CN108059957A - The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping - Google Patents
The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping Download PDFInfo
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- CN108059957A CN108059957A CN201610974106.0A CN201610974106A CN108059957A CN 108059957 A CN108059957 A CN 108059957A CN 201610974106 A CN201610974106 A CN 201610974106A CN 108059957 A CN108059957 A CN 108059957A
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- light output
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- twilight sunset
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- 239000000463 material Substances 0.000 claims abstract description 45
- 150000002500 ions Chemical class 0.000 claims abstract description 12
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims abstract description 5
- 150000001342 alkaline earth metals Chemical class 0.000 claims abstract description 5
- 229910052736 halogen Inorganic materials 0.000 claims abstract description 4
- 150000002367 halogens Chemical class 0.000 claims abstract description 4
- 239000003129 oil well Substances 0.000 claims abstract description 4
- 239000000126 substance Substances 0.000 claims abstract 2
- 238000012879 PET imaging Methods 0.000 claims description 4
- 229910052801 chlorine Inorganic materials 0.000 claims description 4
- 229910052731 fluorine Inorganic materials 0.000 claims description 4
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- 239000000919 ceramic Substances 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 239000013078 crystal Substances 0.000 abstract description 38
- 239000002994 raw material Substances 0.000 description 19
- 239000000460 chlorine Substances 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 9
- 229910000422 cerium(IV) oxide Inorganic materials 0.000 description 5
- 229910052681 coesite Inorganic materials 0.000 description 5
- 229910052906 cristobalite Inorganic materials 0.000 description 5
- 238000005192 partition Methods 0.000 description 5
- 229910001404 rare earth metal oxide Inorganic materials 0.000 description 5
- 239000000377 silicon dioxide Substances 0.000 description 5
- 229910052682 stishovite Inorganic materials 0.000 description 5
- 229910052905 tridymite Inorganic materials 0.000 description 5
- 229910001424 calcium ion Inorganic materials 0.000 description 4
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 3
- 229910052760 oxygen Inorganic materials 0.000 description 3
- 239000001301 oxygen Substances 0.000 description 3
- 229910020187 CeF3 Inorganic materials 0.000 description 2
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 description 2
- 229910003016 Lu2SiO5 Inorganic materials 0.000 description 2
- 150000001450 anions Chemical class 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 238000005303 weighing Methods 0.000 description 2
- 229910004664 Cerium(III) chloride Inorganic materials 0.000 description 1
- 229910001420 alkaline earth metal ion Inorganic materials 0.000 description 1
- 238000000137 annealing Methods 0.000 description 1
- JJWKPURADFRFRB-UHFFFAOYSA-N carbonyl sulfide Chemical compound O=C=S JJWKPURADFRFRB-UHFFFAOYSA-N 0.000 description 1
- VYLVYHXQOHJDJL-UHFFFAOYSA-K cerium trichloride Chemical compound Cl[Ce](Cl)Cl VYLVYHXQOHJDJL-UHFFFAOYSA-K 0.000 description 1
- 239000002178 crystalline material Substances 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000005251 gamma ray Effects 0.000 description 1
- 238000000265 homogenisation Methods 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000008092 positive effect Effects 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 239000004575 stone Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 238000000904 thermoluminescence Methods 0.000 description 1
- 238000003325 tomography Methods 0.000 description 1
Classifications
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- 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
- C09K11/7766—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
- C09K11/7774—Aluminates
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- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Luminescent Compositions (AREA)
Abstract
The invention discloses a kind of low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping, the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping uses following chemical formula：Lu2‑ yYy‑z‑xCexMzSiO5‑n/2Rn, in formula：M represents divalent alkaline-earth metal, and R table halogen family ions, x is greater than or equal to 0.0001, less than or equal to 0.1；Z is greater than or equal to 0.0001, less than or equal to 0.1；N is greater than or equal to 0, less than or equal to 0.01.This material has the characteristics such as High Light Output, fast attenuation, low twilight sunset, crystal property be good, is imaged available for medical PET, oil well logging and other industrial circles.
