Luis Stand

High energy resolution scintillators for nuclear nonproliferation applications

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: AM2X5:Eu, AMX3, and A2MX4:Eu (A = Cs, K; M = Ca, Sr, Ba; X = Br, I) as well as mixed elpasolites Cs2NaREBr3I3: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 KSr2I5: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.

Zero-dimensional Cs4EuX6 (X = Br, I) all-inorganic perovskite single crystals for gamma-ray spectroscopy

Organic–inorganic and all-inorganic halide perovskites have become leading candidates toward high-performance optoelectronic devices and radiation detectors. In this work, we report novel zero-dimensional Cs4EuX6 (X = Br, I) perovskite single crystals as self-activated scintillators with superior performance for gamma-ray spectroscopy. Both Cs4EuBr6 and Cs4EuI6 single crystals grown by the Bridgman method were determined to have the trigonal crystal structure with the Rc space group, and have a melting point of approximately 540 °C. Cs4EuBr6 and Cs4EuI6 exhibit blue emission under UV excitation and high light yields of 78 000 ± 4000 photons per MeV and 53 000 ± 3000 photons per MeV under 137Cs gamma-ray irradiation, respectively. In particular, the former represents the best result achieved for self-activated scintillators thus far. Thermally stimulated luminescence studies and density functional theory calculations elucidate the correlation between halogen vacancies and long-lived emission (afterglow) at room temperature in Cs4EuX6 (X = Br, I) single crystals. Our findings not only demonstrate the high gamma-ray detection efficiency in Cs4EuX6 (X = Br, I), but will further promote the development of 0D metal halide-based novel luminescent and radiation detection materials.

Crystal growth and characterization of selected high-performance scintillators for national security applications (Conference Presentation)

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.