High-performance composite scintillator
10520610 ยท 2019-12-31
Assignee
Inventors
Cpc classification
G01T1/2008
PHYSICS
G01T1/20185
PHYSICS
International classification
Abstract
A composite scintillator includes a matrix material and pieces of at least one scintillator material embedded in the matrix material. The scintillator material is (a) inorganic single-crystalline or ceramic, (b) organic plastic, or (c) glassy; and the embedded scintillator material scintillates in response to at least one of gamma-ray and neutron irradiation.
Claims
1. A composite scintillator, comprising: a matrix material; and pieces of at least one scintillator material embedded in the matrix material, wherein the scintillator material is (a) inorganic single-crystalline, (b) ceramic, (c) organic plastic, or (d) glassy, and is substantially cylindrical or tapered in shape with dimensions of at least 5 mm, and wherein the embedded scintillator material scintillates photons in response to at least one of gamma-ray and neutron irradiation, wherein the matrix material is a material that absorbs photons emitted by the embedded pieces of scintillator material and re-emits photons at a wavelength longer than the wavelength of photons emitted by the embedded pieces of scintillator material, wherein the matrix material also absorbs at least one of gamma rays and neutrons, wherein the matrix material emits photons in response to absorption of gamma rays or neutrons, and wherein the matrix material has a spectral emission range with an integrated area under the emission spectrum that overlaps an integrated area under a quantum efficiency curve of a photodetector configured to measure performance of the composite scintillator, wherein the photodetector is selected from a photomultiplier tube, a silicon photomultiplier, and a silicon avalanche photodiode, and wherein the overlap meets or exceeds 33% of the integrated area under the emission spectrum.
2. The composite scintillator of claim 1, wherein the embedded scintillator material is selected from at least one of the following materials, including Ce-doped compositions: .sup.6Li-enriched Cs.sub.2LiYCl.sub.6 (CLYC), .sup.7Li-enriched Cs.sub.2LiYCl.sub.6 (.sup.7CLYC), unenriched Cs.sub.2LiYCl.sub.6 (nat-CLYC), Cs.sub.2LiLaBr.sub.6 (CLLB), (CsLiLaBr.sub.6).sub.0.9(Cl.sub.6).sub.0.1 (CLLBC), Eu-doped SrI.sub.2, Cs.sub.2HfCl.sub.6, Cs.sub.2HfBr.sub.6, Cs.sub.2HfCl.sub.4Br.sub.2, Cs.sub.2HfCl.sub.2Br.sub.4, Tl-doped NaI, Tl-doped CsI, .sup.6Li-doped glass, and an organic plastic.
3. The composite scintillator of claim 1, wherein the matrix material comprises an organic composition.
4. The composite scintillator of claim 3, wherein the organic composition is polyvinyltoluene with functionalized fluorophores that are excitable by at least one of gamma and neutron radiation.
5. The composite scintillator of claim 1, wherein the matrix material comprises a silicone-based composition with functionalized fluorophores that are excitable by at least one of gamma and neutron radiation.
6. The composite scintillator of claim 1, wherein the pieces of the scintillator material are dispersed through the matrix in a regular three-dimensional pattern.
7. The composite scintillator of claim 1, wherein the pieces of the scintillator material are dispersed through the matrix without a regular three-dimensional pattern.
8. The composite scintillator of claim 1, wherein at least some of the surfaces of the embedded scintillator material are smoothly polished.
9. The composite scintillator of claim 1, wherein at least some of the surfaces of the embedded scintillator material are polished to a ground or matte surface finish.
10. The composite scintillator of claim 1, wherein one surface of the composite scintillator is coupled with a light-collection device, and wherein other surfaces of the composite scintillator are polished to a degree that increases internal reflection and are covered by a reflector.
11. The composite scintillator of claim 1, wherein the composite scintillator has a substantially cylindrical shape.
12. The composite scintillator of claim 1, wherein the composite scintillator has a tapered shape.
13. The composite scintillator of claim 1, wherein the matrix material is a material that absorbs at least 50% of photons emitted by the pieces of scintillator material.