Description
Technical field
The present invention relates to a kind of scintillator materials, are dodged more particularly to a kind of low twilight sunset of the miscellaneous High Light Output of cation-anion co-doping
Bright body material.
Background technology
Scintillator is a kind of material that absorbs and can shine after high energy particle or ray, and this kind of material is widely used in γ and penetrates
In the particle detectors such as line, X-ray and cosmic ray.
Early stage the 1990s, it was found that Ce:Lu2SiO5Scintillator crystal materials (United States Patent (USP)：US4958080), the material
Material has many advantages, such as high density, High Light Output, short die-away time, low-refraction, and patent US6624420 is related to Ce2x(Lu1- yYy)2(1-x)SiO5Scintillator crystal materials, also the same excellent scintillation properties with LSO materials, this kind of material have to height jointly
The high ability prevented of energy ray, can cause the blue emission to decay soon, this crystalloid is used for gamma-ray detection field quickly,
Particularly in positron emission computerized tomography (PET) system.
Common, this kind of scintillator has the disadvantage that the inhomogeneity of light output and energy resolution, i.e. material
Performance crystal different parts have larger otherness, patent US7166845 and US7151261 find by by crystal containing
Implementing high annealing under oxygen environment is conducive to make the oxygen in environment to be diffused into crystals, fills up Lacking oxygen to reach crystal property
The purpose of homogenization；Another shortcoming of this kind of material is that the fluorescence of long die-away time occurs after irradiated in crystalline material, this
Application for PET imaging systems is more unfavorable, and the presence of twilight sunset reduces the resolution ratio of PET system.P.Dorenbost
Deng in " Afterglow and thermoluminescence properties of Lu2SiO5:Ce scintillation
To this twilight sunset of LSO materials in crystals " (J.Phys.Condens.Matter 6 1994, pp.416704180) article
Phenomenon has compared with in-depth study, it is believed that twilight sunset is the intrinsic property of LSO materials.
United States Patent (USP) US2015097385, US7132060 describe divalent alkaline-earth metal and Al ion dopings to LSO and
LYSO crystal twilight sunset has apparent inhibitory action.Applicant has found in an experiment, using the Lu of different chlorinty2O3Raw material is given birth to
The state of long obtained crystal twilight sunset is different, and the crystal twilight sunset compared with high chloride ion content is significantly lower than compared with low chlorine ion content
Crystal, but higher concentration chloride ion content can cause the decline of light output, and applicant is further sent out using anion doped experiment
Existing, suitable fluorine ion introducing can similarly be played the role of reducing twilight sunset, and crystal light output is also more brilliant than undoped fluorine ion
Body light output is higher by 8% or so.When using anion and divalent alkaline-earth metal ion co-doped, twilight sunset can be reduced to
Undoped with preceding less than 10%.
The content of the invention
The present invention provides a kind of miscellaneous High Light Output of cation-anion co-doping low twilight sunset scintillator material, with High Light Output,
The characteristics such as fast attenuation, low twilight sunset, crystal property be good are imaged, oil well logging and other industrial circles available for medical PET.
The present invention is to solve above-mentioned technical problem by following technical proposals：A kind of miscellaneous bloom of cation-anion co-doping is defeated
Go out low twilight sunset scintillator material, which is characterized in that it uses the scintillator material such as following formula：
Lu2-yYy-z-xCexMzSiO5-n/2Rn
In formula：M represents divalent alkaline-earth metal, and R table halogen family ions, x is greater than or equal to 0.0001, less than or equal to 0.1；
Z is greater than or equal to 0.0001, less than or equal to 0.1；N is greater than or equal to 0, less than or equal to 0.01.
Preferably, the M is Ca or Mg.
Preferably, the R is F or Cl.
Preferably, the z is less than or equal to 0.002.
Preferably, the n is less than or equal to 0.0005.
Preferably, the M and R are adulterated simultaneously.
Preferably, the low twilight sunset scintillator material of the miscellaneous High Light Output of the cation-anion co-doping is monocrystalline or ceramics.
Preferably, the low twilight sunset scintillator material of the miscellaneous High Light Output of the cation-anion co-doping can be used for medical treatment PET imagings, stone
Oil well logging.
