Synthesis and scintillation properties of CsGd2Cl7:Ce for gamma ray and neutron detection

In this work, we report on optical and scintillation properties of a new scintillation material CsGd₂Cl₇:Ce. Crystals were grown in vacuum sealed ampoules, and the response to gamma rays and thermal neutrons was characterized. The scintillation light yield was ∼38,000 ph/MeV, and the primary decay time was 60 ns under γ-ray excitation. A thermal neutron response resulting from capture by ¹⁵⁷Gd and ¹⁵⁵Gd and subsequent emission of conversion electrons and X-rays was observed. The crystals exhibited a layered structure with cleavage planes and relatively low hygroscopicity.     

Crystal growth and scintillation properties of Ce and Eu doped LiSrAlF6

Ce and Eu doped LiSrAlF₆ (LiSAF) single crystals for the neutron detection with different dopant concentrations were grown by the micro-pulling-down method (μ-PD). In Ce:LiSAF, intense emission peaks due to Ce³⁺ 5d-4f transitions were observed at approximately 315 and 335 nm in photo- and α-ray induced radio-luminescence spectra. In case of Eu:LiSAFs, an intense emission peak at 375 nm due to Eu²⁺ 5d-4f transition was observed in the radio-luminescence spectra. The pulse height spectra and decay time profiles were measured under ²⁵²Cf neutron irradiation to examine the neutron response. The Ce 3% and Eu 2% doped LiSAF showed the highest light yield of 2860 ph/n with 19 ns main decay time component and 24,000 ph/n with 1610 ns.     

Thermal neutron imaging with rare-earth-ion-doped LiCaAlF6 scintillators and a sealed Cf source

Thermal neutron imaging with Ce-doped LiCaAlF₆ crystals has been performed. The prototype of the neutron imager using a Ce-doped LiCaAlF₆ scintillating crystal and a position sensitive photomultiplier tube (PSPMT) which had 64 multi-channel anode was developed. The Ce-doped LiCaAlF₆ single crystal was grown by the Czochralski method. A plate with dimensions of a diameter of 50×2 mm² was cut from the grown crystal, polished, and optically coupled to PSPMT by silicone grease. The ²⁵²Cf source (<1 MBq) was sealed with 43 mm of polyethylene for neutron thermalization. Alphabet-shaped Cd pieces with a thickness of 2 mm were used as a mask for the thermal neutrons. After corrections for the pedestals and gain of each pixel, we successfully obtained two-dimensional neutron images using Ce-doped LiCaAlF₆.     

Evaluation of large deuterated scintillators for fast neutron detection (E=0.5-20 MeV) using the D(d,n)He, C(d,n) and Al(d,n) reactions

The response of large deuterated liquid scintillators (up to 10 cm diameter by 15 cm) to neutrons 0.5-20 MeV has been studied using the 2.5 MeV neutron generator at the University of Michigan, and the d(d,n), ¹³C(d,n), ²⁷Al(d,n) and other reactions at the University of Notre Dame FN tandem accelerator. The latter utilize 9 and 16 MeV deuteron beams including a pulsed beam, which permitted time-of-flight measurements. Combining pulse-shape discrimination and time-of-flight allows gating on specific neutron energy groups to determine the detector response to specific neutron energies. This will permit accurate simulation of the detector response functions for applications of these detectors in nuclear research and homeland security applications.     

Scintillation properties of Ce-doped LuLiF4 and LuScBO3

The crystals of 1 mol% Ce-doped LuLiF₄ (Ce:LLF) grown by the micro-pulling down (μ-PD) method and 1 mol% Ce-doped LuScBO₃ (Ce:LSBO) grown by the conventional Czochralski (Cz) method were examined for their scintillation properties. Ce:LLF and Ce:LSBO demonstrated ∼80% transparency at wavelengths longer than 300 and 400 nm, respectively. When excited by ²⁴¹Am α-ray to obtain radioactive luminescence spectra, Ce³⁺ 5d-4f emission peaks were detected at around 320 nm for Ce:LLF and at around 380 nm for Ce:LSBO. In Ce:LSBO, the host luminescence was also observed at 260 nm. By recording pulse height spectra under γ-ray irradiation, the absolute light yield of Ce:LLF and Ce:LSBO was measured to be 3600±400 and 4200±400 ph/MeV, respectively. Decay time kinetics was also investigated using a pulse X-ray equipped streak camera system. The main component of Ce:LLF was ∼320 ns and that of Ce:LSBO was ∼31 ns. In addition, the light yield non-proportionality and energy resolution against the γ-ray energy were evaluated.     

