Recent research in manufacturing plastic scintillators via photopolymerization has reported various non-aromatic acrylic-based resins for easy 3D printing. However, the absence of traditionally used aromatic matrices, such as polystyrene or poly(vinyl toluene) (PVT), resulted in a limited scintillation performance. In this research, the feasibility of accommodating a high ratio of PVT with pentaerythritol tetraacrylate was demonstrated by the synthesis of plastic scintillators with efficient pulse shape discrimination. Moreover, the research described the understanding of the current inferior performance of photocured plastics compared to thermally cured analogs and showed 3D printability of studied resins in different shapes.
The development of efficient, robust plastic scintillators with pulse shape discrimination (PSD) has been of much interest in recent years. As is the case with many new technologies, initial formulations for PSD plastics provided new capabilities that have required in-depth research to refine. Herein we describe continued results from extensive optimization studies that have led to the development of PSD plastics with improved scintillation performance and physical properties. Improvements in the formulation for PSD plastics provide a groundwork from which element-loaded PSD plastics can be further advanced. Two separate approaches for incorporating lithium compounds into plastic scintillators are explored based on the identity of the lithium salt used. Aliphatic and aromatic lithium compounds require different methods of incorporation, resulting in different mechanisms of light quenching and reduction in PSD. These quenching mechanisms are explored and discussed for each type of lithium salt. Since at large size physical and scintillation characteristics are much more sensitive to preparation conditions, performance characterization of scaled plastics is described and compared among different formulations.
This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
Radiation Portal Monitors (RPMs) based on polyvinyl toluene (PVT) scintillators have been in use since the 1970s. Recently it has been discovered that under certain conditions PVT scintillators can fog at low temperatures. In collaboration with researchers at national laboratories, Eljen Technology has developed methods for the production of Intrinsic Anti-Fogging Scintillators. The production methods have been scaled up to allow for castings of rods and large sheets of scintillators that are deployable in RPMs and other extreme locations. The work is ongoing. The presentation will focus on the properties of the new scintillators and on the ongoing testing results from exposure to extreme environmental conditions.
Pulse shape discrimination in plastic scintillators has been of much interest in recent years. As with many innovative technologies, initial formulations for PSD plastics provided new capabilities that required much in-depth research to fully develop and refine. Herein we describe results from extensive optimization studies which have led to the development of PSD plastics with markedly improved scintillation performance and physical properties. Results of exploring different plastic matrices as well as a variety of secondary dyes are reported and optimum components are described. Due to the large concentration of additives required to manifest optimal PSD properties in plastic scintillators, the physical stability can be limited and the mechanical properties of PSD plastics are inferior to standard engineering plastics. Practical and theoretical solutions have been developed to address the physical stability and mechanical deformation problems in PSD plastics, and this work has resulted in physically stable scintillators with robust mechanical properties. Performance deterioration on increasing the size of PSD plastics is also addressed. At large sizes, physical and performance characteristics are much more sensitive to preparation conditions and compositional alterations as compared with small scintillators, and efforts to improve these properties are described. Finally, efforts to incorporate aromatic lithium compounds into PSD plastics are summarized and the effects of the lithium compounds on scintillation, stability, and attenuation are discussed.
The detection of neutrons in the presence of gamma-ray fields has important applications in the fields of nuclear physics, homeland security, and medical imaging. Organic scintillators provide several attractive qualities as neutron detection materials including low cost, fast response times, ease of scaling, and the ability to implement pulse shape discrimination (PSD) to discriminate between neutrons and gamma-rays. This talk will focus on amorphous organic scintillators both in plastic form and small-molecule organic glass form. The first section of this talk will describe recent advances and improvements in the performance of PSD-capable plastic scintillators. The primary advances described in regard to modification of the polymer matrix, evaluation of new scintillating dyes, improved fabrication conditions, and implementation of additives which impart superior performance and mechanical properties to PSD-capable plastics as compared to commercially-available plastics and performance comparable to PSD-capable liquids. The second section of this talk will focus on a class of small-molecule organic scintillators based on modified indoles and oligophenylenes which form amorphous glasses as PSD-capable neutron scintillation materials. Though indoles and oligophenylenes have been known for many decades, their PSD properties have not been investigated and their scintillation properties only scantily investigated. Well-developed synthetic methodologies have permitted the synthesis of a library of structural analogs of these compounds as well as the investigation of their scintillation properties. The emission wavelengths of many indoles are in the sensitive region of common photomultiplier tubes, making them appropriate to be used as scintillators in either pure or doped form.
