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Optical Engineering

High-temperature spectral hole burning on samarium(II) in single crystals of the lead fluorohalide structure family and in thin films of calcium fluoride

Hans Bill, Raivo Jaaniso, Hans R. Hagemann, D. Lovy, Alain Monnier, Marc Schnieper

Published Aug 1, 1995• 30 citations

Abstract

When modern spectral hole burning applications for high-density information storage under noncryogenic temperatures are envisioned, it is necessary to develop new frequency-selective photoactive materials for this purpose. Mixed compounds of the PbFCI family, doped with samarium (II) ions, exhibit promising and true room-temperature hole burning capabilities. We investigate this class of systems (and related ones) by combining material synthesis and high-resolution spectroscopy. Whole groups of isomorphous crystals were synthesized with varying degrees of halide anion and/or cation substitutions. Thin films of fluoride-based materials were made in a laboratory-built molecular beam epitaxy system. An extended x-ray study, differential thermal analysis, luminescence, and Raman measurements allowed the characterization of the materials. Formal models were developed for both the inhomogeneous zero-phonon optical line shapes of the Samarium (II) and the time evolution of hole burning.

DOI: 10.1117/12.201813

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When modern spectral hole burning applications for high-density information storage under noncryogenic temperatures are envisioned, it is necessary to develop new frequency-selective photoactive materials for this purpose. Mixed compounds of the PbFCI family, doped with samarium (II) ions, exhibit promising and true room-temperature hole burning capabilities. We investigate this class of systems (and related ones) by combining material synthesis and high-resolution spectroscopy. Whole groups of isomorphous crystals were synthesized with varying degrees of halide anion and/or cation substitutions. Thin films of fluoride-based materials were made in a laboratory-built molecular beam epitaxy system. An extended x-ray study, differential thermal analysis, luminescence, and Raman measurements allowed the characterization of the materials. Formal models were developed for both the inhomogeneous zero-phonon optical line shapes of the Samarium (II) and the time evolution of hole burning.

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.

Multicomponent thin films with spectral hole burning capacity at room temperature were synthesized by using molecular beam and pulsed laser deposition techniques All materials were activated by Sm2+ in low-symmetry alkaline earth sites, the synthesis involved the control of ionic diffiision rate during multilayer growth and special reduction of Samarium. Enhancement of hole burning rate by 1–2 orders is obtained in nanocrystalline films as compared to bulk and microcrystalline materials New hypothetic mechanism involving the creation of Sm-defect (photochromic) centers is proposed for reversible photoburning

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+.

Two-photon persistent hole burning is observed at T = 296 K in 5 D 1 – 7 F 0 and 5 D 0 – 7 F 0 transitions of Sm 2+ ions in substitutionally disordered SrFCl 1/2 single crystals, showing the ratio of inhomogeneous to homogeneous linewidth of 20 ÷ 25. The minimum hole widths of 3.5 cm -1 and 2.6 cm -1 , respectively, were determined for these transitions. In fact, the applicability of persistent spectral hole burning, known as a low-temperature high-resolution spectroscopic method and a potential basis for the use of a new–spectral–dimension in optical data storage and processing, is demonstrated for the first time at room temperature in inorganic materials.

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.