A neutron Albedo system with time rejection for landmine and IED detection

A neutron Albedo system has been developed for imaging of buried landmines and improvised explosive devices (IEDs). It involves irradiating the ground with fast neutrons and subsequently detecting the thermalized neutrons that return. A scintillating ⁶Li loaded ZnS(Ag) screen with a sensitive area of 40 cm×40 cm is used as a thermal neutron detector. Scintillation light is captured by orthogonal arrays of wavelength-shifting fibers placed on either side of the scintillator surface and then transferred to X and Y multi-pixel PMTs. A timing circuit, used with pulsed neutron sources, records the time when a neutron detection takes place relative to an external synchronization pulse from the pulsed source. Experimental tests of the Albedo system performance have been done in a sand box with a ²⁵²Cf neutron source (no time gating) and with pulsed D-D (2.6 MeV) neutrons from the Defense R&D Ottawa Van de Graaff accelerator (with time gating). Information contained in the time evolution of the thermal neutron field provided improved detection capability and image reconstruction. The detector design is described and experimental results are discussed.     

Detection of SNM by delayed gamma rays from induced fission

The Pulsed Neutron Interrogation Test Assembly (PUNITA) is an experimental device for research in NDA methods and field applicable instrumentation for nuclear safeguards and security applications. PUNITA incorporates a standard 14-MeV (D-T) pulsed neutron generator inside a large graphite mantle. The generator target is surrounded by a thick tungsten filter with the purpose to increase the neutron output and to tailor the neutron energy spectrum. In this configuration a sample may be exposed to a relatively high average thermal neutron flux of about (2.2±0.1)×10³ s⁻¹ cm⁻² at only 10% of the maximum target neutron emission. The sample cavity is large enough to allow variation of the experimental setup including the fissile sample, neutron and gamma detectors, and shielding materials.The response from SNM samples of different fissile material content was investigated with various field-applicable scintillation gamma detectors such as the 3×2 in. LaBr₃ detector. Shielding in the form of tungsten and cadmium was applied to the detector to improve the signal to background ratio. Gamma and neutron shields surrounding the samples were also tested for the purpose of simulating clandestine conduct. The energy spectra of delayed gamma rays were recorded in the range 100 keV-9 MeV. In addition time spectra of delayed gamma rays in the range 3.3-8 MeV were recorded in the time period of 10 ms-120 s after the 14-MeV neutron burst. The goal of the experiment was to optimize the sample/detector configuration including the energy range and time period for SNM detection. The results show, for example, that a 170 g sample of depleted uranium can be detected with the given setup in less than 3 min of investigation. Samples of higher enrichment or higher mass are detected in much shorter time.     

A novel wide range, real-time neutron fluence monitor based on commercial off the shelf gallium arsenide light emitting diodes

Displacement damage produced by high-energy neutrons in gallium arsenide (GaAs) light emitting diodes (LED) results in the reduction of light output. Based on this principle we have developed a simple, cost effective, neutron detector using commercial off the shelf (COTS) GaAs-LED for the assessment of neutron fluence and KERMA at critical locations in the vicinity of the 230 MeV proton therapy cyclotron operated by Westdeutsches Protonentherapiezentrum Essen (WPE). The LED detector response (mV) was found to be linear within the neutron fluence range of 3.0×10⁸-1.0×10¹¹ neutron cm⁻². The response of the LED detector was proportional to neutron induced displacement damage in LED; hence, by using the differential KERMA coefficient of neutrons in GaAs, we have rescaled the calibration curve for two mono-energetic sources, i.e. 1 MeV neutrons and 14 MeV neutrons generated by D+T fusion reaction. In this paper we present the principle of the real-time GaAs-LED based neutron fluence monitor as mentioned above. The device was calibrated using fast neutrons produced by bombarding a thick beryllium target with 14 MeV deuterons from a TCC CV 28 medical cyclotron of the Strahlenklinik University Hospital Essen.     

