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Modern Purification Methods for Liquid Scintillators Intended for Recording Rare Events

— Chromato-mass-spectrometry and UV/VIS spectroscopy are used to study the composition and properties of linear alkyl benzene (LAB) produced in Russia as the basic solvent for production of low-background liquid scintillators. The efficiency of LAB purification by reducing intrinsic radioactivity (U, Th) via water extraction (with addition of a strong chelate, dimethylaminomethylendiphosphonic acid) and sorption on Al{sub 2}O{sub 3} in silica gel is studied. The purification method for removing potassium from scintillation fluors (PPO, BPO, p -terphenyl) is developed. It is shown that U and Th can be efficiently extracted from NdCl{sub 3} water solutions with 0.1 M TOPO solution in pseudocumene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Development of the Scintillation Track Detector Based on Multichannel Photodetectors

— Matrices of silicon photomultipliers (SiPM) are promising multichannel photosensors for scintillation detectors. They can be used to construct tracks of relativistic particles inside detectors. The first detectors based on the direct contact of the SiPM matrices with the surface of the scintillation detector and with the application of Fresnel lenses are developed; promising variants of large detectors for neutrino astrophysics and geophysics are proposed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Stability of Gadolinium-Doped Liquid Organic Scintillators

The technology of preparing a linear-alkylbenzene-based gadolinium-doped liquid organic scintillator (Gd-LOS) as a target material in reactor antineutrino detectors has been developed. Results of longterm measurements of the light yield of Gd-LOS in contact with acryl and stainless steel are presented, which confirm the compatibility of Gd-LOS with these materials. The measurements were performed for two otherwise identical LOS detectors only differing in wall materials of the sensitive volume: acryl versus stainless steel. The results of measurements over about one year showed almost the same, relatively small decreases in the light yield of both detectors. It is concluded that both structural materials can be used in detector parts contacting with Gd-doped scintillator. Such a long-term parallel comparative test was carried out for the first time.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Radiation-Induced Degradation of LiF:W-Based Scintillators

We have studied the laws of, and reasons for, changes in the spectral and kinetic characteristics of cathodoluminescence (CL) of LiF:W scintillators irradiated by nanosecond electron pulses. It is established that the observed CL response distortions are related to the transformation of pre-irradiation defects and the accumulation of new color centers. Optimum conditions of operation of the LiF:W scintillators have been determined: preliminary exposure to a 10{sup 3}- to 10{sup 4}-Gy dose leads to a 1.5- to 2-fold increase in the CL intensity (“small-dose” effect).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Combustion water purification techniques influence on OBT analysing using liquid scintillation counting method

In order to determine organically bound tritium (OBT) from environmental samples, these must be converted into water, measurable by liquid scintillation counting (LSC). For this purpose we conducted some experiments to determine OBT level of a grass sample collected from an uncontaminated area. The studied grass sample was combusted in a Parr bomb. However usual interfering phenomena were identified: color or chemical quench, chemiluminescence, overlap over tritium spectrum because of other radionuclides presence as impurities ({sup 14}C from organically compounds, {sup 36}Cl as chloride and free chlorine, {sup 40}K as potassium cations) and emulsion separation. So the purification of the combustion water before scintillation counting appeared to be essential. 5 purification methods were tested: distillation with chemical treatment (Na{sub 2}O{sub 2} and KMnO{sub 4}), lyophilization, chemical treatment (Na{sub 2}O{sub 2} and KMnO{sub 4}) followed by lyophilization, azeotropic distillation with toluene and treatment with a volcanic tuff followed by lyophilization. After the purification step each sample was measured and the OBT measured concentration, together with physico-chemical analysis of the water analyzed, revealed that the most efficient method applied for purification of the combustion water was the method using chemical treatment followed by lyophilization.

