Dual-strategy co-doped rare earth orthosilicate fast scintillation material, preparation method and application

Abstract

The present invention provides a dual-strategy co-doped rare earth orthosilicate fast scintillation material, a preparation method and an application thereof. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1‑u‑v‑w) Ce 2u M 2v N 2w Si 1‑y Al y O5, wherein 0 < u ≤ 0.05, 0 ≤ v ≤ 0.1, 0 < w ≤ 0.1, 0 ≤ y ≤ 0.1, and v + y > 0, RE represents a rare earth element, selected from at least one of lanthanum, lutetium, yttrium, and gadolinium, the carrier trap suppression dopant element includes aluminum and / or M, selected from at least one of magnesium, calcium, and nickel, and N represents a competitive luminescence center dopant element, selected from at least one of ytterbium, europium, praseodymium, and neodymium. According to the present invention, the scintillation light decay time can be reduced to less than 30 ns.

Description

Technical Field

[0001] The present invention relates to the technical field of scintillation materials, and in particular to a dual-strategy co-doped rare earth orthosilicate fast scintillation material, a preparation method and applications thereof. Background Art

[0002] Inorganic scintillating materials are crystalline energy converters that can convert the energy of high-energy photons (X / gamma rays) or particles (protons, neutrons, etc.) into easily detectable ultraviolet / visible light photons. Detectors made from inorganic scintillating crystals are widely used in high-energy physics, nuclear physics, space physics, nuclear medicine diagnostics (XCT, PET), geological exploration, and safety audits. With the rapid development of nuclear detection and related technologies, the performance requirements for inorganic scintillating crystals have also increased significantly. Currently, traditional scintillating crystals such as NaI(Tl), BGO, and PWO are no longer able to meet existing requirements. Newer generation aluminate and silicate scintillating crystals, due to their high light output and fast decay characteristics, have gradually become a research hotspot.

[0003] Current scintillating materials focus on properties such as high output, fast response, and high density. Research on new scintillating materials is being conducted through the following two methods to enhance and improve material properties: 1) By co-doping different ions, the deficiencies of existing scintillating materials can be improved, and their scintillation properties, such as light yield, can be enhanced; 2) By leveraging the relationship between microscopic defects, co-doping, and scintillation properties, harmful point defects can be reduced and suppressed, thereby reducing the loss of energy conversion caused by non-radiative transitions during the scintillation process.

[0004] With rare earth ion Ce 3+ As an activator, Ce 3+ The 5d→4f parity-allowed transition of ions can be used to obtain high-intensity fast-decay luminescence. The new scintillating materials currently used include Ce:YAG, Ce:GAGG, Ce:LYSO, Ce:GSO, Ce:YAP, Ce:LuAP, etc. Compared with traditional inorganic scintillating crystals such as NaI:Tl, BGO, BaF2 and PWO, Ce: 3+ Ion-doped high-temperature oxide crystals have the characteristics of high light output (about 2-10 times that of BGO crystals) and fast attenuation (about 1 / 5-1 / 20 of BGO crystals). 3+ Ion-doped orthosilicates (lutetium silicate (LSO) crystals and yttrium lutetium silicate (LYSO) crystals) have the characteristics of high light output, fast luminescence decay, a large effective atomic number, and high density. Therefore, they are widely used in medical PET (positron emission tomography) machines and computed tomography (CT scanner) systems in the industrial sector.

[0005] Currently, for Ce 3+In the preparation of ion-doped rare earth orthosilicate scintillating materials, co-doping is an effective method to optimize performance. Co-doping elements include Ca 2+ Mg 2+ 、Al 3+ 、Yb 3+ 、Zn 2+ 、Li + 、Cu 2+ , Pb 2+ 、Dy 3+ 、Tb 3+ 、Na + By adjusting the shallow energy trap concentration in the crystal, the charge state of the luminescent center ions, making the luminescent center Ce tend to occupy the fast luminescent Ce1 position or shortening the luminescent process of the luminescent center, the decay time of the crystal is shortened. 2+ Ion co-doping is the best doping modification method for the comprehensive performance of cerium-doped rare earth orthosilicate scintillating materials. Chinese patent application CN108059957A discloses a scintillator material with high light output and low afterglow, in which the rare earth sites of the scintillating material are Ca 2+ or Mg 2+ Although Ca 2+ Co-doping can significantly or even completely eliminate the shallow energy level traps in YSO:Ce scintillating materials. However, due to the Ca 2+ Co-doping has little effect on the excited state lifetime of the luminescent center, so Ca 2+ The scintillation decay time of co-doped rare earth orthosilicate scintillating materials is still difficult to break the limit of 30ns.

[0006] Therefore, there is an urgent need to provide a scintillation material with an ultrafast decay time. Summary of the Invention

[0007] Existing technology discloses Yb co-doped LSO:Ce materials, but their scintillation decay time has not been studied. Furthermore, research on Pr and Ce co-doped rare earth orthosilicate scintillating materials is also lacking. While Eu and Nd have been studied, because Nd and Eu emit light via 4f-4f transitions, when co-doped with rare earth orthosilicate scintillating materials, they typically exhibit line-spectrum luminescence with millisecond-scale decay. Therefore, they are often used as fluorescent materials or optical storage materials.

[0008] On this basis, the inventors discovered that by combining two types of doping elements, namely optically inert defect suppression elements (at least one of Al and / or Mg, Ca, and Ni) and competitive luminescent elements (at least one of Yb, Eu, Pr, and Nd), and co-doping rare earth orthosilicate scintillating materials with multiple elements, the decay time of the rare earth orthosilicate scintillating materials can be greatly improved, and the present invention was completed on this basis.

[0009] According to the first aspect of the present invention, a dual-strategy co-doped rare earth orthosilicate fast scintillation material is provided. The dual-strategy co-doped rare earth orthosilicate fast scintillation material is a scintillation material co-doped with a carrier trap suppression type doping element and a competitive luminescence center type doping element. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y O5, where 0<u≤0.05, 0≤v≤0.1, 0<w≤0.1, 0≤y≤0.1, and v+y>0,

[0010] The RE represents a rare earth element, and the rare earth element is at least one selected from lanthanum, lutetium, yttrium, and gadolinium.

[0011] The carrier trap suppression doping element includes aluminum and / or M element, and the M element is selected from at least one of magnesium, calcium, and nickel.

[0012] The N represents a competitive luminescence center type doping element, and the competitive luminescence center type doping element is selected from at least one of ytterbium, europium, praseodymium, and neodymium.

[0013] Furthermore, the carrier trap suppression doping element includes aluminum and M element, wherein the aluminum element at least partially occupies the silicon lattice site.

[0014] Furthermore, the rare earth element is yttrium or a solid solution of lutetium and yttrium.

[0015] Furthermore, the rare earth element is a solid solution of lutetium and yttrium, wherein the molar ratio of lutetium to yttrium is 9:1.

[0016] Furthermore, 0.001≤u≤0.005, 0.001≤v≤0.02, 0.004≤w≤0.05.

[0017] Furthermore, 0.003≤y≤0.02.

[0018] Furthermore, the scintillation light decay time of the dual-strategy co-doped rare earth orthosilicate fast scintillation material is less than 30ns.

[0019] According to a second aspect of the present invention, a method for preparing a dual-strategy co-doped rare earth orthosilicate fast scintillation material is provided. The dual-strategy co-doped rare earth orthosilicate fast scintillation material is a scintillation material co-doped with a carrier trap suppression type doping element and a competitive luminescence center type doping element. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M2v N 2w Si 1-y Al y O5, where 0<u≤0.05, 0≤v≤0.1, 0<w≤0.1, 0≤y≤0.1, and v+y>0,

[0020] The RE represents a rare earth element, and the rare earth element is at least one selected from lanthanum, lutetium, yttrium, and gadolinium.

