阅读说明：本技术 一种稀土掺杂钽酸镁系列闪烁发光材料及其制备方法和应用 (Rare earth doped magnesium tantalate series scintillation luminescent material and preparation method and application thereof ) 是由 马云峰 郭超 徐家跃 秦康 吴金成 蒋毅坚 王森宇 于 2021-07-01 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系列闪烁发光材料及其制备方法和应用。本发明的稀土掺杂钽酸镁系列闪烁发光材料的化学组成表达式为：Mg-4Ta-2O-9:RE。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。所发明的闪烁发光材料,在X射线激发下,得到的不同稀土掺杂的Mg-4Ta-2O-9:RE样品光产额在13848～43917ph/MeV。其中样品Mg-4Ta-2O-9：0.25at％Gd光产额最高,是CsI(Tl)的81％,是Mg-4Ta-2O-9(简称MTO)和CdWO-4的2.4倍。(The invention discloses a rare earth doped magnesium tantalate series scintillation luminescent material and a preparation method and application thereof. The chemical composition expression of the rare earth doped magnesium tantalate series scintillation luminescent material is as follows: mg (magnesium) 4 Ta 2 O 9 RE. 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 scintillation luminescent material of the invention can obtain Mg doped with different rare earths under the excitation of X rays 4 Ta 2 O 9 The light yield of the RE sample is 13848-43917 ph/MeV. Wherein sample Mg 4 Ta 2 O 9 :0.25 at% Gd, 81% of CsI (Tl) and Mg 4 Ta 2 O 9 (MTO for short) and CdWO 4 2.4 times of the total weight of the powder.)

1. The rare earth doped magnesium tantalate series scintillation luminescent material is characterized in that the chemical composition expression is Mg₄Ta₂O₉RE, wherein the rare earth doping element RE is Sc³⁺、Lu³⁺、Yb³⁺、Tm³⁺、Er³⁺、Y³⁺、Ho³⁺、Dy³⁺、Tb³⁺、Gd³⁺、Eu^{3 +}、Sm³⁺、Nd³⁺、Pr³⁺、Ce³⁺And La³⁺At least one of (1).

2. The rare earth-doped magnesium tantalate series scintillating light emitting material according to claim 1, wherein the doping atomic percentage of the rare earth doping element RE is 0.25 at%.

3. The rare earth-doped magnesium tantalate series scintillating luminescent material according to claim 1, wherein the light yield of the rare earth-doped magnesium tantalate series scintillating luminescent material is 13848-43917 ph/MeV.

4. The method for preparing the rare earth-doped magnesium tantalate series scintillating luminescent material according to any one of claims 1 to 3, which is characterized by comprising the following steps: MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅And rare earth metal oxide, grinding the raw materials in an agate mortar, adding a solvent for dispersion, uniformly grinding, then putting into a corundum crucible, presintering 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 in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

5. The method according to claim 4, wherein the solvent is absolute ethyl alcohol.

6. The method for preparing rare earth-doped magnesium tantalate series scintillating luminescent materials according to claim 4, wherein the pre-sintering temperature is 1250-1300 ℃ and the time is 3-12 h.

7. The method for preparing rare earth-doped magnesium tantalate series scintillating luminescent materials according to claim 4, wherein the sintering temperature is 1300-1400 ℃ and the sintering time is 6-24 h.

8. The use of the rare earth-doped magnesium tantalate series scintillating luminescent materials of any one of claims 1 to 3 in the field of X-ray detection.

Technical Field

The invention relates to a rare earth doped magnesium tantalate series scintillation luminescent material and a preparation method and application thereof, belonging to the technical field of X-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 crystal is environment-friendly, has no problem that toxic elements pollute the environment from production, processing, application and recovery, has potential application prospect in the aspect of a radiographic probe, but has no report about further improvement of the light yield of MTO.

