A pure inorganic perovskite CsPbBr3 single crystal X-ray detector treated by Kr particle irradiation and a preparation method thereof

CN122909909APending Publication Date: 2026-10-13JILIN UNIVERSITY
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Patent Information

Application Number
CN202611087179.8
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2026-07-21
Publication Date
2026-10-13

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Technical Problem

[0005]针对钙钛矿单晶本征缺陷及传统化学掺杂易引入外源杂质的问题,本发明提供一种经Kr粒子辐照处理的纯无机钙钛矿CsPbBr3单晶X射线探测器及其制备方法

Benefits of technology

[0022](1)通过Kr粒子辐照处理,在不引入化学掺杂的情况下,实现对纯无机钙钛矿CsPbBr3单晶缺陷态的调控;

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Abstract

A kind of pure inorganic perovskite CsPbBr3 Single crystal X-ray detector treated by Kr particle irradiation and its preparation method belong to radiation detection and photoelectric detection technical field.The device is composed of first metal electrode, CsPbBr3 Single crystal and second metal electrode arranged in sequence, after the preparation of the device, it is treated by Kr particle irradiation of specific energy and total dose, so that the internal defect state of CsPbBr3 Single crystal is regulated and passivated under the premise of not introducing exogenous chemical impurities.After treated by Kr particle irradiation, the intrinsic dark current of the device is significantly reduced, and the trap dynamics and transport performance of carriers are greatly improved.Under X-ray irradiation, the detection sensitivity of the device is improved by about 10 times, and the minimum detection limit is greatly reduced to 0.29 mGy air ·s ‑1 The device has excellent transient switching response characteristics and working stability, and is suitable for high-performance X-ray detection and imaging applications.
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Description

Technical Field

[0001] This invention belongs to the field of radiation detection and photoelectric detection technology, specifically relating to a pure inorganic perovskite CsPbBr3 single crystal X-ray detector treated with Kr particle irradiation and its preparation method. Background Technology

[0002] X-ray detectors have wide applications in medical imaging, industrial non-destructive testing, and radiation monitoring. In recent years, halide perovskite materials have been considered strong candidates for next-generation X-ray detection materials due to their high carrier mobility, large X-ray absorption coefficient, and good solution processing properties.

[0003] Compared to organic-inorganic hybrid perovskite materials, pure inorganic perovskite CsPbBr3 single crystals, free of organic components, exhibit higher thermal and radiation stability, making them particularly suitable for high-energy radiation detection applications. However, intrinsic defects are inevitably generated during the growth and device fabrication of CsPbBr3 single crystals. These defect states readily participate in carrier recombination under applied electric fields or radiative excitation, thus limiting carrier transport performance and consequently affecting X-ray detection sensitivity and detection limit.

[0004] Existing methods for controlling defect states in perovskites mostly rely on chemical doping or interface modification. However, these methods often introduce exogenous impurities or increase the complexity of the device structure, which is detrimental to the long-term stability and reproducibility of the device. Therefore, there is an urgent need for a technical solution to effectively control defect states in pure inorganic perovskite single crystals without introducing chemical impurities, in order to further improve their X-ray detection performance. Summary of the Invention

[0005] To address the intrinsic defects of perovskite single crystals and the problem of easily introducing exogenous impurities through traditional chemical doping, this invention provides a pure inorganic perovskite CsPbBr3 single crystal X-ray detector treated with Kr particles and its preparation method.

[0006] The detector comprises a first metal electrode, a CsPbBr3 single crystal, and a second metal electrode arranged sequentially. After the device is fabricated, it is subjected to Kr particle irradiation treatment with a specific energy and total flux. This allows for the regulation and passivation of the defect states inside the CsPbBr3 single crystal without introducing exogenous chemical impurities. This invention irradiates the fabricated perovskite CsPbBr3 single crystal X-ray detector with heavy ion (Kr particle) irradiation treatment with a specific total flux. By utilizing the interaction between high-energy particles and the crystal lattice, the local recombination of the crystal microstructure and effective passivation of defect states are achieved without changing the chemical composition. This significantly improves the carrier (μτ product) transport characteristics, enhances the X-ray detection sensitivity of the device, and reduces the detection limit.

