Scintillators are important materials for radiation detection applications such as homeland security, geological exploration, and medical imaging. Scintillators for nuclear nonproliferation applications in particular must have excellent energy resolution in order to distinguish the gamma-ray signatures of potentially dangerous radioactive sources, such as highly enriched uranium or plutonium, from non-threat radioactive sources such as radioactive tracers used in medical imaging. There is an established need for scintillators with energy resolution in the 1-2% range at 662 keV. However, there are challenges surrounding the development of this new generation of high light yield/high resolution scintillators; for example, the high cost of production due to low crystal yield and slow growth process, and crystal inhomogeneity. We will discuss efforts focused on developing recently discovered high performance scintillators K(Sr,Ba)2I5:Eu, Cs4(Ca,Sr)I6:Eu and Cs2Hf(Cl,Br)6 that have potential for meeting nuclear security needs. Growth parameters for these materials have been optimized, allowing the growth of excellent quality single crystals measuring up to one-inch in diameter via the vertical Bridgman technique at translation rates between 1 and 5 mm/h. These scintillators materials have excellent properties with light yields between 30,000 and 120,000 ph/MeV, and energy resolutions between 2.3 and 4.6% at 662 keV.
The detection of ionizing radiation is important in numerous applications related to national security ranging from the detection and identification of fissile materials to the imaging of cargo containers. A key performance criterion is the ability to reliably identify the specific gamma-ray signatures of radioactive elements, and energy resolution approaching 2% at 662 keV is required for this task. In this work, we present discovery and development of new high energy resolution scintillators for gamma-ray detection. The new ternary halide scintillators belong to the following compositional families: AM<sub>2</sub>X<sub>5</sub>:Eu, AMX3, and A<sub>2</sub>MX<sub>4</sub>:Eu (A = Cs, K; M = Ca, Sr, Ba; X = Br, I) as well as mixed elpasolites Cs<sub>2</sub>NaREBr<sub>3</sub>I<sub>3</sub>:Ce (RE = La, Y). Using thermal analysis, we confirmed their congruent melting and determined crystallization and melting points. Using the Bridgman technique, we grew 6, 12 and 22 mm diameter single crystals and optimized the Eu concentration to obtain the best scintillation performance. Pulse-height spectra under gamma-ray excitation were recorded in order to measure scintillation light output, energy resolution and light output nonproportionality. The KSr<sub>2</sub>I<sub>5</sub>:Eu 4% showed the best combination of excellent crystal quality obtained at fast pulling rates and high light output of ~95,000 photons/MeV with energy resolution of 2.4% at 662 keV.
Conference Committee Involvement (1)
Hard X-Ray, Gamma-Ray, and Neutron Detector Physics XXI
11 August 2019 | San Diego, California, United States