LiTaO3: Tb < 3 + > nanocrystalline glass ceramic capable of capturing carriers as well as preparation method and application of LiTaO3: Tb < 3 + > nanocrystalline glass ceramic

Abstract

The invention discloses LiTaO3: Tb < 3 + > nanocrystalline glass ceramic capable of capturing carriers as well as a preparation method and application of the LiTaO3: Tb < 3 + > nanocrystalline glass ceramic, and belongs to the technical field of solid luminescent materials. The glass ceramic is prepared from 66.67 mol% of H3BO3, 25 mol% of Li2CO3, 8.33 mol% of Ta2O5, and 0.02 mol% to 0.08 mol% of Tb4O7 which is externally doped with the glass ceramic. Through the steps of powder raw material preparation, high-temperature melting, quenching forming, annealing and heat treatment, a LiTaO3 nanocrystalline phase is precipitated in situ in a borate glass matrix, the LiTaO3: Tb < 3 + > nanocrystalline glass ceramic with three different depth traps is formed by doping Tb < 3 + >, the single particle size of the glass ceramic is 121 nm, and the transmittance can reach 93%; the glass ceramic can effectively capture and store carriers by using different types of traps, improves storage of electron hole pairs under X-ray excitation, and can still realize signal reading after X-ray excitation is stopped.

Description

Technical Field

[0001] This invention belongs to the field of solid-state luminescent materials technology, specifically relating to a LiTaO3:Tb material capable of trapping charge carriers. 3+ Nanocrystalline glass ceramics, their preparation methods, and applications. Background Technology

[0002] Delayed-motion X-ray imaging (DXEMI) is an advanced radiation detection method based on energy storage and stimulated readout. Its core principle lies in using scintillator materials with carrier-trapping capabilities. During X-ray irradiation, these materials absorb energy and trap the resulting electron-hole pairs in specific traps within the material. After irradiation ceases, external stimulation releases the trapped carriers, causing them to recombine and emit light, thus storing and delaying the radiation information. This technology exhibits unique advantages in fields such as medical diagnostics, industrial non-destructive testing, security inspection, and high-energy physics experimental recording. Accordingly, developing high-performance scintillators capable of effectively trapping carriers, especially those with deep traps and effective defect states, is crucial for advancing strong-excitation luminescence and high-resolution delayed-motion X-ray imaging techniques.

[0003] Currently, conventional carrier trapping materials mainly rely on plates composed of inorganic phosphors and organic polymer matrices. Although such materials have been commercially applied, this inherent material system has the following limitations: (1) Under repeated X-ray irradiation and thermal stimulation, the organic components are easily degraded, significantly reducing the service life of the composite material; (2) The inorganic powders in the powder-organic composite material are usually micron-sized, and the mismatch between the refractive index of the powder and the organic matrix often makes the material opaque. Therefore, signals can only be recorded and read on the surface of the material, making the imaging data particularly susceptible to environmental degradation and loss; (3) The difficulty in matching the density of the inorganic powder and the organic matrix leads to powder sedimentation, resulting in uneven distribution of carrier trapping particles and affecting the realization of high-resolution delayed X-ray imaging. Therefore, the development of novel carrier trapping materials that can overcome the above limitations is crucial for advancing delayed X-ray imaging.

[0004] Nanostructured glass-ceramics are composite materials composed of nanocrystals embedded in an inorganic glass matrix. They not only exhibit optical properties comparable to corresponding single crystals but also retain the inherent advantages of the glass matrix, such as flexible design, ease of manufacturing, low cost, and simple processing. Compared to the aforementioned inorganic powder-organic composites, glass-ceramics possess superior physical / chemical stability, effectively mitigating aging problems caused by repeated exposure to X-ray radiation. Furthermore, by controlling the crystallization process, functional crystals can be uniformly precipitated in situ at nanoscale within the glass network, fundamentally avoiding the problem of charge carrier trapping and sedimentation of luminescent particles. In addition, the glass matrix itself serves as an excellent encapsulation medium, protecting the functional crystals from environmental corrosion.

[0005] However, not all glass-ceramic systems are suitable for high-resolution delayed X-ray imaging. This application places specific requirements on the materials. First, they must possess extremely high visible light transmittance to ensure that the excitation light can fully penetrate the material thickness to release the deeply stored signal, while simultaneously allowing the generated fluorescence to be emitted with low loss. Second, traps of appropriate depth and concentration must be introduced to effectively capture and store X-ray-excited charge carriers for extended periods. If the traps are too shallow, the signal storage time is short and decays quickly; if the traps are too deep, conventional methods such as heating or infrared lasers are insufficient to effectively release the charge carriers, resulting in insufficient readout sensitivity. Finally, the activating ions, which serve as the luminescent centers, require a crystal field environment to achieve efficient luminescence; therefore, a functional crystalline phase rich in these activating ions must be successfully precipitated within the glass.

