Method of shortening scintillation response of luminescense centres and material of scintillator with shortened scintillation response
10976451 · 2021-04-13
Assignee
Inventors
- Jind{hacek over (r)}ich Hou{hacek over (z)}vi{hacek over (c)}ka (Turnov, CZ)
- Karel Bla{hacek over (z)}ek (Turnov, CZ)
- Petr Horodyský (Moravany, CZ)
- Martin Nikl (Prague, CZ)
- Pavel Bohá{hacek over (c)}ek (Prague, CZ)
Cpc classification
G21K4/00
PHYSICS
International classification
Abstract
Currently, the known method of shortening the scintillation response of scintillation material is to suppress the amplitude-minor slower components of the scintillation response, whereas the possibilities of significant shortening of the amplitude-dominant component of the scintillation response in this method are limited. The invention concerns the method of shortening the scintillation response of scintillator luminescence centres which uses co-doping with Ce or Pr together with co-doping with ions from the lanthanoids, 3d transition metals, 4d transition metals or 5s.sup.2 or 6s.sup.2 ions group. Having had the luminescence centres electrons excited as a result of absorbed electromagnetic radiation, the scintillator created in this method is capable of taking away a part of the energy from the excited luminescence centres via a non-radiative energy transfer, which results in a significant shortening of the time of duration of the amplitude-dominant component of the scintillation response.
Claims
1. A scintillator material based on a garnet with a general chemical formula of A.sub.3B.sub.5O.sub.12 which shortens the scintillation response, wherein said scintillator corresponds to the general chemical formula A.sub.3-x1-x2.sup.1M.sub.x1.sup.2M.sub.x2B.sub.5O.sub.12 where the substituent A is represented by a cation from the Y.sup.3+, Lu.sup.3+, Gd.sup.3+ group or their mixture, the substituent B is represented by a cation from the Al.sup.3+, Ga.sup.3+, Sc.sup.3+, Mo.sup.3+ group or their mixture, the substituent .sup.1M represents the dopant cation from the Ce.sup.3+ or Pr.sup.3+ group, and the substituent .sup.2M represents a mixture of a first co-dopant selected from the group consisting of Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zr, Nb, Mo, Ru, Ag, Ta, W, In, Sn, Sb, Tl, Pb or Bi and a second co-dopant selected from the group consisting of optically inactive ions, Mg.sup.2+ or Ca.sup.2+.
Description
DESCRIPTION OF THE DRAWINGS
(1) The invention shall be clarified more closely in the following drawings, where:
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EXAMPLES OF THE PREFERRED EMBODIMENTS OF THE INVENTION
(18) It is understood that the below stated and depicted specific examples of the invention execution are represented for illustration and not as the limitation of the invention to the stated examples. Experts knowledgeable of the state of technology will find or will be able to ensure, when performing routine experimentation, larger or smaller amount of equivalents to the specific executions of the invention which are described here. These equivalents shall be also included in the extent of the following patent claims.
(19) Active scintillators may be prepared in the form of powder, such as via simple sintering, of an active layer, such as via epitaxial growth or plasma deposition, or of a volume single crystal, such as with the Czochralski, EFG, microPD, Kyropoulos and other methods.
(20) The scintillation response mechanism with known materials is schematically illustrated in
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Example 1—Preparation of Sample of YAG:Ce, YAG:Nd a YAG:Ce Single Crystal Co-Doped with Nd (YAG:Ce, Nd)
(24) Mixtures were prepared of Y.sub.2O.sub.3 and Al.sub.2O.sub.3 binary oxides with the Y.sub.3Al.sub.5O.sub.12 composition, CeO.sub.2 and Al.sub.2O.sub.3 with the Ce.sub.3Al.sub.5O.sub.12 composition, Nd.sub.2O.sub.3 and Al.sub.2O.sub.3 of the Nd.sub.3Al.sub.5O.sub.12 composition when the used materials were of the 5N purity. Mechanical mixing was followed with homogenisation via shaking and isostatic pressing into a block. The blocks were sintered at 1 400° C. for the period of 24 hours in the air and subsequently were partially crushed and inserted into a molybdenum crucible. The YAG:Ce, YAG:Nd and YAG:Ce, Nd single crystals were grown from the mixture via the Czochralski method under a protective hydrogen/argon atmosphere. The composing of melt for growing was selected in such a method that the resulting crystals are of the Y.sub.2.96Nd.sub.0.04Al.sub.5O.sub.12) Y.sub.2.91Nd.sub.0.04Ce.sub.9.95Al.sub.5O.sub.12 a Y.sub.2.95Ce.sub.0.05Al.sub.5O.sub.12 composition to compare their characteristics.
