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Journal of Applied Physics

Persistent spectral hole burning in chalcohalide glasses doped with Eu3+

Woon Jin Chung, Jong Heo

Published May 15, 2002• 1 citation
Publisher

Abstract

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.

DOI
10.1063/1.1467964

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Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations
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.
We present the case of photoionization-induced persistent spectral holeburning in rare earth doped II-VI compounds for high density memory storage. Experimental data on photon-gated holeburning has been presented for different sulfide hosts (MgS, CaS: RE2+ and RE3+). With the proper choice of the host electronic band structure, the optically active rare earth ion and its electronic transitions involved in the holeburning process, we have observed the highest number of persistent holes ever burned in a single electronic transition. Efficient photon-gated holeburning in the 4f7 (8S7/2) - 4f65d1 transition of Eu2+ is a result of photoionization of Eu2+ to Eu3+. These holes have a width of less than 5 GHz, have no detectable erasing effects after thousands of reading cycles, survive thermal cycling up to the room temperature and have infinite lifetime at low temperature (2 K). Although self- gated holeburning is observed with reading laser at higher powers, the photon budget for reading these holes is so small that thousands of reading cycles can be performed without significantly affecting the optical signal. We discuss the unique features of these systems that make them the most promising candidates to date for the holeburning based optical memories.
We present the case of photoionization-induced holeburning in rare-earth-doped II–VI compounds for high-density persistent holeburning. In this case, the photoproduct of holeburning is distributed across the entire zero-phonon line. This maximizes the total number of possible spectral holes that can be burned into an inhomogeneous line as well as produces holes that are photoerasable. Experimental data on photon-gated holeburning in MgS:Eu2+, Eu3+ are presented. With the proper choice of the host electronic band structure, the optically active rare-earth ion and its electronic transitions involved in the holeburning process, to the best of our knowledge we have observed the highest number of photon-gated holes ever burned in a single electronic transition. The features of these holes are that they suffer no detectable erasure after several thousands of read cycles, they survive thermal cycling to ∼150 K, and they are completely photoerasable. A special case of photon-gated holeburning, power-gated holeburning, was employed to demonstrate that, in such systems, a single laser can be used for burning, reading, and erasing of the spectral holes.
The mechanism for highly efficient photoionization spectral hole burning in the 4f7–4f65d1 transition of Eu2+ in MgS host is investigated in detail. The time and power dependencies of the hole depth and its photoerasure are analyzed assuming that a resonant two-photon ionization process initiates the hole burning. The near-room-temperature cycling shifts the hole to low energies, demonstrating the relaxation of an unstable lattice resulting from the hole burning. The characteristics of hole burning change significantly in samples codoped with Ce and Eu. All of these studies support that the mechanism of hole burning is the electron transfer from the Eu2+ ion to the Eu3+ deep trap, both of which are located at the substitutional octahedral sites.
Persistent spectral hole-burning has been reported for singly, Eu-doped, and doubly, Eu- and Sm-doped, CaS phosphors. Efficient photon gated holeburning in the 4f7 (8S7/2)−4f65d1 transition of Eu2+ is a result of photoionization of Eu2+ to Eu3+. These holes have a width of <5 GHz (2 K), survive thermal cycling of the phosphor up to the room temperature, 300 K, and have no detectable deterioration over more than a day of storage time at low temperature (2 K). Although self-gated holeburning is observed with the reading laser at higher powers, the photon budget for reading these holes is so small that in excess of 1000 reading cycles can be performed without destroying the optical signal. The nature of holes burned by photon-gating is found to be very different from the self-gated holes. The characteristics for the holeburning are the same in singly and doubly doped phosphors, suggesting that under the conditions of our experiments, Sm traps do not play any significant role in spectral holeburning. Possibilities of high density optical memory storage using photon-gated holeburning in this THz broad transition are discussed.
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.
We reported the first observation of room-temperature persistent spectral hole burning in Sm2+-doped fluoride glass in the last conference [1]. Room-temperature hole burning had been also observed in Sm2+-doped crystals [2]. We found considerable differences in the hole-burning characteristics between Sm2+-doped glasses and Sm2+-doped crystals: The burning-laser-intensity dependence is approximately linear, and no antihole is observed around the hole burned in Sm2+-doped glasses [3]. More detailed experimental studies are needed to clarify the mechanism of the hole burning in this glass and to explore more efficient hole-burning systems. In this paper, we report several experimental results related to wavelength dependence of the hole burning process.