Scintillation and radioluminescence mechanism in β-GaO semiconducting single crystals.

In this paper, we present the results of experiments on samples of β-GaO single crystals under a project aimed at assessing and improving the scintillation performance of this material by studying scintillation and radioluminescence mechanism and its limitations. In addition to standard experiments, such as scintillation light yields and time profiles, radio-, and thermoluminescence, we developed and tested a new and promising two-beam experiment, in which a sample is excited by an X-ray beam and additionally stimulated by an IR laser diode. Fe and Mg doping compensate for the inherent n-type conductivity of β-GaO to obtain semi-insulating single crystals for large-area substrates and wafers. At the same time, residual Fe and Ir are ubiquitous uncontrolled impurities leached from the Ir crucibles used to grow large bulk crystals by the Czochralski method. For these experiments, we selected four samples cut from the Czochralski grown 2-cm diameter β-GaO single crystal boules; one with a reduced Fe content, two unintentionally Fe- and Ir-doped (UID) with lower and higher Fe content, and one doped with Mg. We find that steady-state radioluminescence spectra measured at temperatures between 10 and 350 K are dominated by the UV emission peaking at about 350-370 nm. Unfortunately, even for the best sample with a reduced Fe-content, the intensity of this emission drops precipitously with the temperature down to about 10 % at 300 K. From the two-beam experiments, we conclude that recombination via inadvertent Fe impurity involving three charge states (2+, 3+, and 4+) may reduce a steady-state UV emission of β-GaO under X-ray excitation by as much as 60-70 %, one-third to one-half of which is due to the recombination (specific for Fe-doped β-GaO) involving the 4+ and 3+ charge states of Fe and the remaining 50-70 % being due to a more familiar route typical of other oxides, involving the 2+ and 3+ charge states of Fe. These losses are at higher temperatures enhanced by a thermally activated redistribution of self-trapped holes (STHs). In addition, the trapping of electrons by Fe and holes by Mg, Fe, and Ir may be responsible for scintillation light loss and reduction of the zero-time amplitude essential for the fast timing scintillation applications. Despite indirect evidence of competitive recombination in β-GaO involving a deep Ir donor level, we could not quantitatively assess losses of the UV steady state radioluminescence light due to the inadvertent Ir impurity.