Phase I Final Report
Explore the source record for details and available documents.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
SEARCH · Engineering Papers
Results for “scintillating nanoparticles”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Scintillation Hydro-Gel for Isotopic Neutron (SHINE): Eco-Friendly Quantum Dot Neutron Detectors
The development of new neutron detectors to replace helium-3 (3He) detectors is imperative due to a worldwide shortage of 3He following the draw down in nuclear weapons production since the end of the Cold War. The United States Department of Homeland Security would like to deploy monitors for the detection of neutron emissions from shipping containers housing illicit nuclear material; however, this effort has been put on hold until new replacements for 3He detectors can be developed. Scintillation Hydro-Gel for isotopic Neutron Emitters (SHINE) is a unique, first of its kind, 6Li-loaded quantum dot gel scintillator developed at INL. By incorporating 6Li with quantum dots in a gel matrix, SHINE displays the best properties of liquid and solid scintillators without their disadvantages such as continuous filtering to keep liquids free of contaminates, slow throughput of containers, higher base component costs, ‘dead’ voids in solid scintillators, and a high loading of 6Li without compromising on light transparency. Additionally, SHINE is completely eco-friendly, a breakthrough in high-efficiency detection systems. SHINE is a unique combination of 6LiCl, a highly water-soluble compound, and InP/ZnS core/shell quantum dots, which are poured into a gel-form using cross-linking polymers. In this presentation, SHINE has been successfully tested for neutron detection and shows promise as both a replacement for current 3He neutron detectors as well as potential use in handheld, compact neutron detection units and antineutrino detection.
36 MATERIALS SCIENCE↗
Development of Plasmonically Cloaked Nanoparticles
An advanced in-pile multi-parameter reactor monitoring system is being proposed in this funding opportunity. The proposed effort brings cutting edge, high-fidelity optical measurement systems into the reactor environment in an unprecedented fashion, including in-core, in-cladding and in-fuel pellet itself. Unlike instrumented leads, the proposed system provides a unique solution to a multi-parameter monitoring need in core while being minimally intrusive in the reactor core. Detector designs proposed herein can monitor fuel compression and expansion in both the radial and axial dimensions as well as monitor linear power profiles and fission rates during the operation of the reactor. In addition to pressure, stress, strain, compression, neutron flux, neutron spectra, and temperature can be observed inside the fuel bundle and fuel rod using the proposed system. The proposed research aims at developing radiation-hard, harsh-environment multi-parameter systems for insertion into the reactor environment. The proposed research holds the potential to drastically increase the fidelity and precision of in-core instrumentation with little or no impact in the neutron economy in the reactor environment while providing a measurement system capable of operation for entire operating cycles. Significant work has been done over the last few years on the use of nanoparticle-based scintillators. Through the use of metamaterials, the PIs aim to develop planar neutron detectors and large-volume neutron detectors. These detectors will have high efficiencies for neutron detection and will have a high gamma discrimination capability.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Tumor Microenvironment Targeting Nano–Bio Emulsion for Synergistic Combinational X-Ray PDT with Oncolytic Bacteria Therapy
Various cancer therapies have been developed, but tumor recurrence with incomplete tumor killing and remaining tumor cells/tissues is frequent in monotherapies. Herein, a nano–bio therapeutic emulsion formulated with multifunctional nanoscintillators and anaerobic Clostridium novyi-NT spores for synergistic image-guided combinational cancer therapy is reported. MRI visible nanoscintillators (NSs) are synthesized with a NaGdF 4 :Tb,Ce@NaGdF 4 core/shell structure for an image-guided X-ray photodynamic therapy (PDT) of the normoxic peripheral tumor. An anaerobic oncolytic bacterium (C. novyi-NT) therapy is combined to treat the hypoxic central tumor tissues. Photosensitizer-coated NSs (PS-NSs) and C. novyi-NT spores are emulsified with clinically available ethiodized oil (Lipiodol) to be the nano–bio therapeutic emulsion and injected into the tumor with computed tomography image guidance. The distribution of nano–bio therapeutic emulsion, including PS-NSs and anaerobic C. novyi-NT spores in the tumor site, is confirmed by both X-ray and T1-weighted magnetic resonance imaging. Following the image-guided X-ray PDT and anaerobic C. novyi- NT combination treatment, apoptotic cell death in cancer tissues, including both peripheral and central tumor regions, is significantly higher than in the control groups. Finally, this combination therapy approach using a nano–bio therapeutic emulsion is expected to overcome the limitations of conventional cancer therapy, resulting in increased cancer-therapeutic efficacy.