[0006] Chinese Patent Publication No. CN114859647A, filed on May 27, 2022, discloses a method for X-ray time-lapse imaging based on microcrystalline glass. The molar ratios of its components are: Na₂CO₃: 10–15 mol%, SiO₂: 40–50 mol%, Al₂O₃: 10–20 mol%, BaF₂: 18–23 mol%, LaF₃: 2–7 mol%, TbF₃: 1–5% mol%. This invention solves the problems of low transparency, poor uniformity, and large particle size in electron-capturing materials in existing technologies, leading to poor physicochemical stability. Although the scintillator increases the types of electron-capturing materials currently available, the Ba₂LaF₇:TbF₃ ratio remains relatively stable at the specified preparation temperature. 3+ Microcrystalline glass exhibits devitrification, resulting in a reduction in transparency of approximately 10%, which is detrimental to high-resolution X-ray time-lapse imaging analysis.

[0007] Chinese patent publication number CN119220260A, filed on December 2, 2024, discloses a scintillator for time-delay imaging, its preparation method, and its application. The main scheme involves a lanthanum-doped fluoride nanocrystal scintillator. The coating layer includes inorganic glass, organic glass, or silicon dioxide. The lanthanum element includes any one of Tb, Eu, Er, Ce, Ce / Tb, Gd / Tb, or Ce / Tb / Gd. The fluoride nanocrystals are Pb4Lu3F. 17 Pb4Lu3F 17 Pb4Lu3F 17 Pb4Lu3F 17 Na5Lu9F 32 Cs 0.02 Na 0.98Either LuF4 or Ba2LaF7. However, in this patent, there is a clear physical interface between the pre-synthesized nanocrystals and the subsequently formed coating layer, making it difficult to achieve a precise match in refractive index. The large number of interfaces will lead to severe visible light scattering, thereby impairing the overall transparency of the material.

[0008] In summary, in the current field of delayed X-ray imaging materials, it is difficult to simultaneously achieve high-performance carrier trapping capability and high optical transparency in a single material. Powder-organic composite materials suffer from low transparency due to severe scattering; some glass-ceramic materials face the risk of devitrification due to improper crystallization control or phase interface matching problems. Therefore, developing a novel glass-ceramic scintillator capable of achieving efficient and controllable in-situ precipitation of functional crystalline phases, ensuring fine grain size, uniform distribution, and good optical compatibility with the glass matrix, thereby maintaining high light transmittance characteristics close to that of optical glass while obtaining excellent carrier trapping performance, has become a technical bottleneck that urgently needs to be overcome by those skilled in the art. This breakthrough is of vital significance for promoting the development of delayed X-ray imaging technology towards higher resolution, longer signal storage time, and greater stability and reliability. Summary of the Invention

[0009] To address the problems existing in the prior art, the present invention provides a LiTaO3:Tb carrier-capturing solution. 3+ Nanocrystalline glass-ceramics, their preparation methods, and applications: The nanocrystalline glass-ceramics can effectively capture and store charge carriers using different types of traps, improve the storage of electron-hole pairs under X-ray excitation, and still achieve signal readout after X-ray excitation stops.

[0010] The technical solution of the present invention is as follows: One of the objectives of this invention is to provide a LiTaO3:Tb solution capable of trapping charge carriers. 3+ The molar ratio of the components in the nanocrystalline glass-ceramic is as follows: The total molar percentage of the above components is 100 mol%, consisting of 66.67 mol% H3BO3, 25 mol% Li2CO3, and 8.33 mol% Ta2O5, with an additional 0.02-0.08 mol% Tb4O7.

[0011] The second objective of this invention is to provide a LiTaO3:Tb solution capable of capturing charge carriers. 3+ The preparation method of nanocrystalline glass ceramics includes the following steps: S1. Weigh the powder raw materials according to the proportions of each group. The component contents are as follows: 66.67 mol% H3BO3, 25 mol% Li2CO3, 8.33 mol% Ta2O5, the total molar amount of the above components is 100 mol%, with 0.02-0.08 mol% Tb4O7 added externally; S2. After grinding the powder raw material evenly, place it in a crucible, put it in a high-temperature furnace to melt it to obtain the precursor glass melt, and quickly pour it into a preheated copper mold. After it is formed, quickly place it in a muffle furnace for annealing to obtain the precursor glass. S3. The precursor glass is placed in a muffle furnace and kept at a constant temperature to induce the in-situ nucleation and growth of the LiTaO3 crystal phase in the glass, thereby obtaining the glass ceramic.