[0007] To achieve the above objectives, the present invention provides a method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles, comprising the following steps:

[0008] (I) Preparation of CsPbBr3 single crystals

[0009] (1) Preparation of precursor solution: Weigh CsBr and PbBr2 in DMSO solvent at a molar ratio of 1:2 to prepare a precursor solution with a CsBr concentration of 0.8~1.0 M;

[0010] (2) Refining and impurity removal: The precursor solution obtained in step (1) is precisely filtered through an organic polytetrafluoroethylene (PTFE) filter membrane with a pore size of 0.22 μm to ensure that the growth environment is free of micron-sized impurities;

[0011] (3) Seed crystal induction and screening: Under inert gas protection (such as in a high-purity nitrogen glove box, maintaining the water and oxygen content to be less than 0.1 ppm), take a small amount of the solution filtered in step (2) and put it into a crystallization container and seal it strictly; place the sealed crystallization container in a light-proof environment and heat it to 85~90℃, increasing the temperature by 1~2℃ every hour until rapid crystallization is induced to form seed crystals. Then, under inert gas protection, select seed crystals with flat surfaces, regular shapes and no twinning phenomenon as seed crystals for later use.

[0012] (4) Isothermal growth: Under the protection of inert gas, the seed crystal obtained in step (3) is put into a crystallization container containing the remaining precursor solution in step (3) and is sealed again; the sealed crystallization container is placed in a light-proof environment and a constant temperature of 80~100℃ for equilibration growth for 10~20 days to obtain CsPbBr3 single crystal.

[0013] (5) Post-processing: Take out the CsPbBr3 single crystal obtained in step (4) while it is still hot, and immediately rinse the surface residual liquid with anhydrous ethanol or toluene to prevent crystallization from damaging the surface morphology when the temperature drops. Then blow it dry with high-purity nitrogen and vacuum dry it.

[0014] (II) Device fabrication

[0015] A physical vapor deposition (PVD) method is used to deposit metal electrodes on both sides of a vacuum-dried CsPbBr3 single crystal at a rate of 0.1–0.5 Å / s, forming an X-ray detector with a metal electrode / CsPbBr3 single crystal / metal electrode structure. Furthermore, the metal electrodes are Au, Ag, Cr, or Cu electrodes, etc., and the PVD is performed under high vacuum conditions, with a vacuum level less than 7.0 × 10⁻⁶. -4 Pa, the thickness of the metal electrode is 20~50 nm.

[0016] In the X-ray detectors prepared under the above conditions, the thickness of the CsPbBr3 single crystal is 1–3 mm, and the effective detection area of ​​the device is 0.2–0.5 cm². 2 .

[0017] (III) Kr particle irradiation pretreatment

[0018] The prepared X-ray detector was placed in a particle beam irradiation system, and... 84 Kr ions were used as the irradiation source for Kr particle irradiation treatment in a vacuum environment (vacuum degree less than 10). -3 Thus, a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles was obtained. The single nucleon energy of the Kr particles was 1~20 MeV / u, the total energy was in the keV~GeV range, and the total flux of Kr particles on the metal electrode surface of the X-ray detector was 6.0×10⁻⁶. 6 ~2.6×10 7 ions / cm 2 The Kr particle irradiation treatment is performed at room temperature. Before acting on the device surface, the Kr particles pass sequentially through a titanium window with a thickness of 20–50 μm and an air layer with a thickness of 40–80 mm. During this process, due to the linear transport characteristics of high-energy heavy ions, the total flux of Kr particles reaching the device surface remains constant. Simultaneously, the titanium window and air layer act as energy-reducing media, causing controlled attenuation of the kinetic energy of the Kr ions. By adjusting the thickness of the titanium window and air layer to attenuate the initial energy of the Kr ions, it is ensured that the ions are precisely deposited at a specific depth (Bragg peak position) inside the crystal with specific residual energy, achieving local recombination of deep-level defect states. Through Kr particle irradiation treatment, the deep-level defect states inside the CsPbBr3 single crystal can be locally recombinated and controlled without changing the chemical composition of the CsPbBr3 single crystal, improving the electrical response characteristics of the device, thereby obtaining a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector treated with Kr particles.

[0019] (iv) X-ray detection performance test conditions

[0020] The fabricated X-ray detector was tested using a commercial X-ray source. The highest tube voltage of the X-ray tube was 70 kV, the maximum power was 12 W, and the X-ray exit window was a 0.25 mm thick beryllium window. Different dose rate conditions were obtained by adjusting the X-ray tube current.

