A rate-type radiation sensing device with dose rate non-linear response and methods of use thereof
The nonlinear response ratio type radiation sensing device using a hybrid probe of NaLuF4:3Pr,5Er and NaLuF4:3Ce nanocrystals solves the problems of low measurement accuracy, complex structure and poor reliability of existing radiation sensors. It achieves high-precision self-calibration and accurate detection over a wide dose rate range, and is suitable for environmental monitoring, biomedical imaging and public safety inspection.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- DALI UNIV
- Filing Date
- 2026-03-05
- Publication Date
- 2026-05-29
AI Technical Summary
Existing radiation sensors suffer from low measurement accuracy, complex structure, poor reliability, poor real-time performance, and poor applicability, making it difficult to meet the demand for high-precision, low-cost, and real-time X-ray dose rate detection in complex environments.
A hybrid sensing probe using NaLuF4:3Pr,5Er and NaLuF4:3Ce nanocrystals is employed. The nonlinear response is achieved through the cross-relaxation process of Pr3+ and Er3+, combined with the linear response of Ce3+. Detection is performed using the fluorescence intensity ratio of the two nanocrystals, avoiding reliance on an additional excitation source and achieving self-calibration.
It achieves high-precision self-calibration detection, accurate detection over a wide dose rate range, has a simple structure that is easy to standardize and produce, adapts to various detection scenarios, and meets the real-time detection needs of environmental monitoring, biomedical imaging, and public safety inspection.
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Abstract
Description
Technical Field
[0001] This invention relates to a method for measuring the nonlinear variation of luminous intensity in a scintillator, belonging to the field of optical measurement. Background Technology
[0002] Radiation sensing technology plays a crucial role in environmental radiation monitoring, biomedical imaging, public safety inspection, and industrial non-destructive testing. Among these, radiation sensing methods based on the scintillation fluorescence properties of nanocrystals have attracted widespread attention due to their advantages such as fast response speed and ease of observation. These devices typically utilize the linear relationship between the scintillation fluorescence intensity of a single luminescent center and the radiation dose rate to achieve dose detection. Furthermore, by comparing two different linear relationships and optimizing the atomic number of the matrix material, as well as controlling the type and concentration of dopant ions, the detection performance can be improved. The formula is as follows: Where I is the scintillation fluorescence intensity, P is the radiation dose rate, and K and B are constants, where K represents the correspondence between the light intensity and dose rate of a single luminous center, and B represents the additional luminous intensity unaffected by X-rays.
[0003] However, existing technologies have several obvious drawbacks: firstly, they require additional excitation sources to maintain the constant. First, the use of linear luminescence intensity for comparison necessitates maintaining a constant term unaffected by X-rays to ensure effective dose rate measurement. This significantly reduces the complexity and reliability of the measurement equipment, making it unsuitable for complex testing environments. Second, it increases the cost and size of the detection instrument. Additional excitation sources may interfere with the instrument's own scintillation fluorescence, affecting the measurement results. To avoid interference, specific excitation sources or separate signal collection devices are required, inevitably increasing the cost and size of the detection instrument. Third, some sensing materials rely on the principle of cumulative dose detection, indirectly calculating the dose rate by accumulating radiation energy over a period of time. This makes it impossible to capture dynamic changes in the dose rate in real time, leading to detection lag in scenarios with rapidly fluctuating radiation dose rates, thus failing to meet real-time monitoring requirements. These shortcomings make it difficult for existing technologies to meet the demands for high-precision, low-cost, and real-time X-ray dose rate detection in complex environments. Summary of the Invention
[0004] The present invention aims to solve the technical problems of low measurement accuracy, complex structure, poor reliability, poor real-time performance and poor applicability of existing radiation sensors, and provides a ratiometric radiation sensing device with nonlinear response to dose rate and its usage method.
[0005] The ratiometric radiation sensing device with nonlinear response to dose rate of the present invention includes an X-ray excitation module, a hybrid sensing probe and a light signal collection module; wherein the hybrid sensing probe is a disc pressed from a uniform mixture of NaLuF4:3Pr,5Er nanocrystals and NaLuF4:3Ce nanocrystals.
[0006] Furthermore, the diameter of the disc is 5-12 mm and the thickness is 1-3 mm;
[0007] Furthermore, in the NaLuF4:3Pr,5Er nanocrystals, Pr 3+ The molar concentration of doping is 3%, Er 3+ The molar concentration of the dopant is 5%.
