阅读说明：本技术 稀土掺杂钽酸镁闪烁发光材料及其制备方法 (Rare earth doped magnesium tantalate scintillation luminescent material and preparation method thereof ) 是由 马云峰 郭超 徐家跃 秦康 吴金成 蒋毅坚 王森宇 于 2021-08-10 设计创作，主要内容包括：本发明公开了一种稀土掺杂钽酸镁闪烁发光材料及其制备方法。所述稀土掺杂钽酸镁闪烁发光材料的化学通式为Mg-(4)Ta-(2)O-(9):RE,其中RE为稀土元素。制备方法为：按化学通式称取原料,将所有原料混合均匀；然后将混合物在空气气氛中依次预烧、煅烧,再自然冷却到室温,研磨即可。本发明中的闪烁发光材料采用高温固相法合成,在空气中稳定存在,工艺安全简单,容易控制。所制得的闪烁发光材料在X射线激发下,得到的不同稀土掺杂的Mg-(4)Ta-(2)O-(9):RE样品,光产额在13848～43917ph/MeV,最高可达CsI(Tl)的81％、Mg-(4)Ta-(2)O-(9)和CdWO-(4)的2.4倍。(The invention discloses a rare earth doped magnesium tantalate scintillation luminescent material and a preparation method thereof. The chemical general formula of the rare earth doped magnesium tantalate scintillation luminescent material is Mg 4 Ta 2 O 9 RE, wherein RE is a rare earth element. The preparation method comprises the following steps: weighing raw materials according to a chemical formula, and uniformly mixing all the raw materials; and then sequentially presintering and calcining the mixture in air atmosphere, naturally cooling to room temperature, and grinding. The scintillation luminescent material is synthesized by a high-temperature solid phase method, stably exists in the air, and is safe and simple in process and easy to control. The prepared scintillation luminescent material is excited by X-rays to obtain Mg doped with different rare earths 4 Ta 2 O 9 RE samples with light yield of 13848-43917 ph/MeV, which can reach 81% of CsI (Tl) and Mg 4 Ta 2 O 9 And CdWO 4 2.4 times of the total weight of the powder.)

1. The rare earth doped magnesium tantalate scintillation luminescent material is characterized in that the chemical general formula is Mg₄Ta₂O₉RE, wherein RE is a rare earth element.

2. Rare earth doping of claim 1The magnesium tantalate scintillating luminescent material is characterized in that RE in the chemical general formula is Sc³⁺、Lu³⁺、Yb³⁺、Tm³⁺、Er³⁺、Y³⁺、Ho³⁺、Dy³⁺、Tb³⁺、Gd³⁺、Eu³⁺、Sm³⁺、Nd³⁺、Pr³⁺、Ce³⁺Or La³⁺。

3. The rare earth doped magnesium tantalate scintillating light emitting material of claim 1, wherein the doping amount of RE in the chemical formula is 0.25 at%.

4. The rare earth-doped magnesium tantalate scintillating luminescent material according to claim 1, wherein the light yield of the rare earth-doped magnesium tantalate scintillating luminescent material under X-ray excitation is 13848-43917 ph/MeV.

5. The method for preparing the rare earth-doped magnesium tantalate scintillating luminescent material according to any one of claims 1 to 4, characterized in that the raw materials are weighed according to the chemical formula and are mixed uniformly; and then sequentially presintering and calcining the mixture in air atmosphere, naturally cooling to room temperature, and grinding.

6. The method for preparing the rare earth doped magnesium tantalate scintillating luminescent material of claim 5, wherein the raw materials are MgO and Ta₂O₅And Sc selected according to the doping element of the general chemical formula₂O₃、Lu₂O₃、Yb₂O₃、Tm₂O₃、Er₂O₃、Y₂O₃、Ho₂O₃、Dy₂O₃、Tb₂O₃、Gd₂O₃、Eu₂O₃、Sm₂O₃、Nd₂O₃、Pr₂O₃、Ce₂O₃Or La₂O₃。

7. The method for preparing a scintillating light-emitting material of rare earth doped magnesium tantalate of claim 5, wherein the addition of MgO is 3 at% excess to the standard ratio.

8. The method for preparing the rare earth doped magnesium tantalate scintillating luminescent material according to claim 5, wherein the pre-sintering temperature is 1250-1300 ℃ and the time is 3-12 hours.

