Two-dimensional lead halide perovskites have demonstrated their potential as high-performance scintillators for X- and gamma-ray detection, while also being low-cost. Here we adopt lithium chemical doping in two-dimensional phenethylammonium lead bromide (PEA)2PbBr4 perovskite crystals to improve the properties and add functionalities with other radiation detections. Li doping is confirmed by X-ray photoemission spectroscopy and the scintillation mechanisms are explored via temperature dependent X-ray and thermoluminescence measurements. Our 1:1 Li-doped (PEA)2PbBr4 demonstrates a fast decay time of 11 ns (80%), a clear photopeak with an energy resolution of 12.4%, and a scintillation yield of 11,000 photons per MeV under 662 keV gamma-ray radiation. Additionally, our Li-doped crystal shows a clear alpha particle/gamma-ray discrimination and promising thermal neutron detection through 6Li enrichment. X-ray imaging pictures with (PEA)2PbBr4 are also presented. All results demonstrate the potential of Li-doped (PEA)2PbBr4 as a versatile scintillator covering a wide radiation energy range for various applications.

hybrid lead halide perovskites are potential candidates for high light yield scintillators as they have small band gaps between 3 and 4 eV and large excitonbinding energy. Here, we discuss the scintillation properties from a total of 11 organic/inorganic hybrid perovskite crystals with two already reported crystals, (PEA) 2 PbBr 4 and (EDBE)PbBr 4 . Their photoluminescence and X-ray luminescence (XL) spectra are dominated by narrow and broad band emissions, and they correspond to free exciton and self-trapped exciton, respectively. The lifetimes derived from time-resolved XL strongly vary from 0.6 to 17.0 ns. These values make this type of compound among the fastest scintillators. For the light yield derived from the XL, we found that only (PEA) 2 PbBr 4 , (EDBE)PbBr 4 , and (BA) 2 PbBr 4 crystals have light yields between 10,000 and 40,000 photons/ MeV. The mechanisms for thermal quenching and afterglow are discussed in order to optimize the light yields. With gamma-ray excitation, we reported the best energy resolution of 7.7% at 662 keV with excellent proportionality. Finally, this study paves the way toward the ultimate high light yield and fast scintillators for medical and homeland security applications.

Commensurate Lithium doping of two-dimensional lead halide perovskites leads to improved scintillation properties, with enhanced light yield, narrower energy resolution, higher radiation hardness and faster scintillation decay.