This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. This work has been supported by the U.S. Department of Energy Office of Nonproliferation Research and Development (NA-22) and by the Defense Threat Reduction Agency (DTRA).
T. Clancy, J. Caggiano, J. McNaney, M. Eckart, M. Moran, V. Glebov, J. Knauer, R. Hatarik, S. Friedrich, R. Zacharias, A. Carpenter, M. Shoup, T. Buczek, M. Yeoman, Z. Zeid, N. Zaitseva, B. Talison, J. Worden, B. Rice, T. Duffy, A. Pruyne, K. Marshall
This paper describes the engineering architecture and function of the neutron Time-of-Flight (nToF) diagnostic suite
installed on the National Ignition Facility (NIF) at Lawrence Livermore National Laboratory (LLNL). These
instruments provide key measures of neutron yield, ion temperature, drift velocity, neutron bang-time, and neutron
downscatter ratio.
Currently, there are five nToFs on three collimated lines-of-site (LOS) from 18m to 27m from Target Chamber Center,
and three positioned 4.5m from TCC, within the NIF Target Chamber but outside the vacuum and confinement boundary
by use of re-entrant wells on three other LOS.
NIF nToFs measure the time history and equivalent energy spectrum of reaction generated neutrons from a NIF
experiment. Neutrons are transduced to electrical signals, which are then carried either by coaxial or Mach-Zehnder
transmission systems that feed divider assemblies and fiducially timed digitizing oscilloscopes outside the NIF Target
Bay (TB) radiation shield wall.
One method of transduction employs a two-stage process wherein a neutron is converted to scintillation photons in
hydrogen doped plastic (20x40mm) or bibenzyl crystals (280x1050mm), which are subsequently converted to an
electrical signal via a photomultiplier tube or a photo-diode.
An alternative approach uses a single-stage conversion of neutrons-to-electrons by use of a thin (0.25 to 2 mm) Chemical
Vapor Deposition Diamond (CVDD) disc (2 to 24mm radius) under high voltage bias. In comparison to the scintillator
method, CVDDs have fast rise and decay times (<ns), have very low residual tails, are insensitive to shot gammas, and
are less sensitive to the neutron signal of interest.
Detection of high-energy neutrons in the presence of gamma radiation background utilizes pulse-shape
discrimination (PSD) phenomena in organics studied previously only with limited number of materials, mostly
liquid scintillators and single crystal stilbene. The current paper presents the results obtained with broader varieties
of luminescent organic single crystals. The studies involve experimental tools of crystal growth and material
characterization in combination with the advanced computer modeling, with the final goal of better understanding
the relevance between the nature of the organic materials and their PSD properties. Special consideration is given to
the factors that may diminish or even completely obscure the PSD properties in scintillating crystals. Among such
factors are molecular and crystallographic structures that determine exchange coupling and exciton mobility in
organic materials and the impurity effect discussed on the examples of trans-stilbene, bibenzyl, 9,10-
diphenylanthracene and diphenylacetylene.
We investigate the laser-induced damage resistance at 355 nm in DKDP crystals grown with varying growth parameters, including temperature, speed of growth and impurity concentration. In order to perform this work, a DKDP crystal was grown over 34 days by the rapid-growth technique with varied growth conditions. By using the same crystal, we are able to isolate growth-related parameters affecting LID from raw material or other variations that are encountered when testing in different crystals. The objective is to find correlations of damage performance to growth conditions and reveal the key parameters for achieving DKDP material in which the number of damage initiating defects is minimized.
