Mechanism of luminescence and efficient energy storage in Lu2SiO5 : Ce3+single crystals

Abstract
The development of high energy physics and medicine has raised the necessity of heavy stintillating materials with a large total gamma quantum absorption cross-section, high quantum output and fast response. Cerium doped lutetium silicate Lu2SiO5 : Ce3+ (LSO) has high density, large effective atomic number and high conversion efficiency. In this work we have reported optical absorption spectroscopy and photoluminescence data for LSO single crystals grown using the modified Musatov method. The absorption spectra show the fundamental intrinsic absorption edge of Lu2SiO5 at ~200 nm and four extrinsic absorption bands of Ce3+ activator near 250—375 nm. The band gap is 6.19 to 6.29 eV depending on optical beam direction. We have confirmed that the extrinsic absorption bands correspond to optical transitions in Ce3+ activator ions localized in two crystallographically non-equivalent CeI and CeII positions. We have estimated that oscillator force for the optical transitions in Ce3+ ions. The photoluminescence spectra excited by 3.49 eV photon energy UV laser contain three bands: ~2.96 eV, ~3.13 eV (CeI) and ~2.70 eV (CeII). The energy structure of electron traps in LSO has been studied with thermally stimulated luminescence, the crystals being exposed to UV with different spectral and energy parameters. All the experimental thermally stimulated luminescence curves contain at least two peaks at 345 and 400 K with a 4 : 1 intensity ratio attributable to electron traps at 0.92—0.96 and1.12—1.18 eV. LSO exposure to high pressure mercury lamp radiation having the highest energy has for the first time showed the presence of traps at 0.88 eV. A model of the energy structure of LSO has been developed. The luminescence mechanism in the material is more complex than purely intracenter one. We show that high excitation energies may lead to ionization by the mechanism hv a + Ce3+ = Ce4+ + e-. We have assumed that the storage of excitation energy involves not only Ce3+ activator but also the conduction band as well as trap states localized near the conduction band.