60 APPLIED LIFE SCIENCES↗
Effects of Quantum Dot Loading on the Radioluminescence Efficiency in Quantum-Dot-Embedded Composites
Nanoparticle-embedded plastic scintillators are an emerging technology for fast, large-area, high-resolution radiation detection and imaging. Here, this study investigates the properties of such composites, focusing on the effects of the quantum dot (QD) concentration on the radioluminescence (RL) intensity, spectra, and dynamics. Experiments using CdSe/CdS QDs in a polymer reveal a superlinear increase in RL with the QD concentration despite optical losses from inner filtering and interparticle interactions. When corrected for inner filtering, RL shows a quadratic concentration dependence, consistent with simple analytical models of improving the secondary electron capture. Practically, the benefits of high QD concentrations are muted by optical losses, but the findings apply to other systems with insulating hosts. In addition to manipulating emission for large effective Stokes shifts, future improvements may come from hosts with higher stopping power and better charge transport, which enable more effective funneling of excitations but without concomitant optical losses associated with high nanoparticle concentrations.
Auger recombination↗
Quantum Shell in a Shell: Engineering Colloidal Nanocrystals for a High-Intensity Excitation Regime
Many optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses. Here, we address this issue by introducing quantum shells with a CdS–CdSe–CdS–ZnS core–shell–shell–shell multilayer structure. Further, the ZnS barrier inhibits the surface carrier decay, which increases the photoluminescence (PL) quantum yield (QY) to 90% while retaining a high biexciton emission QY of 79%. The improved QS morphology allows demonstrating one of the longest Auger lifetimes reported for colloidal NCs to date. The reduction of nonradiative losses in QSs also leads to suppressed blinking in single nanoparticles and low-threshold amplified spontaneous emission. We expect that ZnS-encapsulated quantum shells will benefit many applications exploiting high-power optical or electrical excitation regimes.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Lutetium oxide-based transparent ceramic scintillators
In one embodiment, a transparent ceramic of sintered nanoparticles includes gadolinium lutetium oxide doped with europium having a chemical composition (Lu.sub.1-xGd.sub.x).sub.2-YEu.sub.YO.sub.3, where X is any value within a range from about 0.05 to about 0.45 and Y is any value within a range from about 0.01 to about 0.2, and where the transparent ceramic exhibits a transparency characterized by a scatter coefficient of less than about 10%/cm. In another embodiment, a transparent ceramic scintillator of sintered nanoparticles, includes a body of sintered nanoparticles including gadolinium lutetium oxide doped with a rare earth activator (RE) having a chemical composition (Lu.sub.1-xGd.sub.x).sub.2-YRE.sub.YO.sub.3, where RE is selected from the group consisting of: Sm, Eu, Tb, and Dy, where the transparent ceramic exhibits a transparency characterized by a scatter coefficient of less than about 10%/cm.
36 MATERIALS SCIENCE↗
Magnetic iron oxide nanoparticles for the collection and direct measurement of adsorbed alpha-emitting radionuclides from environmental waters by liquid scintillation analysis
Radioactive contamination in the environment, be it from accidental or intentional release, can create an urgent need to assess water and food supplies, the environment, and monitor human health. Alpha-emitting radionuclides represent the most ionizing, and therefore the most damaging, form of radiation when internalized. Additionally, because of its ease of energy attenuation in solids or liquids, alpha emissions cannot be reliably monitored using non-destructive means. In the event of such an emergency, rapid and efficient methods will be needed to screen scores of samples (food, water, and human excreta) within a short time window. Unfortunately, the assay of alpha-emitting radionuclides using traditional radioanalytical methods is typically labor intensive and time consuming. The creation of analytical counting sources typically requires a series of chemical treatment steps to achieve well performing counting sources. In an effort to devise radioanalytical methods that are fast, require little labor, and minimize the use of toxic or corrosive agents, researchers at PNNL have evaluated magnetite (Fe3O4) nanoparticles as extracting agents for alpha-emitting radionuclides from chemically unmodified aqueous systems. It is demonstrated that bare magnetic nanoparticles exhibit high affinity for representative α-emitting radionuclides (241Am and 210Po) from representative aqueous matrices: river and ground water. Furthermore, use of the magnetic properties of these materials to concentrate the sorbed analyte from the bulk aqueous solution has been demonstrated. The nanoparticle concentrate can be either directly dispensed into scintillation cocktail, or first dissolved and then added to scintillation cocktail as a solution for alpha emission assay by liquid scintillation analysis. Despite the extreme quench caused by the metal oxide suspensions, the authors have demonstrated that quench correction features available on modern liquid scintillation analyzers can be employed to assure that quench-induced analytical biases can be avoided.
