Giulia Hull

Strontium and barium iodide high light yield scintillators

Europium-doped strontium and barium iodide are found to be readily growable by the Bridgman method and to produce high scintillation light yields.

Scintillators With Potential to Supersede Lanthanum Bromide

New scintillators for high-resolution gamma ray spectroscopy have been identified, grown and characterized. Our development efforts have focused on two classes of high-light-yield materials: europium-doped alkaline earth halides and cerium-doped garnets. Of the halide single crystals we have grown by the Bridgman method-SrI2, CaI2, SrBr2, BaI2 and BaBr2-SrI2 is the most promising. SrI2(Eu) emits into the Eu2+ band, centered at 435 nm, with a decay time of 1.2 mus and a light yield of up to 115,000 photons/MeV. It offers energy resolution better than 3% FWHM at 662 keV, and exhibits excellent light yield proportionality. Transparent ceramic fabrication allows the production of gadolinium- and terbium-based garnets which are not growable by melt techniques due to phase instabilities. The scintillation light yields of cerium-doped ceramic garnets are high, 20,000-100,000 photons/MeV. We are developing an understanding of the mechanisms underlying energy dependent scintillation light yield non-proportionality and how it affects energy resolution. We have also identified aspects of optical design that can be optimized to enhance the energy resolution.

Crystal Growth and Scintillation Properties of Strontium Iodide Scintillators

Single crystals of SrI₂:Eu and SrI₂:Ce/Na were grown from anhydrous iodides by the vertical Bridgman technique in evacuated silica ampoules. Growth rates were of the order of 5-30 mm/day. Radioluminescence spectra of SrI₂:Eu and SrI₂:Ce/Na exhibit a broad band due to Eu²⁺ and Ce³⁺ emission, respectively. The maximum in the luminescence spectrum of SrI₂:Eu is found at 435 nm. The spectrum of SrI₂:Ce/Na exhibits a doublet peaking at 404 and 435 nm attributed to Ce³⁺ emission, while additional impurity-or defect-related emission is present at approximately 525 nm. The strontium iodide scintillators show very high light yields of up to 120 000 photons/MeV, have energy resolutions down to 3% at 662 keV (Full Width Half Maximum) and exhibit excellent light yield proportionality with a standard deviation of less than 5% between 6 and 460 keV.

New Organic Crystals for Pulse Shape Discrimination

Efficient, readily-available, low-cost, high-energy neutron detectors can play a central role in detecting illicit nuclear weapons since neutrons are a strong indication for the presence of fissile material such as Plutonium and Highly-Enriched Uranium. The main challenge in detecting fast neutrons consists in the discrimination of the signal from the gamma radiation background. At present, the only well-investigated organic crystal scintillator for fast neutron detection, in a n/gamma mixed field, is stilbene, which while offering good pulse shape discrimination, is not widely used because of its limited availability and high cost.

Scintillator Non-Proportionality: Present Understanding and Future Challenges

Scintillator non-proportionality (the fact that the conversion factor between the energy deposited in a scintillator and the number of visible photons produced is not constant) has been studied both experimentally and theoretically for ~50 years. Early research centered on the dependence of the conversion factor on the species of the ionizing radiation (gamma, alpha, beta, proton, etc.), and researchers during the 1960s discovered a strong correlation between the scintillation efficiency and the ionization density. In more recent years, non-proportionality has been proposed as the reason why the energy resolution of most scintillators is worse than that predicted by counting statistics. While much progress has been made, there are still major gaps in our understanding of both the fundamental causes of non-proportionality and their quantitative link to scintillator energy resolution. This paper summarizes the present state of knowledge on the nature of the light-yield non-proportionality and its effect on energy resolution.

Design of a Facility for Measuring Scintillator Non-Proportionality

While the original Compton coincidence technique provided accurate measurements of electron response in scintillators, the data rate was low and measurements took weeks. We present the conceptual design for a high throughput version that is predicted to collect data at 65 cps, reducing measurement times from weeks to hours. In this design, a collimated 1 mCi 137Cs source will illuminate the scintillator sample from a distance of 18 cm and 5 high-purity germanium (HPGe) detectors placed 10 cm from the scintillator will measure the energy of the scattered gamma ray. The source can be placed in either of two positions spaced 15deg apart, allowing relatively uniform scattering angle coverage from 0deg to 146deg, corresponding to electron energies in the scintillator from 0 to 466 keV. The scintillator will be coupled to a hybrid photodetector (HPD), which has extremely linear response, and the HPDs ability to resolve single photoelectrons provides a built-in calibration mechanism. The output of each HPGe detector and the HPD will be digitized with a free-running 12-bit, 200 MHz ADC, providing accurate measurement of the signal amplitudes and the ability to measure the electron response for different temporal components of the scintillator signals. The facility will be located at Lawrence Livermore National Laboratory (LLNL) and is intended to be made available to the community at large. The goals are to facilitate scintillator development and to understand the nature of the light-yield non-proportionality and its effect on the energy resolution.