[0008] Furthermore, the NaLuF4:3Pr,5Er nanocrystalline material is prepared using NaLuF4 as a matrix via a combination of thermal decomposition and hot-injection techniques. The matrix material NaLuF4, due to its low phonon energy (effectively suppressing nonradiative relaxation), high atomic number (Lu has an atomic number of 71, enabling efficient absorption of X-ray energy), and mature synthesis process, is a suitable substrate for Pr... 3+ With Er 3+ The luminescence of Pr provides a stable crystal environment. 3+ As the main light-emitting center, its 3 P0 energy level towards 3 The H4 energy level transition generates a characteristic narrowband fluorescence at 486 nm, and the intensity response characteristics of this fluorescence are key to realizing nonlinear sensing; Pr 3+ The emission spectrum is as follows Figure 1 As shown. Er 3+ The purpose of introducing it is not to directly participate in luminescence, but to change Pr by constructing specific cross-relaxation paths. 3+ The excited-state population process—under X-ray irradiation, the NaLuF4 matrix absorbs X-ray energy and generates a large number of free electron-hole pairs, which are then transferred to Pr 3+ With Er 3+ Subsequently, cross-relaxation occurs between the excited state energy levels of the two, specifically including 3 P0(Pr)+ 4 I 13 / 2 (Er)→ 1 D2(Pr)+ 4 I 11 / 2 , 3 P0(Pr)+ 4 I 13 / 2 (Er)→ 3 F 3,4 (Pr)+ 4 F 7 / 2 , 3 P0(Pr)+4 I 13 / 2 (Er)→ 3 H6(Pr)+ 4 F 3 / 2,5 / 2 Three key processes. These cross-relaxation processes generate higher-order terms in the population product of two excited states, breaking Pr 3+ The linear response of the ion 3P0 energy level to X-ray dose rate results in a regular nonlinear change in fluorescence intensity at 486 nm with radiation dose rate, thus endowing the nanocrystal with the core characteristic of "dose rate sensitive". The mechanism of cross-relaxation during Pr and Er co-doping is shown in the diagram below. Figure 2 As shown.
[0009] Furthermore, in the NaLuF4:3Ce nanocrystals, Ce 3+ The molar concentration of the doping is 3%.
[0010] Furthermore, the NaLuF4:3Ce nanocrystalline material is prepared using NaLuF4 as a matrix via thermal decomposition. 3+ The doping molar concentration is controlled at 3%, which ensures high luminescence intensity while avoiding concentration quenching. 3+ The luminescence originates from the 5d→4f transition, producing broadband ultraviolet fluorescence in the 270~340nm range, Ce 3+ emission spectrum such as Figure 2 As shown, its luminescence process has two key characteristics: firstly, as a single-doped nanocrystal, Ce... 3+ The 5d energy level is not affected by the Er in NaLuF4:3Pr,5Er nanocrystals. 3+ The influence of the cross-relaxation process; secondly, in the radiation dose rate range of 0~20 mGy / s, Ce 3+ The fluorescence intensity and dose rate consistently maintain a stable linear growth trend, with a linear fitting coefficient of determination R² > 0.999. Based on these two characteristics, the nanocrystal can serve as a "stable reference unit," providing a reliable reference signal for ratiometric sensing and offsetting the influence of external interference on the detection results.
[0011] Furthermore, the mass ratio of NaLuF4:3Pr,5Er nanocrystals to NaLuF4:3Ce nanocrystals is 1:(0.9~1.1). The fabrication of the hybrid sensing probe is crucial for achieving synergistic response between the two nanocrystals. Mixing them at this mass ratio ensures that, under X-ray excitation, the characteristic fluorescence intensities of the two nanocrystals are within a suitable comparison range, avoiding errors in ratio calculation due to either signal being too strong or too weak. When the probe is irradiated by X-rays, the NaLuF4 matrix synchronously absorbs the X-ray energy and transfers it to their respective luminescent centers, while the Ce... 3+ Pr produces a linear response ultraviolet fluorescence 3+The 486nm fluorescence that produces a nonlinear response has a unique correlation between the fluorescence intensity ratio of the two and the change in radiation dose rate. Moreover, this ratio is not affected by fluctuations in probe concentration (such as uneven distribution of local nanocrystals) or drift in detection efficiency (such as changes in spectrometer sensitivity), thus achieving a self-calibration effect.
[0012] Furthermore, the compression is performed using an electric tablet press at a pressure of 60-65 MPa for 1-3 minutes. Under these conditions, the tablet compression ensures a dense probe structure.