actinide↗
Structural, photoluminescence and radioluminescence properties of Eu{sup 3+} doped La{sub 2}Hf{sub 2}O{sub 7} nanoparticles
This study presents the structural, optical, and radioluminescent characterization of newly synthesized europium-doped lanthanum hafnate (La{sub 2}Hf{sub 2}O{sub 7}:xmol%Eu{sup 3+}, x=0 to 35) nanoparticles (NPs) for use as phosphors and scintillation materials. Samples prepared through a combined co-precipitation and molten salt synthetic process were found to crystalize in the pyrochlore phase, a radiation tolerant structure related to the fluorite structure. These samples exhibit red luminescence under ultraviolet and X-ray excitation. Under these excitations, the optical intensity and quantum yield of the La{sub 2}Hf{sub 2}O{sub 7}:xmol%Eu{sup 3+} NPs depend on the Eu{sup 3+} concentration and are maximized at 5%. It is proposed that there is a trade-off between the quenching due to defect states/cross-relaxation and dopant concentration. An optimal dopant concentration allows the La{sub 2}Hf{sub 2}O{sub 7}:5 mol%Eu{sup 3+} NPs to show the best luminescent properties of all the samples. - Graphical abstract: Incident X-ray and UV photons interact with La{sub 2}Hf{sub 2}O{sub 7}: xmol%Eu{sup 3+}(x=1–35) nanoparticles (NPs) to yield strong red luminescence centered at 612 nm. Colored spheres inside NP diagram represent pyrochlore coordination environment of La{sub 2}Hf{sub 2}O{sub 7}:xmol%Eu{sup 3+}. Blue, red, yellow, green and black spheres represent hafnium(IV) atoms, lanthanum(III)/europium(III) atoms, oxygen atoms at 48f site, oxygen atoms at 8b site and oxygen vacancies, respectively. - Highlights: • La{sub 2}Hf{sub 2}O{sub 7}:xmol%Eu{sup 3+} (x=0–35) nanoparticles with weakly-ordered pyrochlore structures were synthesized. • Optically and X-ray excited emission spectra showed strong luminescence centered at 612 nm. • Photoluminescence quantum yield increases with doping concentration up to 5% and decreases at higher concentrations.
36 MATERIALS SCIENCE↗
{sup 6}LiF oleic acid capped nanoparticles entrapment in siloxanes for thermal neutron detection
The good light output of siloxane based scintillators as displayed under γ-rays and α particles has been exploited here to obtain clear and reliable response toward thermal neutrons. Sensitization towards thermal neutrons has been pursued by adding {sup 6}LiF, in form of nanoparticles. Aiming at the enhancement of compatibility between the inorganic nanoparticles and the low polarity, siloxane based surrounding medium, oleic acid-capped {sup 6}LiF nanoparticles have been synthesized by thermal decomposition of Li trifluoroacetate. Thin pellets siloxane scintillator maintained their optical transmittance up to weight load of 2% of {sup 6}Li. Thin samples with increasing {sup 6}Li concentration and thicker ones with fixed {sup 6}Li amount have been prepared and tested with several sources (α, γ-rays, moderated neutrons). Light output as high as 80% of EJ212 under α irradiation was measured with thin samples, and negligible changes have been observed as a result of {sup 6}LiF addition. In case of thick samples, severe light loss has been observed, as induced by opacity. Nevertheless, thermal neutrons detection has been assessed and the data have been compared with GS20, based on Li glass, taken as a reference material.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Size, structure, and luminescence of Nd 2 Zr 2 O 7 nanoparticles by molten salt synthesis
Pyrochlore materials with novel properties are in demand with multifunctional applications such as optoelectronics, scintillator materials, and theranostics. Many reports have already indicated the importance of the synthesis technique for Nd 2 Zr 2 O 7 (NZO) nanoparticles (NPs); however, no explanation has been provided for the reason behind the nature of its phase selectivity. Here, we have explored the structural and optical properties of the NZO NPs synthesized by a molten salt synthesis method. We have synthesized size-tunable NZO NPs and correlated the particle size with their structural behavior and optical performance. All NZO NPs are stabilized in defect fluorite phase. Neutron diffraction provided insight on the behavior of oxygen in the presence of heavy atoms. We have collected bright amalgam of blue and green emission on UV irradiation due to the presence of oxygen vacancies from these NPs. We have carried out in situ XRD and Raman investigations to observe the temperature-induced phase transformation in a controlled argon environment. Interestingly, we have not observed phase change for the molten salt synthesized fluorite NZO NPs; however, we observed phase transformation from a precursor stage to pyrochlore phase by in situ XRD directly. Finally, these observations provide a new strategy to synthesize nanomaterials phase-selectively for a variety of applications in materials science.
