WO2004086089A1 - 熱蛍光線量計用フッ化物単結晶材料及び熱蛍光線量計 - Google Patents
熱蛍光線量計用フッ化物単結晶材料及び熱蛍光線量計 Download PDFInfo
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- WO2004086089A1 WO2004086089A1 PCT/JP2004/003814 JP2004003814W WO2004086089A1 WO 2004086089 A1 WO2004086089 A1 WO 2004086089A1 JP 2004003814 W JP2004003814 W JP 2004003814W WO 2004086089 A1 WO2004086089 A1 WO 2004086089A1
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- WIPO (PCT)
- Prior art keywords
- single crystal
- dosimeter
- thermofluorescence
- fluoride
- crystal material
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Classifications
-
- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21K—TECHNIQUES FOR HANDLING PARTICLES OR IONISING RADIATION NOT OTHERWISE PROVIDED FOR; IRRADIATION DEVICES; GAMMA RAY OR X-RAY MICROSCOPES
- G21K4/00—Conversion screens for the conversion of the spatial distribution of X-rays or particle radiation into visible images, e.g. fluoroscopic screens
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/61—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing fluorine, chlorine, bromine, iodine or unspecified halogen elements
- C09K11/615—Halogenides
- C09K11/616—Halogenides with alkali or alkaline earth metals
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/7732—Halogenides
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K9/00—Tenebrescent materials, i.e. materials for which the range of wavelengths for energy absorption is changed as a result of excitation by some form of energy
-
- C—CHEMISTRY; METALLURGY
- C30—CRYSTAL GROWTH
- C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
- C30B15/00—Single-crystal growth by pulling from a melt, e.g. Czochralski method
-
- C—CHEMISTRY; METALLURGY
- C30—CRYSTAL GROWTH
- C30B—SINGLE-CRYSTAL GROWTH; UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL; PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; APPARATUS THEREFOR
- C30B29/00—Single crystals or homogeneous polycrystalline material with defined structure characterised by the material or by their shape
- C30B29/10—Inorganic compounds or compositions
- C30B29/12—Halides
Definitions
- thermofluoride single crystal material for thermofluorescence dosimeter and thermofluorescence dosimeter
- thermofluorescence dosimeter used for measuring individual exposure dose such as workers engaged in radiation work such as a nuclear power plant, environmental radiation dose in a specific area, or exposure dose at the time of X-ray diagnosis.
- individual exposure dose such as workers engaged in radiation work such as a nuclear power plant, environmental radiation dose in a specific area, or exposure dose at the time of X-ray diagnosis.
- Thermofluorescence dosimeter (generally also called dosimeter) for measuring the personal exposure of workers engaged in radiation work such as nuclear power plants, the environmental radiation dose in a specific area, or the exposure dose during X-ray diagnosis the thermoluminescent dosimeter element for use in), e ⁇ lithium phosphor (L i 2 B 4 0 7 ; called LBO) (e.g., see Patent documents 1 to 3), or lithium-based fluorescent fluoride Body (L i F) (see, for example, Patent Document 4) is used.
- LBO lithium phosphor
- Li F lithium-based fluorescent fluoride Body
- the fluoride as the single crystal material lithium fluoride calcium aluminum single crystal; (see Patent Document 5, 6) to (L i CaAl F 6 called L i CAF) has been developed as an optical part.
- Li CAF has characteristics that can be used as a scintillator (see Non-Patent Documents 1 and 2).
- the power density is as small as 2.94 g / cm 3.
- thermoluminescent phosphors conventionally used in thermofluorescence dosimeter elements do not have satisfactory thermofluorescence efficiency, but have a higher thermofluorescence efficiency. Devices are required.
- Patent Document 3 JP-A-7-35865 (Claims)
- JP 2002-285150A (Claims, paragraph 000 1-0003)
- Patent Document 4 Patent Document 4
- Patent Document 5 Japanese Patent Laid-Open No. 2000-228801 (paragraphs 0001 to 0008 etc.
- JP 2002-234795 A paragraphs 0001 to 0006 etc.