9. The method for preparing the rare earth doped magnesium tantalate scintillating luminescent material according to claim 5, wherein the calcining temperature is 1300-1400 ℃ and the time is 6-24 hours.

10. Use of the rare earth doped magnesium tantalate scintillating luminescent material of any one of claims 1 to 4 in high-energy radiation detection.

Technical Field

The invention relates to Mg for high-energy ray detection₄Ta₂O₉:RE(RE＝Sc³⁺、Lu³⁺、Yb³⁺、Tm³⁺、Er³⁺、Y³⁺、Ho³⁺、Dy³⁺、Tb³⁺、Gd³⁺、Eu³⁺、Sm³⁺、Nd³⁺、Pr³⁺、Ce³⁺、La³⁺) A scintillation luminescent material and a preparation method thereof belong to the technical field of scintillation luminescent materials for high-energy ray detection.

Background

The inorganic scintillation crystal is widely applied to the fields of high-energy physics and nuclear physics, celestial body physics, medical imaging, geological exploration, safety detection, national defense safety and the like. Particularly airport security inspection, customs container inspection and the like, a large number of X-ray imaging probes based on scintillation crystals are needed, and the current mature security inspection probe material mainly comprises CdWO₄Crystals, CsI (Tl) crystals, and the like. CdWO₄Has good radiation stopping power, almost has no afterglow, but has relatively low brightness, and Cd is toxic. Tl has good light yield and radiation stopping power, but its decay time is relatively long and Tl is toxic. Therefore, the search for a novel non-toxic environment-friendly scintillation crystal with excellent performance is an urgent need and development center in the current security inspection application field.

Mg₄Ta₂O₉The (MTO for short) crystal material belongs to hexagonal system, has ilmenite structure, space group P3c1(165), lattice constant a 0.51611nm, c 1.40435nm and V0.32396 nm³。Mg₄Ta₂O₉662keV of crystal¹³⁷The light yield of Cs gamma rays is 13000 + -2000 ph/MeV, and CdWO₄The crystal (12000-15000 ph/MeV) is equivalent to about 24% of CsI (Tl) crystal light yield (52000-56000 ph/MeV); the energy resolution is 6.2 percent and is higher than that of CdWO₄The energy resolution of the crystal is 8.3%, which is comparable to the energy resolution of CsI (Tl) (5.7%); the decay time is 4.5 mu s, which is superior to CdWO₄14 μ s for crystals, longer than 1 μ s for CsI (Tl) crystals. The crystalThe method is environment-friendly, has no problem that toxic elements pollute the environment from production, processing, application and recovery, and has potential application prospect in the aspect of radiographic probes.

From a compositional standpoint, rare earths play a tremendous role in the development of scintillation crystals. Most of rare earth ions (Ce)³⁺→Yb³⁺) The luminescent material has an incompletely filled 4f electron layer, 1639 energy levels in total, and 199177 transitions, and is a huge luminescent treasure bank which is widely used as an activator and a sensitizer of luminescent materials. The unique electronic configuration structure of rare earth ions can lead Mg₄Ta₂O₉The crystal has more excellent luminescence property, when rare earth ions are weakly doped, the crystal can be used as a sensitizer, and the abundant energy level structure of the sensitizer is utilized to absorb and transfer energy to a Ta-O octahedral luminescence center, so that Mg is improved₄Ta₂O₉The light yield of the crystal. When the rare earth ions are heavily doped, they can act as activators, Mg₄Ta₂O₉The energy absorbed by the matrix is transferred to the luminescence center of the rare earth ion, and ultraviolet and visible light is emitted by utilizing the abundant energy level structure of the rare earth ion, so that the rare earth scintillation crystal with excellent scintillation performance is formed.

Disclosure of Invention

The technical problem to be solved by the invention is as follows: how to combine the luminous advantages of rare earth in the field of scintillating materials and mix the rare earth with Mg₄Ta₂O₉(MTO for short) to obtain the rare earth doped magnesium tantalate scintillating material for detecting high-energy ray radiation with high light yield.

In order to solve the technical problem, the invention provides a rare earth doped magnesium tantalate scintillation luminescent material, the chemical general formula of which is Mg₄Ta₂O₉RE, wherein RE is a rare earth element.

