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DOE OSTI2020

Role of Lithium Codoping in Enhancing the Scintillation Yield of Aluminate Garnets

The aim of this work is to clarify the scintillation-yield enhancement in Lu YAG : Pr scintillators obtained by Li codoping via integrated study of the valence state of activators, the preferential site occupancy of Li codopants, and defect structures from experimental and theoretical insights. Here, with Li codoping, the light yield and energy resolution of 10 × 10 × 10 mm 3 Lu YAG : Pr samples are improved from 156000 to 248000 photons/MeV, and 5.3 to 4.3% at 662 keV,respectively.The optical absorption spectra indicate that Li codoping does not induce conversion of stable Pr 3 + to Pr 4 + in Lu YAG : Pr single crystals. Based on the formation energies of substitutional and interstitial Li sites using density-functional-theory (DFT) calculations and the 7 Li nuclear magnetic resonance results, it is shown that the Li ions prefer to dominantly occupy the fourfold coordinated interstitial sites and fourfold coordinated Al sites. The systematic analysis of thermoluminescence glow curves, positron annihilation lifetime spectroscopies, and defect formation energies derived from DFT calculations reveals that the concentration of isolated Lu and Al vacancies as dominant acceptor defects is reduced by Li codoping, whilst the shallow Li i interstitial defects and the deep V O oxygen vacancies are introduced simultaneously. We propose that the lowering of hole trapping at defects resulting from Li codoping contributes to the scintillation-yield enhancement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Detection of uranium-photofission neutrons with a 4 He scintillation detector

The use of photon active interrogation to detect special nuclear material has held significant theoretical promise, as the interrogating source particles, photons, are fundamentally different from one of the main signatures of special nuclear material: neutrons produced in nuclear fission. However, neutrons produced by photonuclear reactions in the accelerator target, collimator, and environment can obscure the fission neutron signal. These (γ, n) neutrons could be discriminated from fission neutrons by their energy spectrum, but common detectors sensitive to the neutron spectrum, like organic scintillators, are typically hampered by the intense photon background characteristic of photon-based active interrogation. In contrast, high-pressure 4 ⁢He-based scintillation detectors are well-suited to photon active interrogation, as they are similarly sensitive to fast neutrons and can measure their spectrum, but show little response to gamma rays. Here, in this work, a photon active interrogation system utilizing a 4 ⁢He scintillation detector and a 9 MeV linac-bremsstrahlung x-ray source was experimentally evaluated. The detector was shown to be capable of operating in intense gamma-ray environments and detecting photofission neutrons from 238 ⁢U when interrogated by this x-ray source. The photofission neutrons show clear spectral separation from (γ, n) neutrons produced in lead, a common shielding material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Scintillation yield from electronic and nuclear recoils in superfluid He 4

Superfluid $^4$He is a promising target material for direct detection of light ($<$ 1 GeV) dark matter. Possible signal channels available for readout in this medium include prompt photons, triplet excimers, and roton and phonon quasiparticles. The relative yield of these signals has implications for the sensitivity and discrimination power of a superfluid $^4$He dark matter detector. Using a 16~cm$^3$ volume of 1.75~K superfluid $^4$He read out by six immersed photomultiplier tubes, we measured the scintillation from electronic recoils ranging between 36.3 and 185~keV$_\mathrm{ee}$, yielding a mean signal size of $1.25^{+0.03}_{-0.03}$~phe/keV$_\mathrm{ee}$, and nuclear recoils from 53.2 to 1090~keV$_\mathrm{nr}$. We compare the results of our relative scintillation yield measurements to an existing semiempirical model based on helium-helium and electron-helium interaction cross sections. As a result, we also study the behavior of delayed scintillation components as a function of recoil type and energy, a further avenue for signal discrimination in superfluid $^4$He.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Crystal Growth and Characterization of Europium-Doped Rubidium Calcium Bromide Scintillators