14. A radiation detection system, comprising: a composite scintillator, comprising a matrix material and pieces of at least one scintillator material embedded in the matrix material, wherein the scintillator material is (a) inorganic single-crystalline, (b) ceramic, (c) organic plastic, or (d) glassy, and is substantially cylindrical or tapered in shape with dimensions of at least 5 mm, and wherein the embedded scintillator material scintillates photons in response to at least one of gamma-ray and neutron irradiation, wherein the composite scintillator has a base surface, and wherein the matrix material is a material that absorbs photons emitted by the embedded pieces of scintillator material and re-emits photons at a wavelength longer than the wavelength of photons emitted by the embedded pieces of scintillator material, wherein the matrix material also absorbs at least one of gamma rays and neutrons, and wherein the matrix material emits photons in response to absorption of gamma rays or neutrons; a photodetector configured to receive and detect photons emitted by the composite scintillator, wherein the matrix material has a spectral emission range with an integrated area under the emission spectrum that overlaps an integrated area under a quantum efficiency curve of the photodetector, wherein the photodetector is selected from a photomultiplier tube, a silicon photomultiplier, and a silicon avalanche photodiode, and wherein the overlap meets or exceeds 33% of the integrated area under the emission spectrum; and a waveguide with two base surfaces at opposite ends of the waveguide, wherein a first of the base surfaces of the waveguide is coupled with the base surface of the composite scintillator, and wherein a second of the base surfaces of the waveguide is coupled with a photodetector.
15. The radiation detection system of claim 14, wherein the base surface of the composite scintillator has a base area, S.sub.1, wherein the first base surface of the waveguide has a base area that is substantially equal to S.sub.1, and wherein the second base surfaces of the waveguide has a base area, S.sub.2, wherein S.sub.2<S.sub.1.
16. The radiation detection system of claim 14, wherein the system is incorporated in a radiation portal monitor, and wherein the composite scintillator is a plate.
17. A method for radiation detection, comprising: absorbing gamma-ray or neutron radiation in pieces of at least one scintillator material embedded in a matrix material, wherein the matrix material and the scintillator together form a composite scintillator, and wherein the scintillator material is (a) inorganic single-crystalline, (b) ceramic, (c) organic plastic, or (d) glassy, and is substantially cylindrical or tapered in shape with dimensions of at least 5 mm; emitting photons from the pieces of scintillator material in response to the absorption of gamma-ray or neutron radiation; absorbing in the matrix material the photons emitted from the pieces of scintillator material; re-emitting photons from the matrix material at a wavelength longer than the wavelength of photons emitted by the embedded pieces of scintillator; absorbing in the matrix material at least one of gamma rays and neutrons and emitting photons in response to the absorption of the at least one of gamma rays and neutrons; and detecting the photons from the matrix material with a photodetector, wherein the matrix material has a spectral emission range with an integrated area under the emission spectrum that overlaps an integrated area under a quantum efficiency curve of the photodetector, wherein the photodetector is selected from a photomultiplier tube, a silicon photomultiplier, and a silicon avalanche photodiode, and wherein the overlap meets or exceeds 33% of the integrated area under the emission spectrum.
18. The method of claim 17, further comprising: absorbing at least one of gamma rays and neutrons in the matrix material; and emitting photons from the matrix material in response to the absorption of gamma rays or neutrons.
19. The method of claim 17, wherein the matrix material absorbs at least 50% of photons emitted by the pieces of scintillator material.
Description
BRIEF DESCRIPTION OF THE DRAWINGS
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(16) In the accompanying drawings, like reference characters refer to the same or similar parts throughout the different views; and apostrophes are used to differentiate multiple instances of the same item or different embodiments of items sharing the same reference numeral. The drawings are not necessarily to scale; instead, an emphasis is placed upon illustrating particular principles in the exemplifications discussed below. For any drawings that include text (words, reference characters, and/or numbers), alternative versions of the drawings without the text are to be understood as being part of this disclosure; and formal replacement drawings without such text may be substituted therefor.