Preferably, RE in the chemical formula is Sc³⁺、Lu³⁺、Yb³⁺、Tm³⁺、Er³⁺、Y³⁺、Ho³⁺、Dy³⁺、Tb³⁺、Gd³⁺、Eu³⁺、Sm³⁺、Nd³⁺、Pr³⁺、Ce³⁺Or La³⁺。

Preferably, the doping amount of RE in the chemical formula is 0.25 at%.

Preferably, the rare earth doped magnesium tantalate scintillation luminescent material has a light yield of 13848-43917 ph/MeV under the excitation of X rays.

The invention also provides a preparation method of the rare earth doped magnesium tantalate scintillation luminescent material, which comprises the steps of weighing raw materials according to a chemical formula, and uniformly mixing all the raw materials; and then sequentially presintering and calcining the mixture in air atmosphere, naturally cooling to room temperature, and grinding.

Preferably, the raw materials are MgO and Ta₂O₅And Sc selected according to the doping element of the general chemical formula₂O₃、Lu₂O₃、Yb₂O₃、Tm₂O₃、Er₂O₃、Y₂O₃、Ho₂O₃、Dy₂O₃、Tb₂O₃、Gd₂O₃、Eu₂O₃、Sm₂O₃、Nd₂O₃、Pr₂O₃、Ce₂O₃Or La₂O₃。

Preferably, the addition amount of MgO is 3 at% excess to the standard ratio.

Preferably, the pre-sintering temperature is 1250-1300 ℃ and the time is 3-12 hours.

Preferably, the calcining temperature is 1300-1400 ℃, and the time is 6-24 hours.

The invention also provides the application of the rare earth doped magnesium tantalate scintillation luminescent material in high-energy ray detection.

The rare earth doped magnesium tantalate system synthesized by adopting a high-temperature solid-phase method can stably exist in the air and has high light output under the excitation of high-energy rays. The invention can provide theoretical and technical support for the design and preparation of the novel scintillator material.

Compared with the prior art, the invention has the following advantages and beneficial effects:

(1) the scintillation luminescent material is synthesized by a high-temperature solid phase method, the preparation process is simple, the operation is safe, and the conditions are easy to control.

(2) The scintillation luminescent material of the invention has no toxicity and radioactive elements, stably exists in the air, and is not easy to deliquesce.

(3) The scintillation luminescent material of the invention can obtain Mg doped with different rare earths under the excitation of X rays₄Ta₂O₉The light yield of RE sample is 13837-43917ph/MeV, which is better than that of undoped Mg₄Ta₂O₉Wherein sample Mg₄Ta₂O₉The Gd light yield is 81% of that of CsI (Tl) and Mg₄Ta₂O₉And CdWO₄2.4 times of the total weight of the powder.

Drawings

FIG. 1 is an X-ray diffraction pattern of a scintillating light-emitting material prepared in each example;

FIG. 2 is Mg₄Ta₂O₉An emission spectrum measured by the Sc scintillation luminescent material with 0.25 at% under the excitation of X ray;

FIG. 3 is Mg₄Ta₂O₉An emission spectrogram of 0.25 at% Lu scintillation luminescent material under the excitation of X-ray;

FIG. 4 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% Yb scintillation luminescent material under the excitation of X ray;

FIG. 5 is Mg₄Ta₂O₉An emission spectrum of the 0.25 at% Tm scintillation luminescent material under the excitation of X rays;

FIG. 6 is Mg₄Ta₂O₉An emission spectrogram of the Er scintillation luminescent material with the concentration of 0.25at percent measured under the excitation of X rays;

FIG. 7 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% of Y scintillation luminescent material under the excitation of X ray;

FIG. 8 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% Ho scintillation luminescent material under the excitation of X ray;

FIG. 9 is Mg₄Ta₂O₉0.25 at% Dy scintillationAn emission spectrum of the luminescent material measured under the excitation of X-rays;

FIG. 10 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% Tb scintillating luminescent material under the excitation of X-ray;

FIG. 11 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% Gd scintillating luminescent material under the excitation of X ray;

FIG. 12 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% Eu scintillating luminescent material under the excitation of X ray;

FIG. 13 is Mg₄Ta₂O₉An emission spectrum measured by 0.25 at% of Sm scintillation luminescent material under the excitation of X rays;

FIG. 14 is Mg₄Ta₂O₉An emission spectrum measured by the Nd scintillation luminescent material at 0.25 at% under the excitation of X ray;

FIG. 15 is Mg₄Ta₂O₉An emission spectrogram of 0.25 at% Pr scintillating luminescent material under the excitation of X ray;

FIG. 16 is Mg₄Ta₂O₉An emission spectrum measured by the 0.25 at% Ce scintillation luminescent material under the excitation of X rays;

FIG. 17 is Mg₄Ta₂O₉Emission spectrum of 0.25 at% La scintillation luminescent material under X-ray excitation.