National security strategies like gamma spectroscopy and high-energy X-ray radiography are limited, in part, by the scintillator used, prompting research into novel materials with improved properties. In this paper, Eu 2+ activated rubidium calcium bromide scintillators were grown via the vertical Bridgman method with a range of dopant concentrations. Light yield, energy resolution, and the afterglow of Rb 4 CaBr 6 :Eu and RbCaBr 3 :Eu improved with increasing Eu 2+ concentration, and scintillation decay time increased. The highest light yields of Rb 4 CaBr 6 :Eu and RbCaBr 3 :Eu were 71000 and 45000 ph/MeV, respectively.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Proton Quenching in Rare-Earth Inorganic Scintillators: GAGG:Ce and YSO:Ce

Scintillator detectors are an integral component of radiation detection systems for a variety of applications such as medical imaging, accelerator diagnostics, and space science. Typically, a scintillator detector’s response is characterized using gamma sources to understand the detection response to different types of radiation, including charged particle detection. However, there exists a nonlinearity of the amount of light produced from an incident gamma ray of specific energy and the light produced from an incident charged particle of the same energy. This important effect, known as quenching, must be accounted for to interpret energies from charged particles incident on detectors. In this article, we present results of quenching parameterization for two types of cerium-doped inorganic scintillators, Y2SiO5:Ce (YSO:Ce) and Gd3Al2Ga3O12:Ce (GAGG:Ce). We measured the light output from incident proton energies from 1 to 25 MeV using a 3-MV tandem accelerator and two reactions: Au(p,p)Au and 3He(d,p)⁴He. Using gamma-ray sources to calibrate the detectors, we compared the measured electron-equivalent energy versus the incident energy expected. Using an adaptation of the Birks semi-empirical formula, we extracted the Birks parameter (kB) to understand quenching. For one of the GAGG:Ce samples, the kB parameter of 0.0072 [g cm-2 MeV-1] is comparable to a similar study where the value of kB was 0.0065 [g cm-2 MeV-1]. For YSO:Ce, no other kB values were found in the literature. Three different types of GAGG:Ce were used to collect measurements of kB as a function of dopant concentration.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Application of the Rossi-alpha method to simulations of HEU and organic scintillators

The International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook contains thousands of high-quality benchmark measurements that include detailed descriptions of experiment designs and exhaustive accounting of uncertainties. These benchmarks are used extensively by the criticality safety and nuclear data communities. A subcritical benchmark involving bare, highly enriched uranium (HEU) has yet to be accepted to the handbook. The Measurement of Uranium Subcritical and Critical (MUSiC) was proposed to address this gap. MUSiC will be performed at the National Criticality Experiments Research Center (NCERC) and will leverage bare HEU hemisphere shells that can be assembled in a variety of configurations. The measurement has the following key benefits: it will be the first set of fast, subcritical measurements of HEU to be submitted to ICSBEP; ten configurations will be measured spanning from nearly no multiplication to critical (e.g., it is a measurement of similar systems with different re activities); measurements of an all-HEU system will be of value for nuclear data validation, providing results that assist in determining biases in both measurements and simulations. A variety of detector systems will be used including a Neutron Multiplicity Array Detector (NoMAD) system (similar to the MC-15), four small volume 0.635 cm (#8960;) × 7.59 cm 3He detectors (ideal for measuring prompt neutron decay constants due to their fast recovery speed), and an array of eight 5.08 cm (#8960;) × 5.08 cm EJ-309 organic scintillator detectors. The focus of this work is the simulation of the subcritical MUSiC configurations including the EJ-309 detectors and the application of the Rossi-α method. The EJ-309 organic scintillator detector array is a new detection system that will be deployed at NCERC. Organic scintillators are ideal for measurements of fast, subcritical systems due to their short time response on the order of nanoseconds.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Design and implementation of the new scintillation light detection system of ICARUS T600