[0013] Furthermore, the mixing described is mechanical mixing.
[0014] Furthermore, the X-ray excitation module is an adjustable dose rate X-ray source used to emit stable X-rays to the hybrid sensing probe to excite the characteristic scintillation fluorescence of the two nanocrystals, NaLuF4:3Pr,5Er and NaLuF4:3Ce.
[0015] Furthermore, the optical signal collection module can detect the characteristic fluorescence of NaLuF4:3Pr,5Er nanocrystals at 480~490nm and the characteristic fluorescence of NaLuF4:3Ce nanocrystals at 270~340nm, achieving accurate acquisition and separation of the two characteristic fluorescence signals, effectively eliminating signal crosstalk interference, and facilitating reading and use by operators.
[0016] The above-described method of using a ratiometric radiation sensing device with nonlinear dose rate response is performed according to the following steps:
[0017] First, the standard curve of the ratiometric radiation sensor was measured: the X-ray excitation source was turned on and preheated to ensure stable dose rate output; the standard radiation dosimeter was placed at the X-ray irradiation position, and the actual output dose rate of the X-ray excitation source was calibrated. The dose rates were set to 1.86, 3.73, 5.6, 7.47, 9.3, 11.2, 13.08, and 14.95 mGy / s, respectively. Under the above dose rates and in an environment without interference from ultraviolet and visible light signals, the fluorescence intensity I1 of the hybrid sensing probe at 480~490nm and the ultraviolet fluorescence intensity I2 at 270~340nm were tested, and the luminous intensity ratio I2 / I1 was calculated. The standard curve was obtained by fitting I2 / I1 as the ordinate and the corresponding dose rate as the abscissa.
[0018] During testing, ensure that the testing environment is free from interference from ultraviolet and visible light signals. Place the hybrid sensing probe and optical signal collection device in the environment where the X-ray dose needs to be tested, set the optical collection integration time, and collect the fluorescence intensity I3 at 480~490nm and the ultraviolet fluorescence intensity I4 at 270~340nm respectively. Calculate the fluorescence intensity ratio LIR = I4 / I3 from the obtained data, and compare the fluorescence intensity ratio LIR with the standard curve to obtain the real-time dose rate value.
[0019] Furthermore, the light collection integration time is 1000~5000ms.
[0020] The nonlinear response ratio-type radiation sensing device of this invention achieves high-precision detection of radiation dose rate by rationally combining two nanocrystalline materials with different sensitivities to radiation dose rate and utilizing the nonlinear response characteristics of their luminescence intensity ratio. This design not only fundamentally eliminates the drawback of relying on an additional excitation source by utilizing the ratio relationship, but also significantly improves the detection accuracy over a wide dose rate range through its nonlinear response characteristics, especially achieving higher relative sensitivity in the low-dose region. Simultaneously, the low phonon energy and high atomic number characteristics of the NaLuF4 matrix endow the nanocrystalline materials with excellent luminescence performance and X-ray absorption capability, effectively avoiding the problem of luminescence quenching. The advantages of this invention are as follows:
[0021] High-precision self-calibration detection: This device uses the fluorescence intensity ratio of two nanocrystals as the detection signal. The ratio method can automatically cancel out common interference factors such as probe concentration fluctuations, detection system efficiency drift, and probe wear changes, eliminating the need for frequent external calibration, significantly improving detection accuracy, and enabling real-time detection.
[0022] Wide dose rate range adaptability: via Pr 3+ With Er 3+ The cross-relaxation design enables NaLuF4:3Pr,5Er nanocrystals to exhibit a nonlinear dose response. Combined with the linear response of NaLuF4:3Ce nanocrystals, accurate detection can be achieved in a wide range of 1.86~14.95Gy / s. At low dose rates (1.86mGy / s), the relative sensitivity can reach 17.71%, which can meet the needs of various detection scenarios from low dose rates to high dose rates without the need to replace the sensing probe or adjust the device structure.
[0023] Simple structure and easy to standardize production: Both types of nanocrystals are prepared by mature thermal decomposition method, with clear process steps, readily available reagents, and controllable costs; the hybrid sensing probe is made by mechanical mixing and pressing, without the need for complex thin film deposition or device integration processes, resulting in high production efficiency and the ability to mass-produce probes of different specifications to suit different application scenarios.