Considerable attention has been paid over the years to the problem of growing high purity KDP and KD*P to meet damage threshold requirements of inertial confinement fusion lasers at LLNL. The maximum fluence requirement for KD*P triplers on the NIF is 14.3 J/cm2 at 351 nm in a 3 ns pulse. Currently KD*P cannot meet this requirement without laser (pre)conditioning. In this overview, recent experiments to understand laser conditioning and damage phenomena in KDP and KD*P are discussed. These experiments have led to a fundamental revision of damage test methods and test result interpretation. In particular, the concept of a damage threshold has given way to measuring performance by damage distributions using beams of millimeter size. Automated R/1 damage test have shown that the best rapidly grown KDP crystals exhibit the same damage distributions as the best conventionally grown KD*P. Continuous filtration of the growth solution and post-growth thermal annealing are shown to increase the damage performance as well.
Development of high damage threshold, 50 cm, rapidly grown KD*P frequency triplers for operation on the National Ignition Facility (NIF) in the 14 J/cm2, 351 nm, 3 ns regime requires a thorough understanding of how the crystal growth parameters and technologies affect laser induced damage. Of particular importance is determining the effect of ionic impurities which may be introduced in widely varying concentrations via the starting salts. In addition, organic particulates can contaminate the solution as leachants from growth platforms or via mechanical ablation. Mechanical stresses in the crystals may also play a strong role in the laser-induced damage distribution (LIDD), particularly in the case of large boules where hydrodynamic forces in the growth tank may be quite high. In order to investigate the effects of various impurities and stresses on laser damage we have developed a dedicated, automated damage test system with diagnostic capabilities specifically designed or measuring time resolved bulk damage onset and evolution. The data obtained makes it possible to construct characteristic damage threshold distributions for each samples. Test results obtained for a variety of DKP samples grown form high purity starting salts and individually doped with Lucite and Teflon, iron, chromium and aluminum show that the LIDD drops with increasing contamination content. The results also show that solution filtration leads to increased damage performance for undoped crystals but is not solely responsible for producing the high LIDDs required by the NIF. The highest LIDD measured on a rapidly grown sample indicate that it is possible to produce high damage threshold material using ultrahigh purity, recrystallized starting salts, continuous filtration and a platform designed to minimize internal stress during growth.
KDP (KH2PO4) single crystals up to 47 cm in size have been grown by the rapid growth technique on the point seed in glass crystallizers of 1000 L in volume at growth rates of 10 to 25 mm/day in both the [001] and [100] directions. Measurement of the optical quality of 41 X 41 cm single crystal plates are presented.
Interest in producing high damage threshold KH2PO4 (KDP) and (DxH1-x)2PO4 (DKDP) for frequency conversion and optical switching applications is driven by the requirements of the National Ignition Facility (NIF) at the Lawrence Livermore National Laboratory. At present only the best crystals meet the NIF system requirements at the third harmonic and only after a laser conditioning process. Neither the mechanism for damage in bulk KDP nor the mechanism for conditioning ins understood. As part of ta development effort to increase the damage thresholds of KDP and DKDP, we have been developing techniques to pinpoint the locations where damage will initiate in the bulk material. After we find these locations we will use other measurement techniques to determine how these locations differ from the other surrounding materials and why they cause damage. This will allow crystal growers to focus their efforts to improve damage thresholds. Historically, damage thresholds have increased it is believed as a consequence of increased purity of the growth solution and through the use of constant filtration during the growth process. As a result we believe that damage is caused by defects in the crystals and have conducted a series of experiments using light scatter to locate these defects and to determine when and where damage occurs. In this paper we present results which show a low correlation between light scatter from bulk defects in KDP and the initiation sites for damage. We have also studied the effects of thermal conditioning on light scatter, strain induced birefringence and damage threshold. We have seen evidence that regions of high strain also exhibit lower damage threshold than the surrounding lower strain material. When thermally conditioned, these crystals show a decrease in some of the strong linear scattering features and a decrease in the strain birefringence while the damage threshold in these regions increased to that of the surrounding bulk material.