(25) Small discs were cut from the prepared single crystals of 1 mm thickness and 10 mm diameter which were optically polished for the subsequent measurement of the spectra and scintillation responses.
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Example 2 Preparation of Sample of YAG:Ce Single Crystal Co-Doped with Ho (YAG:Ce, Ho)
(27) In the total amount of 5 g, the Y.sub.2O.sub.3, Al.sub.2O.sub.3, CeO.sub.2 and Ho.sub.2O.sub.3 binary oxides of the 5N purity were mixed in the ratio of the chemical Y.sub.2.91Ho.sub.004Ce.sub.005Al.sub.5O.sub.12 formula. After mechanical mixing and grinding in the grinding mortar there followed a two-stage sintering: in the first stage at 1 300° C. for the period of 24 hours, in the second stage at 1 400° C. for the period of 24 hours, in the air. The material was again mechanically ground in the grinding mortar between the individual steps. The powder was inserted into a molybdenum crucible and in the protective atmosphere of 70% argon/30% hydrogen a single crystal was drawn in the shape of a rod with the EFG method through a molybdenum die. The Y.sub.2.96Nd.sub.0.04Al.sub.5O.sub.12 and Y.sub.2.95Ce.sub.0.05Al.sub.5O.sub.12 single crystals were prepared in the same method to compare their characteristics. Small discs of 1 mm thickness were cut from the prepared single crystal rods of 4 mm diameter which were optically polished for the subsequent measuring of spectra and scintillation responses.
(28) The overlap of the emission band of the Ce.sup.3+ centre with maximum at 525 nm and absorption transition of the centre Ho.sup.3+ 5I.sub.8=.sup.5S.sub.2, .sup.5F.sub.4 centre with the maximum at 530-540 nm (W. T. Carnal) et al, J. Chem. Phys. 90, no. 7, 3443, 1989) in the spectrum range of 500-595 nm which corresponds to FWHM of the Ce.sup.3+ centre emission, causes the acceleration of the amplitude-dominant component of the scintillator response which is depicted in
Example 3 Preparation of Sample of YAP:Pr Single Crystal and YAP:Pr Single Crystal Co-Doped with Gd (YAP:Pr, Gd)
(29) The YAP:Pr and YAP:Pr, Gd single crystals were prepared and grown analogously according to Example 2 when the Y.sub.2O.sub.3, Al.sub.2O.sub.3, Gd.sub.2O.sub.3 and Pr.sub.8O.sub.11 binary oxides of the 5N purity were mixed in the ratio of the Y.sub.0.995Pr.sub.0.005AlO.sub.3, Y.sub.0.985Gd.sub.0.01Pr.sub.0.005AlO.sub.3 and Y.sub.0.945Gd.sub.0.05Pr.sub.0.005AlO.sub.3 chemical formulas. The spectra and scintillation responses were measured analogously as in Example 2.