36 MATERIALS SCIENCE↗
Samarium-Activated La 2 Hf 2 O 7 Nanoparticles as Multifunctional Phosphors
Recent developments in the field of designing novel nanostructures with various functionalities have pushed the scientific world to design and develop high-quality nanomaterials with multifunctional applications. Here, we propose a new kind of doped metal oxide pyrochlore nanostructure for solid-state phosphor, X-ray scintillator, and optical thermometry. The developed samarium-activated La 2 Hf 2 O 7 (LHOS) nanoparticles (NPs) emit a narrow and stable red emission with lower color temperature and adequate critical distance under near-UV and X-ray excitations. When the LHOS NPs are exposed to an energetic X-ray beam, the Sm 3+ ions situated at the symmetric environment get excited along with those located at the asymmetric environment, which results in a low asymmetry ratio of Sm 3+ under radioluminescence compared to photoluminescence. High activation energy and adequate thermal sensitivity of the LHOS NPs highlight their potential as a thermal sensor. Our results indicate that these Sm 3+ -activated La 2 Hf 2 O 7 NPs can serve as a multifunctional UV, X-ray, and thermographic phosphor
36 MATERIALS SCIENCE↗
Evaluating Brightness and Stability of Cathodoluminescence from Colloidal Semiconductor Nanocrystals
Cathodoluminescence offers promise as a technique for correlation of atomic structure with electronic structure at the level of individual nanoparticles or even defects, with the ability to analyze complex nanostructures at length-scales far below those typically available to optical spectroscopy. Unlike other forms of electron microscopy, cathodoluminescence offers direct insights into the electronic structure of the visualized sample. Despite reports more than 10 years ago of individual nanoparticle cathodoluminescence, effective cathodoluminescence collection from colloidal semiconductor materials is relatively rare and remains challenging due to the instability of materials under the conditions of electron beam irradiation. In this work, to clarify the roadblocks for cathodoluminescence analysis of colloidal nanocrystals, we attempt a comprehensive study of the cathodoluminescence properties of semiconductor quantum shells, which have a thin concentric CdSe shell surrounding CdS nanoparticles, then surrounded by a further concentric CdS shell. These same materials were recently demonstrated to show promising scintillation performance in radioluminescence measurements, including high brightness (up to 100 ph/keV) and excellent durability. Comparative quantum yield measurements are designed to assess the brightness of semiconductor nanocrystal films, which show that the quantum shells are much less bright under electron irradiation compared to X-ray photons. Instability of CL emission is assigned to charging effects on the samples—and not thermal effects—through a series of voltage, current, dwell time, and atmospheric pressure experiments.
cathodoluminescence↗
Enhanced UV light detection using wavelength-shifting properties of Silicon nanoparticles
Detection of UV photons is becoming increasingly necessary with the use of noble gases and liquids in elementary particle experiments. Cerenkov light in crystals and glasses, scintillation light in neutrino, dark matter, and rare decay experiments all require sensitivity to UV photons. New sensor materials are needed that can directly detect UV photons and/or absorb UV photons and re-emit light in the visible range measurable by existing photosensors. It has been shown that silicon nanoparticles are sensitive to UV light in a wavelength range around ~ 200 nm. UV light is absorbed and re-emitted at wavelengths in the visible range depending on the size of the nanoparticles. Initial tests of the wavelength-shifting properties of silicon nanoparticles are presented here that indicate by placing a film of nanoparticles in front of a standard visible-wavelength detecting photosensor, the response of the sensor is significantly enhanced at wavelengths < 320 nm.