[0021] The carrier trap suppression doping element includes aluminum and / or M element, and the M element is selected from at least one of magnesium, calcium, and nickel.

[0022] The N represents a competitive luminescence center type doping element, and the competitive luminescence center type doping element is selected from at least one of ytterbium, europium, praseodymium, and neodymium. The preparation method comprises the following steps:

[0023] S1, weigh the rare earth source compound, Ce source compound, carrier trap suppression type dopant source compound, competitive luminescence center type dopant source compound, and SiO2 respectively so that the chemical formula based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1- y Al y O5, and fully mix the raw materials to obtain mixed powder;

[0024] S2, pressing the mixed powder into a shape, and then subjecting the mixed powder to a solid phase reaction at 1000-2000° C. for 5-200 hours to obtain the dual-strategy co-doped rare earth orthosilicate fast scintillation material.

[0025] Furthermore, the carrier trap suppression type dopant source compound includes aluminum oxide and / or a compound containing an M element, and the compound containing an M element includes one or more of an oxide, a silicide, and a carbonate of the M element.

[0026] Furthermore, the competitive luminescence center type dopant source compound includes one or more of oxides, silicides, and carbonates of the N element.

[0027] Furthermore, in step S2, the temperature of the solid phase reaction is 1300-1600° C., and the time is 10-50 hours.

[0028] Furthermore, the dual-strategy co-doped rare earth orthosilicate fast scintillation material is a single crystal, and the preparation method further comprises the following steps:

[0029] S3, placing the material obtained in step S2 into a container, heating it to melt it, and slowly crystallizing the single crystal from the melt.

[0030] According to the third aspect of the present invention, there is provided the application of the dual-strategy co-doped rare earth orthosilicate fast scintillation material of any embodiment of the first aspect in any field including high energy physics, nuclear physics, space physics, nuclear medicine imaging diagnosis, industrial non-destructive testing, safety auditing, geology and mineral and oil well exploration, and environmental testing.

[0031] The above technical solution of the present invention has at least one of the following beneficial effects:

[0032] According to the dual-strategy co-doped rare earth orthosilicate fast scintillation material of the embodiment of the present invention, by combining a carrier trap suppression dopant element (aluminum and / or M element, M element selected from at least one of magnesium, calcium, and nickel) with a competing luminescence center dopant element (at least one of ytterbium, europium, praseodymium, and neodymium) to co-dope into the scintillation material, the scintillation decay time performance is significantly improved;

[0033] In some embodiments, by optimizing and adjusting the doping amounts of carrier trap suppression dopant elements and competing luminescence center dopant elements, for example, 0.001≤u≤0.005, 0.001≤v≤0.02, and 0.004≤w≤0.05, the scintillation decay time of the cerium-doped rare earth orthosilicate scintillating material can be reduced to below 30 ns.

[0034] In some embodiments, an M element such as Ca is added to a cerium-doped rare earth orthosilicate scintillating material. 2+ With Al 3+ Simultaneous doping, Ca 2+ Due to its large ionic radius and strong electron-withdrawing properties, it mainly occupies the RE1 site, Al 3+ Because of Si 4+ The close ionic radius and the Al-O bond are very similar to the Si-O bond, at least partially occupying the Si lattice site, thereby achieving the simultaneous doping of rare earth lattice sites and silicon lattice sites, making Ce 3+ The emission peak is blue-shifted and the broadening is reduced, the Ce1 content is greatly increased, and the luminescence decay time is significantly shortened; and due to the point defect Al Si ' and Ca Lu ' is formed at the same time, resulting in a large amount of Ce 3+ Transformed into stable Ce 4+ To maintain charge balance, thus bypassing Ce 3+ The initial hole capture process of emission further shortens the scintillation decay time;

[0035] The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to the present application can be well applied to any field including high-energy physics, nuclear physics, space physics, nuclear medicine imaging diagnosis, industrial non-destructive testing, safety audit, geology and mineral and oil well exploration, and environmental testing due to its extremely short scintillation decay time. BRIEF DESCRIPTION OF THE DRAWINGS

[0036] Figure 1 The X-ray diffraction patterns of LYSO:Ce single crystals co-doped with different doping amounts of Ca and Al;

[0037] Figure 2 This is the scintillation decay time spectrum of Ca co-doped YSO:Ce single crystal;

[0038] Figure 3 This is the scintillation decay time spectrum of Ca and Yb co-doped YSO:Ce single crystal;

[0039] Figure 4 is the scintillation decay time spectrum of Ca co-doped LYSO:Ce ceramics;

[0040] Figure 5 This is the scintillation decay time spectrum of Ca and Eu co-doped LYSO:Ce ceramics;

[0041] Figure 6 This is the scintillation decay time spectrum of Mg and Pr co-doped LYSO:Ce ceramics;

[0042] Figure 7 This is the scintillation decay time spectrum of Ni and Yb co-doped LYSO:Ce single crystal;

[0043] Figure 8 This is the scintillation decay time spectrum of Al and Yb co-doped LYSO:Ce ceramics;

[0044] Figure 9 This is the scintillation decay time spectrum of Al and Eu co-doped LYSO:Ce ceramics;

[0045] Figure 10 This is the scintillation decay time spectrum of Al and Nd co-doped LYSO:Ce ceramics;

[0046] Figure 11 This is the scintillation decay time spectrum of Al, Ca, and Yb co-doped LYSO:Ce single crystal. DETAILED DESCRIPTION

[0047] To make the objectives, technical solutions, and advantages of the embodiments of the present invention more clear, the technical solutions of the present invention will be clearly and completely described below in conjunction with the embodiments of the present invention. Obviously, the described embodiments are only some embodiments of the present invention, not all embodiments. Based on the described embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field are within the scope of protection of the present invention.

[0048] The following first describes the dual-strategy co-doped rare earth orthosilicate fast scintillation material according to an embodiment of the present application.

[0049] The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to the embodiment of the present application is a scintillation material co-doped with a carrier trap suppression type doping element and a competitive luminescence center type doping element. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y O5, wherein 0<u≤0.05, 0≤v≤0.1, 0<w≤0.1, 0≤y≤0.1, and v+y>0, RE represents a rare earth element, the rare earth element is selected from at least one of lanthanum, lutetium, yttrium, and gadolinium, the carrier trap suppression type doping element includes aluminum and / or M element, the M element is selected from at least one of magnesium, calcium, and nickel, N represents a competitive luminescence center type doping element, the competitive luminescence center type doping element is selected from at least one of ytterbium, europium, praseodymium, and neodymium.

[0050] According to the dual-strategy co-doped rare earth orthosilicate fast scintillation material of the present invention, by combining a carrier trap suppression dopant element (aluminum and / or M element, M element selected from at least one of magnesium, calcium, and nickel) with a competing luminescence center dopant element (at least one of ytterbium, europium, praseodymium, and neodymium) to co-dope the scintillating material, the scintillation decay time of the cerium-doped rare earth orthosilicate scintillating material can be reduced, and the scintillation decay time performance is significantly improved. Due to its fast scintillation decay performance characteristics, it can be better applied in high-energy physics, nuclear physics, space physics, nuclear medical imaging diagnosis, industrial non-destructive testing, safety auditing, geology, mineral and oil well exploration, and environmental monitoring.

