A first-principles study of co-doping in lanthanum bromide

It was recently shown that the energy resolution of Ce-doped LaBr$_3$ scintillator radiation detectors can be crucially improved by co-doping with Sr, Ca, or Ba. Here we outline a mechanism for this enhancement on the basis of electronic structure calculations. We show that Sr dopants create and bind to Br vacancies, resulting in stable neutral complexes. The association with Sr causes the deep vacancy level to move toward the conduction band edge. This is essential for reducing the effective carrier density available for Auger quenching during thermalization of hot carriers. Subsequent de-trapping of electrons from the complexes can activate Ce dopants that have previously captured a hole leading to luminescence. This mechanism implies an overall reduction of Auger quenching of free carriers, which is expected to improve the linearity of the photon light yield with respect to the energy of incident electron or photon. Optical properties of the Ce-Sr-vacancy triple complex are discussed and compared to experiment. Prepared by LLNL under Contract DE-AC52-07NA27344.