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DOE OSTI2024

Studies of Cherenkov photon production in PbF 2 crystals using proton beams at Fermilab

Future lepton colliders such as the FCC-ee, CEPC, ILC, or a muon collider will collect large data samples that allow precision physics studies with unprecedented accuracy, especially when the data is collected by innovative state-of-the-art detectors. An electromagnetic calorimeter based on scintillating crystals, designed to separately record Cherenkov and scintillation light, can achieve precision measurements of electrons and photons without sacrificing jet energy resolution, given adequate light collection efficiency and separation. This paper presents initial measurements from a program aimed at developing such a calorimeter system for future colliders. Finally, we focus on using PbF 2 crystals to enhance the understanding of Cherenkov light collection, marking the first step in this endeavor.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Thallium-based scintillators for high-resolution gamma-ray spectroscopy: Ce 3+ - doped Tl 2 LaCl 5 and Tl 2 LaBr 5

In this paper we report on the crystallographic and scintillation properties of Tl 2 LaCl 5 :Ce 3 + and Tl 2 LaBr 5 :Ce 3 + , two novel thallium-containing high-resolution scintillators for gamma-ray spectroscopy. Crystals of Tl 2 LaCl 5 :Ce 3 + and Tl 2 LaBr 5 :Ce 3 + were grown by the Vertical Bridgman method up to 1-inch diameter and 1-inch long. Single crystals of Tl 2 LaCl 5 :Ce 3 + and Tl 2 LaBr 5 :Ce 3 + belong to the orthorhombic system with space group 62 and have a density of 5.16 and 5.98 g/cm 3 , respectively. The scintillators show high light yields of up to 68,000 photons/MeV, excellent gamma-ray energy resolution of ≤ 3% at 662 keV, a fast scintillation decay, and a proportional response over a wide range of energies from 32 keV up to 1275 keV. Density Functional Theory calculations show that the Ce 3 + energy levels are inside the bandgap despite the smaller bandgap of Tl 2 LaCl 5 and Tl 2 LaBr 5 compared to K 2 LaCl 5 and K 2 LaBr 5 . Finally, a systematic Ce 3 + concentration study was performed for Tl 2 LaCl 5 :Ce 3 + and trends observed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Crystal Growth, Optical and Scintillation Properties of Eu 2+ -doped TlSr 2 Br 5

Crystals of undoped and Eu 2+ -doped TlSr 2 Br 5 of up to 16 mm in diameter and 50 mm in length were grown by the Vertical Bridgman technique. TlSr 2 Br 5 has the monoclinic crystal structure with space group P21/c. Its density and Z eff are 5.03 g/cm 3 and 58.6, respectively. Radioluminescence spectra of undoped and Eu 2+ -doped TlSr 2 Br 5 feature a broad emission band peaking at about 440 nm for undoped and 520 nm for Eu 2+ -doped crystals. The light yield of undoped TlSr 2 Br 5 is 42,000 ph/MeV, which increases to 55,000 ph/MeV for Eu 2+ -doped crystals. The energy resolution at 662 keV ( 137 Cs) is about 5 – 6% (FWHM). As a result, the scintillation decay of undoped and Eu 2+ -doped TlSr 2 Br 5 is of the order of 100s of nanoseconds.

Bridgman technique↗

DOE OSTI2021

Crystal growth, density functional theory, and scintillation properties of Tl 3 LnCl 6 :Ce 3+ and TlLn 2 Cl 7 :Ce 3+ (Ln = Y, Gd)

In this paper we report on the crystal growth, density functional theory (DFT) calculations and scintillation properties of Tl 3 LnCl 6 :Ce and TlLn 2 Cl 7 :Ce(Ln = Y, Gd). Crystals were grown by the Vertical Bridgman technique up to 16 mm in diameter and 25 mm long. Crystals of Tl 3 YCl 6 :Ce and Tl 3 GdCl 6 :Ce belong to the family of the Nesohalides which have the monoclinic crystal structure. Crystals of TlY 2 Cl 7 :Ce and TlGd 2 Cl 7 :Ce belong to the family of the Phyllohalides which have either the monoclinic or the orthorhombic crystal structure. We report the light yields of these Nesohalides and Phyllohalides are typically on the order of 35,000–40,000 ph/MeV.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Characterization and pulse-shape discrimination of a multi-stacked structure of ZnS: Ag/PMMA for fast-neutron detection in high-flux environments