The positive effect of the present invention is：One, the miscellaneous LYSO crystal of cation-anion co-doping, have higher light output (>
32000Ph/MeV)；Two, the miscellaneous LYSO crystal of cation-anion co-doping has decays faster, and three, the miscellaneous LYSO of cation-anion co-doping is brilliant
Body has shorter twilight sunset.
Specific embodiment
Present pre-ferred embodiments are given below, with the technical solution that the present invention will be described in detail.
The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping of the present invention uses the scintillator material such as following formula：
Lu2-yYy-z-xCexMzSiO5-n/2Rn
In formula：M represents divalent alkaline-earth metal, and R table halogen family ions, x is greater than or equal to 0.0001, less than or equal to 0.1；
Z is greater than or equal to 0.0001, less than or equal to 0.1；N is greater than or equal to 0, less than or equal to 0.01.
The M is Ca or Mg.The R is F or Cl.Z is less than or equal to 0.002.N is less than or equal to 0.0005.M and
R is adulterated simultaneously.The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping of the present invention is monocrystalline or ceramics.
Embodiment 1：It is miscellaneous with high purity rare earth oxides Lu that cation-anion co-doping is not carried out203(Cl ion concentrations for 50ppm with
Under), Y2O3、CeO2And SiO2For raw material, first pre-burning raw material is to remove H before dispensing2O and CO2.By Lu1.85Y0.148Ce0.002SiO5
Partition is ground uniformly than accurately weighing to amount to 2KG raw materials and be sufficiently mixed.Mixed raw material briquet under 200MPa pressure,
Then put material block into Muffle furnace, 15h is sintered at 1400 DEG C and obtains LYSO polycrystalline.Polycrystalline LYSO is dosed into single crystal growing furnace
Crystal growth is carried out, crucible internal diameter is 80mm, after crystal grows up to, is slowly dropped to room temperature.After crystal is come out of the stove, cut sample and carry out performance survey
Examination.
Embodiment 2：Ca ion dopings
With high purity rare earth oxides Lu203(Cl ion concentrations are below 50ppm), Y2O3、CeO2And SiO2, CaO for original
Material, first pre-burning raw material is to remove H before dispensing2O and CO2.By Lu1.85Y0.145Ce0.002Ca0.003SiO5Partition than accurately weighs total
2KG raw materials are simultaneously sufficiently mixed grinding uniformly.Then mixed raw material briquet under 200MPa pressure puts material block into Muffle
In stove, sintering 15h obtains LYSO polycrystalline at 1400 DEG C.Polycrystalline LYSO is dosed into single crystal growing furnace, carries out crystal growth, crucible
Internal diameter is 80mm, after crystal grows up to, is slowly dropped to room temperature.After crystal is come out of the stove, cut sample and be tested for the property.
Embodiment 3：F ion is adulterated
With high purity rare earth oxides Lu203(Cl ion concentrations are below 50ppm), Y2O3、CeO2And SiO2、CeF3For original
Material, first pre-burning raw material is to remove H before dispensing2O and CO2.By Lu1.85Y0.148Ce0.002SiO4.9998F0.0004Partition than accurately weighs
It amounts to 2KG raw materials and is sufficiently mixed grinding uniformly.Then mixed raw material briquet under 200MPa pressure is put material block into
In Muffle furnace, sintering 15h obtains LYSO polycrystalline at 1400 DEG C.Polycrystalline LYSO is dosed into single crystal growing furnace, carries out crystal growth,
Crucible internal diameter is 80mm, after crystal grows up to, is slowly dropped to room temperature.After crystal is come out of the stove, cut sample and be tested for the property.
