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Journal of the Optical Society of America B

Persistent infrared spectral hole burning of Tb^3+ in the glasslike mixed crystal Ba_1−x_−yLaxTbyF_2+x_+y

S. P. Love, J. A. Campbell, Carl E. Mungan, Albert J. Sievers

Published May 1, 1992• 28 citations
Publisher

Abstract

Persistent IR spectral holes that exhibit glasslike characteristics—highly nonexponential low-temperature relaxation behavior and a broad distribution of barrier heights observable in thermal-cycling studies—have been produced in the inhomogeneously broadened 4.5-μm 7F6 → 7F5 electronic absorption band of the Tb3+ ion in the mixed crystal Ba1−x−yLaxTbyF2+x+y. Investigations of six compositions, ranging from x = 0, y = 0.005 to x = 0.30, y = 0.05, reveal no hole burning for the x = 0, y = 0.005 case and a hole-burning quantum efficiency of the order of 5 × 10−7 with a weak dependence of the lanthanide fraction for x + y ≥ 0.05. For all compositions with x + y ≥ 0.05 hole behavior is virtually identical, with both the widths and the peak positions of the distributions of relaxation rates and barrier heights for these mixed crystals being typical of those found for glasses.

DOI
10.1364/josab.9.000794

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Persistent IR spectral holes that exhibit glasslike characteristics—highly nonexponential low-temperature relaxation behavior and a broad distribution of barrier heights observable in thermal-cycling studies—have been produced in the inhomogeneously broadened 4.5-μm 7F6 → 7F5 electronic absorption band of the Tb3+ ion in the mixed crystal Ba1−x−yLaxTbyF2+x+y. Investigations of six compositions, ranging from x = 0, y = 0.005 to x = 0.30, y = 0.05, reveal no hole burning for the x = 0, y = 0.005 case and a hole-burning quantum efficiency of the order of 5 × 10−7 with a weak dependence of the lanthanide fraction for x + y ≥ 0.05. For all compositions with x + y ≥ 0.05 hole behavior is virtually identical, with both the widths and the peak positions of the distributions of relaxation rates and barrier heights for these mixed crystals being typical of those found for glasses.
Efficient persistent spectral hole burning in Eu3+-doped sulfide glasses was observed with the addition of CsBr or KBr. Holes in these glasses showed high initial growth rates, thermal barrier heights, and low relaxation rates. It was also possible to form independent multiholes on the inhomogeneously broadened absorption spectrum. One-photon absorption of the burning light and corresponding reduction of Eu3+ into Eu2+ via interaction with local conduction (or charge transfer) bands are the main processes for hole burning.
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
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.
With a ring dye laser persistent spectral hole-burning was measured by fluorescence excitation spectroscopy in the zero-phonon lines of the 2llg ↔ 2llu transition in KI:S2 − and of the 3H4 → 3P0 transition of a defect center with three D− ions in SrF2:Pr3+:D−and also in the zero-phonon line at 462.5 nm of a color center in neutron-irradiated and annealed α-Al2O3. In all three lines holes with a width in the order of 1 GHz could be obtained at 1.5 K with single frequency laser. With broad-band laser in KI:S2 − and SrF2:Pr3+:D− spectral redistribution within the full range of inhomogeneous broadening could be observed which are explained by a photophysical model based on barrier crossing in asymmetric double-well-potentials. In the case of sapphire a photobleaching process is dominant which is effective also for nonselective excitation, and the holes are thermoresistant up to 300 K.
Persistent spectral hole burning is observed in Sm(2+)-doped glasses at room temperature. The holes are burned in the (7)F(0) ? (5)D(0), (5)D(1) lines of the Sm(2+) ions in three kinds of fluoride glass. The dependence of the burning efficiency on the sample and on the burning intensity is measured. The intensity dependence is approximately linear, and no antihole is observed around the burned hole. The hole-burning mechanism is discussed. The temperature dependence of the homogeneous width is also measured.
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.