- LiCaAlF 6 Ce crystal: a new scintillator A. Gektin, N. Shiran, S. Neic eva, V. Govicyuk, A. Bensalah, T. Fukuda and K. Shimamura, Nuclear Instruments and Methods in Physics Research A 486 (2002 274—277. Disclosure of the Invention
- an object of the present invention is to provide a fluoride single crystal material for a thermofluorometer having higher thermoluminescence efficiency than conventional materials and a thermofluorescence dosimeter using the same.
- the present inventors have found that a lithium fluoride aluminum single crystal doped with a predetermined element or in which a part of a calcium site is substituted with the predetermined element has a very high thermoluminescence efficiency.
- the present invention has been completed.
- a first embodiment of the present invention is a fluoride single crystal material for a thermofluorescence dosimeter used for a thermofluorescence dosimeter, represented by Li XAl F 6 , wherein X is C a, S r, Mg and A thermofluorescence dosimeter characterized by containing at least one selected from the group consisting of Ce, Na, Eu, Nd, Pr, Tm, Tb, and Er as a dopant. In fluoride single crystal material.
- the X is mainly composed of Y that is Ca or Sr, and is substituted with Z that is an element selected from the group consisting of Mg and Ba.
- thermofluorescence dosimeter element made of the single crystal material for a thermofluorescence dosimeter according to any one of the first to third embodiments, and a holder for holding the thermofluorescence dosimeter element.
- thermofluorescence dosimeter characterized by comprising:
- thermofluorescence dosimeter having higher thermoluminescence efficiency than conventional materials and a thermofluorescence dosimeter using the same.
- FIG. 1 is a graph showing the measurement results of the thermal fluorescence dose intensity of Test Example 1 in Example 1 and Comparative Example.
- FIG. 2 is a graph showing the measurement results of the thermal fluorescence dose intensity of Test Example 1 in Example 2 and Comparative Example.
- FIG. 3 is a graph showing the measurement results of the thermofluorescence dose intensity of Test Example 1 in Example 3 and Comparative Example.
- FIG. 4 is a graph showing the measurement results of the irradiation dose dependency of the thermofluorescent dose intensity of Test Example 2 in Example 3 and Comparative Example. BEST MODE FOR CARRYING OUT THE INVENTION
- Thermoluminescent dosimeter for fluoride single crystal material of the present invention are represented by L i XAl F 6, X Is selected from the group consisting of Ca, Sr, Mg and Ba.
- X is preferably mainly composed of calcium (Ca) or strontium (Sr).
- X is mainly calcium
- a part of calcium may be replaced by strontium.
- X is mainly composed of Ca or Sr
- a part thereof may be substituted with at least one of Mg and Ba
- Ca or Sr is represented by Y
- Mg or Ba is represented by Y.
- the fluoride single crystal material for a thermofluorescence dosimeter comprises at least one selected from Ce, Na, Eu, Nd, Pr, Tm, Tb, and Er as a dopant. It is preferred to contain. This is because it is necessary to improve the thermofluorescence efficiency.
- thermofluorescence dosimeter of the present invention Since the fluoride single crystal material for a thermofluorescence dosimeter of the present invention is used for a thermofluorescence dosimeter element, it is necessary to obtain a high quality and homogeneous bulk crystal. In order to obtain such a Balta crystal, it is preferable to use the following production method.
- the fluoride single crystal material for a thermofluorescence dosimeter of the present invention is preferably produced by a melt growth method or a solution growth method, but in order to produce the rare earth fluoride of the present invention, It is preferable to manufacture by a melt growth method or a solution growth method depending on the conditions described above.
- the fluoride single crystal of the present invention is prepared from a melt or a solution obtained by removing impurities by a melt growth method or a solution growth method in an atmosphere of an inert gas such as Ar. It becomes possible.
- thermofluorescence dosimeter of the present invention will be described in more detail.
- the fluoride single crystal material for a thermofluorescence dosimeter of the present invention is a powdered or polycrystalline fluoride raw material, namely, lithium fluoride (LiF), calcium fluoride (CaF 2 ), aluminum fluoride (A1 A raw material for matrix such as F 3 ) is charged into the crucible at a predetermined mixing ratio, and a raw material for dopant such as cerium fluoride (CeF 3 ) is filled in the crucible as necessary.