[0051] In addition, the carrier trap suppression doping element in the dual-strategy co-doped rare earth orthosilicate fast scintillation material of the present application may include aluminum and M elements at the same time, wherein the aluminum element at least partially occupies the silicon lattice site.

[0052] Specifically, the rare earth orthosilicate scintillating material is doped with M element and aluminum at the same time, with Ca 2+ With Al 3+As an example, Figure 1 Shows Ca 2+ With Al 3+ The doping amount is 0.1% (based on the chemical formula of the ingredients is Lu 1.797 4Y 0.2 Ce 0.0006 Ca 0.002 Si 0.999 Al 0.001 O5 single crystal) and 0.3% (based on the chemical formula of the ingredients is Lu 1.7934 Y 0.2 Ce 0.0006 Ca 0.006 Si 0.997 Al 0.003 O5 single crystal) and the X-ray diffraction pattern of LYSO:Ce material (i.e., undoped Ca 2+ With Al 3+ ), doped only with Al 3+ And its doping amount is 0.6% (equivalent to the atomic percentage of Si, (based on the chemical formula of the ingredients is Lu 1.7994 Y 0.2 Ce 0.0006 Si 0.994 Al 0.006 O5 single crystal) X-ray diffraction pattern, and X-ray diffraction standard pattern. Figure 1 It can be seen that all the diffraction peaks recorded in the figure can be obtained by (Lu 1.81 Y 0.19 )SiO5 structure index (PDF#97-015-9308), and there is no impurity peak. In addition, compared with LYSO:Ce material, Al 3+ The doped X-ray diffraction peak shifts to a lower angle, indicating that doping increases the unit cell volume. 3+ Radius 56pm, rare earth RE 3+ Ionic radius>100pm, Si 4+ Radius 40pm, if Al 3+ Replace rare earth RE 3+ The lattice position will inevitably lead to a decrease in the unit cell volume, that is, the increase in the unit cell volume indicates that the Al 3 + Occupies the Si lattice site. Moreover, after Ca and Al co-doping, the diffraction peak further shifts to a smaller angle. This is related to the larger radius of Al 3+ , Ca 2+ Replace Lu respectively 3+ 、Si 4+ , and their synergistic effect further increases the unit cell volume. 2+ Due to its large ionic radius and strong electron-withdrawing properties, it mainly occupies the RE1 site, Al 3+Because of Si 4+ The close ionic radius and the Al-O bond are very similar to the Si-O bond, at least partially occupying the Si lattice site, thereby achieving the simultaneous doping of rare earth lattice sites and silicon lattice sites, making Ce 3+ The emission peak is blue-shifted and the broadening is reduced, and the Ce1 content is greatly increased, which significantly shortens the luminescence decay time; and due to the point defect Al Si ' and Ca Lu ' is formed at the same time, resulting in a large amount of Ce 3+ Transformed into stable Ce 4+ To maintain charge balance, thus bypassing Ce 3+ The initial hole capture process of emission further shortens the scintillation decay time.

[0053] And because Al 3+ After co-doping, some ions will occupy the Si lattice site, and the ion distance between the silicon site and the rare earth site Spacing between rare earth lattice ions Smaller, so Co-doping has a more significant effect on regulating the excited state lifetime of Ce luminescence centers. 3+ When the , M elements exist at the same time, there will be an obvious synergistic enhancement effect, which has better ability to control the flicker decay time.

[0054] Furthermore, the rare earth element is preferably lutetium or yttrium, or a solid solution of both; more preferably, a solid solution of both lutetium and yttrium, wherein the molar ratio of lutetium:yttrium is 9:1. By introducing Y, which is cheaper, has a lower melting point, and a larger ionic radius, into LSO:Ce crystals, and combining it with lutetium Lu at the aforementioned molar ratio to prepare a solid solution LYSO:Ce, this can lower the melting point, reduce costs (raw materials and electricity costs for single crystal growth), reduce defect levels, and optimize crystal performance.

[0055] The dual-strategy co-doped rare earth orthosilicate fast scintillation material and its preparation method of the present application are further explained below with reference to specific examples.

[0056] It should be noted that the concentrations of Ce, M, and N dopants in the following embodiments are the atomic ratios of the number of atoms of Ce, M, and N elements to the total number of atoms occupying rare earth sites in the chemical formula of the ingredients, and are calculated as follows:

[0057] The chemical formula is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y The Ce doping concentration C in the rare earth orthosilicate material of O5 Ce=2u / [2(1-uvw)+2u+2v+2w]×100at.%=100uat.%; Similarly, the doping concentration of M is C N =2v / [2(1-uvw)+2u+2v+2w]=100v at.%; similarly, the N doping concentration C N =2w / [2(1-uvw)+2u+2v+2w]=100wat.%.

[0058] In addition, the concentration of the Al dopant in the embodiment is designed according to the silicon sites occupied by the dopant. Therefore, the doping concentration of Al is the atomic ratio of the number of Al atoms to the total number of atoms occupying silicon sites in the chemical formula of the dopant, and is calculated as follows:

[0059] The chemical formula is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y The doping concentration of Al in rare earth orthosilicate materials of O5 Al =y / [(1-y)+y]×100at.%=100y at.%.

[0060] Example 1 (Preparation of Ca and Yb co-doped YSO:Ce material)

[0061] Non-transparent: Mix the ingredients in the molar ratio of Y2O3:CeO2:CaO:Yb2O3:SiO2=(0.999-vw):0.002:2v:w:1 (v=0.002, 0.004; w=0.01, 0.02, 0.03), mix them thoroughly, put the mixture into a corundum crucible, put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Yb 2w SiO5 polycrystalline powder.

[0062] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Yb 2w SiO5 transparent ceramics.

[0063] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressure, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding.2(0.999-v-w) Ce 0.002 Ca 2v Yb 2w SiO5 single crystal.

[0064] Table 1 Scintillation decay time of Ca and Yb co-doped YSO:Ce single crystals with different doping concentrations

[0065]

[0066] Figure 3 The scintillation decay time spectra of YSO:Ce, YSO:Ce, 0.2% Ca, 1.0% Yb, YSO:Ce, 0.4% Ca, 2.0% Yb, and YSO:Ce, 0.4% Ca, 3.0% Yb single crystals are shown, with the fitted decay times being 71.2ns, 27.2ns, 12.1ns, and 8.3ns, respectively. For comparison, single crystals doped with a single strategy, i.e., carrier trap suppression, were also prepared under the same process conditions, and the experimental results under the same experimental conditions are shown in Figure 2. Figure 2 shown. Figure 2 The scintillation decay time spectra of YSO:Ce, YSO:Ce, 0.2% Ca, YSO:Ce, 0.4% Ca, and YSO:Ce, 1.0% Ca single crystals are shown, and the fitted decay times are 71.2ns, 54.3ns, 39.2ns, and 38.9ns, respectively. Figure 2 Only the case of Ca doping up to 1.0at% is shown. This is because in the experiment, when more doping is added, the surface tension of the melt is significantly reduced, resulting in the inability to grow crystals smoothly (the crystal data of the Ca doping amount of 1.0at% is measured for the block solidified after cooling in the iridium crucible). Even if crystals are grown by chance, the significant difference between the ionic radius of Ca and Lu / Y will cause the crystals to be distorted, cracked and contain a large number of inclusions, which has no practical application value. This also means that in the case of single-strategy doping (doping with carrier defect suppression type doping elements), the improvement of the scintillation decay time reaches its limit when the doping amount reaches 1.0%. Figure 2 and Figure 3 It can be seen that although doping with only a single defect suppression element Ca can accelerate the decay time of YSO:Ce crystal to a certain extent, it is difficult to break the 30ns limit. Figure 3As shown in Table 1, without the introduction of carrier trapping and competing luminescence center dopants (i.e., YSO:Ce), the flicker decay time is 71.2ns. By simultaneously introducing these two doping elements, the flicker decay time is improved. By adjusting the appropriate component ratio, the decay time can be further improved relative to YSO:Ce with increasing Ca and Yb doping levels. Further analysis shows that co-doping with higher levels of Ca (≥0.2%, i.e., v ≥ 0.002) and Yb (≥1.0%, i.e., w ≥ 0.01) significantly accelerates the decay time (below 30ns).