[0021] Compared with the prior art, the present invention has the following beneficial effects:

[0022] (1) By irradiating Kr particles, the defect states of pure inorganic perovskite CsPbBr3 single crystals can be controlled without introducing chemical doping.

[0023] (2) After being irradiated with Kr particles, the dark current of the X-ray detector is reduced and the response current of the device under X-ray irradiation is significantly increased.

[0024] (3) The X-ray detection sensitivity of the fabricated X-ray detector is improved, and the detection limit is correspondingly reduced; the detection sensitivity of the device is improved by about 10 times (from 101 μC·Gy at a bias voltage of 10 V). air -1 ·cm -2 Increased to 1010 μC·Gy air -1 ·cm -2 Meanwhile, the minimum detection limit was significantly reduced to 0.29 mGy. air ·s -1 ;

[0025] (4) The X-ray detector obtained still maintains good working stability under high bias voltage and irradiation conditions, and has excellent transient switching response characteristics and working stability, making it suitable for high-performance X-ray detection and imaging applications. Attached Figure Description

[0026] Figure 1 The following are physical images and structural characterization diagrams of the pure inorganic perovskite CsPbBr3 single crystals prepared in the embodiments and comparative examples of this invention; wherein, (a) is an optical photograph of the obtained CsPbBr3 single crystal, and (b) is a comparison of the X-ray diffraction (XRD) test spectrum of the single crystal with the simulated standard spectrum.

[0027] Figure 2 : A schematic diagram of the structure of the pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles according to the present invention; as shown in the figure. Figure 2 As shown, the X-ray detector is composed of a first metal electrode, a CsPbBr3 single crystal, and a second metal electrode. The first metal electrode and the second metal electrode are respectively disposed on opposite sides of the CsPbBr3 single crystal, forming a bulk device structure of metal / CsPbBr3 / metal. In the embodiment of the present invention, Au is selected as the metal electrode.

[0028] Figure 3 The current signal response curve acquired in real time by the X-ray detector described in this invention during Kr particle irradiation treatment; such as... Figure 3 As shown, when the device is subjected to Kr particle irradiation, a source meter is connected (applying a DC bias voltage of 1V or 10V). The significant spike in the current signal (i.e. the prominent part of the signal) in the figure is the real-time current response curve of the detector to Kr ions, which intuitively reflects the dynamic change of current during the high-energy particle irradiation process.

[0029] Figure 4The present invention provides a comparison curve of the current response of the X-ray detector before and after Kr particle irradiation under X-ray irradiation conditions; for example... Figure 4 As shown, the figure contains four sub-figures (a), (b), (c), and (d), which respectively illustrate the steady-state and transient photoelectric response characteristics of the device before and after irradiation, as detailed below: Figure 4 (a) and Figure 4 (b) shows the current density-voltage (IV) characteristic curves of the device before and after Kr particle irradiation, respectively. (Comparison) Figure 4 (a) and Figure 4 (b) It can be seen that within the bias range of 0–10 V, the dark current of the device decreased significantly after Kr particle irradiation treatment; simultaneously, under the same X-ray dose rates (e.g., 1 mGy / s and 2 mGy / s), the photocurrent density of the irradiated device increased significantly. This indicates that Kr particle irradiation treatment effectively passivates internal crystal defects, reduces leakage current, and significantly improves carrier transport and collection efficiency. Figure 4 (c) and Figure 4 (d) The transient current-time (It) response curves of the device before and after Kr particle irradiation are shown respectively, illustrating the dynamic current response characteristics of the device under different bias voltages (5 V and 10 V) and stepwise varying X-ray dose rates (105 μGy / s to 2.00 mGy / s) when the X-ray source is repeatedly turned on and off. (Comparison) Figure 4 (c) and Figure 4 (d) shows that after being irradiated with Kr particles, the device not only maintained stable square wave step switching response characteristics, but also achieved an order-of-magnitude improvement in steady-state photocurrent response values ​​at various test dose rates, further demonstrating the significant effect of irradiation treatment on improving the dynamic response sensitivity of the device.