From a compositional standpoint, rare earths play a tremendous role in the development of scintillation crystals. Most of rare earth ions (Ce)³⁺-Yb³⁺) Utensil for cleaning buttockThe total energy level of 1639 electron layers with incomplete filling is up to 199177 transition numbers, which is a huge luminescence treasure base and has been widely used as activator and sensitizer of luminescent materials. However in Mg₄Ta₂O₉Rare earth ions are doped in the material, but the rare earth ions are rarely reported.

Disclosure of Invention

The technical problem solved by the invention is as follows: how to further increase Mg₄Ta₂O₉The light yield of the crystal.

In order to solve the technical problem, the invention provides a rare earth doped magnesium tantalate series scintillation luminescent material, the chemical composition expression of which is Mg₄Ta₂O₉RE, wherein the rare earth doping element RE is Sc³⁺、Lu³⁺、Yb³⁺、Tm³⁺、Er³⁺、Y³⁺、Ho³⁺、Dy³⁺、Tb³⁺、Gd³⁺、Eu³⁺、Sm³⁺、Nd³⁺、Pr³⁺、Ce³⁺And La³⁺At least one of (1).

Preferably, the doping proportion of the rare earth doping element RE is 0.25 at%.

Preferably, the light yield of the rare earth doped magnesium tantalate series scintillation luminescent material is 13848-43917 ph/MeV.

The invention also provides a preparation method of the rare earth doped magnesium tantalate series scintillating luminescent material, which comprises the following steps: MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅And rare earth metal oxide, grinding the raw materials in an agate mortar, adding a solvent for dispersion, uniformly grinding, then putting into a corundum crucible, presintering 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 in air atmosphere, naturally cooling to room temperature, and uniformly grinding to finally obtain the product.

Preferably, the solvent is absolute ethyl alcohol.

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

Preferably, the sintering temperature is 1300-1400 ℃, and the time is 6-24 h.

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

Compared with the prior art, the invention has the following 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, the conditions are easy to control, and the scintillation luminescent material has no toxic or radioactive elements, has high light output under the excitation of high-energy rays, stably exists in the air and is not easy to deliquesce;

2. the invention utilizes the unique electronic configuration structure of rare earth ions to 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 to form a rare earth scintillation crystal with excellent scintillation performance;

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 13837-43917 ph/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 accordance with an embodiment of the invention;

FIG. 2 is Mg₄Ta₂O₉0.25 at% Sc scintillating luminescent material emission measured under X-ray excitationA spectrogram;

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 Mg₄Ta₂O₉An emission spectrogram of the 0.25 at% Dy scintillating luminescent material is 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 Mg₄Ta₂O₉0.25 at% Pr scintillating luminescent materialMeasuring an emission spectrogram of the material under the excitation of X rays;

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

A preparation method of rare earth (Sc) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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, 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% Sc (at% represents atomic percent). As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). Mg as shown in FIG. 2₄Ta₂O₉0.25 at% Sc, which indicates 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

A preparation method of a rare earth (Lu) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

weighing according to stoichiometric ratioMgO，Ta₂O₅，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 graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). Mg as shown in FIG. 3₄Ta₂O₉0.25 at% Lu, indicating 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

A method for preparing rare earth (Yb) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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, 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 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). Mg as shown in FIG. 4₄Ta₂O₉0.25 at% Yb, shows an emission wavelength of 343nm, a full width at half maximum of 89nm, and an emission spectrum excited by 30keV X-rayLight 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

A preparation method of a rare earth (Tm) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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 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% Sc curve. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). Mg as shown in FIG. 5₄Ta₂O₉0.25 at% Tm, indicating 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 of the total length of the film, and the full width at half maximum is 20 nm.