We report the experimental results of impurity contamination and laser-induced damage investigations on rapidly grown potassium dihydrogen phosphate (KDP) crystals. Using absorption spectroscopy and chemical analysis, we determined the impurity distribution in the different growing sectors of KDP single crystals. The level of impurity was dependent on the starting materials and growth rate. We also studied the influence of impurities on the laser-induced damage in fast grown KDP. The laser damage threshold in the impurity- rich prismatic sector is same as in the high purity pyramidal sector within the experimental error. Meanwhile, the laser damage threshold (LDT) at the boundary of the prismatic and pyramidal sectors is less than half of that in the bulk. Furthermore, we found that the thermal annealing of the crystal eliminated the weakness of this sector boundary and increased its LDT to the same level as in the bulk of the crystal. Our result suggests that laser damage occurred in the vicinity of a high, localized strain field.
Potassium dihydrogen phosphate (KDP) has traditionally been used as a nonlinear optical material for frequency conversion to produce second and third harmonic radiation. A high laser induced damage threshold for KDP crystals is required for high power laser applications, such as laser fusion. High quality KDP crystals for such applications can be produced by a recently developed rapid crystal growth method. We report the results of an impurity contamination study in raidlygrown KDP crystals. Using absorption spectroscopy, we identified the impurity contamination in the different growth sectors of the crystals. We show that the level of contamination depends on the growth rate achieved during the rapid growth. The impurities observed by absorption spectroscopy are identified as the origin of lattice distortion and optical birefringence in the KDP crystals. The study of impurity incorporation during crystal growth is important for understanding the damage mechanism of KDP.
Large solid state lasers such as Beamlet and the proposed National Ignition Facility require optical materials with extremely high damage thresholds. Potassium dihydrogen phosphate (KDP) and its deuterated analog (KD*P) both require some form of conditioning to reach the design fluence of these lasers. Both the bulk material and the crystal surfaces must have damage thresholds in excess of 16 J/cm2 at 1053 nm and 11 J/cm2 at 351 nm for 3- ns pulselengths. The use of ultrafiltration techniques has been demonstrated to produce bulk material with damage thresholds exceeding these requirements with the use of R:1 laser conditioning. More recent results at LLNL using large-area laser conditioning and thermal annealing are described for a variety of state-of-the-art KDP and KD*P crystals. Results on thermally annealed KD*P with a deuteration range of 60% to 80% are also presented, and compared to those of ordinary KDP.
The results of the two-dimensional theory of four-wave mixing (AIM) in the double phase-conjugate mirror geometry are compared with the experiment in a cubic Photorefractive BinTiao crystal. It is shown experimentally that this scheme can he used to determine the averaged surface relief of a scattering object.
High degrees of linear polarization of laser radiation and sensitivity to its variation are achieved by applying frequency converters using nonlinear crystals as polarizers and analyzers. The factors leading to distortion of linear polarization of light in such devices are identified. A KD*P polarimeter with extinction ratio of 5 (DOT) 10-9 is developed on the basis of a quasi-CW picosecond YAG laser.
Comparative analysis of main optical characteristics of KDP crystals grown by traditional technique at growth rates up to 1 mm/day and by rapid growth technique at growth rates ranging from 15 to 40 mm/day is carried out. The results on anomalous biaxiality absorption ard scattering of light effective nonlinear susceptibility and bulk laser damage threshold of crystals are given. It is shown that the increase of the crystal growth rate by more than one order does not deteriorate the crystal optical quality.
On the basis of the metastable zone investigations the optimal conditions for adenine sulphate solution stability were found. These made it possible to apply the novel high rate growth technique developed for KDP-family crystals group to the nucleic acid base crystals. The optical quality of adenine sulphate crystals grown at the rate about five times higher than the traditional one thus reducing the growth period six or seven times is sufficient not only for Raman spectroscopy but even for the normal reflection one.
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