54 ENVIRONMENTAL SCIENCES↗

Science-Driven Candidate Search for New Scintillator Materials FY 2013 Annual Report

This annual report presents work carried out during Fiscal Year (FY) 2013 at Pacific Northwest National Laboratory (PNNL) under the project entitled “Science-Driven Candidate Search for New Scintillator Materials” (Project number: PL13-SciDriScintMat-PD05) and led by Dr. Fei Gao. This project is divided into three tasks, namely (1) Ab initio calculations of electronic properties, electronic response functions and secondary particle spectra; (2) Intrinsic response properties, theoretical light yield, and microscopic description of ionization tracks; and (3) Kinetics and efficiency of scintillation: nonlinearity, intrinsic energy resolution, and pulse shape discrimination. Detailed information on the findings and insights obtained in each of these three tasks are provided in this report. Additionally, papers published this fiscal year or currently in review are included in Appendix together with presentations given this fiscal year.

Intrinsic Energy Resolution↗

Science-Driven Candidate Search for New Scintillator Materials: FY 2014 Annual Report

This annual reports presents work carried out during Fiscal Year (FY) 2014 at Pacific Northwest National Laboratory (PNNL) under the project entitled “Science-Driven Candidate Search for New Scintillator Materials” (Project number: PL13-SciDriScintMat-PD05) and led by Drs. Fei Gao and Sebastien N. Kerisit. This project is divided into three tasks: 1) Ab initio calculations of electronic properties, electronic response functions and secondary particle spectra; 2) Intrinsic response properties, theoretical light yield, and microscopic description of ionization tracks; and 3) Kinetics and efficiency of scintillation: nonproportionality, intrinsic energy resolution, and pulse shape discrimination. Detailed information on the results obtained in each of the three tasks is provided in this Annual Report. Furthermore, peer-reviewed articles published this FY or currently under review and presentations given this FY are included in Appendix. This work was supported by the National Nuclear Security Administration, Office of Nuclear Nonproliferation Research and Development (DNN R&D/NA-22), of the U.S. Department of Energy (DOE).

scintillation, nonproportionality, Monte Carlo sim↗

Technical Scope of Work: Proton Induced Radiation Damage in Crystal Scintillators

This is a technical scope of work (TSW) between the Fermi National Accelerator Laboratory (Fermilab) and the experimenters of California Institute of Technology who have committed to participate in beam tests to be carried out during the 2014 Fermilab Test Beam Facility program. The goal of this investigation is to understand the proton-induced radiation damage in candidate fast crystal scintillators for future HEP experiments. Degradations of the optical and scintillation properties, including emission and transmittance spectra, light output, decay time and light response uniformity, will be measured before and after each step of proton irradiation at Fermilab with a defined fluence. The irradiation will start with a fluence of 10 10 /cm 2 and going up in four steps to 10 13 /cm 2 .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Temperature and dopant concentration effects on proton light quenching in rare-earth inorganic scintillators [Slides]

Rare-earth inorganic scintillators have characteristics that offer optimal detection qualities for space applications as long a quenching is considered; Incident proton and electron response was measured in four different rare-earth inorganic scintillators of interest; We observed: A temperature effect on quenching for GAGG type detectors. A dopant concentration/decay time effect on quenching for GAGG detectors; Extracting the Birks’ factor for future detectors will improve the analysis of data.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Tritium Betavoltaic Powered Sensor Platforms: Power Augmentation with Scintillating Particles

Betavoltaics (BV) are long-life power sources that typically convert beta particle radiation into electricity. Largely, the radioactive decays within the source go unharvested by the device. This work seeks to augment the power generation of BV devices by integration of scintillating particles within the radiative getter to convert beta emission which would otherwise not leave the getter into usable light for power generation. Silica-covered barium fluoride scintillating particles were integrated into a tritiated water getter. Power generation was increased from 100s of nW to µW levels with the addition of 0.2 wt. % particles into the getter. Nanowatt-scale sensor platforms were demonstrated with the µW BV devices and the maximum possible lifetime of such platforms was estimated. As this technique enables higher power density BV devices from conventional Si semiconductors (compared to wider bandgap BVs), the further implementation may lower the barrier-to-deployment of these long-life power/sensor platforms.