[0030] Figure 5 The present invention presents a comparison curve of the X-ray detection sensitivity and detection limit of the X-ray detector before and after Kr particle irradiation treatment. Figure 5 (a) and Figure 5 (b) shows the linear fitting curves of X-ray photocurrent density versus dose rate at 5 V and 10 V bias voltages for the device before and after Kr particle irradiation (before Kr). The slope of the fitted line represents the X-ray detection sensitivity of the device. (Comparison) Figure 5 (a) and Figure 5 (b) It can be seen that the sensitivity of the control group device before treatment is 40 μC·Gy at 5 V and 10 V bias voltages, respectively.air -1 ·cm -2 and 101 μC·Gy air -1 ·cm -2 After being irradiated with Kr particles, the device's sensitivity at 5 V and 10 V bias voltages was significantly improved to 540 μC·Gy. air -1 ·cm -2 and 1010 μC·Gy air -1 ·cm -2 The results show that irradiation treatment improved the detection sensitivity of the device by more than 10 times under different bias voltages. Figure 5 (c) and Figure 5 (d) These are linear fitting curves of the signal-to-noise ratio (SNR) as a function of X-ray dose rate at 5 V and 10 V biases, respectively, for the device before (Before Kr) and after (After Kr) irradiation. According to the SNR=3 criterion (shown by the black dashed line in the figure), the x-axis of the intersection of the fitted line and the SNR=3 dashed line represents the device's lowest detection limit. (Comparison) Figure 5 (c) and Figure 5 (d) It can be seen that the untreated control group device has a higher detection limit at 5 V and 10 V bias voltages, which is 5.37 mGy. air ·s -1 and 4.14 mGy air ·s -1 After Kr particle irradiation, the device's dark current noise floor was significantly reduced, and its detection limits at 5 V and 10 V bias voltages were substantially reduced to 0.25 mGy. air ·s -1 and 0.29 mGy air ·s -1 The detection limit is far below the standard dose rate requirement for conventional medical X-ray diagnostics, demonstrating that Kr particle irradiation treatment enhances the device's ability to detect weak signals. Detailed Implementation

[0031] Comparative Example 1: Conventional CsPbBr3 single-crystal X-ray detector without Kr particle irradiation treatment

[0032] (1) Preparation of CsPbBr3 single crystals:

[0033] Precursor preparation: In a glove box filled with high-purity nitrogen, with the water and oxygen contents both less than 0.1 ppm, CsBr and PbBr2 were weighed at a molar ratio of 1:2 and dissolved in 5 mL of dimethyl sulfoxide (DMSO) solvent. The mixture was continuously stirred magnetically at room temperature to prepare a precursor solution with a CsBr concentration of 0.9 M and a PbBr2 concentration of 1.8 M.

[0034] Purification and impurity removal: The precursor solution is precisely filtered through an organic polytetrafluoroethylene (PTFE) membrane with a pore size of 0.22 μm to ensure that the growth environment is free of micron-sized impurities.

[0035] Controlled growth: 1 mL of the filtered precursor solution was transferred to a clean glass bottle and sealed tightly. The bottle was heated to 90°C in a dark environment, with the temperature increased by 1°C every hour until rapid crystallization was induced to form seed crystals. Seed crystals with smooth surfaces, regular shapes, and no twins were selected under inert gas protection. These seed crystals were then placed into a crystallization container containing the remaining 4 mL of precursor solution and grown at a constant temperature of 100°C for 15 days to obtain CsPbBr3 single crystals. The morphology of the obtained CsPbBr3 single crystals was observed, and X-ray diffraction (XRD) tests were performed. The results are as follows: Figure 1 As shown. From Figure 1 As shown in the optical photograph (a), the prepared CsPbBr3 single crystal is orange in color, with a regular appearance and a smooth surface, exhibiting good macroscopic bulk continuity and light transmittance. Figure 1 As shown in the XRD pattern of (b), the actual test curve (upper part) of the single crystal sample is in high agreement with the simulated standard curve (lower part) of the CsPbBr3 single crystal. The actual test pattern only shows sharp diffraction peaks of specific crystal planes, without other polycrystalline diffraction peaks or impurity phase peaks. This indicates that the pure inorganic perovskite CsPbBr3 single crystal prepared by this controlled growth method does not contain obvious impurity phases and has extremely high crystal quality and good crystal plane orientation.

[0036] Post-processing: The obtained CsPbBr3 single crystal was taken out while hot and immediately rinsed with anhydrous ethanol to remove residual liquid on the surface to prevent crystallization from damaging the surface morphology when cooled. Then it was dried with high-purity nitrogen and placed in a vacuum drying oven to obtain a CsPbBr3 single crystal with a thickness of 2 mm.