Embodiment 4：F, Ca ion dopings
With high purity rare earth oxides Lu203(Cl ion concentrations are below 50ppm), Y2O3、CeO2And SiO2、CeF3、CaO
For raw material, first pre-burning raw material is to remove H before dispensing2O and CO2.By Lu1.85Y0.145Ce0.002Ca0.003SiO4.9998F0.0004Partition ratio
Accurate weigh amounts to 2KG raw materials and is sufficiently mixed grinding uniformly.Then mixed raw material briquet under 200MPa pressure will
Material block puts Muffle furnace into, and 15h is sintered at 1400 DEG C and obtains LYSO polycrystalline.Polycrystalline LYSO is dosed into single crystal growing furnace, is carried out
Crystal growth, crucible internal diameter are 80mm, after crystal grows up to, are slowly dropped to room temperature.After crystal is come out of the stove, cut sample and be tested for the property.
Embodiment 5：Cl, Ca ion doping
With high purity rare earth oxides Lu203(Cl ion concentrations are below 50ppm), Y2O3、CeO2And SiO2、CeCl3、CaO
For raw material, first pre-burning raw material is to remove H before dispensing2O and CO2.By Lu1.85Y0.145Ce0.002Ca0.003SiO4.9998Cl0.0004Partition
It is ground uniformly than accurately weighing to amount to 2KG raw materials and be sufficiently mixed.Mixed raw material briquet under 200MPa pressure, then
It puts material block into Muffle furnace, 15h is sintered at 1400 DEG C and obtains LYSO polycrystalline.Polycrystalline LYSO is dosed into single crystal growing furnace, into
Row crystal growth, crucible internal diameter are 80mm, after crystal grows up to, are slowly dropped to room temperature.After crystal is come out of the stove, cut sample and carry out performance survey
Examination.
The results are shown in Table 1 for the die-away time of 5 embodiments, light output, twilight sunset etc. above.
Table 1
In table, composition 4 uses F ion and Ca ion co-dopeds, can will be improved undoped with LYSO crystal light output
10% or so, corresponding twilight sunset recovery time is 1/10 undoped with crystal.
The low twilight sunset scintillator material of the above-mentioned miscellaneous High Light Output of cation-anion co-doping can be used for medical PET imagings, oil is surveyed
Well and other industrial circles.
Particular embodiments described above, the technical issues of to the solution of the present invention, technical solution and advantageous effect carry out
It is further described, it should be understood that the above is only a specific embodiment of the present invention, is not limited to
The present invention, within the spirit and principles of the invention, any modification, equivalent substitution, improvement and etc. done should be included in this
Within the protection domain of invention.
Claims (8)
- A kind of 1. low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping, which is characterized in that the cation-anion co-doping The low twilight sunset scintillator material of miscellaneous High Light Output uses following chemical formula：Lu2-yYy-z-xCexMzSiO5-n/2RnIn formula：M represents divalent alkaline-earth metal, and R table halogen family ions, x is greater than or equal to 0.0001, less than or equal to 0.1；Z is big In or equal to 0.0001, less than or equal to 0.1；N is greater than or equal to 0, less than or equal to 0.01.
- 2. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described M is Ca or Mg.
- 3. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described R is F or Cl.
- 4. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described Z is less than or equal to 0.002.
- 5. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described N is less than or equal to 0.0003.
- 6. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described M and R are adulterated simultaneously.
- 7. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping is monocrystalline or ceramics.
- 8. the low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping as described in claim 1, which is characterized in that described The low twilight sunset scintillator material of the miscellaneous High Light Output of cation-anion co-doping can be used for medical treatment PET imagings, oil well logging.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112630818A (en) * | 2020-11-16 | 2021-04-09 | 中国科学院上海硅酸盐研究所 | Silicon-site-doped improved rare earth orthosilicate scintillation material and preparation method and application thereof |
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| CN103249805A (en) * | 2010-11-16 | 2013-08-14 | 圣戈班晶体及检测公司 | Luminescent material comprising a doped rare earth silicate |
| CN104508192A (en) * | 2012-04-13 | 2015-04-08 | 泽克泰克光子学有限公司 | Multi-doped lutetium based oxyorthosilicate scintillators having improved photonic properties |
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2016
- 2016-11-07 CN CN201610974106.0A patent/CN108059957A/en active Pending
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| CN1250526A (en) * | 1998-01-12 | 2000-04-12 | Tasr有限公司 | Scintillating substance and scintillating wave-guide element |
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