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In this work the Bridgman crystal growth and scintillation properties of both undoped and Tl-doped Cs 3 Cu 2 I 5 are presented. This material is very attractive for gamma and X-ray detection applications, with a density of 4.53 g/cm3 and effective atomic number of 51.9. Undoped Cs 3 Cu 2 I 5 had a light yield of 41,500 photons/MeV, with an energy resolution of 4.4% at 662 keV. Thallium doping at 0.5 mol % resulted in a much-improved scintillation response, in which light yield increased to 98,200 photons/MeV and energy resolution reduced to 3.3% at 662 keV. The X-ray excited emission is centered at 442 nm for the undoped and 500 nm for the Tl-doped crystals. The undoped emission is broad, typical of excitonic emission, while thallium doping results in an even broader band with features of both the undoped and thallium defect-mediated emissions. • Transparent single crystals of undoped Cs 3 Cu 2 I 5 and Cs 3 Cu 2 I 5 (Tl) were grown via the Bridgman technique. • Phase purity was established via powder XRD analysis. • Undoped Cs 3 Cu 2 I 5 has 41,500 photons/MeV and 4.4% energy resolution at 662 keV. • Tl doping at 0.5 mol% improves light yield to 98,200 photons/MeV and energy resolution to 3.3%. [ABSTRACT FROM AUTHOR]

Recently discovered scintillators Cs 4 SrI 6 :Eu and Cs 4 CaI 6 :Eu have shown promising properties for gamma-ray detection in homeland security applications, with <4% energy resolution (at 662 keV) and light yields above 50,000 ph/MeV. However, a thorough investigation of the effects of europium concentration has not yet been conducted. In this work, Eu2+ concentration was varied from 0.5 mol% to 9 mol%, and Ø7 mm single crystals were grown from the melt via the vertical Bridgman method. Scintillation performance was evaluated as a function of Eu2+ concentration to determine the optimal amount. The observed trend was improved energy resolution and higher light yield with increasing Eu2+ concentration up to 7 mol%. The best energy resolution achieved was 3.2% for Cs 4 SrI 6 :Eu 7% and 3.6% for Cs 4 CaI 6 :Eu 7%. Their respective light yields were 71,000 ph/MeV and 69,000 ph/MeV. • Photoluminescence and radioluminescence emission show weak dependence on europium concentration in Cs4SrI6:Eu and Cs4CaI6:Eu. • A maximum light yield of 78,000 ph/MeV is obtained with 9 mol% europium in Cs4SrI6:Eu. • An energy resolution of 3.2% at 662 keV is achieved with 7 mol% europium in Cs4SrI6:Eu. [ABSTRACT FROM AUTHOR]

KCaI 3 :Eu single crystals exhibit favorable scintillation properties and have potential for use in domestic security applications requiring radioisotope identification. The anisotropic thermal expansion of the orthorhombic unit cell of this perovskite-type scintillator has been investigated using in-situ high temperature X-ray diffraction on powdered samples. Samples from single crystals of both pure and Eu-doped KCaI 3 grown by the Bridgman method were used for comparison. Expansion with temperature along the b -axis is greatest with an average linear coefficient of thermal expansion of ≈ (41–46) x 10 −6  K −1 resulting from the weaker bonding between alternating layers of K and Ca parallel to the b -axis. Thermal expansion in each of the KCaI 3 samples has the highest degree of anisotropy with respect to the b and c axis with ratio ᾱ b /ᾱ c of 1.4–1.5. Additionally, we identify the predominant cleavage plane in KCaI 3 as (0 -3 -1) based upon Laue reflection imaging. [ABSTRACT FROM AUTHOR]

KCaI 3 :Eu crystals have been identified as very promising for use in spectroscopic detector applications related to nuclear nonproliferation and domestic security efforts. Initial studies have shown for small crystals a few mm 3 in size with 3% europium dopant concentration, a high light yield of >70,000 ph/MeV and energy resolution of ≈3% at 662 keV is attainable which is comparable with the highest performance scintillators discovered. In this work, single crystals of KCaI 3 with a range of Eu 2+ doping between 0 and 5 at% substituting for Ca 2+ were grown at 22 mm diameter and their performance for gamma-ray spectroscopy studied. Comparisons among crystals approximately Ø22 mm×22 mm (8.4 cm 3 or ≈0.5 in 3 ) provide a more accurate understanding of how scintillation performance changes with Eu doping and increased crystal size. KCaI 3 in the undoped form is shown to be a highly efficient intrinsic scintillator with a defect-related emission at 404 nm which coexists with the Eu 2+ 5d–4f emission in low dopant concentrations and is completely re-absorbed in more heavily doped crystals. For larger crystals, effects from self-absorption due to Eu activation become more evident by a near doubling of decay time for 0.5 in 3 crystals as the activator is increased from 0.5 to 5.0 at% Eu. Comparisons of pulse-height spectra obtained for Ø22 mm×22 mm cylinders with varying Eu concentration suggests best performance is achieved using lower Eu additions closer to 0.5–1.0 at%. Using a modified crystal packaging featuring an offset reflector geometry, 0.5 in 3 crystals of KCaI 3 :Eu can attain under 4% energy resolution at 662 keV. [ABSTRACT FROM AUTHOR]

Yb2+ was investigated as a potential alternative activator for Cs 4 SrI 6 and Cs 4 CaI 6 scintillators for the first time, as opposed to the previously studied Eu2+ activator. Single crystals with nominal Yb2+ concentrations of 0.5 mol%, 1 mol%, and 3 mol% were grown in Ø7 mm ampoules using the vertical Bridgman method. Luminescence and scintillation properties were evaluated as a function of Yb2+ concentration and host compound. The 5 d → 4 f electronic transition of Yb2+ was observed for both the Sr- and Ca-containing compositions. X-ray induced radioluminescence emission was centered between 449 nm and 463 nm depending on Yb2+ concentration and host compound. Both the spin-allowed and spin-forbidden transitions were observed in photoluminescence emission spectra and were centered at 446 nm and 476 nm, respectively, for both compounds. The best scintillation performance was achieved with Cs 4 CaI 6 :Yb 1 mol%, which had a 3.5% energy resolution at 662 keV and 43,000 ph/MeV light yield. To our knowledge this is the best energy resolution ever reported for a Yb2+-doped scintillator. Additional Cs 4 CaI 6 :Yb 1% crystals were grown in Ø12 mm ampoules to investigate the size dependence of scintillation properties, as well as crystal homogeneity. • Single crystals of Cs4CaI6:Yb and Cs4SrI6:Yb were grown using the vertical Bridgman technique. • Cs4CaI6:Yb 1% has an energy resolution of 3.5% at 662 keV and light yield of 43,000 ph/MeV. • Emission from the Yb2+ spin-allowed and spin-forbidden transitions are both observed in photoluminescence spectra.. [ABSTRACT FROM AUTHOR]