An aliovalently calcium-doped cerium tribromide (CeBr3:Ca2+) crystal was prepared with a gamma-energy resolution (FWHM) of 3.2% at the 137Cs 662 keV gamma energy. We completed a crystal assessment and calculated the predictive performance and physical characteristics using density functional theory (DFT) formalism. Detector performance, characteristics, calcium doping concentration, and crystal strength are reported. The structural, electronic, and optical properties of CeBr3 crystals were investigated using the DFT within generalized gradient approximation. Specifically, we see excellent linearity of photons per unit energy with the aliovalent CeBr3:Ca2+ crystal. Proportionality of light yield is one area of performance in which Ce-doped and Ce-based lanthanide halides excel. Maintaining proportionality is the key to producing a strong, high-performance scintillator. Relative light yield proportionality was measured for both doped and undoped samples of CeBr3 to ensure no loss in performance was incurred by doping. The light output and proportionality for doped CeBr3, however, appears to be similar to that of undoped CeBr3. The new crystal was subjected to additional testing and evaluation, including a benchmark spectroscopy assessment. Results, which present energy resolution as a function of energy, are summarized. Typical spectroscopy results using a 137Cs radiation source are shown for our crystallites with diameters <1 cm. We obtain energy resolution of 3.2% before packing the crystallite in a sealed detector container and 4.5% after packing. Spectra were also obtained for 241Am, 60Co, 228Th, and background to illustrate the spectrosocopic quality of CeBr3:Ca2+ over a broader energy range.
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