Neutronic design and simulated performance of Peking University Neutron Imaging Facility (PKUNIFTY)

The Peking University Neutron Imaging Facility (PKUNIFTY) is a Radio Frequency Quadruple (RFQ) accelerator based system. The fast neutrons are produced by 2 MeV deuterons bombarding beryllium target. The moderator, reflector, shielding and collimator have been optimized with Monte-Carlo simulation to improve the neutron beam quality. The neutrons are thermalized in water cylinder of Φ26×26 cm² with a polyethylene disk in front of Be target. The size of deuteron beam spot is optimized considering both the thermal neutron distribution and the demand of target cooling. The shielding is a combination of 8 cm thick lead and 42 cm thick boron doped polyethylene. The thermal neutrons are extracted through a rectangular inner collimator and a divergent outer collimator. The thermal neutron beam axis is perpendicular to the D⁺ beam line in order to reduce the fast neutron and the γ ray components in the imaging beam. When the neutron yield is 3×10¹² n/s and the L/D is 50, the thermal neutron flux is 5×10⁵ n/cm²/s at the imaging plane, the Cd ratio is 1.63 and the n/γ ratio is 1.6×10¹⁰ n/cm²/Sv.     

Evaluation of a LiI(Eu) neutron detector with coincident double photodiode readout

Previous work showed that enriched ⁶Li halide scintillation crystal is a good candidate for portable neutron-sensitive detectors. Photodiode readout is a good alternative to PMT in compact devices. These detectors are often required to work in presence of a strong gamma background. Therefore, great discrimination against gamma rays is crucial. Because of the high Q-value of the ⁶Li(n,α)³H reaction, the light yield of a neutron capture signal corresponds to 3-4 MeV gamma equivalent in spite of the quenching effect of heavily charged particles. As a result, energy discrimination is quite effective against gamma signals generated in thin crystals. However, direct gamma interactions inside the photodiode can create pulses whose amplitude is large enough to interfere with thermal neutron peak. This study shows an innovative design based on coincident readout to solve this problem. In this design, two photodiodes are attached on both sides of the LiI crystal. The output signal is only accepted when both photodiodes give out coincident output. The method is proved to effectively suppress background in the neutron window in a 420 mR/h ¹³⁷Cs field down to the level of natural background.     

Beryllium neutron activation detector for pulsed DD fusion sources

A compact fast neutron detector based on beryllium activation has been developed to perform accurate neutron fluence measurements on pulsed DD fusion sources. It is especially well suited to moderate repetition-rate (<0.2 Hz) devices, such as the plasma focus or Z-pinch. The detector comprises a beryllium metal sheet sandwiched between two large-area xenon-filled proportional counters. A methodology for calculating the absolute response function of the detector using a “first principles” approach is described. This calibration methodology is based on the ⁹Be(n,α)⁶He cross-section, energy calibration of the proportional counters, and numerical simulations of neutron interactions and beta-particle paths using MCNP5. The response function R(E_n) is determined over the neutron energy range 2-4 MeV. The count rate capability of the detector has been studied and the corrections required for high neutron fluence measurements are discussed. For pulsed DD neutron fluencies >3×10⁴ cm⁻², the statistical uncertainty in the fluence measurement is better than 1%. A small plasma focus device has been employed as a pulsed neutron source to test two of these new detectors, and their responses are found to be practically identical. Also the level of interfering activation is found to be sufficiently low as to be negligible.     

Crystal growth and thermal neutron scintillation response of Ce doped KLiYF5

K⁶Li(Y_1−xCe_x)F₅ (x = 0.003, 0.02) single crystals were grown from the melt using the precise atmosphere control type Micro-Pulling-Down (μ-PD) method to examine their potential as a new thermal neutron scintillators. The grown crystals were single-phase materials as confirmed by XRD. The crystals demonstrated 40-60% transmittance above 320 nm and Ce³⁺ 5d-4f luminescence observed around 340 nm when exited by α-ray. The radio luminescence measurements under thermal neutron excitation (²⁵²Cf) demonstrated the light yield of 890 (Ph/neutron) and the decay time excited by α-ray exhibited 20 and 259 ns.     