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(31) The overlap of the emission band of the Pr.sup.3+ centre with absorption transition of the centre Gd.sup.3+ 8S.sub.7/2.fwdarw..sup.6I.sub.x at 270-275 nm (W. T. Carnal) et al, J. Chem. Phys. 90, no. 7, 3443, 1989) in the spectrum range of 235-285 nm which corresponds to FWHM of the Pr.sup.3+ centre emission, causes a non-radiative energy transfer from the Pr.sup.3+ centre to the Gd.sup.3+ centre which results in the acceleration of the amplitude-dominant component 1 in the scintillator response which is depicted in
Example 4 Preparation of Sample of YAP:Pr Single Crystal and YAP:Pr Single Crystal Co-Doped with Tb (YAP:Pr, Tb)
(32) The YAP:Pr and YAP:Pr co-doped with Tb single crystals were prepared and grown analogously according to Example 1. A mixture of Y.sub.2O.sub.3 and Al.sub.2O.sub.3 binary oxides was prepared with the ratio 1:1. Mechanical mixing was followed with homogenisation shaking and isostatic pressing into a block. The blocks were sintered at 1 400° C. for the period of 24 hours in the air and subsequently were partially crushed and inserted into a tungsten crucible. To complete stoichiometry, the Al.sub.2O.sub.3, Tb.sub.4O.sub.7 and Pr.sub.6O.sub.11 oxides were used with materials of the 4N purity. Single crystal with Y.sub.0.995Pr.sub.0.005AlO.sub.3, Y.sub.0.985Tb.sub.0.01Pr.sub.0.005AlO.sub.3 and Y.sub.0.945Tb.sub.0.05Pr.sub.0.005AlO.sub.3 chemical formulas were prepared from the stated materials. The spectra and scintillation responses were measured analogously as in Example 1.
(33) The overlap of the emission band of the Pr.sup.3+ centre with maximum at 247 nm and the lowest absorption band transition 4f-5d of the Tb.sup.3+ centre in range of 250-280 nm (K. S. Sohn et al, J. Electrochem. Soc., 147 (9) 3552, 2000) in the spectrum range of 235-285 nm which corresponds to FWHM of the Pr.sup.3+ centre emission, causes a non-radiative energy transfer from the Pr.sup.3+ centre to the Tb.sup.3+ centre which results in the acceleration of the amplitude-dominant component 1 in the scintillator response. It is depicted in
Example 5 Preparation of Sample of LGSO:Ce Single Crystal and LGSO:Ce Single Crystal Co-Doped with Dy (LGSO:Ce, Dy)
(34) The LGSO:Ce and LGSO:Ce co-doped with Dy single crystals were prepared and grown with the Czochralski method from iridium crucible under the protective atmosphere of nitrogen with traces of oxygen. The starting materials for growing the single crystal analogously according to Example 1 were the Lu.sub.2O.sub.3 and SiO.sub.2, Gd.sub.2O.sub.3 and SiO.sub.2, CeO.sub.4 and SiO.sub.2 and Dy.sub.2O.sub.3 and SiO.sub.2 binary oxides mixtures with the purity of 5N. The result of growth were the single crystals of the (Lu.sub.0.53Gd.sub.0.40Ce.sub.0.01).sub.2SiO.sub.5, and (Lu.sub.0.57Gd.sub.0.40Ce.sub.0.01Dy.sub.0.02).sub.2SiO.sub.5 chemical formulas. The spectra and scintillation responses were measured analogously as in Example 1.
(35) The overlap of the emission band of the Ce.sup.3+ centre with marked maximum 3 at 425 nm and FWHM 400-465 nm and absorption transitions 4f-4f from the basic state of .sup.6H.sub.15/2 to higher 4f states .sup.4I.sub.15/2 and .sup.4G.sub.1/12 and .sup.4M.sub.21/2 of the Dy.sup.3+ centre in the range of 400-455 nm (W. T. Carnal) et al, J. Chem. Phys. 90, no. 7, 3443, 1989), which is depicted in
Example 6—Preparation of Sample of YSO:Ce Single Crystal
(36) The YSO:Ce single crystal was prepared and grown analogously according to Example 4. The Y.sub.2O.sub.3, SiO.sub.2 and CeO.sub.4 binary oxides of 5N purity were mixed which resulted in a single crystal of the (Y.sub.0.99Ce.sub.0.01).sub.2SiO.sub.5 chemical formula. The spectra and scintillation responses were measured analogously as in Example 1.