[0067] Example 2 (Preparation of Ca and Eu co-doped YSO:Ce material)

[0068] Non-transparent: Mix the ingredients in the molar ratio of Y2O3:CeO2:CaO:Eu2O3:SiO2=(0.999-vw):0.002:2v:w:1 (v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05). After mixing thoroughly, put the powder mixture into a corundum crucible and place it in a muffle furnace. Calcinate at 1600℃ for 10h to cause solid phase reaction to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Eu 2w SiO5 polycrystalline powder.

[0069] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Eu 2w SiO5 transparent ceramics.

[0070] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressure, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.999-v-w) Ce 0.002 Ca 2v Eu 2w SiO5 single crystal.

[0071] Table 2 Scintillation decay time of Ca and Eu co-doped YSO:Ce ceramics with different doping concentrations

[0072]

[0073] Combined with Table 2, it can be seen that by adjusting the appropriate component ratio, the decay time can be further improved relative to YSO:Ce with increasing Ca and Eu doping amounts; further analysis shows that higher (≥0.2%, i.e. v ≥ 0.002) Ca and (≥0.8%, i.e. w ≥ 0.008) Eu co-doping will significantly accelerate the decay time (below 30ns).

[0074] Example 3 (Growth of Ca and Pr Co-doped YSO:Ce Scintillating Material)

[0075] The single crystal was grown by the Czochralski method.

[0076] Non-transparent: Molar ratio of Y2O3:CeO2:CaO:Pr6O 11 :SiO2=(0.999-vw):0.002:2v:w / 3:1(v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Pr 2w SiO5 polycrystalline powder.

[0077] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Pr 2w SiO5 transparent ceramics.

[0078] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressure, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.999-v-w) Ce 0.002 Ca 2v Pr 2w SiO5 single crystal.

[0079] Table 3 Scintillation decay time of Ca and Pr co-doped YSO:Ce ceramics with different doping concentrations

[0080]

[0081] Combined with Table 3, it can be seen that by adjusting the appropriate component ratio, the decay time can be further improved relative to YSO:Ce with increasing Ca and Pr doping levels; further analysis shows that higher (≥0.2%, i.e. v ≥ 0.002) Ca and (≥0.8%, i.e. w ≥ 0.008) Pr co-doping will significantly accelerate the decay time (below 30ns).

[0082] Example 4 (Preparation of Ca and Nd co-doped YSO:Ce material)

[0083] Non-transparent: Mix the ingredients in the molar ratio of Y2O3:CeO2:CaO:Nd2O3:SiO2=(0.999-vw):0.002:2v:w:1 (v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05). After mixing thoroughly, put the powder mixture into a corundum crucible and place it in a muffle furnace. Calcinate at 1600℃ for 10h to cause solid phase reaction to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Nd 2w SiO5 polycrystalline powder.

[0084] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Y 2(0.999-v-w) Ce 0.002 Ca 2v Nd 2w SiO5 transparent ceramics.

[0085] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressure, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.999-v-w) Ce 0.002 Ca 2v Nd 2w SiO5 single crystal.

[0086] Table 4 Scintillation decay time of Ca and Nd co-doped YSO:Ce ceramics with different doping concentrations

[0087]

[0088] Combined with Table 4, it can be seen that with the increase of Ca and Nd doping amounts, the decay time can be continuously improved relative to YSO:Ce; when the doping concentration reaches (≥0.2%, i.e. v ≥ 0.002) Ca and (≥0.8%, i.e. w ≥ 0.008) Nd co-doping, the decay time is greatly accelerated and is less than 30ns.

[0089] Example 5 (Preparation of Ca and Yb co-doped LYSO:Ce scintillating material)

[0090] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Yb2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.001, 0.002, 0.003, 0.004; w=0.002, 0.004, 0.006, 0.02, 0.05), mix the ingredients thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace, and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb 2w SiO5 polycrystalline powder.

[0091] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb 2w SiO5 transparent ceramics.

[0092] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb 2w SiO5 single crystal.

[0093] Table 5 Scintillation decay time of Ca and Yb co-doped LYSO:Ce ceramics with different doping concentrations

[0094]

[0095] Table 5 shows that, compared to LYSO:Ce scintillating material, co-doping with lower doping concentrations (0.1%, i.e., v ≥ 0.001) of Ca and (0.2%, i.e., w = 0.002) of Yb can significantly accelerate decay time (below 30ns). Furthermore, as the Ca and Yb doping levels increase, the decay time can be further improved relative to LYSO:Ce.

[0096] Example 6 (Preparation of Ca and Eu co-doped LYSO:Ce scintillating material)

[0097] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Eu2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.002, 0.004; w=0.002, 0.004, 0.006, 0.02, 0.05). After mixing thoroughly, put the powder mixture into a corundum crucible and place it in a muffle furnace. Calcinate at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w SiO5 polycrystalline powder.

[0098] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w SiO5 transparent ceramics.

[0099] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w SiO5 single crystal.

[0100] Table 6 Scintillation decay time of Ca and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0101]

[0102] Figure 5 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.2% Ca, 0.2% Eu, LYSO:Ce, 0.2% Ca, 0.4% Eu, LYSO:Ce, 0.4% Ca, 0.6% Eu, LYSO:Ce, 0.4% Ca, 2.0% Eu, and LYSO:Ce, 0.4% Ca, 5.0% Eu ceramics are shown, and the fitted decay times are 42.3ns, 28.5ns, 17.2ns, 13.5ns, 9.3ns, and 6.9ns, respectively. For comparison, ceramics with a single strategy, i.e., carrier trap suppression doping, were also prepared under the same process conditions, and the experimental results under the same experimental conditions are shown in Figure 2. Figure 4 shown. Figure 4 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.2%Ca, LYSO:Ce, 0.4%Ca, and LYSO:Ce, 1.0%Ca ceramics are shown, and the fitted decay times are 42.3ns, 34.5ns, 32.3ns, and 31.8ns, respectively. Figure 4 Only the case where the Ca doping amount reaches 1.0 at% is shown, which is the same as the above-mentioned embodiment 1. Figure 4 and Figure 5 It can be seen that although doping with only a single defect suppression element Ca can accelerate the decay time of LYSO:Ce ceramics to a certain extent, it is difficult to break the 30ns limit. Figure 5 As shown in Table 6, Ca and Eu co-doping improves the flicker decay time compared to LYSO:Ce ceramics. Co-doping with (≥0.2%) Ca and (≥0.2%) Eu significantly accelerates the decay time (below 30ns). Furthermore, as the Ca and Eu doping levels increase, the decay time significantly improves compared to LYSO:Ce.

[0103] Example 7 (Growth of Ca and Pr Co-doped LYSO:Ce Scintillating Material)

[0104] The single crystal was grown by the Czochralski method.

[0105] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:CaO:Pr6O 11 :SiO2=(0.899-vw):0.1:0.002:2v:w / 3:1(v=0.001、0.002、0.003、0.004;w=0.003、0.005、0.007、0.02、0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w SiO5 polycrystalline powder.

