PNNL

Abstract

In semiconductors, defects often assist non-radiative relaxation. However, Tl doping can significantly suppress the non-radiative relaxation in alkali halides to increase scintillation efficiency. Without the Tl, it is known that the creation of Frenkel pairs at self-trapped excitons, assisted by excited electron and hole relaxations, is the reason for the non-radiative relaxation. Here we show by first-principles calculation that Tl doping introduces Tl p states inside the band gap to trap the excited electrons. The trapping is highly effective to within several ps, as revealed by time-dependent density functional theory calculations. It alters the non-radiative relaxation process to result in a noticeable increase in the relaxation barrier from 0.3 to 0.63 eV, which reduces the non-radiative relaxation by roughly a factor of 105 at room temperature.