Detailed Description

In order to make the invention more comprehensible, preferred embodiments are described in detail below with reference to the accompanying drawings.

Example 1

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Sc₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1250 ℃ for 3 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1300 ℃ for 6 hours in air atmosphere, and naturally cooling to room temperatureAnd (4) uniformly grinding after warming to obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Sc curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 2, Mg₄Ta₂O₉0.25 at% Sc, an emission wavelength of 352nm, a full width at half maximum of 109nm, and a luminous intensity of Mg₄Ta₂O₉2.4 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Sc has a light yield of 31450 ph/MeV.

Example 2

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Lu₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1250 ℃ for 3 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1300 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Lu curve. As can be seen from the curves in the figure, all diffraction peaks correspond to the diffraction peaks of the standard diffraction (PDF # 38-1458). As shown in FIG. 3, Mg₄Ta₂O₉0.25 at% Lu shows that the emission wavelength is 354nm, the full width at half maximum is 109nm, and the luminous intensity is Mg₄Ta₂O₉1.6 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Lu has a light yield of 21394 ph/MeV.

Example 3

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Yb₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1250 ℃ for 3 hours in air atmosphere, and automatically calciningAnd cooling to room temperature, pouring the raw materials out, continuously and fully grinding in an agate mortar, then putting the raw materials into a corundum crucible, sintering for 6 hours at 1300 ℃ in air atmosphere, naturally cooling to room temperature, and grinding uniformly to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉And a Yb curve of 0.25 at%. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 4, Mg₄Ta₂O₉0.25 at% Yb, an emission wavelength of 343nm, a full width at half maximum of 89nm, and a luminous intensity of Mg₄Ta₂O₉1.1 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Yb has a light yield of 13837 ph/MeV.

Example 4

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Tm₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1250 ℃ for 3 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1300 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉And a Tm curve of 0.25 at%. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 5, Mg₄Ta₂O₉0.25 at% Tm in 30keV X-ray excitation emission spectrum, which shows that the emission wavelength is 355nm, the full width at half maximum is 82nm, and the luminous intensity is Mg₄Ta₂O₉1.6 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉The light yield of 0.25 at% Tm is 20471 ph/MeV. Also shown in the XEL chart is Tm³⁺Is/are as follows¹D₂→³F₄Energy level transition, peak position at 459nm, and luminous intensity at Mg₄Ta₂O₉1.3 times ofThe full width at half maximum is 20 nm.

Example 5

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Er₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1260 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1330 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉Er curve of 0.25 at%. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 6, Mg₄Ta₂O₉0.25 at% Er shows that the emission wavelength is 348nm, the full width at half maximum is 96nm, and the luminous intensity is Mg₄Ta₂O₉1.2 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉The light yield of 0.25 at% Er was 15620 ph/MeV.

Example 6

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Y₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1260 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1330 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Y curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 7, Mg₄Ta₂O₉0.25 at% Y, an X-ray excitation emission spectrum of 30keV showed an emission wavelength of 344nm,the full width at half maximum is 95nm, and the luminous intensity is Mg₄Ta₂O₉2.2 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Y has a light yield of 28152 ph/MeV.

Example 7

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Ho₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1260 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1330 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉And 0.25 at% Ho curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 8, Mg₄Ta₂O₉0.25 at% Ho, which shows an emission wavelength of 349nm, a full width at half maximum of 117nm, and a luminous intensity of Mg₄Ta₂O₉1.2 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Ho has a light yield of 15353 ph/MeV.

Example 8

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Dy₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1260 ℃ for 6 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1330 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Dy curve. As can be seen from the curves in the figure, all diffraction peaks diffract the standardPeaks (PDF #38-1458) correspond. As shown in FIG. 9, Mg₄Ta₂O₉An emission spectrum of 30keV X-ray excited emission of 0.25 at% Dy has an emission wavelength of 350nm, a full width at half maximum of 91nm, and a luminous intensity of Mg₄Ta₂O₉1.1 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Dy has a light yield of 13693 ph/MeV. Dy is also shown in the XEL diagram³⁺Is/are as follows⁴F_9/2→⁶H_13/2Energy level transition, peak position at 579nm, and luminous intensity at Mg₄Ta₂O₉0.9 times of the total length of the film, and the full width at half maximum is 12 nm.