Example 5

A preparation method of a rare earth (Er) -doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，Er₂O₃Grinding the raw materials in an agate mortar, adding absolute ethyl alcohol as a dispersing agent, uniformly grinding, then putting into a corundum crucible, and putting in an air atmosphere at 1 DEGPresintering at 260 ℃ for 6 hours, naturally cooling to room temperature, pouring the raw materials out of an agate mortar, continuously and fully grinding, then putting the raw materials into a corundum crucible, sintering at 1330 ℃ for 12 hours in air atmosphere, naturally cooling to room temperature, and uniformly grinding to 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). Mg as shown in FIG. 6₄Ta₂O₉0.25 at% Er, and 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

A preparation method of rare earth (Y) doped magnesium tantalate series scintillating luminescent materials comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 7₄Ta₂O₉0.25 at% Y, indicating that the emission wavelength is 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

A preparation method of a rare earth (Ho) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 8₄Ta₂O₉0.25 at% Ho, indicating that the emission wavelength is 349nm, the full width at half maximum is 117nm, and the luminous intensity is 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

A preparation method of a rare earth (Dy) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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 are compared with the standardThe diffraction peaks (PDF #38-1458) correspond. Mg as shown in FIG. 9₄Ta₂O₉0.25 at% Dy, and shows that the emission wavelength is 350nm, the full width at half maximum is 91nm, and the luminous intensity is 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 459nm, and luminous intensity at Mg₄Ta₂O₉1.3 times of the total length of the film, and the full width at half maximum is 20 nm.

Example 9

A preparation method of rare earth (Tb) doped magnesium tantalate series scintillating luminescent materials comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 10₄Ta₂O₉0.25 at% Tb, indicating that its emission wavelength is 359nm, full width at half maximum is 98nm and its luminous intensity is 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

A preparation method of rare earth (Gd) -doped magnesium tantalate series scintillating luminescent materials comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 11₄Ta₂O₉0.25 at% Gd, which has an emission wavelength of 345nm, a full width at half maximum of 92nm, and a light emission intensity of 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

A preparation method of rare earth (Eu) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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 curves in the figure, allThe diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). Mg as shown in FIG. 12₄Ta₂O₉0.25 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, the light yield is 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

A preparation method of rare earth (Sm) doped magnesium tantalate series scintillating luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 13₄Ta₂O₉0.25 at% Sm, shows an emission spectrum excited by 30keV X-rays and has an emission wavelength of 348nm, a full width at half maximum of 86nm and a luminous intensity of 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

A preparation method of a rare earth (Nd) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

in stoichiometric ratioMgO and Ta are weighed respectively₂O₅，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. As can be seen from the graph, all diffraction peaks correspond to the standard diffraction peaks (PDF # 38-1458). Mg as shown in FIG. 14₄Ta₂O₉0.25 at% Nd, showing an emission wavelength of 345nm, a full width at half maximum of 90nm, and a luminous intensity of 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

A preparation method of rare earth (Pr) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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). Mg as shown in FIG. 15₄Ta₂O₉0.25 at% Pr, indicating a half-height emission wavelength of 347nmWidth of 98nm and 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

A preparation method of rare earth (Ce) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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, and uniformly grinding to finally obtain 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). Mg as shown in FIG. 16₄Ta₂O₉0.25 at% Ce, and an emission spectrum of 30keV X-ray excitation showing that the emission wavelength is 375nm, the full width at half maximum is 124nm, and the luminous intensity is 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

A preparation method of a rare earth (La) doped magnesium tantalate series scintillation luminescent material comprises the following steps:

MgO and Ta are respectively weighed according to the stoichiometric ratio₂O₅，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 then putting into the corundum crucibleGrinding uniformly to 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). Mg as shown in FIG. 17₄Ta₂O₉0.25 at% La, showing an emission wavelength of 347nm, a full width at half maximum of 89nm, and a luminous intensity of Mg₄Ta₂O₉1.7 times of the total amount of Mg, and detecting to obtain Mg₄Ta₂O₉The light yield of 0.25 at% La was 22752 ph/MeV.

While the invention has been described with respect to a preferred embodiment, it will be understood by those skilled in the art that various changes in form and details may be made therein without departing from the spirit and scope of the invention.