Single Crystalline Films of Ce³⁺-Doped Y₃Mg_xSi_yAl_5−x−yO₁₂ Garnets: Crystallization, Optical, and Photocurrent Properties

Abstract

This research focuses on LPE growth, and the examination of the optical and photovoltaic properties of single crystalline film (SCF) phosphors based on Ce3+-doped Y3MgxSiyAl5−x−yO12 garnets with Mg and Si contents in x = 0–0.345 and y = 0–0.31 ranges. The absorbance, luminescence, scintillation, and photocurrent properties of Y3MgxSiyAl5−x−yO12:Ce SCFs were examined in comparison with Y3Al5O12:Ce (YAG:Ce) counterpart. Especially prepared YAG:Ce SCFs with a low (x, y 2+ and Mg2+–Si4+ codopants also showed a photocurrent that increased with rising Mg2+ and Si4+ concentrations. Mg2+ excess was systematically present in as-grown Y3MgxSiyAl5−x−yO12:Ce SCFs. The as-grown SCFs of these garnets under the excitation of α–particles had a low light yield (LY) and a fast scintillation response with a decay time in the ns range due to producing the Ce4+ ions as compensators for the Mg2+ excess. The Ce4+ dopant recharged to the Ce3+ state after SCF annealing at T > 1000 °C in a reducing atmosphere (95%N2 + 5%H2). Annealed SCF samples exhibited an LY of around 42% and similar scintillation decay kinetics to those of the YAG:Ce SCF counterpart. The photoluminescence studies of Y3MgxSiyAl5−x−yO12:Ce SCFs provide evidence for Ce3+ multicenter formation and the presence of an energy transfer between various Ce3+ multicenters. The Ce3+ multicenters possessed variable crystal field strengths in the nonequivalent dodecahedral sites of the garnet host due to the substitution of the octahedral positions by Mg2+ and the tetrahedral positions by Si4+. In comparison with YAG:Ce SCF, the Ce3+ luminescence spectra of Y3MgxSiyAl5−x−yO12:Ce SCFs greatly expanded in the red region. Using these beneficial trends of changes in the optical and photocurrent properties of Y3MgxSiyAl5−x−yO12:Ce garnets as a result of Mg2+ and Si4+ alloying, a new generation of SCF converters for white LEDs, photovoltaics, and scintillators could be developed.

Keywords

• luminescence
• single crystalline films
• liquid-phase epitaxy
• Mg²⁺–Si⁴⁺-based garnet
• Ce³⁺-doped
• phosphor converters