The Micro-Layered Fast Neutron Detector (MLFD) is a proton-recoil scintillator that incorporates the basic concept of a Hornyak button detector with an improved design using a layered structure of ZnS:Ag and PMMA (polymethyl methacrylate). The MLFD was predicted to have low sensitivity to gamma rays, hence pulse shape discrimination was performed to determine the gamma-ray contribution. Presented in this paper are the pulse-shape discrimination characteristics of the MLFD. Additionally, the charge integration technique was employed to discriminate between the neutrons and gamma rays using a fast digitzer. The MLFD was found to exhibit excellent neutron/gamma-ray discrimination, with the highest Figure-of-Merit (FoM) being 4.56. With PSD, the neutron signal is distinct from gamma-ray, Ĉerenkov and electronic noise signals. This clear separation was achieved due to the large differences in decay times of the neutron and gamma-ray-induced pulses in the ZnS:Ag phosphor. The MLFD can be employed in high gamma-ray exposure fields, up to at least 1287.7 mR/hr, without appreciable degradation in PSD performance.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Investigation of the competition between Tl + and Ce 3+ scintillation in Tl2LiYCl6:Ce, an elpasolite scintillator

Li-containing elpasolite scintillators are currently investigated for their ability to detect both thermal neutrons and gamma photons with a single inorganic crystal. The scintillation is typically triggered by using an activator such as Ce. However, when Tl, also a luminescent ion, is present in the matrix, competition between the two centers Tl and Ce can occur. In this study, we are using Ce doped Tl 2 LiYCl 6 to investigate this competition. To this end, the Ce (which substitutes Y) concentration is varied from 0 to 1 in the Tl 2 LiY 1-x CexCl 6 composition. In the low concentration range in which Ce remains a dopant, the photo- and radioluminescence spectra show that the scintillation of Tl 2 LiYCl 6 :Ce is mostly dominated by recombination on intrinsic luminescent centers. For cerium concentrations higher than x = 0.02, very different emissions can be easily distinguished from the photo- and radioluminescence of undoped and low Ce doped Tl 2 LiYCl 6 crystals. These emissions are attributed to the formation of a second phase Tl 2 CeCl 5 , identified by X-ray diffraction. We conclude that the intrinsic luminescence related to Tl dominates the scintillation in the range of concentration for which Ce does substitute on the Y-site.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Crystal Growth Scale-Up and Stability of RbSr 2 X 5 :Eu Scintillators

The discovery and development of new scintillation materials support national security needs. In these applications, large volumes of scintillator crystals are needed to achieve efficient screening for contraband. Therefore, one important step in the discovery of new scintillator compositions is testing their feasibility for scale-up and their stability. In this work, high-quality Ø22 mm crystals of two new scintillators RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu were grown via the Vertical Bridgman method, and their scintillation properties were characterized. Here, the Ø22 mm RbSr 2 I 5 :Eu crystals could be grown with fast translation rates up to 3.5 mm/h. Both RbSr 2 Br 5 :Eu and RbSr 2 I 5 :Eu had high scintillation performance, including light yields of 46,000 and 61,000 ph/MeV, respectively, for Ø22 × 35 mm crystals. Additionally, properties related to physical stability were investigated, including the coefficients of thermal expansion via high-temperature X-ray diffraction (HTXRD) as well as moisture sensitivity. HTXRD confirmed the absence of solid–solid phase transitions and showed that RbSr 2 Br 5 had minimal thermal expansion anisotropy compared to RbSr 2 I 5 and some other inorganic metal halide scintillators, which favors the growth of large-sized crystals.

36 MATERIALS SCIENCE↗

DOE OSTI2024

WoRDMAp Outbrief: Workshop on Radiation Detection Materials [Slides]

Project Goal: Identify pathway to reliably grow and fabricate high-performance radiation detectors for use in a variety of nonproliferation applications. 1. Create 3 working groups (semiconductors, inorganic and organic scintillators) that bring together international R&D subject-matter experts (national laboratories, industry, and academia), end users, and mission stakeholders 2. Reach expert consensus views regarding current materials related technology gaps and define prioritized R&D directions required to resolve these gaps 3. Envisage the future state of next-generation radiation detection materials and quantify the benefits to nuclear security applications 4. Provide a comprehensive expert report to DNN R&D program office to serve as roadmap with recommendations for future high-impact office investment in radiation-detection materials development

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2026

Scintillator Library

This website provides measured scintillation properties of many inorganic and organic materials and citations to published papers in which the original measurements were reported. It is intended for two main uses: a web-accessible reference to useful scintillation detector materials and properties; an aid in developing fundamental theories or empirical relations between basic material properties and scintillation performance. To this end, both strong and weak scintillators have been included as well as those where sensitive measurements have not detected any scintillation emissions.