DETAILED DESCRIPTION
(17) The foregoing and other features and advantages of various aspects of the invention(s) will be apparent from the following, more-particular description of various concepts and specific embodiments within the broader bounds of the invention(s). Various aspects of the subject matter introduced above and discussed in greater detail below may be implemented in any of numerous ways, as the subject matter is not limited to any particular manner of implementation. Examples of specific implementations and applications are provided primarily for illustrative purposes.
(18) Unless otherwise herein defined, used or characterized, terms that are used herein (including technical and scientific terms) are to be interpreted as having a meaning that is consistent with their accepted meaning in the context of the relevant art and are not to be interpreted in an idealized or overly formal sense unless expressly so defined herein. For example, if a particular composition is referenced, the composition may be substantially (though not perfectly) pure, as practical and imperfect realities may apply; e.g., the potential presence of at least trace impurities (e.g., at less than 5%) can be understood as being within the scope of the description. Likewise, if a particular shape is referenced, the shape is intended to include imperfect variations from ideal shapes, e.g., due to manufacturing tolerances. Percentages or concentrations expressed herein can be in terms of weight or volume. Processes, procedures and phenomena described below can occur at ambient pressure (e.g., about 50-120 kPafor example, about 90-110 kPa) and temperature (e.g., 20 to 50 C.for example, about 10-35 C.) unless otherwise specified.
(19) Although the terms, first, second, third, etc., may be used herein to describe various elements, these elements are not to be limited by these terms. These terms are simply used to distinguish one element from another. Thus, a first element, discussed below, could be termed a second element without departing from the teachings of the exemplary embodiments.
(20) Spatially relative terms, such as above, below, left, right, in front, behind, and the like, may be used herein for ease of description to describe the relationship of one element to another element, as illustrated in the figures. It will be understood that the spatially relative terms, as well as the illustrated configurations, are intended to encompass different orientations of the apparatus in use or operation in addition to the orientations described herein and depicted in the figures. For example, if the apparatus in the figures is turned over, elements described as below or beneath other elements or features would then be oriented above the other elements or features. Thus, the exemplary term, above, may encompass both an orientation of above and below. The apparatus may be otherwise oriented (e.g., rotated 90 degrees or at other orientations) and the spatially relative descriptors used herein interpreted accordingly.
(21) Further still, in this disclosure, when an element is referred to as being on, connected to, coupled to, in contact with, etc., another element, it may be directly on, connected to, coupled to, or in contact with the other element or intervening elements may be present unless otherwise specified.
(22) The terminology used herein is for the purpose of describing particular embodiments and is not intended to be limiting of exemplary embodiments. As used herein, singular forms, such as a and an, are intended to include the plural forms as well, unless the context indicates otherwise. Additionally, the terms, includes, including, comprises and comprising, specify the presence of the stated elements or steps but do not preclude the presence or addition of one or more other elements or steps.
(23) Additionally, the various components identified herein can be provided in an assembled and finished form; or some or all of the components can be packaged together and marketed as a kit with instructions (e.g., in written, video or audio form) for assembly and/or modification by a customer to produce a finished product.
(24) The composite scintillator (CS) includes and may essentially consist of two or three different materials, M, A and/or B. Materials A and B are formed into various-sized pieces that may have any geometric shape, including right cylinders, prisms, disks, spheres, and irregularly shaped pieces as if formed from the crushing of a larger piece. Where the material A and/or B is a cylinder, the cylinder can have a diameter, e.g., in the range of 1-100 mm and a height from 1-100 mm. Materials A and/or B are contained (encapsulated) by M and may occupy, in total, a volume of 1% to 95% of the total composite volume. A cylindrical composite scintillator can have a diameter as small as 25 mm and can have a thickness in a wide range of, e.g., 5 mm to 2 m.
