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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Photon-Gated Spectral Hole-Burning in a Polymer Doped with a Mixture of Several Zn-Benzoporphyrin Derivatives

B. Luo, Jean‐Pierre Galaup

Published Jan 1, 1994• 0 citations
Publisher

Abstract

Photochemical spectral hole-burning (PSHB) has attracted particular attention in the past decade because of its potential for frequency domain optical storage. In order to apply PSHB to a practical optical memory, the material should have high burning temperature, high thermal stability, erasability and high frequency multiplexing. Two ways are possible to increase the storage density: one is to narrow the homogeneous line width, the other is to broaden the inhomogeneous line width. In previous works, the larger inhomogeneous line width (greater than 1,000 cm–1) has been reached in polymethylmethacrylate (PMMA) doped with two kinds of Zn-benzoporphyrin derivatives with roughly the same hole-burning efficiencies [1]. In this paper, the authors investigate systematically the optical properties of Zn-benzoporphyrin derivatives, their hole-burning mechanisms, thermal stability and electron-phonon coupling in cellulose acetate (CA) and in PMMA matrices. The choice of CA was motivated mainly by the fact this polymer allows to prepare samples with excellent optical quality.

DOI
10.1364/shbs.1994.wd28

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Low Temperature Physics•Nov 1, 2006•1 citation
Photochemical spectral hole-burning (PSHB) has attracted particular attention in the past decade because of its potential for frequency domain optical storage. In order to apply PSHB to a practical optical memory, the material should have high burning temperature, high thermal stability, erasability and high frequency multiplexing. Two ways are possible to increase the storage density: one is to narrow the homogeneous line width, the other is to broaden the inhomogeneous line width. In previous works, the larger inhomogeneous line width (greater than 1,000 cm–1) has been reached in polymethylmethacrylate (PMMA) doped with two kinds of Zn-benzoporphyrin derivatives with roughly the same hole-burning efficiencies [1]. In this paper, the authors investigate systematically the optical properties of Zn-benzoporphyrin derivatives, their hole-burning mechanisms, thermal stability and electron-phonon coupling in cellulose acetate (CA) and in PMMA matrices. The choice of CA was motivated mainly by the fact this polymer allows to prepare samples with excellent optical quality.
Recently, the interests in optical memory based on persistent spectral hole burning (PSHB) are increased because of its possibility of the application to high density optical memory. PSHB was observed for an organic dye doped in polymer and rear earth or transition metal doped in inorganic crystal or glasses up to now. Since PSHB was observed by two Russian groups (Gorokhovskii et al. and Kharlamov et al.) for free base phthalocyanine in a n-octane Shpol'skii matrix1 and for perylene and 9-aminoacridine molecules in glassy ethanol matrix2, PSHB materials are studied primarily for the polymer doped with an organic dye. But such materials can make hole only at very low temperature. Room temperature PSHB phenomena were observed on Sm2+ doped fluoride crystals3-5 and glasses6 recently, however these materials' Гih(inhomogeneous line width)/Гh(homogeneous line width)'s which are the parameters of data multiplicity in PSHB optical memory are an order of unity. For the application of PSHB materials to optical memory, high operating temperature, high Гih/Гh, and rapid reaction rate are wanted. Glass has a superiority on the view point of optical memory application because of its broad inhomogeneous line width and productivity. Our group has discovered room temperature PSHB for Sm2+ in borate glass systems whose Гih/Гh is 24.7 PSHB for rear earth metal in glass matrix has not been studied seriously, yet. It is thought that the study of the relationship between the optical hole and glass structure is necessary.
Persistent spectral hole burning (PSHB) has attracted much attention due not only to its usefulness in high resolution spectroscopy but also to its applicability to wavelength multiplexed optical memory.1) Though its application is still far from realization, potentially 103 times higher storage density would be attainable. Technological breakthrough is largely concerned with the issue of optimizing storage materials. For the formation of persistent holes, the existence of both photoreactive centers and a solid matrix is essential, and therefore, the comprehension of intramolecular and intermolecular electron-phonon interaction is of great importance. We have already proposed one working hypothesis in connection with the latter, which emphasizes the possibility of controlling the mesoscopic structure of the materials.2-4)
In addition to its importance for the optical spectroscopy of solids, photochemical spectral hole burning (PSHB) has attracted great interest due to its potential use in high density optical data storage [1]. By encoding information as a function of frequency an enormous increase in storage is possible compared to conventional optical storage materials. The most optimistic estimates predict an increase given by the ratio of the inhomogeneous linewidth to the homogeneous linewidth of the optical transition responsible for hole burning. Until now, however, there have been relatively few investigations of the practical limitations to storing a large number of spectral holes [2,3]. We describe here a recent experiment in which 2000 grayscale images were successfully recorded as holograms in the PSHB material chlorin in polyvinylbutyral. In holographic spectral hole burning the relative phase of the interfering light waves used to prepare the hologram has a strong influence on diffraction properties and, hence, on crosstalk between adjacent holograms [4]. By controlling the phase and frequency during burning in a novel manner, we have minimized crosstalk between the stored images.
Photochemical hole burning (PHB) is a topic of attracting increasing interest from spectroscopic viewpoints as well as from the practical prospects for ultra-high-density frequency-domain optical storage. Recent advances in PHB study are reviewed mainly focusing on the effects of chemical structure of guest ions and molecules as well as host matrices on the efficiency of hole formation and its temperature dependence, low energy excitation modes and Debye-Waller factors in amorphous matrices, and the mechanism of photon-gated PHB.
The persistent spectral hole-burning (PSHB) phenomenon has been known since 1974. It is still an important research area for the study of the intimacy of complex molecular systems in the solid state, revealing high-resolution spectra, photophysics, photochemistry, and dynamics of molecular doped amorphous media, organic as well as inorganic. From another point of view, PSHB allows the engraving of any spectral structures in the inhomogeneous absorption band profile of molecular doped amorphous hosts or ion doped crystals cooled down to liquid helium temperatures. Therefore, a PSHB material is programmable in the spectral domain and consequently it can be transformed in an optical processor capable of achieving user-defined optical functions. Some aspects of both fields are illustrated in the present paper. Concerning the search for efficient PSHB materials, the hole-burning performances and the photophysics of polymer and xerogel based systems are compared. The problem of high-temperature persistent spectral hole-burning materials and the search for new frequency selective photosensitive systems for fast optical pulse processing at 800nm are considered. Regarding the points treated, inorganic hosts based on silicate xerogels or porous glasses have shown the best results. Moreover, by combining inorganic and organic capabilities or by grafting organic species to the host, hybrid xerogels have not yet revealed all possibilities. Also, the interest of two-photon materials for engraving spectral features with near-infrared or infrared light is developed. As an introduction to possible applications of PSHB material, the basics of spectro-temporal holography are remembered and a demonstrative experiment using a naphthalocyanine-doped polymer film is described, proving that the temporal aberration free recompression of ultrashort light pulses is feasible, therefore opening a way for applications in ultrashort light pulse shaping. Aspects for a comparison between cw hole-burning and femtosecond spectro-temporal experiments are considered, and prospects for coherent control of light fields or photochemical processes are also evoked.