Hole self-trapping in the Y3Al5O12 and Lu3Al5O12 garnet crystals

TL;DR

This study investigates hole self-trapping mechanisms in Y3Al5O12 and Lu3Al5O12 garnet crystals using EPR and TSL, revealing stable O- hole centers and their thermal behaviors up to 150 K.

Contribution

It provides detailed insights into the nature, stability, and thermal properties of hole self-trapping centers in garnet crystals, including their energies and interactions.

Findings

Holes are predominantly self-trapped at oxygen ions forming O- centers.

Self-trapped holes are thermally stable up to about 100 K, increasing to 150 K near acceptor ions.

Hole ionization energies are approximately 0.25-0.26 eV for pure O- centers and 0.41-0.45 eV when stabilized by acceptors.

Abstract

The processes of hole localization in the Y3Al5O12 and Lu3Al5O12 single crystals were investigated by electron paramagnetic resonance (EPR) and thermally stimulated luminescence (TSL). It was found that holes created by x-ray irradiation at 77 K are predominantly self-trapped at regular oxygen ions forming O- hole center. This self-trapped hole (STH) center is thermally stable to about 100 K in both YAG and LuAG crystals. At higher temperatures, thermally liberated holes are retrapped at oxygen ions in the vicinity of an acceptor ion such as Mg2+ and Al_{Y} or Al_{Lu} antisite ion that leads to increase of the thermal stability of the trapped hole to app. 150 K. TSL measurements show two composite glow peaks in the temperature range of 77 - 280 K, the temperature positions of which well correlate with the thermal stability of the O- centers. The hole thermal ionization energy was determined from a numerical fit of the TSL peaks within the model of second order kinetics. It is in the range of 0.25 - 0.26 eV for the O- STH center, and increases to 0.41 - 0.45 eV for O- center stabilized by the acceptor. Revealed O- centers can be attributed to O- small polarons formed mainly due to the hole stabilization by short-range interaction with the surrounding lattice.