[0037] (2) Fabrication of Au / CsPbBr3 / Au devices: Using a perforated metal mask (usually a stainless steel mask), the device is fabricated under a vacuum of less than 7.0 × 10⁻⁶. -4In a Pa thermal evaporation system, Au was vapor-deposited onto both sides of a vacuum-dried CsPbBr3 single crystal at a rate of 0.3 Å / s to obtain a 30 nm thick gold electrode. The effective detection area of ​​the device was 0.25 cm². 2 (That is, the area of ​​the overlapping part of the metal electrodes on the top and bottom sides of the single crystal, which is the effective area for receiving X-ray excitation and collecting charge carriers).

[0038] (3) X-ray sensitivity test

[0039] X-ray sensitivity testing was performed on the Au / CsPbBr3 / Au device under darkroom conditions. The top gold electrode served as the anode, and the bottom gold electrode as the cathode. A DC bias of 5 V and 10 V was continuously applied between the anode and cathode via a source meter to ensure stable operation. These DC biases are exemplary voltages and can be adjusted according to device size and testing conditions in practical applications. X-rays were directly irradiated into the device and incident on the internal CsPbBr3 single crystal.

[0040] By adjusting the tube current of the X-ray source, multiple sets of different X-ray dose rate conditions were obtained, namely 105 μGy / s, 431 μGy / s, 1.04 mGy / s, 1.64 mGy / s, and 2 mGy / s. The steady-state current response of the device was measured under each dose rate condition.

[0041] The steady-state current measured under non-X-ray irradiation conditions is defined as the dark current, while the steady-state current measured under X-ray irradiation conditions is defined as the photocurrent. The net photocurrent is obtained by subtracting the dark current from the photocurrent, and then further divided by the effective detection area of ​​the device to obtain the corresponding current density.

[0042] Plotting X-ray dose rate on the x-axis and current density on the y-axis, a linear fit was performed on multiple sets of data. The slope of the fitted line was defined as the X-ray sensitivity of the device. After unit conversion, the sensitivity unit is μC·Gy. air -1 ·cm -2 The detection limit test measures the current fluctuation of the device in the dark and calculates its variance (noise current). Combining the above sensitivity, the lowest detection limit of the device is calculated using the industry-known signal-to-noise ratio (SNR) of 3. The x-coordinate of the intersection of the fitted line and the dashed line with SNR=3 is the lowest detection limit of the device.

[0043] Test: Test display (corresponding) Figure 4 and Figure 5 (Before Kr), the control group device had X-ray sensitivities of 40 μC·Gy at 5 V and 10 V bias voltages, respectively. air-1 ·cm -2 and 101 μC·Gy air -1 ·cm -2 The detection limits are as high as 5.37 mGy. air ·s -1 and 4.14 mGy air ·s -1 .

[0044] Example 1: CsPbBr3 single-crystal X-ray detector irradiated with Kr particles

[0045] (1) Preparation of CsPbBr3 single crystal: According to the ratio and process in Comparative Example 1, the crystal was grown at 100℃ for 15 days, and then post-processed to obtain a CsPbBr3 single crystal with a thickness of 2 mm.

[0046] (2) Fabrication of Au / CsPbBr3 / Au devices: Same as Comparative Example 1, using a perforated metal mask as the mask, under a vacuum degree not exceeding 7.0 × 10⁻⁶. -4 In a Pa thermal evaporation system, Au was vapor-deposited onto both sides of a vacuum-dried CsPbBr3 single crystal at a rate of 0.3 Å / s to obtain a 30 nm thick gold electrode. The effective detection area of ​​the device was 0.25 cm². 2 (That is, the area of ​​the overlapping part of the metal electrodes on the top and bottom sides of the single crystal, which is the effective area for receiving X-ray excitation and collecting charge carriers.)

[0047] (3) Kr particle irradiation pretreatment: The device obtained in step (2) is placed in a particle beam irradiation system for irradiation treatment. The beamline vacuum at the irradiation terminal is maintained at 6.0 × 10⁻⁶. -8 Approximately mbar (high vacuum environment). Using... 84 Kr ions were used as the irradiation source, with an initial extraction energy set at 15.50 MeV / u (i.e., single nucleon energy, total particle energy approximately 1302 MeV). Upon exiting the terminal irradiation, the ion beam passed through a 30 μm thick titanium window and a 60 mm air layer before reaching the device surface. In this embodiment, the total terminal irradiation fluence of Kr ions was controlled to be 1.0 × 10⁻⁶. 7 ions / cm 2 The entire irradiation process is maintained at room temperature to avoid secondary damage to the crystal due to thermal effects, thereby obtaining a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles with specific total energy and total flux.