[0106] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w SiO5 transparent ceramics.

[0107] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w SiO5 single crystal.

[0108] Table 7 Scintillation decay time of Ca and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0109]

[0110] As shown in Table 7, co-doping with Ca and Pr can further improve the decay time compared to LYSO:Ce. Co-doping with (≥0.1%) Ca and (≥0.3%) Pr can significantly accelerate the decay time (below 30ns). Furthermore, the decay time improves further with increasing Ca and Pr doping levels.

[0111] Example 8 (Preparation of Ca and Nd co-doped LYSO:Ce scintillating material)

[0112] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Nd2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.001, 0.002, 0.003, 0.004; w=0.002, 0.004, 0.006, 0.02, 0.05). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid-phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w SiO5 polycrystalline powder.

[0113] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w SiO5 transparent ceramics.

[0114] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w SiO5 single crystal.

[0115] Table 8 Scintillation decay time of Ca and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0116]

[0117] As shown in Table 8, co-doping with Ca and Nd can improve the decay time compared to LYSO:Ce. Co-doping with (≥0.1%) Ca and (≥0.2%) Nd can significantly accelerate the decay time (below 30ns). The decay time further improves with increasing Ca and Nd doping levels.

[0118] Example 9 (Preparation of Mg and Yb co-doped LYSO:Ce scintillating material)

[0119] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Yb2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.001, 0.002, 0.003, 0.005, 0.01; w=0.002, 0.004, 0.006, 0.015, 0.02, 0.05), mix the ingredients thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace, and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w SiO5 polycrystalline powder.

[0120] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w SiO5 transparent ceramics.

[0121] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w SiO5 single crystal.

[0122] Table 9 Scintillation decay time of LYSO:Ce ceramics with different doping concentrations of Mg and Yb

[0123]

[0124] As shown in Table 9, compared to LYSO:Ce scintillating materials, a lower doping concentration (0.1%) of Mg and (0.2%, i.e., w = 0.001) of Yb can significantly accelerate the decay time (below 30ns). Furthermore, the decay time can be further improved with increasing Mg and Yb doping levels.

[0125] Example 10 (Preparation of Mg and Eu co-doped LYSO:Ce scintillating material)

[0126] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Eu2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.001, 0.002, 0.003, 0.005, 0.01; w=0.001, 0.002, 0.003, 0.02, 0.05), mix the ingredients thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace, and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w SiO5 polycrystalline powder.

[0127] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w SiO5 transparent ceramics.

[0128] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w SiO5 single crystal.

[0129] Table 10 Scintillation decay time of LYSO:Ce ceramics with different doping concentrations of Mg and Eu

[0130]

[0131]

[0132] As shown in Table 10, compared to LYSO:Ce scintillating material, a lower doping concentration (0.1%) of Mg and (0.1%) of Eu can significantly accelerate the decay time (below 30ns). With increasing Mg and Eu doping levels, the decay time is further improved relative to LYSO:Ce.

[0133] Example 11 (Growth of Mg and Pr Co-doped LYSO:Ce Scintillating Material)

[0134] The single crystal was grown by the Czochralski method.

[0135] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:MgO:Pr6O 11 :SiO2=(0.899-vw):0.1:0.002:2v:w / 3:1(v=0.001、0.002、0.003、0.005、0.01;w=0.003、0.005、0.006、0.02、0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2w SiO5 polycrystalline powder.

[0136] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2wSiO5 transparent ceramics.

[0137] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2w SiO5 single crystal.

[0138] Table 11 Scintillation decay time of LYSO:Ce ceramics with different doping concentrations of Mg and Pr

[0139]

[0140] Figure 6 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.1% Mg, 0.3% Pr, LYSO:Ce, 0.2% Mg, 0.5% Pr, LYSO:Ce, 0.3% Mg, 0.6% Pr, LYSO:Ce, 0.5% Mg, 2.0% Pr, and LYSO:Ce, 1.0% Mg, 5.0% Pr ceramics are shown, and the fitted decay times are 42.3ns, 26.7ns, 18.5ns, 13.7ns, 9.5ns, and 6.4ns, respectively. Figure 6 As shown in Table 11, Mg and Pr co-doping improves the scintillation time relative to LYSO:Ce ceramics. Co-doping with (≥0.1%) Mg and (≥0.3%) Pr significantly accelerates the decay time (below 30ns). Furthermore, increasing the Mg and Pr doping levels further improves the decay time relative to LYSO:Ce ceramics.

[0141] Example 12 (Preparation of Mg and Nd co-doped LYSO:Ce scintillating material)

[0142] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Nd2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.001, 0.002, 0.003, 0.005, 0.01; w=0.002, 0.004, 0.006, 0.02, 0.05), mix the ingredients thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace, and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w SiO5 polycrystalline powder.

[0143] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w SiO5 transparent ceramics.

[0144] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w SiO5 single crystal.

[0145] Table 12 Scintillation decay time of LYSO:Ce ceramics with different doping concentrations of Mg and Nd

[0146]

[0147] Table 12 shows that, compared to LYSO:Ce scintillating material, a lower doping concentration (0.1%) of Mg and 0.2%, or w = 0.001%, of Nd can significantly accelerate decay time (below 30ns). Furthermore, increasing the Mg and Nd doping levels further improves decay time relative to LYSO:Ce.

[0148] Example 13 (Preparation of Ni and Yb co-doped LYSO:Ce scintillating material)

[0149] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Yb2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.002, 0.003, 0.006; w=0.004, 0.006, 0.015). After mixing thoroughly, put the powder mixture into a corundum crucible and place it in a muffle furnace. Calcinate at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w SiO5 polycrystalline powder.

[0150] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w SiO5 transparent ceramics.

[0151] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w SiO5 single crystal.

[0152] Table 13 Scintillation decay time of Ni and Yb co-doped LYSO:Ce single crystals with different doping concentrations

[0153]

[0154] Figure 7 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.2% Ni, 0.4% Yb, LYSO:Ce, 0.3% Ni, 0.6% Yb, and LYSO:Ce, 0.6% Ni, 1.5% Yb single crystals are shown, and the fitted decay times are 42.3ns, 19.7ns, 15.3ns, and 9.8ns, respectively. Figure 7 As shown in Table 13, Ni and Yb co-doping improves the scintillation decay time compared to LYSO:Ce single crystals. Co-doping with (≥0.2%) Ni and (≥0.4%) Yb significantly accelerates the decay time (below 30ns). Furthermore, as the Ni and Yb doping levels increase, the decay time significantly improves compared to LYSO:Ce.

[0155] Example 14 (Preparation of Ni and Eu co-doped LYSO:Ce scintillating material)

[0156] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Eu2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1(v=0.001、0.002、0.003、0.01、0.02;w=0.001、0.002、0.003、0.02、0.05), mix the ingredients thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w SiO5 polycrystalline powder.

[0157] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w SiO5 transparent ceramics.

[0158] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w SiO5 single crystal.

[0159] Table 14 Scintillation decay time of Ni and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0160]

[0161] As shown in Table 14, compared to LYSO:Ce ceramics, even with a relatively low doping concentration (0.1%) of Ni and (0.1%) of Eu, the decay time can be significantly accelerated (below 30ns). Furthermore, as the Ni and Eu doping levels increase, the decay time can be further improved relative to LYSO:Ce.

[0162] Example 15 (Growth of Ni and Pr Co-doped LYSO:Ce Scintillating Material)

[0163] The single crystal was grown by the Czochralski method.