- a fluoride single crystal is produced from the obtained melt or solution.
- the method for producing a single crystal from the melt or solution obtained in this manner is not particularly limited, and a pulling method, a Bridgman method, or the like may be used.
- the temperature of the melt is kept close to the melting point of each compound, and the seed crystal is pulled at a speed of 0.1 to 1 OmmZh while rotating at 1 to 50 rpm to generate bubbles in the crystal. ⁇
- Transparent high-quality single crystals without a scattering center can be obtained.
- the fluoride single crystal for a thermofluorescence dosimeter obtained in this way is useful as a thermofluorescence dosimeter element. .
- thermofluorescence dosimeter element obtained by cutting such a fluoride single crystal into a predetermined size is used as a thermofluorescence dosimeter while being held in a predetermined holder, and is used for radiation, for example, X-ray, ⁇ , neutron beam. Absorbs and accumulates, and is generated later when heated by the reader The radiation dose can be determined by detecting the thermofluorescent dose.
- a commercially available bulk pulverized raw material having a purity of 99.99%, Li F, Ca F 2 , and A 1 F 3 were mixed at a molar ratio of 1.01: 1: 1.01 and used as a dopant.
- each 1 mol% of C e F 3 ⁇ Pi N a F Te was added 1 mole%, which was Hama charge in the crucible. It was placed as a single crystal manufacturing furnace, 10- 4 to draw a vacuum until 10 5 torr extent, as it is about 700 ° and heated in a vacuum furnace to about C. Moisture and oxygen in raw materials were removed.
- CF 4 gas and argon gas (volume ratio 50:50) were introduced into the single crystal production furnace, and the raw materials were heated and melted in a mixed gas atmosphere, and were kept in a liquid state for 3 hours. At this time, all the impurities that appeared on the liquid surface disappeared by reacting with CF 4 gas.
- a seed crystal was brought into contact with the melt, and a single crystal was grown and produced in the c-axis direction at a pulling speed of lmm / h and a rotation speed of 15 rpm. Crystals produced have a diameter of about 18. 5 mm, a length of about 8 Omm, bubbles, cladding click, liked Yatta ring centers without such a clear and high-quality L i C a A 1 F 6 : Ce, N a single It was a crystal.
- CF 4 gas and argon gas (volume ratio 50:50) were introduced into a single crystal production furnace, and the raw materials were heated and melted in a mixed gas atmosphere, and kept in a liquid state for 3 hours. At this time, all the impurities that appeared on the liquid surface disappeared by reacting with CF 4 gas. Next, the seed crystal was brought into contact with the melt, pulled up in the c-axis direction at a speed of lmm / h, and rotated at 15 rpm to grow and produce a single crystal.
- the produced crystal is a transparent and high-quality Li SrAlF 6 : Ce.Na single crystal with a diameter of about 18.5 mm and a length of about 80 mm, without bubbles, cracks, and a scattering center. there were. (Example 3)
- a commercially available crushed pulp raw material having a purity of 99.99%, Li F, C a F 2 , and A 1 F 3 were mixed at a molar ratio of 1.01: 1: 1.01 and used as a dopant. Then, 1 mol% of EuF 3 was added, and this was filled in a crucible. It was placed as a single crystal manufacturing furnace, 10- 4 ⁇ ; L 0- evacuated and pressurized to about 5 torr, moisture-oxygen as about 7 00 ° heated furnace, the raw material in a vacuum to about G Removed.
- CF 4 gas and argon gas (volume ratio 50:50) were introduced into the single crystal production furnace, and the raw material was heated and melted in a mixed gas atmosphere, and kept in a liquid state for 3 hours. At this time, all the impurities that appeared on the liquid surface were eliminated by reacting with CF 4 gas.