(25) One or more pieces of material A 12 and/or B 16 are contained in a volume of material M 14 to form a composite scintillator 10, as shown in
(26) Material A and/or B is a single-crystal scintillator responsive to neutron and/or gamma-ray irradiation. Material A and/or B may be single crystals that are grown from the melt by the Bridgman, or Bridgman-Stockbarger, travelling zone, Czochralski, or Kyropolous methods; or from vapor by physical-vapor-transport or chemical-vapor-transport methods; or from solution by standard solution-crystal-growth techniques. Materials A and/or B may be a glassy material and may be formed by the hot-drawn process, rod-in-tube technique, melt spinning, or extrusion. Materials produced by any of the above techniques are cut to appropriate size and polished to the required surface finish.
(27) Material A and/or B emits photons (i.e., scintillates) when it absorbs the neutron and/or gamma-ray radiation. Material A emits photons in the wavelength range of .sub.1-.sub.2, with peak emission at .sub.A, as shown in plot 1 of
(28) Material M may be an organic or silicone-based scintillator with an integrated flurophore that is responsive to gamma-ray and/or neutron irradiation, emitting over the wavelength range of .sub.7-.sub.8 (
(29) The performance of the composite scintillator, as described above, imposes limitations on the selection of materials for A and/or B and matrix M. First, the spectral emission of A and/or B must partially or totally overlap the absorption spectrum of matrix M. For efficient performance of the composite scintillator, it is advantageous that 50-100% of the energy emitted by A and/or B is absorbed by M. The second requirement is that the energy absorbed by M is re-emitted, by the so-called wavelength shifting phenomenon, at wavelengths longer than those emitted by A and/or B. That is, the peak emission wavelength of M, .sub.M in
(30) The energy resolution (ER) and the figure of merit (FOM, as described earlier) of the composite scintillator formed of materials A and/or B and M is influenced by the geometry and volume fraction of A and/or B. In general, shapes with high ratios of volume to surface area are preferred as they offer lower probability of absorption and scattering of light at the interfaces of A and/or B and M. Thus, regular-shaped cylinders or spheres are advantageous over crushed pieces. The ER of the composite scintillator is a function of the volume of A and/or B in the composite. The ER increases with an increasing volume fraction of A and/or B from zero up to a specific volume fraction, hereafter referred to as .sub.max, beyond which, it stays constant. The value of .sub.max is determined by the properties of A and/or B and M, the size and shape of A and/or B, and the size of the composite scintillator. For the composite scintillator 10 of
(31) In cases where the matrix M 14 has an organic composition, the composite scintillator 10 is fabricated by first casting a base layer of matrix M 14 at the bottom of a mold, which can be, for example, cylindrical. After the base layer has cured to the extent that it is mildly hardened and able to support the crystals, the crystals of material A 12 and/or B 16 are placed on top of the base layer. Once the base layer is hardened and the crystals 12/16 are rigidly attached to the base layer, the uncured plastic (material M 14) is poured into the mold to cover the base and the crystals 12/16, to a height that extends over the top of the crystals 12/16, and then cured. In the case in which crushed crystals of material A 12 and/or B 16 are used, the total volume of the material M 14 may be slightly cured to increase its viscosity, the crushed material dispersed and embedded within the volume, and then the entire composite 10 fully cured. In the case that material M 14 is already in a solid piece, holes may be bored or machined, crystals of material A 12 and/or B 16 embedded, and the open volume sealed. In the cases where material M 14 is not a plastic, then a similar procedure with respect to the placement and encapsulation of the crystals 12/16 is followed.
(32) The wavelength shifting process that occurs in a composite scintillator is advantageous when the shifted emission brings the emitted photons to wavelengths where photodetectors, such as photo-multiplier tubes (PMT), silicon photomultipliers (SiPMs), or silicon avalanche photodiodes (SiAPDs) have their greatest quantum efficiency. Most standard bialkali or superbialkali PMTs are sensitive in the range of 200 to 700 nm, with maximum quantum efficiency occurring in the range 350 to 430 nm. Likewise, SiPMs such as the J-type from SenSL Technologies Ltd. of Cork, Ireland, are sensitive in the range of 200 to 900 nm, with peak quantum efficiency occurring at 420 nm. The quantum efficiency of SiAPDs is highest in the range of 500-800 nm.