[0048] (4) Comparative Test: The test was conducted under the same conditions as Comparative Example 1. The test results are shown (corresponding to...). Figure 4 and Figure 5 After irradiation (“After Kr”), the device’s sensitivity at 5 V and 10 V bias voltages increased to 540 μC·Gy. air -1 ·cm -2 and 1010 μC·Gy air -1 ·cm -2 This represents an order-of-magnitude increase; simultaneously, the detection limits at 5 V and 10 V have been significantly reduced to 0.25 mGy. air ·s -1 and 0.29 mGy air ·s -1 This demonstrates that irradiation treatment improves detection performance.

Claims

1. A method for fabricating a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector treated with Kr particles, comprising the following steps: (I) Preparation of CsPbBr3 single crystals (1) Preparation of precursor solution: Weigh CsBr and PbBr2 in DMSO solvent at a molar ratio of 1:2 to prepare precursor solution; (2) Refining and impurity removal: The precursor solution obtained in step (1) is precisely filtered to ensure that the growth environment is free of micron-sized impurities; (3) Seed crystal induction and screening: Under the protection of inert gas, take a small amount of the solution filtered in step (2) and put it into the crystallization container and seal it strictly; place the sealed crystallization container in a light-proof environment and heat it to 85~90℃, increasing the temperature by 1~2℃ every hour until the rapid crystallization is induced to form seed crystals. Then, under the protection of inert gas, select seed crystals with flat surfaces, regular shapes and no twinning phenomenon as seed crystals. (4) Isothermal growth: Under the protection of inert gas, the seed crystal obtained in step (3) is put into a crystallization container containing the remaining precursor solution in step (3) and is sealed again; the sealed crystallization container is placed in a light-proof environment and a constant temperature of 80~100℃ for equilibration growth for 10~20 days to obtain CsPbBr3 single crystal. (5) Post-processing: Take out the CsPbBr3 single crystal obtained in step (4) while it is still hot, and immediately rinse the surface residual liquid with anhydrous ethanol or toluene to prevent crystallization from damaging the surface morphology when the temperature drops. Then blow it dry with high-purity nitrogen and vacuum dry it. (II) Device fabrication A metal electrode was deposited on both sides of a vacuum-dried CsPbBr3 single crystal using physical vapor deposition, forming an X-ray detector with a metal electrode / CsPbBr3 single crystal / metal electrode structure. (III) Kr particle irradiation pretreatment The prepared X-ray detector was placed in a particle beam irradiation system, and... 84 Using Kr ions as an irradiation source, Kr particles are irradiated in a vacuum environment to obtain a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles.

2. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: Precursor solutions with CsBr concentrations of 0.8–1.0 M were prepared.

3. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: Precision filtration is achieved through an organic polytetrafluoroethylene filter membrane with a pore size of 0.22 μm.

4. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: Metal electrodes were deposited at a rate of 0.1–0.5 Å / s.

5. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: The metal electrode is an Au electrode, an Ag electrode, a Cr electrode, or a Cu electrode.

6. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: Physical vapor deposition is performed under high vacuum conditions, wherein the vacuum level is less than 7.0 × 10⁻⁶. -4 Pa, the thickness of the resulting metal electrode is 20~50 nm.

7. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: In the obtained X-ray detectors, the thickness of the CsPbBr3 single crystal is 1–3 mm, and the effective detection area of ​​the device is 0.2–0.5 cm². 2 .

8. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 1, characterized in that: The vacuum level of Kr particle irradiation treatment is less than 10. -3 Pa, the single nucleon energy of the Kr particles is 1~20 MeV / u, the total energy is in the keV to GeV range, and the total flux of Kr particles on the surface of the metal electrode of the X-ray detector is 6.0 × 10⁻⁶. 6 ~2.6×10 7 ions / cm 2 The Kr particle irradiation treatment was carried out at room temperature.

9. The method for preparing a pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles as described in claim 8, characterized in that: Before acting on the device surface, Kr particles pass through a titanium window with a thickness of 20-50 μm and an air layer of 40-80 mm.

10. A pure inorganic perovskite CsPbBr3 single-crystal X-ray detector irradiated with Kr particles, characterized in that: It is prepared by the preparation method described in any one of claims 1 to 9.