- a seed crystal was brought into contact with the melt, and a single crystal was grown and produced in the c-axis direction at a pulling speed of lmm / h and a rotation speed of 15 rpm. Crystals produced has a diameter of about 1 8. 5 mm length of about 80 mm, air bubbles, cracks, liked Yatta ring center of which without a clear and high-quality L i C a A 1 F 6 : was E u single crystal . (Example 4)
- a commercially available bulk milled raw material having a purity of 99.99%, Li F, S r F 2 , and A 1 F 3 were mixed in a molar ratio of 1.01: 1: 1.01 to obtain a dopant. Then, 1 mol% of EuF 3 was added, and this was filled in a crucible. It was placed as a single crystal manufacturing furnace, 10-4 to 10-5 1: Pull vacuum to about orr, it about 7 0 o ° Moisture and oxygen was heated in a vacuum furnace, the raw material up to about c Was removed.
- CF 4 gas and argon gas (volume ratio 50:50) were introduced into the single crystal production furnace, and the raw material was heated and melted in a mixed gas atmosphere, and kept in a liquid state for 3 hours. At this time, all the impurities that appeared on the liquid surface were eliminated by reacting with CF 4 gas.
- a seed crystal was brought into contact with the melt, and a single crystal was grown and produced in the c-axis direction at a pulling speed of lmmZh at a rotation speed of 15 rpm. Crystals produced have a diameter of about 1 8. 5 mm, a length of about 80 mm, air bubbles, cracks, liked Yatta ring center of which without a clear and high-quality L i S r A 1 F 6 : in E u single crystal there were.
- a lithium fluoride single crystal (L i F: M g, T i) doped with Mg and T i was prepared by a known method. (Test example 1)
- thermofluorescent dose when each single crystal was heated at 0.2 ° CZ sec was measured.
- LiF Mg
- Ti is the mainstream because TLD can more accurately examine the effects on living organisms.
- the upper limit of the measurement range is several Gy.
- Example 3 Eu slope of the approximate straight line obtained from the measurement results of the single crystal Doo is equal, L i C a a 1 F 6: Eu is, L i F: Mg, since it shows a very good correlation with T i, of tissue equivalent L i F: Mg, and T i Similarly, it is clear that the effects on living organisms are very easy to study.
- L i CaAlF 6 Eu has linearity equivalent to L i F: Mg, T i, and L i F: Mg, T i It showed that the measurement range capability was almost equivalent to.
- the relative thermofluorescence dose was Li C a A 1 F 6 : Eu, 3.7 times, and Li S r A 1 F 6 : E u was 29.2 times.
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Abstract
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JP2005504032A JPWO2004086089A1 (ja) | 2003-03-24 | 2004-03-22 | 熱蛍光線量計用フッ化物単結晶材料及び熱蛍光線量計 |
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JP2003-080963 | 2003-03-24 | ||
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JP2006251690A (ja) * | 2005-03-14 | 2006-09-21 | Kanazawa Univ | イメージングプレート並びにそれを用いた放射線画像情報記録読取装置及び放射線画像情報読取方法 |
WO2009119378A1 (ja) * | 2008-03-24 | 2009-10-01 | 株式会社トクヤマ | 中性子検出用シンチレーターおよび中性子検出装置 |
WO2011145651A1 (ja) * | 2010-05-18 | 2011-11-24 | 株式会社トクヤマ | 中性子線検出器、中性子線検出用シンチレーターおよび中性子線とγ線とを弁別する方法 |
WO2012011506A1 (ja) * | 2010-07-21 | 2012-01-26 | 国立大学法人広島大学 | ホスウィッチ型熱中性子検出器 |
WO2012011505A1 (ja) * | 2010-07-21 | 2012-01-26 | 国立大学法人広島大学 | 放射線検出器 |
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JP2006251690A (ja) * | 2005-03-14 | 2006-09-21 | Kanazawa Univ | イメージングプレート並びにそれを用いた放射線画像情報記録読取装置及び放射線画像情報読取方法 |
WO2009119378A1 (ja) * | 2008-03-24 | 2009-10-01 | 株式会社トクヤマ | 中性子検出用シンチレーターおよび中性子検出装置 |
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WO2011145651A1 (ja) * | 2010-05-18 | 2011-11-24 | 株式会社トクヤマ | 中性子線検出器、中性子線検出用シンチレーターおよび中性子線とγ線とを弁別する方法 |
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JP5894916B2 (ja) * | 2010-07-21 | 2016-03-30 | 国立大学法人広島大学 | ホスウィッチ型熱中性子検出器 |
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