42 ENGINEERING↗

Hadron-Induced Radiation Damage in Fast Heavy Inorganic Scintillators

Fast and heavy inorganic scintillators with suitable radiation tolerance are required to face the challenges presented at future hadron colliders of high energy and intensity. Up to 5 GGy and 5 × 1018 neq/cm2 of one-MeV-equivalent neutron fluence is expected by the forward calorimeter at the Future Hadron Circular Collider. This paper reports the results of an investigation of proton- and neutron-induced radiation damage in various fast and heavy inorganic scintillators, such as LYSO:Ce crystals, LuAG:Ce ceramics, and BaF2 crystals. The experiments were carried out at the Blue Room with 800 MeV proton fluence up to 3.0 × 1015 p/cm2 and at the East Port with one MeV equivalent neutron fluence up to 9.2 × 1015 neq/cm2, respectively, at the Los Alamos Neutron Science Center. Experiments were also carried out at the CERN PS-IRRAD proton facility with 24 GeV proton fluence up to 8.2 × 1015 p/cm2. Research and development will continue to develop LuAG:Ce ceramics and BaF2:Y crystals with improved optical quality, F/T ratio, and radiation hardness.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Interplanetary Scintillation

Interplanetary scintillation (IPS) has been used as a diagnostic of solar wind speed and interplanetary plasma turbulence, allowing inference of speed and electron density power spectrum close to the Sun and out of the ecliptic. In that context, IPS is 'signal' and provides scientifically interesting data. IPS is also of interest because amplitude and phase perturbations imposed on radio waves are 'noise' for telemetry and precision Doppler tracking of deep space probes and for some radio astronomical observations. This paper briefly reviews the connection between scattering observables and the electron density power spectrum. Interplanetary phase scintillation on time scales of 100 to 10 000 seconds is an important noise in mass determinations of small solar system bodies during space-probe fly-bys and in searches for low-frequency gravitational radiation.

waves deep space probes electron density power spe↗

A Global Model for Estimating Atmospheric Phase Scintillation Statistics

Since 2007, the National Aeronautics and Space Administration (NASA) has been collecting atmospheric phase turbulence data from various NASA ground stations throughout the world. The goal of these measurement campaigns has been to generate statistics to characterize the local site turbulence conditions and their impact on widely distributed ground based antenna arrays. This is of critical importance for the situation of uplink arraying, in which a priori knowledge of the fast varying turbulent conditions of water vapor in the troposphere may not be known, and will impact the power combining efficiency of ground based transmitting arrays. Therefore, the design of these type of systems will be dependent on the local climatology of the particular ground station site. Based on the 30+ station years of data collected characterizing atmospheric phase scintillation statistics at various sites, a global model is presented which attempts to predict the average phase statistics of a generic site based on local surface weather data, such as surface pressure, temperature, relative humidity, wind speed, and median wind direction. A model is proposed and based on a standard log power distribution similar to amplitude scintillation models trained on the existing data sets and shows reasonable accuracy against existing data sets.

propagation↗

Fast Neutron Spectroscopy with Organic Scintillation Detectors in a High-Radiation Environment

Organic scintillators with pulse shape discrimination capability are widely used in both research and practical applications of neutron detection. The neutron and gamma-ray identification performance of the detector depends on the classification algorithms, noise filters and pileup rejection criteria in a high-flux bremsstrahlung radiation environment. In this paper, a technique has been developed and implemented for the neutron detection with multiple filter and discrimination steps, which to a high confidence level eliminates counting of gamma-ray pulses. Such a technique is merited when making measurements in a high flux bremsstrahlung and secondary fluorescence environment. The EJ-309 and stilbene detectors coupled to the digital data acquisition system were used for the calibration assessments with standard gamma-ray and neutron sources such as 137Cs, 60Co, 252Cf, and Am-Be. The MCNPX-PoliMi and GEANT4 toolkits were used to simulate the light output and the optical photon transport in the scintillators and create detector response functions for each type of detector. The neutron spectrum unfolding algorithm, GRAVELW, was used to recreate and calibrate with the Am-Be as final step before applying the neutron detection system to extract fusion neutron spectra generated in an intense bremsstrahlung radiation environment. This new technique described offers the user the ability to measure neutron spectra in a high-flux gamma-ray field and tune the parameters to meet required filtering needs.