[0164] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:NiO:Pr6O 11 :SiO2=(0.899-vw):0.1:0.002:2v:w / 3:1(v=0.001、0.002、0.003、0.006、0.01、0.02;w=0.003、0.005、0.007、0.01、0.02、0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w SiO5 polycrystalline powder.

[0165] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w SiO5 transparent ceramics.

[0166] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w SiO5 single crystal.

[0167] Table 15 Scintillation decay time of Ni and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0168]

[0169]

[0170] As shown in Table 15, Ni and Pr co-doping can improve the decay time relative to LYSO:Ce. Co-doping with (≥0.1%) Ni and (≥0.3%) Pr can significantly accelerate the decay time (below 30ns). Furthermore, increasing the Ni and Pr doping levels further improves the decay time relative to LYSO:Ce.

[0171] Example 16 (Preparation of Ni and Nd co-doped LYSO:Ce scintillating material)

[0172] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Nd2O3:SiO2=(0.899-vw):0.1:0.002:2v:w:1 (v=0.002, 0.003, 0.01, 0.02; w=0.004, 0.006, 0.02, 0.05). After mixing thoroughly, put the powder mixture into a corundum crucible and put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w SiO5 polycrystalline powder.

[0173] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w SiO5 transparent ceramics.

[0174] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w SiO5 single crystal.

[0175] Table 16 Scintillation decay time of Ni and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0176]

[0177] Combined with Table 16, it can be seen that Ni and Nd co-doping can improve the decay time compared to LYSO:Ce. Co-doping with (≥0.2%) Ni and (≥0.4%) Nd can significantly accelerate the decay time (below 30ns). Furthermore, as the Ni and Nd doping levels increase, the decay time can be significantly improved compared to LYSO:Ce.

[0178] Example 17 (Preparation of Al and Yb Co-doped LYSO:Ce Scintillating Material)

[0179] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:Yb2O3:SiO2:Al2O3=(0.899-w):0.1:0.002:w:(1-y):y / 2 (y=0.003, 0.006, 0.01, 0.02; w=0.005, 0.01, 0.02, 0.05). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Yb 2w Si 1-y Al y O5 polycrystalline powder.

[0180] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Yb 2w Si 1-y Al y O5 transparent ceramic.

[0181] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-w) Y 0.2 Ce 0.002 Yb 2w Si 1-y Al y O5 single crystal.

[0182] Table 17 Scintillation decay time of Al and Yb co-doped LYSO:Ce ceramics with different doping concentrations

[0183]

[0184] Figure 8 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.3%Al, 0.5%Yb, LYSO:Ce, 0.6%Al, 0.5%Yb, LYSO:Ce, 0.6%Al, 1.0%Yb, LYSO:Ce, 1.0%Al, 2.0%Yb, and LYSO:Ce, 2.0%Al, 5.0%Yb ceramics are shown, and the fitted decay times are 42.3ns, 22.6ns, 19.2ns, 17.8ns, 7.7ns, and 3.6ns, respectively. Figure 8As shown in Table 17, Al and Yb co-doping improves the scintillation decay time compared to LYSO:Ce ceramics. Co-doping with (≥0.3%) Al and (≥0.5%) Yb significantly accelerates the decay time (below 30ns). Furthermore, as the Al and Yb doping levels increase, the decay time significantly improves compared to LYSO:Ce.

[0185] Example 18 (Preparation of Al and Eu co-doped LYSO:Ce scintillating material)

[0186] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:Eu2O3:SiO2:Al2O3=(0.899-w):0.1:0.002:w:(1-y):y / 2 (y=0.006, 0.01, 0.02; w=0.002, 0.004, 0.006, 0.02, 0.05), mix them thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace, and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Eu 2w Si 1-y Al y O5 polycrystalline powder.

[0187] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Eu 2w Si 1-y Al y O5 transparent ceramic.

[0188] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-w) Y 0.2 Ce 0.002 Eu 2w Si 1-y Al y O5 single crystal.

[0189] Table 18 Scintillation decay time of Al and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0190]

[0191] Figure 9 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.6%Al, 0.2%Eu, LYSO:Ce, 0.6%Al, 0.4%Eu, LYSO:Ce, 1.0%Al, 0.6%Eu, LYSO:Ce, 1.0%Al, 2.0%Eu, and LYSO:Ce, 2.0%Al, 5.0%Eu ceramics are shown, and the fitted decay times are 42.3ns, 21.3ns, 18.0ns, 16.6ns, 9.9ns, and 6.7ns, respectively. Figure 9 As shown in Table 18, Al and Eu co-doping improves the flicker decay time compared to LYSO:Ce ceramics. Co-doping with (≥0.6%) Al and (≥0.2%) Eu significantly accelerates the decay time (below 30ns). Furthermore, as the Al and Eu doping levels increase, the decay time significantly improves compared to LYSO:Ce.

[0192] Example 19 (Growth of Al and Pr Co-doped LYSO:Ce Scintillating Material)

[0193] The single crystal was grown by the Czochralski method.

[0194] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:Pr6O 11 :SiO2:Al2O3=(0.899-w):0.1:0.002:w / 3:(1-y):y / 2(y=0.001、0.002、0.003、0.01、0.02;w=0.003、0.005、0.007、0.02、0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Pr 2w Si 1-y Al y O5 polycrystalline powder.

[0195] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Pr 2w Si 1-y Al y O5 transparent ceramic.

[0196] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-w) Y 0.2 Ce 0.002 Pr 2w Si 1-y Al y O5 single crystal.

[0197] Table 19 Scintillation decay time of Al and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0198]

[0199] As shown in Table 19, Al and Pr co-doping can improve decay time relative to LYSO:Ce. Co-doping with (≥0.1%) Al and (≥0.3%) Pr can significantly accelerate decay time (below 30ns). Furthermore, increasing the Al and Pr doping levels further improves decay time relative to LYSO:Ce.

[0200] Example 20 (Preparation of Al and Nd Co-doped LYSO:Ce Scintillating Material)

[0201] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:Nd2O3:SiO2:Al2O3=(0.899-w):0.1:0.002:w:(1-y):y / 2 (y=0.003, 0.006, 0.01, 0.02; w=0.002, 0.004, 0.006, 0.02, 0.05). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Nd 2w Si 1-y Al y O5 polycrystalline powder.

[0202] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-w) Y 0.2 Ce 0.002 Nd 2w Si 1-y Al y O5 transparent ceramic.

[0203] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-w) Y 0.2 Ce 0.002 Nd 2w Si 1-y Al y O5 single crystal.

[0204] Table 20 Scintillation decay time of Al and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0205]

[0206]

[0207] Figure 10 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.3%Al, 0.2%Nd, LYSO:Ce, 0.3%Al, 0.4%Nd, LYSO:Ce, 0.6%Al, 0.6%Nd, LYSO:Ce, 1.0%Al, 2.0%Nd, and LYSO:Ce, 2.0%Al, 5.0%Nd ceramics are shown, and the fitted decay times are 42.3ns, 28.9ns, 19.7ns, 12.4ns, 9.5ns, and 4.8ns, respectively. Figure 10 As shown in Table 20, Al and Nd co-doping improves the scintillation decay time compared to LYSO:Ce ceramics. Co-doping with (≥0.3%) Al and (≥0.2%) Nd significantly accelerates the decay time (below 30ns). Furthermore, as the Al and Nd doping levels increase, the decay time significantly improves compared to LYSO:Ce.

