered. Limitations for very large capacity PSHB memories put by the number of impurity molecules to store one bit are discussed. Doped with impurities optical fiber memory is proposed as a means to have low impurity concentration simultaneously with a large number of the impurities to store one bit. Bit-by-bit (digital) storage is compared to the distributed one and the advantages of the two versions of the latter -- PSHB holography and PSHB modeling of neural networks -- are considered. An experiment of simultaneous read-out over coordinates and frequency in neural network modeling is described. Requirements to PSHB materials and possibilities of the existence of materials effective at high temperatures are discussed.
Zero-phonon lines in impurity optical spectra and their inhomogeneous broadening are discussed. Photoburning of persistent spectral holes is not only an effective method to eliminate the inhomogeneous broadening and perform high resolution spectroscopy, but it serves also as a powerful tool to control by means of illumination the absorption coefficient and refractive index of the matter. It opens new horizons for frequency-selective optical memories, data storage and data processing. Hole burning by picosecond pulses and the time-and space-domain holography based on it are discussed and the results of the experiments described.
The low temperature spectra of absorption and luminescence of a wide variety of impurity doped organic and inorganic solids comprise very narrow (io 1O cm1) and intense zero-phonon lines (zPL). They arise from the purely electronic transistions in the impurities i.e. from the changes of the electronic state not accompanied by creation or annihilation of the phonons of the host solid. (ZPL may be called the optical analog of the M5sbauer line), Because of their narrowness ZPL's are very sensitive to even very slight differences in the crystal fields at the 1oca tions of impurities and the ZPL spectruim of a body of impu.rities displays a large inhomogeneous broadening (formula available on paper).
It is acknowledged that inhomogeneous absorption bands consisting of narrow homogeneous zero-phonon lines (ZPL) can be used for the purpose of optical data storage in the frequency dimension /1/. Persistent spectral hole-burning (PSHB) /2,3/ has made it feasible to preserve the recorded frequency domain information for a practically unlimited period of time. Via PSHB the inhomogeneous distribution function of the resonance frequencies of the impurity zero-phonon lines can be altered in an almost arbitrary fashion. This, in turn, makes it possible to manipulate the absorption coefficient and correlated to it index of refraction of the optical storage media. On this basis it has been proposed to use PSHB for the shaping of laser pulses via Fourier synthesis /4/. Holographic storage of time domain optical signals in PSHB media was proposed by Mossberg /5/. In the first experiments on the PSHB time domain holography the reproduction of various temporal shapes of picosecond pulses was demonstrated in dye doped polymers cooled to liquid helium temperature /6/. Earlier Zuikov et al. observed correlation between the temporal shapes of nanosecond excitation laser pulses and photon echo signals /7/. Since that time a variety of experiments on time domain holography in different resonant media have been reported (see /8/ and references therein).