[0024] The nonlinear response ratiometric radiation sensing device of the present invention can solve the defects of the prior art such as low measurement accuracy, weak anti-interference ability, poor wide dose adaptability and insufficient real-time performance, and meet the needs of high-precision and real-time detection of X-ray dose rate in multiple scenarios such as environmental monitoring, biomedical imaging, and public safety inspection. Attached Figure Description
[0025] Figure 1 For Pr 3+ The emission spectrum and its specific transition energy level diagram;
[0026] Figure 2 For Ce 3+ The emission spectrum;
[0027] Figure 3 The emission spectrum of the hybrid sensing probe in Example 1;
[0028] Figure 4 This is a diagram illustrating the mechanism of cross-relaxation when the hybrid sensing probe is co-doped with Pr and Er in Example 1.
[0029] Figure 5 Ce in Example 1 3+ and Pr 3+ The graph shows the change in the integral intensity ratio of the emission spectrum as a function of dose rate.
[0030] Figure 6 This is a schematic diagram of the ratiometric radiation sensing device with nonlinear response to dose rate in Example 1, where 1 is an X-ray excitation module, 2 is a hybrid sensing probe, 3 is an optical signal collection module, and 4 is a standard radiation dosimeter. Detailed Implementation
[0031] The beneficial effects of the present invention will be verified using the following examples.
[0032] Example 1: The ratiometric radiation sensing device with nonlinear response to dose rate in this example consists of an X-ray excitation module 1, a hybrid sensing probe 2, and a light signal collection module 3; wherein the hybrid sensing probe 2 is a disc with a diameter of 10 mm and a thickness of 2 mm, which is formed by uniformly mixing NaLuF4:3Pr,5Er nanocrystals and NaLuF4:3Ce nanocrystals at a mass ratio of 1:1 and pressing them together.
[0033] The preparation method of NaLuF4:3Pr,5Er nanocrystals is as follows:
[0034] (1) First, prepare the reagents required for the experiment: 1M PrCl3・6H2O methanol solution, 1M ErCl3・6H2O methanol solution, 1M LuCl3・6H2O methanol solution, 0.5M NaOH methanol solution, and 0.5M NH4F methanol solution. All reagents are analytical grade and do not require additional purification.
[0035] (2) Add 30 μL of PrCl3 methanol solution, 50 μL of ErCl3 methanol solution, 920 μL of LuCl3 methanol solution (total rare earth ion content 1 mmol), 10 mL of oleic acid (OA, as a surfactant), and 15 mL of octadecene (ODE, as a solvent) to a 50 mL three-necked flask. Probe with argon gas and heat the mixture at 180 °C for 45 minutes, then allow it to cool naturally to room temperature. After cooling, slowly add 5 mL of NaOH methanol solution and 6.6 mL of NH4F methanol solution to the flask, raise the temperature to 50 °C and maintain for 45 minutes. Then slowly raise the temperature to 110 °C and maintain for 15 minutes to remove excess methanol and water from the system and prevent subsequent contamination. The reaction continued, generating bubbles. Finally, the temperature was rapidly increased to 300℃ at a rate of 7℃ / min and maintained for 2 hours to allow nanocrystal growth. After the reaction was completed, the system was cooled to room temperature, and 5 mL of ethanol was added to the solution containing the nanocrystals to precipitate them. The precipitate was then collected by centrifugation at 8000 rpm for 5 minutes. The precipitate was washed three times with a 1:1 volume ratio of ethanol and methanol to remove residual OA and ODE. Finally, the precipitate was dispersed in 10 mL of cyclohexane to obtain a uniform NaLuF4:3Pr,5Er nanocrystal dispersion. The dispersion was then centrifuged at 8000 rpm for 5 minutes to obtain the precipitate. After drying, NaLuF4:3Pr,5Er nanocrystal powder was obtained.
[0036] The preparation method of NaLuF4:3Ce nanocrystals is as follows:
[0037] (1) First, prepare the reagents required for the experiment: 1M CeCl3 methanol solution, 1M LuCl3·6H2O methanol solution, 0.5M NaOH methanol solution, and 0.5M NH4F methanol solution. All reagents are analytical grade.