Shook, L. [University of California, Berkeley, CA ↗

NASA NTRS1971

Modification of codes NUALGAM and BREMRAD, Volume 1

The NUGAM2 code predicts forward and backward angular energy differential and integrated distributions for gamma photons and fluorescent radiation emerging from finite laminar transport media. It determines buildup and albedo data for scientific research and engineering purposes; it also predicts the emission characteristics of finite radioisotope sources. The results are shown to be in very good agreement with available published data. The code predicts data for many situations in which no published data is available in the energy range up to 5 MeV. The NUGAM3 code predicts the pulse height response of inorganic (NaI and CsI) scintillation detectors to gamma photons. Because it allows the scintillator to be clad and mounted on a photomultiplier as in the experimental or industrial application, it is a more practical and thus useful code than others previously reported. Results are in excellent agreement with published Monte Carlo and experimental data in the energy range up to 4.5 MeV.

Steyn, J. J.↗

DOE OSTI2024

Gallium oxide semiconductor-based large volume ultrafast radiation hard spectroscopic scintillators

We report on the development of the first-ever inorganic radiation-hard moisture-insensitive large volume spectroscopic semiconductor-based scintillator with less than 2 ns decay time and light yields as high as 8000 ph/MeV. Despite extensive research into scintillator materials, the quest for an ideal scintillator combining ultrafast decay times (akin to BaF 2 and Yb-doped scintillators such as Lu 2 O 3 :Yb), high light yields (exceeding 2000 photons per MeV), spectroscopic capabilities, and exceptional radiation hardness remain unfulfilled. In this study, we demonstrate and report for the first time the viability of large-volume (up to 20 mm thickness) gallium oxide (β-Ga 2 O 3 ) semiconductor-based scintillators for applications requiring these properties. These β-Ga 2 O 3 scintillators were grown using the fast turnaround (~2 days) crucible-free optical float zone (FZ) technique. The high light yield and ultrafast decay time of these high-purity n-type semiconductors with free carrier concentration of 6 × 10 17 cm –3 are attributed to native defects, specifically oxygen vacancies (V O ) and gallium–oxygen vacancy pairs (V Ga –V O ), generated during optimized FZ growth. The ultrafast decay, along with high light yield, enables excellent timing resolution and high count rate detection for applications like time-of-flight positron emission tomography, physics experiments, and nuclear safety. The radiation hardness of these devices has been documented in a separate publication.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2022

Structural Changes in Molten Salt Fuel and/or Waste Stream Compounds Cs 2 UCl 6 and Cs 2 UO 2 Cl 4 from Room Temperature to Melting and Related Materials [Slides]

Perovskite phases have been explored in recent literature as waste forms for long term storage of radioactive waste from molten salt reactors specifically. Synthesis of new halide perovskite phases can inform these efforts as well as molten salt reactor chemistry in general. Inorganic perovskites have also shown promise as new scintillating materials for detection of X-rays and gamma rays. Modifying the structure and chemistry of these compounds, perhaps with organic components, could be used to synthesize new scintillating compounds or modify the properties of existing ones. Both U 6+ and U 4+ readily form compounds with a striking similarity to vacancy ordered perovskites (Cs 2 UO 2 Cl 4 and Cs 2 UCl 6 ). Each of these compounds is relevant to molten salt reactor chemistry and/or waste streams. These phases could from in uranium chloride salt systems or waste streams: Cs being a fission product.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

350 ps Ultrafast room-temperature scintillation realized on CsPbBr 3 -based single crystals via Br 2 over-doping