ICARUS T600 is the far detector of the Short Baseline Neutrino program at Fermilab (U.S.A.), which foresees three Liquid Argon Time Projection Chambers along the Booster Neutrino Beam line to search for LSND-like sterile neutrino signal. The T600 detector underwent a significant overhauling process at CERN, introducing new technological developments while maintaining the already achieved performances. The realization of a new liquid argon scintillation light detection system is a primary task of the detector overhaul. As the detector will be subject to a huge flux of cosmic rays, the light detection system should allow the 3D reconstruction of events contributing to the identification of neutrino interactions in the beam spill gate. The design and implementation of the new scintillation light detection system of ICARUS T600 is described.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Study of scintillation light collection, production and propagation in a 4 tonne dual-phase LArTPC

The 3×1×1 m3 demonstrator is a dual phase liquid argon time projection chamber that has recorded cosmic rays events in 2017 at CERN. The light signal in these detectors is crucial to provide precise timing capabilities. The performance of the photon detection system, composed of five PMTs, are discussed. The collected scintillation and electroluminescence light created by passing particles has been studied in various detector conditions. In particular, the scintillation light production and propagation processes have been analyzed and compared to simulations, improving the understanding of some liquid argon properties.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Manufacturing and characterization of a boron-loaded fast-cured plastic organic scintillator

A novel fast-cured, boron-loaded, plastic organic scintillator was developed and characterized. A diisopropylnaphthalene-containing scintillator was manufactured in minutes with the addition of two commercially available fast-curing monomers, isobornyl acrylate (IBOA) and 1,6-Hexanediol dimethacrylate (HDDMA). Further, the light yield of the device was measured to be approximately 70% relative to a similarly sized, but several-year-aged, EJ-276 detector. Using a coincidence capture technique, the neutron capture light output was found to be 87.7 ± 4.2 keVee, which was 1.47 ± 0.07 greater than the light output from a 59.5 keV electron. Producing a viable fast-cured and thermal-neutron-sensitive detector enables the capability to pursue cost-effective 3D printed thermal neutron detectors in a timely manner.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Development of a large-mass, low-threshold detector system with simultaneous measurements of athermal phonons and scintillation light

For this work, we have combined two low-threshold detector technologies to develop a large-mass, low-threshold detector system that simultaneously measures the athermal phonons in a sapphire detector while an adjacent silicon high-voltage detector detects the scintillation light from the sapphire detector. This detector system could provide event-by-event discrimination between electron and nuclear events due to the difference in their scintillation light yield. While such systems with simultaneous phonon and light detection have been demonstrated earlier with smaller detectors, our system is designed to provide a large detector mass with high amplification for the limited scintillation light. Future work will focus on at least an order of magnitude improvement in the light collection efficiency by having a highly reflective detector housing and custom phonon mask design to maximize light collection by the silicon high-voltage detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Total neutron cross-section measurement on CH with a novel 3D-projection scintillator detector

In order to extract neutrino oscillation parameters, long-baseline neutrino oscillation experiments rely on detailed models of neutrino interactions with nuclei. These models constitute an important source of systematic uncertainty, partially because detectors to date have been blind to final state neutrons. Three-dimensional projection scintillator trackers comprise components of the near detectors of the next generation long-baseline neutrino experiments. Due to the good timing resolution and fine granularity, this technology is capable of measuring neutron kinetic energy in neutrino interactions on an event-by-event basis and will provide valuable data for refining neutrino interaction models and ways to reconstruct neutrino energy. Two prototypes have been exposed to the neutron beamline at Los Alamos National Laboratory (LANL) in both 2019 and 2020, with neutron energies between 0 and 800 MeV. In order to demonstrate the capability of neutron detection, the total neutron-scintillator cross section as a function of neutron energy is measured and compared to external measurements. The measured total neutron cross section in scintillator between 98 and 688 MeV is 0.36 ± 0.05 barn.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Next-generation neutron detection using a 6 Li glass scintillator composite

