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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Room Temperature Hole-Burning in Sm2+-doped Borate Glasses

Kimihiko Hirao

Published Jan 1, 1994• 0 citations
Publisher

Abstract

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.

DOI
10.1364/shbs.1994.thg1

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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.
Summary form only given. Persistent spectral hole burning (PSHB) of rare-earth-doped inorganic materials has attracted much attention in view of application to high-density optical memories. In particular, it seems that the glass materials are advantageous for application in wavelength-selective optical devices, as well as the memory devices, because of their large inhomogeneous linewidth. The wavelength-selective devices are key components in the wavelength-division multiplexing system, which is important for the next-generation optical communication technology. The problem for practical application lies in the fact that PSHB of rare-earth ions in glasses is usually observed only at temperature below 20 K. However, room-temperature PSHB has been observed recently for Sm/sup 2+/-doped crystals and glasses.
Persistent spectral hole burning (PSHB) is expected to be a mechanism for future ultrahigh density multi-wavelength optical memory whose density can be higher than the conventional optical memory by 10 to 104 times. PSHB optical memories are mainly studied for dye-doped polymers, but the hole burning temperatures for such poleymers are limited to tempertures lower than 140 K [1], Recently room-temperature PSHB has been observed in Sm2+ doped halide crystals [2-4] and glasses [5], and borate glasses [6]. The halide crystals are not bulk single crystals but polycrystals.
For next generation high density optical storage, extensive studies on persistent spectral hole burning (PSHB) have been performed, because they have a large potential for a high density frequency-domain optical data storage. PSHB has been observed at room temperature in Sm-doped crystals and glasses. Among them, glasses are considered to be more favorable than single crystals, due to their wide inhomogeneous line width and easy process for mass production. In the study, we developed a new glass mixture which shows room temperature PSHB with a inhomogeneous line width broadened up to 70 cm/sup -1/. The PSHB was characterized by investigating the time decay pattern of fluorescence and the excitation spectra.
Persistent spectral hole burning (PSHB) was discovered in organic molecular system in 1974[1]. Five years later, PSHB in inorganic materials was discovered in NaF by R. M. Macfarlane et al [2]. In 1985, A. Winnacker et al [3] first observed photon gated spectral hole burning in BaFCl: Sm2+ at 2K. Hole burning(HB) is useful in high resolution spectroscopy. It is also of crucial importance for the application to frequency domain optical storage. The storage density is proportional to the ratio of inhomogeneous linewidth(Γi) to the homogeneous linewidth(Γh), N(= Γi/Γh). The inhomogeneous linewidth of 5D0-TF0 transition of Sm2+ is 16GHz and the hole width is 25MHz in BaFCl at 2K[3]. For this material, the inhomogeneous linewidth changes only moderately with the temperature; On the other hand, the homogeneous linewidth increases rapidly as the temperature rises. Then, a small value of N(~2) can be estimated when HB temperature is raised to 77K. That means, it is difficult to burn a hloe in the inhomogeneous line in BaFCl:Sm2+ at 77K. To maintain a reasonable storage capacity or to study HB at a quite high temperature, a large inhomogeneous linewidth is in great request.
Persistent spectral hole burning (PSHB) was performed for several porphyrin molecules imbedded in polymer hosts and rare-earth ion Sm2+ doped in BaFCl0.5Br0.5 matrix. Power saturation and broadening effects for hole depth and width were observed. The dynamical process of hole formation was measured and explanation by population rate equations was given. Quantum efficiency of photochemical hole burning was investigated. For BaFCl0.5Br0.5:Sm2+ the capacity of data storage was estimated according to the result of multiple hole burning.
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.