[0012] Furthermore, the melting temperature of the high-temperature furnace in S2 is 1300-1350℃. Furthermore, the high-temperature furnace melting time in S2 is 20-30 min. Furthermore, the preheating temperature of the copper mold in S2 is 150-200℃. Furthermore, the annealing temperature in the muffle furnace in S2 is 250-350℃. Furthermore, the annealing time in the muffle furnace in S2 is 9-11 h. Furthermore, in S3, the holding temperature of the precursor glass placed in the muffle furnace is 610-630℃. Furthermore, in S3, the pre-conducting glass is kept in the muffle furnace for 1-3 hours. The third objective of this invention is to provide a LiTaO3:Tb solution capable of trapping charge carriers. 3+ Application of nanocrystalline glass ceramics in X-ray time-lapse imaging. Compared with the prior art, the beneficial effects of the present invention are as follows: 1. This invention is the first to propose a one-step melt-heat treatment method for preparing a LiTaO3:Tb material capable of capturing charge carriers. 3+ Nanocrystalline glass-ceramics are first developed by high-temperature melting of a specific combination of raw materials based on a specific molar ratio, followed by rapid cooling to form a completely amorphous precursor glass mass. This ensures highly uniform mixing of all components, laying the foundation for subsequent uniform crystallization. Then, through controlled heat treatment at a specific temperature, lithium tantalate (LiTaO3) nanocrystalline phases are induced to nucleate and grow in situ from the supersaturated glass network. These nanocrystalline phases are densely embedded as functional units within a continuous borate glass matrix, resulting in a "crystalline-amorphous" composite bulk material. This fundamentally avoids the technical problems of uneven powder dispersion, severe interface scattering, and the introduction of organic components found in existing technologies.

[0013] 2. The carrier-capturing LiTaO3:Tb designed in this invention 3+Nanocrystalline glass-ceramics possess ideal physicochemical properties. Regarding optical transparency, the in-situ precipitated LiTaO3 nanocrystals are smaller than the visible light wavelength and have excellent refractive index matching with the borate glass matrix, greatly suppressing light scattering. The Scherrer equation confirms that the individual particle size is 121 nm, and the transmittance in the visible light region can reach over 90%. Regarding carrier trapping ability, Tb... 3+ Ion doping, acting as luminescent centers, synergistically introduces multi-depth traps with the LiTaO3 lattice and glass-crystal interface. Thermoluminescence spectroscopy analysis confirms the existence of three distinct trap energy levels at 382 K, 425 K, and 495 K, corresponding to depths of 0.764 eV, 0.85 eV, and 0.99 eV, respectively. This coexistence system of shallow, medium, and deep traps possesses efficient and tunable carrier trapping capabilities, providing a physical basis for hierarchical carrier storage and on-demand release. Furthermore, the material exhibits excellent physicochemical stability. The annealing process effectively eliminates residual internal stresses formed by rapid cooling of the glass melt, reducing the possibility of bulk cracking. Even under high-energy radiation, the material maintains a dense structure and good mechanical strength. Overall, the material possesses excellent resistance to radiation aging and thermal stability, can withstand repeated X-ray irradiation without performance degradation, and has a long service life.

[0014] 3. This invention innovatively utilizes LiTaO3:Tb to capture charge carriers. 3+ Nanocrystalline glass-ceramics possess significant comprehensive advantages in the field of X-ray time-lapse imaging. Firstly, the excellent bulk transparency of these glass-ceramics allows excitation heat or light to fully penetrate the entire material volume during imaging readout, uniformly releasing signals stored in both deep and shallow regions, while simultaneously enhancing the Tb generated during excitation. 3+ Characteristic fluorescence can be transmitted to the detector with low loss. As shown in the examples, this material can achieve a spatial resolution of over 20.0 lp / mm under thermal excitation at 450K, clearly reproducing the details of the standard line pair card and the internal structure of the target object. The imaging quality is superior to that of traditional composite materials that suffer from signal blurring due to scattering. Secondly, in the glass-ceramic trap structure at different depths, the 0.764 eV shallow trap slowly releases charge carriers at room temperature to generate initial afterglow; the two deep traps at 0.85 eV and 0.99 eV firmly capture charge carriers, allowing X-ray latent image information to be stably stored for up to 7 days at room temperature, extending the readability window and solving the technical problems of low delayed imaging resolution and short storage time of existing glass-ceramic scintillators. In addition, this glass-ceramic is a ready-to-use solid bulk material that does not require subsequent molding and processing. The preparation process is simple, has a short cycle, and low raw material cost, making it very suitable for large-scale industrial production and possessing ideal commercial value and application prospects. Attached Figure Description