Example 9

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Tb₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1280 ℃ for 9 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1350 ℃ for 18 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Tb. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 10, Mg₄Ta₂O₉0.25 at% Tb, an emission wavelength of 359nm, a full width at half maximum of 98nm and a luminous intensity of Mg₄Ta₂O₉1.9 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Tb has a light yield of 24463 ph/MeV. In addition, Tb is also shown in the XEL graph³⁺Is/are as follows⁵D₄→⁷F₅Energy level transition, peak position at 552nm, and luminous intensity of Mg₄Ta₂O₉0.5 times of the total length of the film, and the full width at half maximum is 13 nm.

Example 10

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Gd₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1280 ℃ for 9 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1350 ℃ for 18 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Gd curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 11, Mg₄Ta₂O₉0.25 at% Gd, the emission wavelength of the 30keV X-ray excitation emission spectrum is 345nm, the full width at half maximum is 92nm, and the luminous intensity is Mg₄Ta₂O₉3.4 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Gd has a light yield of 43917 ph/MeV.

Example 11

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Eu₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1280 ℃ for 9 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1350 ℃ for 18 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Eu curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 12, Mg₄Ta₂O₉0.25 at% Eu, shows an emission wavelength of 347nm, a full width at half maximum of 91nm, and a luminous intensity of Mg₄Ta₂O₉2.2 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Eu having a light yield of 28653 ph/MeV. Further, Eu is shown in the XEL chart³⁺Is/are as follows⁵D₀→⁷F₂Energy level transition, peak position at 612nm, and luminous intensity at Mg₄Ta₂O₉2.9 times of the total length of the film, and the full width at half maximum is 10 nm.

Example 12

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Sm₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1280 ℃ for 9 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1350 ℃ for 18 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Sm curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 13, Mg₄Ta₂O₉0.25 at% Sm in a 30keV X-ray excitation emission spectrum shows that the emission wavelength is 348nm, the full width at half maximum is 86nm, and the luminous intensity is Mg₄Ta₂O₉1.1 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Sm has a light yield of 13848 ph/MeV.

Example 13

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Nd₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1300 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1400 ℃ for 24 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉And a curve of 0.25 at% Nd. From the figureAs can be seen from the curves, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 14, Mg₄Ta₂O₉0.25 at% Nd, an emission spectrum of 30keV X-ray excitation shows that the emission wavelength is 345nm, the full width at half maximum is 90nm, and the luminous intensity is Mg₄Ta₂O₉2.1 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉The light yield of 0.25 at% Nd was 27079 ph/MeV.

Example 14

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Pr₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1300 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1400 ℃ for 24 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Pr curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 15, Mg₄Ta₂O₉0.25 at% Pr of the fluorescent material shows an emission wavelength of 347nm, a full width at half maximum of 98nm and a luminous intensity of Mg₄Ta₂O₉1.7 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Pr has a light yield of 21492 ph/MeV.

Example 15

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，Ce₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1300 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1400 ℃ for 24 hours in air atmosphere, naturally cooling to room temperature, uniformly grinding,finally obtaining the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉0.25 at% Ce curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 16, Mg₄Ta₂O₉0.25 at% Ce shows an emission wavelength of 375nm, a full width at half maximum of 124nm and a luminous intensity of Mg₄Ta₂O₉1.1 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉0.25 at% Ce has a light yield of 14264 ph/MeV.

Example 16

Respectively weighing MgO and Ta according to the stoichiometric ratio of 4.1097:1:0.005₂O₅，La₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, presintering at 1300 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, pouring the raw materials out of the agate mortar, continuously and fully grinding, then putting into the corundum crucible, sintering at 1400 ℃ for 24 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

The X-ray diffraction peak of the product is as Mg in figure 1₄Ta₂O₉And a curve of 0.25 at% La. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). As shown in FIG. 17, Mg₄Ta₂O₉0.25 at% La shows that the emission wavelength is 347nm, the full width at half maximum is 89nm, and the luminous intensity is Mg₄Ta₂O₉1.8 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉The light yield of 0.25 at% La was 22752 ph/MeV.