[0208] Example 21 (Preparation of Al, Ca, and Yb Co-doped LYSO:Ce Scintillating Material)

[0209] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Yb2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.001, 0.002; w=0.001, 0.005, 0.01). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb2w Si 1-y Al y O5 polycrystalline powder.

[0210] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb 2w Si 1-y Al y O5 transparent ceramic.

[0211] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Yb 2w Si 1-y Al y O5 single crystal.

[0212] Table 21 Scintillation decay time of Al, Ca, and Yb co-doped LYSO:Ce crystals with different doping concentrations

[0213]

[0214] Figure 11 The scintillation decay time spectra of LYSO:Ce, LYSO:Ce, 0.3% Al, 0.1% Ca, 0.1% Yb, LYSO:Ce, 0.3% Al, 0.1% Ca, 0.5% Yb, LYSO:Ce, 0.6% Al, 0.2% Ca, 1.0% Yb crystals are shown, and the fitted decay times are 42.3ns, 24.4ns, 13.8ns, and 7.2ns, respectively. Figure 11 As shown in Table 21, co-doping with Al, Ca, and Yb improves the scintillation decay time relative to LYSO:Ce crystals. Co-doping with (≥0.3%) Al, (≥0.1%) Ca, and (≥0.1%) Yb significantly accelerates the decay time (below 30ns). Furthermore, as the doping levels of Al, Ca, and Yb increase, the decay time significantly improves relative to LYSO:Ce.

[0215] Example 22 (Preparation of Al, Ca, and Yb Co-doped LYSO:Ce Scintillating Material)

[0216] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Yb2O3:SiO2:Al2O3=(0.9-uvw):0.1:2u:2v:w:(1-y):y / 2 (u=0.001, 0.002, 0.003, 0.004, 0.005; y=0.003; v=0.001; w=0.001). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid-phase reaction to obtain Lu 2(0.9-u-v-w) Y 0.2 Ce 2u Ca 2v Yb 2w Si 1-y Al y O5 polycrystalline powder.

[0217] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.9-u-v-w) Y 0.2 Ce 2u Ca 2v Yb 2w Si 1-y Al y O5 transparent ceramic.

[0218] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.9-u-v-w) Y 0.2 Ce 2u Ca 2v Yb 2w Si 1-y Al y O5 single crystal.

[0219] Table 22 Scintillation decay time of Al, Ca, and Yb co-doped LYSO:Ce crystals with different Ce doping concentrations

[0220]

[0221] Combined with Table 22, it can be seen that when the concentrations of defect suppression elements Al and Ca and the concentration of competing luminescence center Yb remain unchanged, the effect of accelerating the flicker decay time by only changing the Ce concentration is relatively limited, and there is a similar improvement effect in the concentration range of 0.1%-0.5%.

[0222] Example 23 (Preparation of Al, Ca, and Eu Co-doped LYSO:Ce Ceramics)

[0223] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Eu2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05). After mixing thoroughly, put the powder mixture into a corundum crucible and put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w Si 1-y Al y O5 polycrystalline powder.

[0224] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w Si 1-y Al y O5 transparent ceramic.

[0225] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Eu 2w Si 1-y Al y O5 single crystal.

[0226] Table 23 Scintillation decay time of Al, Ca, and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0227]

[0228] Example 24 (Growth of Al, Ca, and Pr Co-doped LYSO:Ce Scintillating Material)

[0229] The single crystal was grown by the Czochralski method.

[0230] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:CaO:Pr6O11 :SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w / 3:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w Si 1-y Al y O5 polycrystalline powder.

[0231] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w Si 1-y Al y O5 transparent ceramic.

[0232] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Pr 2w Si 1-y Al y O5 single crystal.

[0233] Table 24 Scintillation decay time of Al, Ca, and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0234]

[0235] Example 25 (Preparation of Al, Ca, and Nd Co-doped LYSO:Ce Scintillating Material)

[0236] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:CaO:Nd2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.004; w=0.008, 0.01, 0.02, 0.05). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w Si 1-y Al y O5 polycrystalline powder.

[0237] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w Si 1-y Al y O5 transparent ceramic.

[0238] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ca 2v Nd 2w Si 1-y Al y O5 single crystal.

[0239] Table 25 Scintillation decay time of Al, Ca, and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0240]

[0241] Example 26 (Preparation of Al, Mg, and Yb Co-doped LYSO:Ce Scintillating Material)

[0242] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Yb2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.005; w=0.004, 0.006, 0.015, 0.02). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w Si 1-y Al y O5 polycrystalline powder.

[0243] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w Si 1-y Al y O5 transparent ceramic.

[0244] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Yb 2w Si 1-y Al y O5 single crystal.

[0245] Table 26 Scintillation decay time of Al, Mg, and Yb co-doped LYSO:Ce ceramics with different doping concentrations

[0246]

[0247] Example 27 (Preparation of Al, Mg, and Eu Co-doped LYSO:Ce Scintillating Material)

[0248] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Eu2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.005, 0.01; w=0.002, 0.003, 0.02) and mix them thoroughly. Then, put the powder mixture into a corundum crucible and put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w Si 1-y Al y O5 polycrystalline powder.

[0249] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w Si 1-y Al y O5 transparent ceramic.

[0250] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Eu 2w Si 1-y Al y O5 single crystal.

[0251] Table 27 Scintillation decay time of Al, Mg, and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0252]

[0253] Example 28 (Growth of Al, Mg, and Pr Co-doped LYSO:Ce Scintillating Material)

[0254] The single crystal was grown by the Czochralski method.

[0255] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:MgO:Pr6O 11:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w / 3:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.005, 0.01; w=0.005, 0.006, 0.02) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2w Si 1-y Al y O5 polycrystalline powder.

[0256] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2w Si 1-y Al y O5 transparent ceramic.

[0257] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Pr 2w Si 1-y Al y O5 single crystal.

[0258] Table 28 Scintillation decay time of Al, Mg, and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0259]

[0260] Example 29 (Preparation of Al, Mg, and Nd Co-doped LYSO:Ce Scintillating Material)

[0261] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:MgO:Nd2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.005, 0.01; w=0.004, 0.006, 0.02). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w Si 1-y Al y O5 polycrystalline powder.

[0262] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w Si 1-y Al y O5 transparent ceramic.

[0263] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Mg 2v Nd 2w Si 1-y Al y O5 single crystal.

[0264] Table 29 Scintillation decay time of Al, Mg, and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0265]

[0266] Example 30 (Preparation of Al, Ni, and Yb Co-doped LYSO:Ce Scintillating Material)

[0267] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Yb2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.006; w=0.004, 0.006, 0.015, 0.02). After mixing thoroughly, the powder mixture is placed in a corundum crucible and placed in a muffle furnace and calcined at 1600°C for 10 hours to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w Si 1-y Al y O5 polycrystalline powder.

[0268] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w Si 1-y Al y O5 transparent ceramic.

[0269] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Yb 2w Si 1-y Al y O5 single crystal.

[0270] Table 30 Scintillation decay time of Al, Ni, and Yb co-doped LYSO:Ce ceramics with different doping concentrations

[0271]

[0272] Example 31 (Preparation of Al, Ni, and Eu Co-doped LYSO:Ce Scintillating Material)

[0273] Non-transparent: Mix the ingredients in the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Eu2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.01, 0.02; w=0.002, 0.003, 0.02) and mix them thoroughly. Then, put the powder mixture into a corundum crucible and put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w Si 1-y Al y O5 polycrystalline powder.

[0274] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w Si 1-y Al y O5 transparent ceramic.

[0275] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Eu 2w Si 1-y Al y O5 single crystal.