(33) The shift in the wavelength of peak emission towards the more-sensitive wavelength range of the photodetector results in a higher measured light yield and a better energy resolution (i.e., a lower numerical value of ER). Thus, a wavelength shift towards 350-430 nm is advantageous when PMTs or SiPMs are being used, and a shift towards the 500-800 nm range is advantageous when APDs are used. The better matched the peak emission wavelength of the composite scintillator is to the peak in the quantum efficiency of the photodetector, the better the response will be in terms of light yield and energy resolution recorded. Thus, an advantageous feature of material M is its ability to shift a material's spectral emission distribution to wavelengths that better overlap with wavelengths corresponding to the maximum quantum efficiency of the selected photodetector.
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(37) In particular embodiments, a composite scintillator is formed from pieces of single-crystal A 12 and matrix M 14, where crystal A 12 can be any scintillator crystal responsive to gamma-ray and neutron irradiation, including but not restricted to the following Ce-doped compositions: .sup.6Li-enriched Cs.sub.2LiYCl.sub.6 (CLYC), .sup.7Li-enriched Cs.sub.2LiYCl.sub.6 (.sup.7CLYC), Cs.sub.2LiYCl.sub.6 without Li-enrichment (nat-CLYC), Cs.sub.2LiLaBr.sub.6 (CLLB), and (CsLiLaBr.sub.6).sub.0.9 (Cl.sub.6).sub.0.1 (CLLBC).
(38) In particular embodiments, a composite scintillator is formed from pieces of single crystal A 12 and matrix M 14, where crystal A 12 can be any scintillator crystal responsive only to gamma-ray irradiation, including but not restricted to NaI(Tl), CsI(Tl), Cs.sub.2HfCl.sub.6, and SrI.sub.2(Eu).
(39) In particular embodiments, a composite scintillator is formed from pieces of single crystals A 12 and/or B 16 and matrix M 14, where crystal A 12 can be any scintillator crystal responsive to gamma-ray and neutron irradiation, and crystal B 16 can be any scintillator crystal responsive to gamma-ray irradiation.
(40) In particular embodiments, a composite scintillator is formed from pieces of crystal A 12 and/or crystal B 16 and matrix M 14, where crystal A 12 can be any scintillator crystal responsive to gamma-ray irradiation, and where crystal B 16 can be any scintillator crystal or doped glass responsive to neutron irradiation, such as .sup.6Li-doped glass.
(41) In particular embodiments, a composite scintillator is formed from pieces of single crystal A 12 and/or B 16 and matrix M 14, where crystals A 12 and/or B 16 are responsive to gamma-ray and/or neutron radiation, and where matrix M 14 is any material that absorbs gamma rays and/or neutrons and emits photons, such as PVT (e.g., EJ-290) or .sup.6Li-loaded plastic (EJ-270).
(42) In particular embodiments, a composite scintillator is formed from pieces of single crystal A 12 and/or B 16 and matrix M 14, where crystals A 12 and/or B 16 are responsive to gamma-ray and/or neutron radiation, and where matrix M 14 is any material that absorbs neutron irradiation and emits photons.
(43) In particular embodiments, a composite scintillator is formed from pieces of single crystal A 12 and matrix M 14, where matrix M 14 is an organic scintillator, such as PVT (e.g., EJ-290 PVT).
(44) In particular embodiments, a composite scintillator is formed from pieces of single crystal A 12 and matrix M 14, where matrix M 14 is a silicone-based material.
(45) In particular embodiments, a composite scintillator is formed from pieces of crystal A 12 and/or B 16 embedded in matrix M 14 and is coupled to a light guide made of matrix M.
(46) In particular embodiments, the spectral emission of matrix M 14 is in the range that matches the peak quantum efficiency of bialkali or superbialkali photomultiplier tubes (PMTS).
(47) In particular embodiments, the spectral emission of matrix M 14 is in the range that matches (or substantially matches) the peak quantum efficiency of silicon photomultipliers (SiPMs).
(48) In particular embodiments, the spectral emission of matrix M 14 is in the range that matches (or substantially matches) the peak quantum efficiency of silicon avalanche photodiodes (SiAPDs).