Neutron Detector, Organic Scintillator, PulseShape↗

Impacts of Atmospheric Ultrafast Kelvin Waves on Radio Scintillations in the Equatorial Ionosphere

We present a statistical analysis of the amplitudes of GPS scintillations (S4 index) observed throughout 2008–2010 using the satellite radio occultation measurements of the Constellation Observing System for Meteorology, Ionosphere, and Climate (COSMIC). Here, for the first time, periodic variability in the occurrence of S4 is investigated using these data. Significant variations of S4 with periods of 2.5-4 days (quasi-3 days) are identified from the observations during postsunset hours (1900-2400 local time) between 15°S-15°N magnetic latitude during this 3-year interval. Coherence analyses of these variations with the geomagnetic Ap index, solar EUV irradiance, and atmospheric wind measurements from an equatorial mesosphere meteor radar at Thumba, India (8.5°N, 77°E) are performed, providing a measure of the relationship between variations in the scintillations and potential drivers. The quasi-3-day variations in S4 are found to covary with the variations of the three drivers examined. In particular, the S4 signatures are found to be coherent with the atmospheric ultrafast Kelvin (UFK) planetary waves characterized by the zonal wind measurements of the radar. This study shows that these UFK waves are as important as the solar and geomagnetic drivers in forcing the day-to-day variations of the occurrence of equatorial spread F.

Ultra Fast Kelvin planetary wave↗

Radoptic Effect in InP and GaN for Ultrafast Scintillator Applications

Ultrafast scintillators are the subject of current research in an effort to better resolve ultrafast phenomena in high-energy density physics (HEDP) experiments. Despite extensive research on new scintillator materials, the essential mechanism of energy absorption, excitation, and photo-emission has remained unchanged for over 50 years. Recently, a new class of semiconductor detector has been developed using the radoptic effect, or the change of refractive index when subjected to radiation, in an attempt to record events faster than conventional scintillators.1 This study was designed for the observation of the radoptic effect by optical interferometry in different semiconductors (InP, InP:S, GaN, and GaN:Mg) to experimentally determine the fastest and most sensitive materials for the optimization of current radsensors.

InP, GaN, radoptic, scintillator, ultrafast↗

Feasibility Testing of Delayed Scintillator Screens for Indirect Digital Neutron Radiography of Irradiated Nuclear Fuel

Neutron radiography provides information about the internal condition of irradiated nuclear fuels. Traditionally, neutron radiography of highly radioactive irradiated nuclear fuels has been done with film using indirect radiography methods.[1] While indirect film neutron radiography is insensitive to gamma radiation from radioactive samples, it is a time-consuming and labor-intensive process. Digital neutron radiography requires a fraction of the time to produce a neutron radiograph compared to film-based processes. However, electronic components of digital radiography systems can easily be damaged by gamma radiation, which typically precludes use of digital systems for examination of highly radioactive objects, though recent work has demonstrated that some digital neutron radiography systems can indeed directly examine such samples.[2,3] This paper describes experiments performed using a hybrid transfer-digital method with an activated scintillator screen that can record an image that is subsequently read by a digital camera. The screens used in this study use a dysprosium neutron converter that records a latent image in the form of activation while in a neutron beam, then is physically transported away from the beam and sample to a digital camera elsewhere to record the image while the activated dysprosium decays and the adjacent scintillator produces light from interactions with the decay radiation. This approach could accelerate radiographic examination of irradiated nuclear fuels compared to the current transfer method with film. Current indirect imaging infrastructure was modified and augmented with a digital system. A digital neutron radiograph of a highly-radioactive irradiated nuclear fuel pins was produced in ~20 minutes, which is a significant improvement compared to the current process that takes almost a full day to produce a radiograph.

99 GENERAL AND MISCELLANEOUS↗