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The Journal of Chemical Physics

Photoluminescence and spectral holeburning in europium-doped MgS nanoparticles

Zameer U. Hasan, Sameh I. Dardona, Aras Konjhodzic

Published Dec 8, 2005• 5 citations
Publisher

Abstract

Luminescence and power-gated spectral holeburning studies have been performed on Eu-doped MgS nanoparticles. These particles are atomically tailored to produce and control the relative concentration of Eu(2+) and Eu(3+), which is necessary for power-gated holeburning. The spectral holes are permanent at low temperatures. Optical studies show that the electron-phonon coupling is stronger in nanoparticles than in thin films or microparticles of the same material. This is the reason for inherently broader spectral holes in nanoparticles as compared to microparticle or thin-film samples. Temperature broadening of spectral holes in nanoparticles follows a T(2.4) behavior, a faster rate than thin films or microparticles. This behavior can be attributed to the glassy nature of the particles produced.

DOI
10.1063/1.2107467

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Journal of the Optical Society of America B•Feb 1, 2001•3 citations
Luminescence and power-gated spectral holeburning studies have been performed on Eu-doped MgS nanoparticles. These particles are atomically tailored to produce and control the relative concentration of Eu(2+) and Eu(3+), which is necessary for power-gated holeburning. The spectral holes are permanent at low temperatures. Optical studies show that the electron-phonon coupling is stronger in nanoparticles than in thin films or microparticles of the same material. This is the reason for inherently broader spectral holes in nanoparticles as compared to microparticle or thin-film samples. Temperature broadening of spectral holes in nanoparticles follows a T(2.4) behavior, a faster rate than thin films or microparticles. This behavior can be attributed to the glassy nature of the particles produced.
In this paper we report optical hole-burning in nano- particles of MgS doped with Eu. Nano-particles have been produced by quench condensing the laser-ablated vapors from a solid target. Particle size has been controlled by the pressure of the ambient gas in the chamber. Our experiments produced particles as small as 20 nano-meters in size. Optical data shows typical fluorescence enhancement associated with the confined geometries. Results have been presented on optical properties, the hole-burning characteristics, and the broadening of holes at elevated temperatures.
In the form of micro-particles europium doped alkaline earth sulfides have been shown to exhibit high density of permanent spectral holes. The photon-gated spectral holeburning (PGHB) in these systems provided the most promising characteristics of any material known to date. These spectral holes can be used as optical memory. However, for any optical storage device either large size single crystals or thin films are required. Thin films of these materials are grown by Pulsed Laser Deposition (PLD) technique. This fast and simple growth technique is superior the single crystal growth or the molecular beam epitaxy (MBE) as far as the holeburning properties are concerned. Transparent glassy MgS:Eu and CaS:Eu films have been grown and tested for the spectral holeburning properties. Critical parameters such as the relative concentration of Eu2+ and Eu3+, and optical quality of thin films have been investigated. Int his paper we report on the growth and the high-density optical holeburning in these films. The density of spectral holes has been further increased by burning in multiple Eu-centers in a material and by depositing multiple layers of thin films of different materials in a stack.
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.
Previously we have reported the largest number of photon- gated spectral holes ever burned in a solid. This has interest in their applications in optical storage. However, multiple holeburning in MgS:Eu resulted in noticeable erasure of the previously burned holes. This was attributed to the mechanism of holeburning in this material where both Eu2+ and Eu3+ are stable ions. In gated holeburning, Eu2+ ions are ionized. Eu3+ that form deep traps, capture the electrons generated during the holeburning and are converted to Eu2+. The Zero Phonon Line (ZPL) of these newly formed Eu2+ ions are randomly distributed across the inhomogeneous line causing a partial erasure of the holes burned earlier. This reduces the efficiency of holeburning. Co-doping of MgS:Eu and CaS:Eu with different rare earth (RE) ions has been investigated to provide deep electron traps other than Eu3+. Furthermore, co-doping provides the opportunity to burn holes in multiple ZPLs belonging to different REs, thus increasing the storage density many folds.
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.
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.