47 OTHER INSTRUMENTATION↗
Gadolinium-loaded gel scintillators for neutron and antineutrino detection
A gadolinium (Gd) loaded scintillation gel (Gd-ScintGel) compound allows for neutron and gamma-ray detection. The unique gel scintillator encompasses some of the best features of both liquid and solid scintillators, yet without many of the disadvantages associated therewith. Preferably, the gel scintillator is a water soluble Gd-DTPA compound and water soluble fluorophores such as: CdSe/ZnS (or ZnS) quantum dot (Q-dot) nanoparticles, coumarin derivatives 7-hydroxy-4-methylcoumarin, 7-hydroxy-4-methylcoumarin-3-acetic acid, 7-hydroxycoumarin-3-carboxylic acid, and Alexa Fluor 350 as well as a carbostyril compound, carbostyril 124 in a stable water-based gel, such as methylcellulose or polyacrylamide polymers. The Gd-loaded ScintGel allows for a homogenious distribution of the Gd-DTPA and the fluorophores, and yields clean fluorescent emission peaks. A moderator, such as deuterium or a water-based clear polymer, can be incorporated in the Gd-ScintGel. The gel scintillators can be used in compact detectors, including neutron and antineutrino detectors.
36 MATERIALS SCIENCE↗
High-Z Sensitized Plastic Scintillators: A Review
The need for affordable and reliable radiation detectors has prompted significant investment in new radiation detector materials, due to concerns about national security and nuclear nonproliferation. Plastic scintillators provide an affordable approach to large volume detectors, yet their performance for high-energy gamma radiation is severely limited by the small radiation stopping power inherent to their low atomic number. Although some sensitization attempts with organometallics were made in the 1950s to 1960s, the concomitant decrease in light yield has limited the usefulness of these sensitized detectors. Recently, with new knowledge gained during the rapid development of organic optoelectronics and nanotechnology, there has been a revived interest in the field of heavy element sensitized plastic scintillators. In this paper, the recent efforts on sensitized plastic scintillators are summarized. Basic scintillator physics is first reviewed. The discussion then focuses on two major thrusts in the field: sensitization with: (1) organometallics and (2) oxide and fluoride nanoparticles. The design rationales and major results are examined in detail, with existing limitations and possible future pathways discussed. Lastly, special attention is paid to the underlying energy deposition and transfer processes, as these determine the key performance metrics such as light yield and radioluminescence decay lifetime.
36 MATERIALS SCIENCE↗
Wavelength-shifting properties of luminescence nanoparticles for high energy particle detection and specific physics process observation
Here, ultraviolet (UV) photon detection is becoming increasingly important in the quest to understand the fundamental building blocks of our universe. Basic properties of neutrinos and Dark Matter are currently being explored through interactions with noble elements. In response to interactions with fundamental particles, these elements emit scintillation photons in the UV range. However, most available detectors have poor response in the UV so it is typically necessary to shift UV to a wavelength, matching the sensitivity of the viable detectors. We report on development of UV-enhanced photosensors using wavelength-shifting properties of nanoparticles. Several nanoparticle coatings were tested for absorption of UV light with subsequent emission in the visible wavelength for high energy particle detection. ZnS:Mn, Eu, ZnS: Mn, CuCy (Copper Cysteamine) and CdTe nanoparticles all exhibited enhanced detection for wavelengths in the range 200-320 nm in several different tests, while ZnS:Ag and CdS nanoparticle showed little or no enhancement in that range. In addition, various LaF3:Ce nanoparticle concentrations in approximately constant thickness of 2,5-diphenyloxazole (PPO)/polystyrene bases were also tested to optimize the nanoparticle concentration for the best outcome. Our studies indicated that ZnS:Mn, Eu, ZnS: Mn, Cu-Cy, CdTe and LaF 3 :Ce nanoparticles show potential for light detection from fundamental particle interactions.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