Development of neutron radiography facility for boiling two-phase flow experiment in Kyoto University Research Reactor

To visualize boiling two-phase flow at high heat flux by using neutron radiography, a new neutron radiography facility was developed in the B-4 beam hole of KUR. The B-4 beam hole is equipped with a supermirror neutron guide tube with a characteristic wavelength of 1.2 Å, whose geometrical parameters of the guide tube are: 11.7 m total length and 10 mm wide ×74 mm high beam cross-section. The total neutron flux obtained from the KUR supermirror guide tube is about 5×10⁷ n/cm² s with a nominal thermal output of 5 MW of KUR, which is about 100 times what is obtainable with the conventional KUR neutron radiography facility (E-2 beam hole). In this study a new imaging device, an electric power supply (1200 A, 20 V), and a thermal hydraulic loop were installed. The neutron source, the beam tube, and the radiography rooms are described in detail and the preliminary images obtained at the developed facility are shown.     

Basic study of single crystal fibers of Pr:Lu3Al5O12 scintillator for gamma-ray imaging applications

Single-crystalline fibers were grown from 0.25, 0.70, and 1.50 mol% Pr-doped Lu₃Al₅O₁₂ (LuAG) melts by the micro-pulling down (μ-PD) method with a diameter of 0.3-0.5 mm and a length of about 200 mm. They were cut to 10 mm long specimens, and their scintillation properties, including light yield and decay time profile, were examined. These results were compared with corresponding properties of the specimens (0.8×0.8×10 mm³) cut from the bulk crystals produced by conventional Czochralski (CZ) growth. The μ-PD-grown fibers demonstrated relatively low light yield and had the same decay time constant when compared with those of the samples cut from the CZ-grown crystals. The fiber crystals were used to assemble scintillating arrays with dimensions of Ø 0.5×10 mm²×20 pixels and Ø 0.3×10 mm²×30 pixels coated by a BaSO₄ reflector. After optical coupling with a position sensitive photomultiplier tube, the fiber-based arrays demonstrated acceptable imaging capability with a spatial resolution of about 0.5 mm.     

Crystal growth and characterization of CuI single crystals by solvent evaporation technique

Cuprous iodide (CuI) crystals are grown by slow evaporation technique in three different solvents. Large CuI single crystals with dimensions of 7.5 mm × 5 mm × 3 mm are obtained in pure acetonitrile solvent at 40 °C. The as-grown crystals are analyzed by X-ray diffraction, energy-dispersive X-ray analysis, differential scanning calorimetry, current-voltage characteristic and photoluminescence spectrum. The results show that the CuI crystal has the zinc-blende structure with no secondary phase. The elemental Cu/I ratio is 1.09:1. The melting point of the crystal is 875 K and two phase transitions occur from room temperature to its melting point. The electrical conductivity of CuI platelet crystal is in the range of 1.11-2.38 Ω⁻¹ cm⁻¹. Under ultraviolet excitation, the CuI crystals exhibit three emission bands with peak positions at 426, 529 and 671 nm. The nature of the luminescence is discussed.     

High-fidelity MCNP modeling of a D-T neutron generator for active interrogation of special nuclear material

Fast and robust methods for interrogation of special nuclear material (SNM) are of interest to many agencies and institutions in the United States. It is well known that passive interrogation methods are typically sufficient for plutonium identification because of a relatively high neutron production rate from ²⁴⁰Pu [1]. On the other hand, identification of shielded uranium requires active methods using neutron or photon sources [2]. Deuterium-deuterium (2.45 MeV) and deuterium-tritium (14.1 MeV) neutron-generator sources have been previously tested and proven to be relatively reliable instruments for active interrogation of nuclear materials [3] and [4]. In addition, the newest generators of this type are small enough for applications requiring portable interrogation systems.Active interrogation techniques using high-energy neutrons are being investigated as a method to detect hidden SNM in shielded containers [4] and [5]. Due to the thickness of some containers, penetrating radiation such as high-energy neutrons can provide a potential means of probing shielded SNM. In an effort to develop the capability to assess the signal seen from various forms of shielded nuclear materials, the University of Michigan Neutron Science Laboratory’s D-T neutron generator and its shielding were accurately modeled in MCNP. The generator, while operating at nominal power, produces approximately 1×10¹⁰ neutrons/s, a source intensity which requires a large amount of shielding to minimize the dose rates around the generator. For this reason, the existing shielding completely encompasses the generator and does not include beam ports. Therefore, several MCNP simulations were performed to estimate the yield of uncollided 14.1-MeV neutrons from the generator for active interrogation experiments. Beam port diameters of 5, 10, 15, 20, and 25 cm were modeled to assess the resulting neutron fluxes. The neutron flux outside the beam ports was estimated to be approximately 2×10⁴ n/cm² s.     

