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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Inhomogeneous Broadening and Persistent Spectral Hole-Burning of Divalent Samarium Ions In Alkaline Earth Metal Halides

Jiahua Zhang, Xiangjun Wang, Shihua Huang, Jiaqi Yu

Published Jan 1, 1991• 0 citations

Abstract

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.

DOI: 10.1364/pshb.1991.fa3

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Aug 13, 1993•0 citations

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.

Spectral hole burning acting as a high resolution spectroscopic technique has potential applications on high density optical storage. The present paper report the research results on inhomogeneous broadening, fluorescence line narrowing, high temperature persistent spectral hole burning, mechanism of hole burning, hole burning dynamics and thermal stability of spectral holes. We designed and prepared new material system of divalent samarium ion doped alkaline earth metal fluoridehalides for high temperature hole burning. Room temperature hole burning and spectral hole with longer lifetime were performed. Various local configurations were distinguished by using time resolved spectroscopy. Spectral redistribution induced by hole burning indicates that trivalent samarium ions act as electron traps. Hole burning dynamics was analyzesed by using Block theory.

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.

Materials of MyM’1-yFClxBr1-x:Sm2+ have been widely applied in spectral hole-burning since the first observation of persistent spectral hole-burning in BaFCl:Sm2+ at 2K was reported by A. Winnaker, etc. in 1985[1]. From then on, hole-burning in BaFCl0.5Br0.5:Sm2+ at 77K[2] in SrFCl and Mg0.5Sr0.5FCl0.5Br0.5:Sm2+ at room temperature[3, 4] were reported. Room temperature hole-buring of Sm2+ in fluorohafnate glasses[5,6] were reported in recent years also. These materials are of potential use in high temperature hole- burning. But comparing to organic materials, they have lower hole- burning efficiency and narrower inhomogenous line width. In order to apply spetral hole- buring in frequency domain optical storage, it is important to improve these materials.

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.

Photon gated spectral hole-burning was first observed in a samarium doped crystal, BaFCl:Sm2+ [1]. This material was of interest to the developement of optical memories as the holes were found to be stable to room temperature thermal cycling. Holes could be burnt at liquid helium temperatures but as the temperature was raised the line quickly became homogeneously broadened. The addition of bromine to the melt succeeded in broadening the inhomogeneous linewidths to about 2 nm through substitutional disorder [2] and persistent holes were observed at 77 K [3]. Subsequently, a study of the parameters for spectral hole-burning in a BaFCl0.5Br0.5:Sm2+ crystalline powder was performed [4] and the highest temperature for which persistent hole-burning had been observed was raised to 133 K. Here we report spectral hole-burning at room temperature (figure 1) in a related compound, Sr0.5Mg0.5FCl0.5Br0.5:Sm2+.

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.