[0276] Table 31 Scintillation decay time of Al, Ni, and Eu co-doped LYSO:Ce ceramics with different doping concentrations

[0277]

[0278] Example 32 (Growth of Al, Ni, and Pr Co-doped LYSO:Ce Scintillating Material)

[0279] The single crystal was grown by the Czochralski method.

[0280] Non-transparent: Molar ratio Lu2O3:Y2O3:CeO2:NiO:Pr6O 11:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w / 3:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.006, 0.01; w=0.005, 0.007, 0.01, 0.02) were prepared and mixed thoroughly. The powder mixture was placed in a corundum crucible and placed in a muffle furnace and calcined at 1600℃ for 10h to cause solid phase reaction to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w Si 1-y Al y O5 polycrystalline powder.

[0281] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w Si 1-y Al y O5 transparent ceramic.

[0282] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Pr 2w Si 1-y Al y O5 single crystal.

[0283] Table 32 Scintillation decay time of Al, Ni, and Pr co-doped LYSO:Ce ceramics with different doping concentrations

[0284]

[0285] Example 33 (Preparation of Al, Ni, and Nd Co-doped LYSO:Ce Scintillating Material)

[0286] Non-transparent: According to the molar ratio of Lu2O3:Y2O3:CeO2:NiO:Nd2O3:SiO2:Al2O3=(0.899-vw):0.1:0.002:2v:w:(1-y):y / 2(y=0.003, 0.006; v=0.002, 0.003, 0.01, 0.02; w=0.004, 0.006, 0.02,) prepare the ingredients, mix them thoroughly, put the powder mixture into a corundum crucible, put it into a muffle furnace and calcine it at 1600℃ for 10h to cause solid phase reaction, and obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w Si 1-y Al y O5 polycrystalline powder.

[0287] Transparent: Mix the ingredients according to the above molar ratio, mix them thoroughly, press the mixture into blocks under 5000MPa cold isostatic pressing, and allow solid phase reaction to occur in a vacuum hot press to remove bubbles and voids as much as possible to obtain Lu 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w Si 1-y Al y O5 transparent ceramic.

[0288] Single crystal: The mixture is pressed into a block under 2500MPa cold isostatic pressing, placed in an iridium crucible, heated by induction and fully melted, and then slowly pulled from the melt to grow a single crystal of a preset size after seeding. 2(0.899-v-w) Y 0.2 Ce 0.002 Ni 2v Nd 2w Si 1-y Al y O5 single crystal.

[0289] Table 33 Scintillation decay time of Al, Ni and Nd co-doped LYSO:Ce ceramics with different doping concentrations

[0290]

[0291] Through the above embodiments, combined with different compositions and different processes, the dual-strategy co-doped rare earth orthosilicate fast scintillation material of the present application was prepared.

[0292] It should be noted that, in the above embodiments, only the performance conclusions of the ceramics or single crystals of some compositions of Examples 1 to 22 are recorded. In fact, the ceramics or single crystals obtained in the embodiments with other components and other processes all have results consistent with the conclusions of Examples 1 to 22, and their redundant description is omitted here.

[0293] The above is a preferred embodiment of the present invention. It should be pointed out that for ordinary technicians in this technical field, several improvements and modifications can be made without departing from the principles of the present invention. These improvements and modifications should also be regarded as within the scope of protection of the present invention.

Claims

1. A dual-strategy co-doped rare earth orthosilicate fast scintillation material, characterized in that: The dual-strategy co-doped rare earth orthosilicate fast scintillation material is a scintillation material co-doped with a carrier trap suppression type doping element and a competitive luminescence center type doping element. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y O5, where 0<u≤0.05, 0≤v≤0.1, 0<w≤0.1, 0≤y≤0.1, and v+y>0, The RE represents a rare earth element, and the rare earth element is at least one selected from lanthanum, lutetium, yttrium, and gadolinium. The carrier trap suppression doping element includes aluminum and / or M element, and the M element is selected from at least one of magnesium, calcium, and nickel. The N represents a competitive luminescence center type doping element, and the competitive luminescence center type doping element is selected from at least one of ytterbium, europium, praseodymium, and neodymium.

2. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to claim 1, characterized in that: The carrier trap suppression doping element includes aluminum and M elements, wherein the aluminum element at least partially occupies silicon sites.

3. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to claim 1, characterized in that: The rare earth element is yttrium or a solid solution of lutetium and yttrium.

4. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to claim 1, characterized in that: The rare earth element is a solid solution of lutetium and yttrium, wherein the molar ratio of lutetium to yttrium is 9:

1.

5. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to claim 1, characterized in that: 0.001≤u≤0.005, 0.001≤v≤0.02, 0.004≤w≤0.

05.

6. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to claim 5, characterized in that: 0.003≤y≤0.02。 7. The dual-strategy co-doped rare earth orthosilicate fast scintillation material according to any one of claims 1 to 6, characterized in that: The scintillation light decay time of the dual-strategy co-doped rare earth orthosilicate fast scintillation material is less than 30ns.

8. A method for preparing a dual-strategy co-doped rare earth orthosilicate fast scintillation material, characterized in that: The dual-strategy co-doped rare earth orthosilicate fast scintillation material is a scintillation material co-doped with a carrier trap suppression type doping element and a competitive luminescence center type doping element. The chemical formula of the dual-strategy co-doped rare earth orthosilicate fast scintillation material based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y O5, where 0<u≤0.05, 0≤v≤0.1, 0<w≤0.1, 0≤y≤0.1, and v+y>0, The RE represents a rare earth element, and the rare earth element is at least one selected from lanthanum, lutetium, yttrium, and gadolinium. The carrier trap suppression doping element includes aluminum and / or M element, and the M element is selected from at least one of magnesium, calcium, and nickel. The N represents a competitive luminescence center type doping element, and the competitive luminescence center type doping element is selected from at least one of ytterbium, europium, praseodymium, and neodymium. The preparation method comprises the following steps: S1, weigh the RE source compound, Ce source compound, carrier trap suppression type dopant source compound, competitive luminescence center type dopant source compound, and SiO2 respectively so that the chemical formula based on the raw material ratio is RE 2(1-u-v-w) Ce 2u M 2v N 2w Si 1-y Al y O5, and fully mix the raw materials to obtain mixed powder; S2, pressing the mixed powder into a shape, and then subjecting the mixed powder to a solid phase reaction at 1000-2000° C. for 5-200 hours to obtain the dual-strategy co-doped rare earth orthosilicate fast scintillation material.

9. The preparation method according to claim 8, characterized in that The carrier trap suppression type dopant source compound includes aluminum oxide and / or a compound containing an M element. The compound containing an M element includes one or more of an oxide, a silicide, and a carbonate of the M element.

10. The preparation method according to claim 8, characterized in that The competitive luminescence center type dopant source compound includes one or more of oxides, silicides, and carbonates of the N element.

11. The preparation method according to claim 8, characterized in that In step S2, the temperature of the solid phase reaction is 1300-1600° C., and the time is 10-50 hours.

12. The preparation method according to claim 8, characterized in that The dual-strategy co-doped rare earth orthosilicate fast scintillation material is a single crystal, and the preparation method further comprises the following steps: S3, placing the material obtained in step S2 into a container, heating it to melt it, and slowly crystallizing the single crystal from the melt.

13. Application of the dual-strategy co-doped rare earth orthosilicate fast scintillation material according to any one of claims 1 to 7 in the fields of high energy physics, nuclear physics, space physics, nuclear medical imaging diagnosis, industrial non-destructive testing, safety auditing, geology and mineral and oil well exploration, and environmental testing.

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