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Scintillator materials based on certain types of activated alkali metal rare earth halide materials are described. In one embodiment, the material contains CsLaBr4 with Ce(III) ions substituted for a portion of the La component. The scintillator or other detector materials can be in monocrystalline or polycrystalline form. Radiation detectors that use the scintillators are also described, as are related methods for detecting high-energy radiation.