Synthesis and characterisation of the garnet-related Li ion conductor, Li5Nd3Sb2O12

In this paper the synthesis, conductivity, and structure of the garnet-related Li ion conductor, Li₅Nd₃Sb₂O₁₂, are reported. As for the related Li₅La₃M₂O₁₂ (M = Nb, Ta) materials, this phase shows high Li ion conductivity, with a conductivity at 300 °C of 9.2 × 10⁻³ S cm⁻¹. Structural studies using neutron diffraction indicate a cubic unit cell, space group Ia-3d, with Li located in two partially occupied sites. One of the sites is the traditional garnet structure tetrahedral site, while the other Li site is considerably more distorted. Although the latter is nominally a six coordinate site, a close inspection suggests that the coordination could be described as distorted tetrahedral, with the remaining two bonds being significantly longer (≈2.6 Å).     

Detecting fissionable materials in a variety of shielding matrices via delayed gamma and neutron photofission signatures—Part 2: Experimental results

Successful detection of fissionable material contained in a variety of matrices was demonstrated by photon active interrogation of fissionable and inert target materials. Samples were irradiated with pulsed 15 MeV photons generated by a LINAC and tungsten electron/photon converter, operating at 15 Hz. Matrix materials included air (no matrix), wood, water, and lead. A unique dual mode gamma/neutron detector was used to acquire data from both fission product gamma and fission product neutron emission. Neutron emission was recorded by detecting the 478 keV capture gamma from the ¹⁰B (n,α)⁷Li reaction, generating a photopeak in the recorded gamma spectrum. Two signatures were found to correctly differentiate between the fissionable target (²³⁸U) and inert targets (lead, steel, air, and beryllium), with substantial differences in delayed gamma and neutron signatures for fissionable and inert materials in all cases. The signatures are simple to compute and are not significantly affected by system variations or interferences expected during cargo scanning.     

Synthesis, structure, growth and physical properties of a novel organic NLO crystal: 1,3-Dimethylurea dimethylammonium picrate

A novel noncentrosymmetric crystal was prepared from 1,3-dimethylurea dimethylammonium picrate, C₁₁H₁₈N₆O₈ (DMUP), which was designed for second harmonic generation. DMUP crystals exist in noncentro symmetric space group Cmc2₁ with unit cell dimensions a = 14.288(4) Å, b = 17.023(5) Å, c = 6.8268(13) Å, α = β = γ = 90° and volume = 1660.5(8) Å³. The crystal structure of DMUP has been determined using single crystal X-ray diffraction studies. The single crystals of DMUP were successfully grown by the slow evaporation method with dimensions 10 mm × 4 mm × 3 mm using dimethylformamide as solvent. The structural perfection of the grown crystals has been analysed by High-resolution X-ray diffraction (HRXRD) rocking curve measurements. Powder test with Neodymium-doped Yttrium aluminum garnet (Nd:YAG) laser radiation shows a high second harmonic generation (SHG). The laser induced surface damage threshold for the grown crystal was measured using Nd:YAG laser.     

Magnetic and dielectric study of R0.5Sr0.5MnO3 (R = Gd, Tb and Dy)

Magnetic and dielectric properties of perovskite manganites R_0.5Sr_0.5MnO₃ (R = Gd, Tb and Dy) have been investigated. DC and AC magnetic measurements showed short-range glassy magnetic ordering at T_g ∼ 40 K. Such ordering was observed by neutron diffraction and is ascribable to the size mismatch of R³⁺ and Sr³⁺ settled randomly at the same crystallographic site. Dielectric constants for each material were ∼1000-10,000 between ∼50 and ∼300 K and showed broad maximums above T_g. Dielectric dispersion showed poor coherency of the motion of polar regions, plausibly because of the size-mismatch effect; both the magnetic and dielectric properties of this system are governed by the randomness at the R/Sr site. The tan δ and EXAFS data suggest that the dielectric response is rooted in a transfer of the Mn-3d electrons.