Performance of a Facility for Measuring Scintillator Non-Proportionality

We have constructed a second-generation Compton coincidence instrument, known as the Scintillator Light Yield Non-proportionality Characterization Instrument (SLYNCI), to characterize the electron response of scintillating materials. While the SLYNCI design includes more and higher efficiency HPGe detectors than the original apparatus (five 25%-30% detectors versus one 10% detector), the most novel feature is that no collimator is placed in front of the HPGe detectors. Because of these improvements, the SLYNCI data collection rate is over 30 times higher than the original instrument. In this paper, we present a validation study of this instrument, reporting on the hardware implementation, calibration, and performance. We discuss the analysis method and present measurements of the electron response of two different NaI:Tl samples. We also discuss the systematic errors of the measurement, especially those that are unique to SLYNCI. We find that the apparatus is very stable, but that careful attention must be paid to the energy calibration of the HPGe detectors.

Progress in Studying Scintillator Proportionality: Phenomenological Model

We present a model to describe the origin of non-proportional dependence of scintillator light yield on the energy of an ionizing particle. The non-proportionality is discussed in terms of energy relaxation channels and their linear and non-linear dependences on the deposited energy. In this approach, the scintillation response is described as a function of the deposited energy deposition and the kinetic rates of each relaxation channel. This mathematical framework allows both a qualitative interpretation and a quantitative fitting representation of scintillation non-proportionality response as function of kinetic rates. This method was successfully applied to thallium doped sodium iodide measured with SLYNCI, a new facility using the Compton coincidence technique. Finally, attention is given to the physical meaning of the dominant relaxation channels, and to the potential causes responsible for the scintillation non-proportionality. We find that thallium doped sodium iodide behaves as if non-proportionality is due to competition between radiative recombinations and non-radiative Auger processes.

Strontium iodide scintillators for high energy resolution gamma ray spectroscopy

Recently SrI2, a scintillator patented by Hofstadter in 1968, has been rediscovered and shown to possess remarkable scintillation properties. The light output of SrI2:Eu2+ has been measured to be even higher than previously observed and exceeds 120,000 photons/MeV, making it one of the brightest scintillators in existence. The crystal also has excellent energy resolution of less than 3% at 662 keV. The response is highly linear over a wide range of gamma ray energies. The emission of SrI2:Eu2+ and SrI2:Ce3+/Na+ is well-matched to both photomultiplier tubes and blue-enhanced silicon photodiodes. While SrI2:Eu2+ is relatively slow, SrI2:Ce3+/Na+ has a fast response. SrI2 crystals with many different dopant concentrations have been grown and characterized. In this presentation, crystal growth techniques as well as the effects of dopant concentration on the scintillation properties of SrI2, over the range 0.5% to 8% Eu2+ and 0.5% to 2% Ce3+/Na+, will be discussed in detail.

Measurements of NaI(Tl) Electron Response: Comparison of Different Samples

This paper measures the sample to sample variation in the light yield proportionality of NaI(Tl), and so explores whether this is an invariant characteristic of the material or whether it depends on the chemical and physical properties of the tested samples. We report on the electron response of nine crystals of NaI(Tl), differing in shape, volume, age, manufacturer and quality. The proportionality has been measured at the SLYNCI facility in the energy range between 3.5 to 460 keV. We observe that while samples produced by the same manufacturer at approximately the same time have virtually identical electron response curves, there are significant sample to sample variations among crystals produced by different manufacturers or at different times. In an effort to correlate changes in the electron response with details of the scintillation mechanism, we characterized other scintillation properties, including the gamma response and the x-ray excited emission spectra and decay times, for the nine crystals. While sample to sample differences in these crystals were observed, we have been unable to identify the underlying fundamental mechanisms that are responsible for these differences.