Neutron detectors are crucial in fundamental science, nuclear security, safeguards, and civil applications. 3 He-filled gas proportional counters are the gold standard for thermal neutron detection, prized for their efficiency, neutron/gamma discrimination, and stability; however, the scarcity of 3 He has prompted the search for alternatives. Here, we introduce a neutron detector design based on a scintillating composite consisting of 6 Li glass scintillator particles dispersed in an organic matrix. A detector consisting of this scintillating composite, photomultiplier tubes (PMTs) for optical detection, and electronics for reading out the PMT signal in both pulse and current modes was prototyped and characterized using various neutron and gamma sources. The prototype achieves a measured intrinsic detection efficiency of 6.70 ± 0.01%, a die-away time of 10.3 ± 0.1 μs, a negligible gamma misidentification probability, and response linearity up to at least 3.7 × 10 6 incident neutrons/s established via a cross-calibration technique. This detector holds the potential to outperform traditional 3 He-gas-based neutron detection systems, offering a viable alternative amidst the ongoing 3 He shortage and promising advancements in neutron detection technology.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Devising novel methods for the controlled synthesis with morphology and size control of scintillator materials

Nanoscale scintillators represent an important class of materials underlying the functioning of high resolution, high ‘light yield’ radiation detection equipment, applicable for medicine in addition to security and environmental monitoring. This current study has focused on the controlled synthesis of Cs 2 ZnX 4 (X = Cl, Br) not only due to its very fast and promising radioluminescence decay time but also because no reliable synthesis protocols have been reported for producing nanoscale motifs of this material, to date. Solution-based methods can be used to synthesize products, possessing different, discrete morphologies with the ability to dictate particle size and shape. Specifically, we have demonstrated that a hot injection technique can be used to fabricate nanoscale rods and plates. Using this method, we systematically studied the effect of varying reaction variables, such as (i) reaction temperature, (ii) surfactants, and (iii) reaction time. As synthesized nanorods of Cs 2 ZnCl 4 possessed lengths of 101.3 ± 24.4 nm with widths of 17.3 ± 4.5 nm, whereas Cs 2 ZnBr 4 , created under identical conditions, were characterized by lengths of 206 ± 50 nm and widths of 26.7 ± 12.6 nm. Ligand-assisted re-precipitation (LARP) was used to produce the corresponding micron-sized particles. Under these conditions, we successfully synthesized spindles and spherical particles of Cs 2 ZnCl 4 with sizes of 1.58 ± 0.16 μm and 1.03 ± 0.34 μm, respectively, whereas plates of Cs 2 ZnBr 4 were prepared with average sizes of 0.76 ± 0.21 μm. High resolution synchrotron mapping, using the hard X-ray nanoprobe at NSLS II, was used to confirm the expected spatial distribution of Cs, Zn, and Cl within the as-produced crystals. Nanorods of Cs 2 ZnCl 4 and Cs 2 ZnBr 4 were subsequently tested for scintillation light yield and decay times. Preliminary results showed that Cs 2 ZnCl 4 maintained a light yield of 100–300 photons per MeV with a fast decay component of 2.6 ns. Finally, the Cs 2 ZnBr 4 analogue did not give rise to any perceptible scintillation emission.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Gas scintillation mitigation in gas Cherenkov detectors for inertial confinement fusion (invited)

Gas Cherenkov detectors provide a time resolved measurement of the fusion burn in inertial confinement fusion experiments. The fusion rate delivers critical benchmark figures, such as burn width and bang time. Recent detector improvements pushed temporal resolution to 10 ps to make burn width measurements on igniting targets possible. First high temporal resolution measurements using CO 2 gas fills had a background signal with a long decay length (tail), which was caused by gas scintillation. This gas scintillation limits the ability of the detector to resolve short burn width and high frequency features in the fusion rate measurements. A thorough investigation of the cause of the tail and mitigation options for gas scintillation is presented here. As a near-term resolution, neon gas is being used to extract fusion burn histories. Paths forward for the next generation of gas Cherenkov detectors are identified including the usage of oxygen as a Cherenkov medium.