(37) A sufficient increase in temperature leads practically with every luminescence centre to the appearance of non-radiative thermal quenching of luminescence which can be utilized, too, for the shortening of the period of duration of the dominant component 1 in the scintillation response. In case of the emission band of both the Ce.sup.3+ centres, marked here as the P curve and the Q curve, in the host YSO crystal, the thermal quenching of both the P and Q centres occurs at approximately 350 K, as shown in
(38) It is clear from Examples 1 to 6 that the utilization of the first co-dopant results in a significant acceleration in the time of duration of amplitude-dominant component of the scintillation response. The scintillation response consists also of slower components where it is possible to decrease intensity. This simultaneous action occurs with materials according to the following example of invention execution:
Example 7—Preparation of Sample of Single Crystals LuAG:Ce and LuAG:Ce Co-Doped with Nd and LuAG:Ce Doubly Co-Doped with Nd and Mg (LuAG:Ce, Nd and LuAG:Ce, Nd, Mg)
(39) The LuAG:Ce and LuAG:Ce co-doped with Nd and LuAG:Ce doubly do-doped with Nd and Mg single crystals were prepared and grown analogously according to Example 2 when the Lu.sub.2O.sub.3, Al.sub.2O.sub.3, CeO.sub.2, Nd.sub.2O.sub.3 and MgO binary oxides of 5N purity were mixed in the ratio of the Lu.sub.2.91Nd.sub.0.02Ce.sub.0.05Mg.sub.0.02Al.sub.5O.sub.12 and Lu.sub.2.93Nd.sub.0.02Ce.sub.0.05Al.sub.5O.sub.12 and Lu.sub.2.95Ce.sub.0.05Al.sub.5O.sub.12 chemical formulas. The spectra and scintillation responses were measured analogously as in Example 2.
(40) The overlap of the emission band of the Ce.sup.3+ centre with maximum at 525 nm and absorption band transitions of the centre Nd.sup.3+ 4I.sub.9/2>.sup.4G.sub.5/2, .sup.4G.sub.7/2 Nd3+ 4I9/2□4G5/2,4G7/2 (W. T. Carnal) et al, J. Chem. Phys. 90, no. 7, 3443, 1989) in the spectrum range of 500-595 nm which corresponds to FWHM of the Ce.sup.3+ centre emission, causes a non-radiative energy transfer from the Ce.sup.3+ centre to the Nd.sup.3+ centre which results in the acceleration of the amplitude-dominant component 1 in the scintillation response which is depicted in
(41) In other example of execution, the first co-dopant can be from the 3d transition metals group—Ti, V, Cr, Mn, Fe, Co, Ni, Cu, 4d transition metals group—Zr, Nb, Mo, Ru, Rh, Ag, 5d transition metals group—Ta, W, 5s.sup.2 ions—In, Sn, Sb, or from the 6s.sup.2 ions group—Tl, Pb, Bi. In another example of execution the Ca.sup.2+ cation can be used as the second co-dopant.
Example 8—Preparation of Sample of Single Crystals Gd.SUB.3.Ga.SUB.3.Al.SUB.2.O.SUB.12.:Ce (GGAG:Ce), GGAG:Nd and GGAG:Ce Co-Doped with Nd (GGAG:Ce, Nd)
(42) The Gd.sub.3Ga.sub.3Al.sub.2O.sub.12:Ce (GGAG:Ce) single crystal was prepared and grown analogously according to Example 1 when the Gd.sub.2O.sub.3, Ga.sub.2O.sub.3, Al.sub.2O.sub.3, CeO.sub.2 and Nd.sub.2O.sub.3 binary oxides of 5N purity were mixed. The GGAG:Ce single crystal was grown from the mixture via the Czochralski method under a protective hydrogen/argon atmosphere, the composition of melt for the growth was selected in such a method that the resulting crystal was composed in the ratio of the Gd.sub.2.955Nd.sub.0.03Ce.sub.0.015Ga.sub.3Al.sub.2O.sub.12 chemical formula. Analogously as in Example 1, the spectra and scintillation responses were subsequently measured. The Gd.sub.2.97Nd.sub.0.03Ga.sub.3Al.sub.2O.sub.12 and Gd.sub.2.985Ce.sub.0.15Ga.sub.3Al.sub.2O.sub.12 single crystals were prepared in the same method to compare their characteristics.