Ultrafast scintillators are essential for next-generation radiation detection, positron emission tomography, and high-speed medical imaging. All-inorganic CsPbBr 3 perovskites are attractive candidates because of their high stopping power, and excellent optical quality, yet their long carrier lifetimes result in slow scintillation responses on the order of hundreds of nanoseconds. Here, we demonstrate that controlled over-doping with Br 2 produces CsPbBr 3.03 single crystals with sub-nanosecond scintillation at room temperature while preserving crystal quality. Single crystals grown by the Bridgman method exhibit high transparency and maintain the orthorhombic perovskite structure. Br 2 over-doping induces a slight lattice expansion (about 0.42% increase in unit-cell volume) while maintaining the orthorhombic perovskite phase and high optical transparency. Optical absorption reveals a slight redshift of the absorption edge after Br 2 introduction, indicating a modified defect landscape. Time-resolved photoluminescence and radioluminescence measurements show that Br 2 doping creates dense and efficient recombination centers that reduce the scintillation decay time from more than 100 ns in undoped crystals to 350 ps under 5.486 MeV α-particle excitation, and the scintillation decay time decreases by two orders of magnitude. The doped crystals also achieve a spatial resolution of 12 lp mm −1 in X-ray imaging. These results reveal a defect-engineering route for achieving ultrafast scintillation in halide perovskites and highlight the potential of Br 2 -modified CsPbBr 3 for fast timing applications.

Li, Zongxiao [Chinese Academy of Sciences (CAS), N↗

DOE OSTI2023

Long-Lived and Bright Biexcitons in Quantum Dots with Parabolic Band Potentials

Multiple exciton physics in semiconductor nanocrystals play an important role in optoelectronic devices. Here, this work investigates radially alloyed CdZnSe/CdS nanocrystals with suppressed Auger recombination due to the spatial separation of carriers, which also underpins their performance in optical gain and scintillation experiments. Due to suppressed Auger recombination, the biexciton lifetime is greater than 10 ns, much longer than most nanocrystals. The samples show optical gain, amplified spontaneous emission, and lasing at thresholds <2 excitons per particle. They also show broad gain bandwidth (>500 meV) encompassing 4 amplified spontaneous emission bands. Similarly enabled by slowed multiple exciton relaxation, the samples display strong performance in scintillating films under X-ray illumination. The CdZnSe/CdS samples have fast radioluminescence rise (<80 ps) and decay times (<5 ns), light yields up to 6700 photonsMeV -1 , and the demonstrated capacity for incorporation into large area films for scintillation imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Colorimetric radiation detector

A low cost, rapid, flexible radiation detector uses inorganic metal halide precursors and dyes that respond to self-quenching hybrid scintillation. Remote, high-contrast, laser sensing can be used to determine when exposure of the detector to radiation occurs (even temporally).

Boyle, Timothy J.↗

DOE OSTI2023

Colorimetric radiation detector

Garzon, Fernando Henry↗

DOE OSTI2023

Influence of fluorescent dopants on the vat photopolymerization of acrylate-based plastic scintillators for application in neutron/gamma pulse shape discrimination

Plastic scintillators, a class of solid-state materials used for radiation detection, were additively manufactured with vat photopolymerization. The photopolymer resins consisted of a primary dopant and a secondary dopant dissolved in a bisphenol A ethoxylate diacrylate-based matrix. The absorptive dopants significantly influence important print parameters, for example, secondary dopants decrease the light penetration depth by a factor > 12×. The primary dopant 2,5-diphenyloxazole had minimal impact on the printing process even when loaded at 25 % by mass of the resin. Working curve measurements, which relate energy dose to cure depth, were performed as a function of feature size to further assess the influence of dopants. Photopatterns smaller than 150 µm width had apparent increases in critical energy dose compared to larger photopatterns, while all resins maintained printed features in line gratings with 50 µm of separation. Printed scintillator monoliths were compared to scintillators cast by traditional molding, demonstrating that the layer-by-layer printing process does not decrease scintillation response. In conclusion, a maximum light output of 31 % of a benchmark plastic scintillator (EJ-200) and successful pulse shape discrimination were achieved with 20 % by mass 2,5-diphenyloxazole as the primary dopant and 0.1 % by mass 9,9-dimethyl-2,7-distyrylfluorene as the secondary dopant in printed scintillator samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Influence of irrigation approaches and spatial geolocation on tritium speciation, uptake and depuration

Pine needles and tree cores from a tritium (T) contaminated phytoremediation forest at the Savannah River Site (SRS in Aiken, SC) Mixed Waste Management Facility (MWMF) were measured for total T and T speciation and compared to other locations at the SRS and the surrounding area. Tree core ages ranged from 9 to 14 years old, covering over half of the ~20-year on-going remediation efforts, while pine needles represent more recent time periods of 1-to-2-year increments. Remedial irrigation efforts at the MWMF are found to directly influence the pine needle T concentrations. The T content in the MWMF samples is higher than non-irrigated needle samples from other locations around the SRS. Furthermore, the different forms of organic bound T are preferentially stored in tree core tissue, compared to pine needles where tritiated water dominates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