47 OTHER INSTRUMENTATION↗

DOE OSTI2020

Measurement of Liquid Argon Scintillation Light Properties by means of an Alpha Source placed inside the CERN 10-PMT LAr Detection System

A particle detection system that exploits the scintillation light produced by ionizing particles in liquid argon (LAr) has been assembled at CERN. The system is based on 10 large-area photomultiplier tubes (PMT) immersed in a 1500-liter dewar filled with liquid argon and equipped with an extendible feed-through and mechanical support for an alpha source (241Am). The position of the source can be changed with respect to the PMT plane in vertical and horizontal directions. Arrays of silicon photomultiplier (SiPM) photodetectors, integrated in the source support, are used for the data acquisition trigger and to define the t0 of the light generation. PMT and SiPM signals can be recorded at different distances and different positions allowing the measurement of some of the LAr scintillation light properties. The system was studied and characterized in detail, and physics results on LAr scintillation properties are expected soon.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Development, characterisation, and deployment of the SNO+ liquid scintillator

A liquid scintillator consisting of linear alkylbenzene as the solvent and 2,5-diphenyloxazole as the fluor was developed for the SNO+ experiment. This mixture was chosen as it is compatible with acrylic and has a competitive light yield to pre-existing liquid scintillators while conferring other advantages including longer attenuation lengths, superior safety characteristics, chemical simplicity, ease of handling, and logistical availability. Its properties have been extensively characterized and are presented here. This liquid scintillator is now used in several neutrino physics experiments in addition to SNO+.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Secondary scintillation properties of multi-layer THGEMs operated in low-pressure CF 4 and Ar/5%Xe

We present a measurement of the secondary scintillation yield produced by two-layer Thick Gas Electron Multipliers (M-THGEMs) in pure Tetrafluoromethane (CF 4 ) gas and in Ar mixed with 5% Xe in low-pressures down to 20 Torr. The detector was irradiated with 5.49 MeV alpha particles from a low-rate 241-Am source. The secondary scintillation light generated during the gas avalanche process was read out by a Hamamatsu photomultiplier tube (model R8520-406), sensitive to a broad wavelength range (160–650 nm). The avalanche charge was collected on the bottom electrode of M-THGEM and correlated to the scintillation light on an event-by-event basis. We observed that, for both gas types, the value of the photon to electron production ratio (0.4 ph/el in CF 4 and 0.1 ph/el in Ar/5%Xe) increases with the thickness of the M-THGEM electrodes and varies significantly with the pressure, being higher at lower values. The decrease in electroluminescence yield at higher pressures is much more pronounced in the Ar/Xe mixture. In addition, because of a larger gas avalanche volume, the electroluminescence light yield is larger in thicker M-THGEM structures. Presented results are particularly useful for designing the next generation of Optical-readout Time Projection Chambers (O-TPCs) operated at low-pressure CF 4 ; applications include experimental nuclear physics with rare isotope beams, dark matter detection with directional sensitivity and observation of the Migdal effect in a low-pressure Optical TPC.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

A laserball calibration device for the SNO+ scintillator phase

Located 2 km underground in SNOLAB, Sudbury, Canada, SNO+ is a large scale liquid scintillator experiment that primarily aims to search for neutrinoless double beta decay. Whilst SNO+ has light and radioactive calibration sources external to the inner volume, an internally deployed optical source is necessary for the full characterization of the detector model. A laser diffuser ball developed for SNO has previously demonstrated to be an effective optical calibration device for both SNO and SNO+ water phase. Since the introduction of liquid scintillator for SNO+, the material compatibility, cleanliness, and radiopurity requirements of any materials in contact with the internal medium have increased. Improving on the original SNO laserball design, a new laserball calibration device has been developed for the SNO+ scintillator phase with the goal of measuring the optical properties of the detector and performing routine PMT gain and timing calibrations. Simulations have been written to model the diffusion properties to optimise optical and temporal performance for calibration. Prototype laserballs have been built and characterised, demonstrating sub-ns timing resolution and a quasi-isotropic light distribution.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