(49) In particular embodiments, the spectral emission of matrix M 14 is in the range that matches (or substantially matches) the peak quantum efficiency of the photodetector used to measure the performance of the composite scintillator.
(50) In particular embodiments, a composite scintillator is fabricated with pieces of crystal A 12 and/or B 16 placed in matrix M 14 in a regular pattern in three dimensions.
(51) In particular embodiments, a composite scintillator is fabricated with pieces of crystal A 12 placed in matrix M 14 without any regular pattern.
(52) In particular embodiments, all or some of the surfaces of crystal A 12 volumes are polished to a very smooth surface prior to placement into matrix M 14.
(53) In particular embodiments, all or some of the surfaces of crystal A 12 volumes are polished to a ground or matte surface prior to placement into matrix M 14.
(54) In particular embodiments, all of the surfaces of the composite scintillator, except for the surface coupled to the light-collection device, are polished to a matte finish to increase internal reflection and are covered by a reflector 22.
(55) In particular embodiments, the composite scintillator is cylindrical.
(56) In particular embodiments, a composite scintillator is formed from pieces of material A 12 and/or B 16 embedded in matrix M 14, where matrix M 14 has a tapered shape, such as a frustrum.
(57) In particular embodiments, as shown in
(58) In particular embodiments, the composite scintillator 10 is a plate with dimensions suitable for use in radiation portal monitors.
(59) A system that includes (a) a composite scintillator 10 comprising matrix M 14 and crystals A 12 and/or B 16, and (b) a photo-detection element is disclosed, where the spectral emission of crystal A 12 and matrix M 16 obey the relationship .sub.A and/or .sub.B< or close to .sub.M and certainly <.sub.6; .sub.3<.sub.5; .sub.4<.sub.6, 60%, and the emission spectrum of matrix M 14 overlaps with the wavelength range of the high-quantum-efficiency range of the photo-detection element.
(60) In describing embodiments of the invention, specific terminology is used for the sake of clarity. For the purpose of description, specific terms are intended to at least include technical and functional equivalents that operate in a similar manner to accomplish a similar result. Additionally, in some instances where a particular embodiment of the invention includes a plurality of system elements or method steps, those elements or steps may be replaced with a single element or step. Likewise, a single element or step may be replaced with a plurality of elements or steps that serve the same purpose. Further, where parameters for various properties or other values are specified herein for embodiments of the invention, those parameters or values can be adjusted up or down by 1/100.sup.th, 1/50.sup.th, 1/20.sup.th, 1/10.sup.th, .sup.th, .sup.rd, , .sup.rd, .sup.th, .sup.th, 9/10.sup.th, 19/20.sup.th, 49/50.sup.th, 99/100.sup.th, etc. (or up by a factor of 1, 2, 3, 4, 5, 6, 8, 10, 20, 50, 100, etc.), or by rounded-off approximations thereof, unless otherwise specified. Moreover, while this invention has been shown and described with references to particular embodiments thereof, those skilled in the art will understand that various substitutions and alterations in form and details may be made therein without departing from the scope of the invention. Further still, other aspects, functions, and advantages are also within the scope of the invention; and all embodiments of the invention need not necessarily achieve all of the advantages or possess all of the characteristics described above. Additionally, steps, elements and features discussed herein in connection with one embodiment can likewise be used in conjunction with other embodiments. The contents of references, including reference texts, journal articles, patents, patent applications, etc., cited throughout the text are hereby incorporated by reference in their entirety for all purposes; and all appropriate combinations of embodiments, features, characterizations, and methods from these references and the present disclosure may be included in embodiments of this invention. Still further, the components and steps identified in the Background section are integral to this disclosure and can be used in conjunction with or substituted for components and steps described elsewhere in the disclosure within the scope of the invention. In method claims (or where methods are elsewhere recited), where stages are recited in a particular orderwith or without sequenced prefacing characters added for ease of referencethe stages are not to be interpreted as being temporally limited to the order in which they are recited unless otherwise specified or implied by the terms and phrasing.