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Example 9—Fast Scintillation Detector of Secondary Electrons
(44) A double-sided polished scintillation disk with the diameter of 10 mm and thickness of 1 mm was manufactured from the Y.sub.0.985Tb.sub.0.01 Pr.sub.0.005AlO.sub.3 crystal, grown in Example 4. On surface it was provided with aluminium coating of the thickness of 50 nm. The disc was glued in the face of the all-sides polished cylinder from quartz glass. Positive potential+10 kV is lead to the aluminium coating. The positive potential attracts electrons to the scintillation disk and inside it, fast light flashes are created. The quartz cylinder leads light pulses from the scintillation disc to the fast optical detector. The assembly of the scintillation disc and quartz cylinder is placed in the electronic scanning microscope chamber and enables to detect the signal of secondary electrons with a time response of 5 ns/pxl.
Example 10—Fast Scintillation Detector of Secondary Electrons
(45) A plate with the diameter of 15 mm and thickness of 2 mm in epitaxial quality was polished from the undoped YAG single crystal. 20 μm thick layer of Gd.sub.2955Nd.sub.003Ce.sub.0015Ga.sub.3Al.sub.2O.sub.12 was applied onto the surface of the plate via the LPE (Liquid Phase Epitaxy) method. The scintillation disc was worked and except for one head surface, the epitaxial layer was polished off. A thin conductive ITO coating was coated onto the surface with the LPE layer. The disc was glued in the face of the all-sides polished cylinder from quartz glass. Positive potential+10 kV is lead to the aluminium coating. The positive potential attracts electrons to the scintillation disk and inside it, fast light flashes are created. The quartz cylinder leads light pulses from the scintillation disc to the fast optical detector. The assembly of the scintillation disc and quartz cylinder is placed in the electronic scanning microscope chamber and enables to detect the signal of secondary electrons. When compared to the same detector which contains a polished YAG:Ce disc, this detector has a higher light yield and operates with a shorter time response.
Example 11 Single Crystal Detector for PET Applications
(46) The LYSO:Ce co-doped with Dy and GGAG:Ce co-doped with Nd single crystals were grown via the Czochralski method. Elements of 2×2×10 mm, polished from all sides, were prepared from each single crystal. From these elements the modules (matrix) were composed with the size of 8×8 elements (pixels) which were optically separated from each other. Both the matrices were connected together optically with the accuracy of minimally 0.1 mm, pixel to pixel. The whole element was inserted in a plastic casing and the crystal was optically connected with 64-pixel APD. The whole module was used in a positron scanner for tumour imaging in small animals, with a high special resolution and speed.
Example 12—Fast Detector for High Energy Particles Detection
(47) A LuAG:Ce, Nd, Mg single crystal was grown via the Czochralski method according to Example 7 with a higher concentration of Nd in such a method that the response of the single crystal on the cerium centre was 20 ns. Fibres of the size 1×1×140 mm were prepared from the single crystal and all the surfaces were polished. A pixel detector was assembled from the fibres so that the fibres were interlaid with a tungsten sheet of 1 mm thickness. The detector contained 8×8 fibres. The detector was constructed in such a method that there were no optical leaks among the individual fibres. The pixels were insulated from each other with tungsten. The detector was connected at its end with a 64-pixel APD. The detector was used as an electromagnetic calorimeter to detect high energy particles originating in a proton-proton collider with the timing of 25 ns. Due to its short response this solution significantly increased the efficiency of particles detection.
INDUSTRIAL APPLICABILITY
(48) Scintillators with a shortened time of response according to the invention will be utilized in medical applications, working with ionizing radiation, such as positron emission tomography (PET) or CT, in scientific applications, such as in various calorimetric detectors, and in industry, particularly in detectors for the quality control of internal structures of mass produced products, such as chips, or e.g. during border controls.