[0015] Figure 1This is a differential scanning calorimetry test image of the precursor glass described in Embodiment 3 of the present invention; Figure 2 The X-ray diffraction patterns of the precursor glass and glass ceramic described in Embodiment 3 of the present invention are shown below. Figure 3 The ultraviolet-visible-near-infrared transmission spectrum of the glass-ceramic described in Example 3 of this invention; Figure 4 This is the afterglow emission spectrum of the glass-ceramic excited by X-rays as described in Embodiment 3 of the present invention; Figure 5 This is a Gaussian peak curve of the pyroelectric spectrum of the glass-ceramic described in Embodiment 3 of the present invention; Figure 6 This is a schematic diagram of the glass-ceramic X-ray time-lapse imaging system described in Embodiment 3 of the present invention; Figure 7 The image is a line-pair card image of the glass-ceramic X-ray time-lapse imaging described in Embodiment 3 of the present invention; Figure 8 This is an X-ray time-lapse image of the glass-ceramic described in Embodiment 3 of the present invention. Detailed Implementation

[0016] The present invention will be further described below with reference to preferred embodiments. The endpoints and any values ​​of the ranges disclosed in the present invention are not limited to the precise ranges or values. These ranges or values ​​should be understood to include values ​​close to these ranges or values. For numerical ranges, the endpoint values ​​of the various ranges, the endpoint values ​​of the various ranges and individual point values, and individual point values ​​can be combined with each other to obtain one or more new numerical ranges, which should be regarded as specifically disclosed herein. Unless otherwise specified, the experimental methods in the following embodiments are conventional methods, performed in accordance with the techniques or conditions described in the literature in this field or in accordance with the product instructions.

[0017] Unless otherwise specified, all materials and reagents used in the following examples are commercially available.

[0018] Example 1 This embodiment provides a LiTaO3:Tb solution capable of capturing charge carriers. 3+ The preparation method of nanocrystalline glass ceramics includes the following steps: S1. Analytical grade H3BO3, Li2CO3, Ta2O5 and Tb4O7 powder with a purity of 99.99% were accurately weighed in a molar ratio of 66.67 mol%: 25 mol%: 8.33 mol%: 0.02 mol%. S2. Grind the above powder raw material in an agate mortar until uniform, then place it in an alumina crucible and melt it in a high-temperature furnace at 1300℃ for 20 min. Then quickly pour the precursor glass melt into a copper mold preheated at 150℃. After forming, quickly place it in a muffle furnace at 250℃ for annealing for 9 h to obtain the precursor glass. S3. The obtained precursor glass is kept in a muffle furnace at 610℃ for 1 h to induce the in-situ precipitation of the LiTaO3 crystal phase in the glass, thus obtaining a glass-ceramic scintillator with a high crystallinity of LiTaO3 crystal phase that can capture charge carriers.

[0019] Example 2 This embodiment provides a LiTaO3:Tb solution capable of capturing charge carriers. 3+ The preparation method of nanocrystalline glass ceramics includes the following steps: S1. Analytical grade H3BO3, Li2CO3, Ta2O5 and Tb4O7 powder with a purity of 99.99% were accurately weighed in a molar ratio of 66.67 mol%: 25 mol%: 8.33 mol%: 0.02 mol%. S2. Grind the above powder raw material in an agate mortar until uniform, then place it in an alumina crucible and melt it in a high-temperature furnace at 1325℃ for 25 minutes. Then quickly pour the precursor glass melt into a preheated copper mold at 175℃. After forming, quickly place it in a muffle furnace at 300℃ for annealing for 10 hours to obtain the precursor glass. S3. The obtained precursor glass is kept in a muffle furnace at 620℃ for 2 h to induce the in-situ precipitation of the LiTaO3 crystal phase in the glass, thus obtaining a glass-ceramic scintillator with a high crystallinity of LiTaO3 crystal phase that can capture charge carriers.

[0020] Example 3 This embodiment provides a LiTaO3:Tb solution capable of capturing charge carriers. 3+ A method for preparing nanocrystalline glass-ceramics includes the following steps: S1. Analytical grade H3BO3, Li2CO3, Ta2O5 and Tb4O7 powder with a purity of 99.99% were accurately weighed in a molar ratio of 66.67 mol%: 25 mol%: 8.33 mol%: 0.06 mol%. S2. Grind the above powder raw material in an agate mortar until uniform, then place it in an alumina crucible and melt it in a high-temperature furnace at 1300℃ for 25 minutes. Then quickly pour the precursor glass melt into a copper mold preheated at 175℃. After forming, quickly place it in a muffle furnace at 300℃ for annealing for 10 hours to obtain the precursor glass. S3. The obtained precursor glass is kept in a muffle furnace at 630℃ for 2 h to induce the in-situ precipitation of the LiTaO3 crystal phase in the glass, thus obtaining a glass-ceramic scintillator with a high crystallinity of LiTaO3 crystal phase that can capture charge carriers.

[0021] Example 4 This embodiment provides a LiTaO3:Tb solution capable of capturing charge carriers. 3+ A method for preparing nanocrystalline glass-ceramics includes the following steps: S1. Analytical grade H3BO3, Li2CO3, Ta2O5 and Tb4O7 powder with a purity of 99.99% were accurately weighed in a molar ratio of 66.67 mol%: 25 mol%: 8.33 mol%: 0.08 mol%. S2. Grind the above powder raw material in an agate mortar until uniform, then place it in an alumina crucible and melt it in a high-temperature furnace at 1350℃ for 30 min. Then quickly pour the precursor glass melt into a preheated copper mold at 200℃. After forming, quickly place it in a muffle furnace at 300℃ for annealing for 11 h to obtain the precursor glass. S3. The obtained precursor glass is kept in a muffle furnace at 630℃ for 3 h to induce the in-situ precipitation of the LiTaO3 crystal phase in the glass, thus obtaining a glass-ceramic scintillator with a high crystallinity of LiTaO3 crystal phase that can capture charge carriers.

[0022] Performance testing 1. Differential scanning calorimetry test Differential scanning calorimetry was used to test the glass-ceramic scintillator prepared in Example 3. The test results are as follows: Figure 1 As shown. Figure 1 Differential scanning calorimetry (DSC) curves show that the glass transition temperature T of the glass-ceramic scintillator is... g The first exothermic peak temperature T C1 The second exothermic peak temperature T C2 The temperatures were approximately 585℃, 639℃, and 653℃, respectively. Selecting 630℃ as the crystallization heat treatment temperature is reasonable. This confirms that the in-situ precipitation of the LiTaO3 crystal phase can be precisely induced by controlling the heat treatment temperature, providing a process basis for achieving high crystallinity and high transparency glass ceramics.

[0023] 2. Crystal structure analysis The glass-ceramic scintillator prepared in Example 3 was tested using an X-ray diffractometer, and the X-ray diffraction pattern is shown below. Figure 2 As shown. Figure 2X-ray diffraction data showed that LiTaO3 crystal phase precipitated in the glass matrix after heat treatment. The corresponding particle size was calculated to be 121 nm according to the Scherrer formula, confirming that the glass ceramic was successfully obtained. It is smaller than the wavelength of visible light and has the structural basis to achieve high transmittance and low light dispersion.

[0024] 3. Optical transmittance test The glass-ceramic scintillator prepared in Example 3 was tested using a UV / Vis / NIR spectrophotometer. The UV-Vis / NIR transmittance spectrum is as follows: Figure 3 As shown. Figure 3 The ultraviolet-visible-near-infrared transmission spectroscopy results show that the glass-ceramic has excellent optical transparency, with a transmittance of over 90% and up to 93% in the visible light region, which meets the optical requirements for signal penetration and collection in high-resolution X-ray time-lapse imaging.

[0025] 4. X-ray excited afterglow emission luminescence test Using an FLS1000 fluorescence spectrometer combined with a self-made testing system consisting of an X-ray source, integrating sphere, sample stage, and FLS1000 fluorescence spectrometer, the steady-state afterglow emission spectrum of the glass-ceramic scintillator prepared in Example 3 was measured under the condition of X-ray irradiation for 1 minute followed by X-ray source shutdown. The X-ray excited afterglow emission spectrum is shown in the figure. Figure 4 As shown in the figure, obvious luminescence can be observed, with the peaks at 489nm, 545nm, 586nm, and 623nm attributed to Tb, respectively. 3+ of 5 D4 to 7 F6 7 F5 7 F4 7 The F3 transition indicates that Tb 3+ Successful incorporation into the LiTaO3 lattice as a luminescent center provides a guarantee for subsequent carrier capture and release luminescence mechanisms based on trap energy levels.

[0026] 5. Defect Analysis The 0.06 mol% Tb doped material obtained in Example 3 3+ LiTaO3:Tb 3+ The thermoluminescence Gaussian distribution curve of glass-ceramics is as follows: Figure 5 As shown. By Figure 5It can be seen that there are three types of traps in this material, distributed at 382K, 425K, and 495K respectively. Calculations using the corresponding formulas show that the depths of these traps are 0.764 eV, 0.85 eV, and 0.99 eV, respectively. A shallow trap exists at 0.764 eV, which can be slowly released at room temperature with a long afterglow. Two deep traps exist at 0.85 eV and 0.99 eV, which are difficult to release at room temperature, ensuring the electron-hole pair structure in LiTaO3:Tb at room temperature. 3+ It maintains high stability for 7 days in microcrystalline glass.

[0027] 6. X-ray time-lapse imaging effect test Use such as Figure 6 The X-ray time-lapse imaging system shown was used to test the X-ray time-lapse imaging effect of the glass-ceramic scintillator described in Example 3. The glass-ceramic was irradiated at 60 kV and 200 μA for 1 minute, then the radiation source was turned off. After waiting 5 minutes, the glass-ceramic was placed on a heating stage and heated to 450 K before a photograph was recorded. The test results are as follows: Figure 7-8 As shown.

[0028] This glass-ceramic material was used to obtain X-ray time-lapse imaging standard line pair cards, such as... Figure 7 As shown, at 450K, a 20.0 lp / mm exceeding the standard line-to-card limit can be clearly observed.

[0029] Using this glass-ceramic to obtain X-ray time-lapse images, such as Figure 8 As shown, the internal structure of the target object can be clearly observed, and high-quality X-ray time-lapse imaging results can be obtained.

[0030] The above description is merely an embodiment of the present invention and does not limit the patent scope of the present invention. Any equivalent modifications made based on the content of the present invention specification and drawings, or direct or indirect applications in related technical fields, are similarly included within the patent protection scope of the present invention.

Claims

1. A LiTaO3:Tb catalyst capable of trapping charge carriers 3+ Nanocrystalline glass-ceramics, characterized in that, The molar ratios of its components are as follows: The total molar percentage of the above components is 100 mol%, consisting of 66.67 mol% H3BO3, 25 mol% Li2CO3, and 8.33 mol% Ta2O5, with an additional 0.02-0.08 mol% Tb4O7.

2. A LiTaO3:Tb carrier-capturing device as described in claim 1 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, Includes the following steps: S1. Weigh the powder raw materials according to the proportions of each group. The component contents are as follows: 66.67 mol% H3BO3, 25 mol% Li2CO3, 8.33 mol% Ta2O5, the total molar amount of the above components is 100 mol%, with 0.02-0.08 mol% Tb4O7 added externally; S2. After grinding the powder raw material evenly, place it in a crucible, put it in a high-temperature furnace to melt it to obtain the precursor glass melt, and quickly pour it into a preheated copper mold. After it is formed, quickly place it in a muffle furnace for annealing to obtain the precursor glass. S3. The precursor glass is placed in a muffle furnace and kept at a constant temperature to induce the in-situ nucleation and growth of the LiTaO3 crystal phase in the glass, thereby obtaining the glass ceramic.

3. The carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The melting temperature of the high-temperature furnace in S2 is 1300-1350℃.

4. A carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The high-temperature furnace melting time in S2 is 20-30 min.

5. The carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The preheating temperature of the copper mold in S2 is 150-200℃.

6. The carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The annealing temperature in the muffle furnace in S2 is 250-350℃.

7. A carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The annealing time in the muffle furnace in S2 is 9-11 h.

8. The carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The holding temperature of the precursor glass in the muffle furnace in S3 is 610-630℃.

9. A carrier-capturing LiTaO3:Tb according to claim 2 3+ A method for preparing nanocrystalline glass ceramics, characterized in that, The holding time of the precursor glass in the muffle furnace in S3 is 1-3 hours.

10. A carrier-capturing LiTaO3:Tb prepared by the method according to any one of claims 2-9 3+ Application of nanocrystalline glass ceramics in X-ray time-lapse imaging.

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