[0038] (2) Add 30 μL of CeCl3 methanol solution, 970 μL of LuCl3 methanol solution (total rare earth ion content 1 mmol), 10 mL of oleic acid (OA, as a surfactant), and 15 mL of octadecene (ODE, as a solvent) to a 50 mL three-necked flask, purge with argon gas, heat the mixture at 180 °C for 45 minutes, and then allow it to cool naturally to room temperature. After cooling, slowly add 5 mL of NaOH methanol solution and 6.6 mL of NH4F methanol solution to the flask, raise the temperature to 50 °C and hold for 45 minutes. Then slowly raise the temperature to 110 °C and hold for 15 minutes to remove excess methanol and water from the system and prevent subsequent reactions. Bubbles should be generated; finally, the temperature is rapidly increased to 300℃ at a rate of 7℃ / min and maintained for 2 hours to grow nanocrystals; after the reaction is completed, the system is cooled to room temperature, ethanol is added to the solution containing nanocrystals to precipitate the nanocrystals, and then the precipitate is collected by centrifugation at 8000 rpm for 5 minutes; the precipitate is washed 3 times with a 1:1 volume ratio of ethanol and methanol to remove residual OA and ODE, and finally the precipitate is dispersed in 10 mL of cyclohexane to obtain a uniform NaLuF4:3Ce nanocrystal dispersion, and then the precipitate is obtained by centrifugation at 8000 rpm for 5 minutes. After drying, NaLuF4:3Ce nanocrystal powder is obtained.
[0039] The preparation process of the hybrid sensing probe is as follows: NaLuF4:3Pr,5Er nanocrystalline powder and NaLuF4:3Ce nanocrystalline powder are placed in an agate mortar at a mass ratio of 1:1 and manually ground for 15 minutes to ensure that the two powders are mixed evenly; the mixed powder is poured into a circular tablet mold with a diameter of 10mm, flattened, and then placed in an electric tablet press, where a pressure of 63.7MPa is applied and maintained for 1 minute; after depressurization, the pressed sheet is removed to obtain the hybrid sensing probe, which has a thickness of 2mm.
[0040] The emission spectrum of the hybrid sensing probe prepared in Example 1 is shown below. Figure 3 As shown, from Figure 3 It can be seen that there is a broad and strong ultraviolet emission band in the 270–340 nm range, corresponding to Ce in NaLuF4:3Ce nanocrystals. 3+ The 5d→4f transition occurs; simultaneously, a distinct narrow-band emission peak is observed near 480–490 nm, originating from Pr in NaLuF4:3Pr,5Er nanocrystals. 3+ The transition from ³P0 to ³H4 occurs. The two emission signals are clearly separated and do not overlap, indicating that the fluorescence signal from the hybrid probe is easy to separate and acquire, providing a reliable spectral basis for subsequent ratio calculations.
[0041] The mechanism diagram of cross-relaxation when Pr and Er are co-doped in the hybrid sensing probe prepared in Example 1 is shown below. Figure 4As shown, under X-ray excitation, Pr 3+ The ³P0 energy level and Er 3+ of 4 I 13 The multipath energy transfer processes that occur between the / 2 energy levels include 3 P0(Pr)+ 4 I 13 / 2 (Er)→ 1 D2(Pr)+ 4 I 11 / 2 , 3 P0(Pr)+ 4 I 13 / 2 (Er)→ 3 F 3,4 (Pr)+ 4 F 7 / 2 , 3 P0(Pr)+ 4 I 13 / 2 (Er)→ 3 H6(Pr)+ 4 F 3 / 2,5 / 2 There are three key processes. These cross-relaxation processes introduce higher-order terms for the excited-state population, causing Pr 3+ The 486nm fluorescence intensity exhibits a nonlinear response relationship with the dose rate, which becomes the key physical mechanism for realizing ratiometric, self-calibrating detection.
[0042] The debugging and testing process for the ratiometric radiation sensor with nonlinear dose rate response in this embodiment is as follows:
[0043] I. Measurement of the Standard Curve for a Ratio-Type Radiation Sensing Device: Turn on the X-ray excitation source and preheat for 15 minutes to ensure stable dose rate output. Place the standard radiation dosimeter 4 at the X-ray irradiation position and calibrate the actual output dose rate of the X-ray excitation source. Set dose rates of 1.86, 3.73, 5.6, 7.47, 9.3, 11.2, 13.08, and 14.95 mGy / s respectively. Under these dose rates and in an environment free from UV and visible light interference, test the fluorescence intensity I1 at 486 nm and the UV fluorescence intensity I2 at 300 nm of the hybrid sensing probe, and calculate the luminescence intensity ratio I2 / I1. Plot the dose rate on the x-axis and I2 / I1 on the y-axis to obtain the standard curve, as shown below. Figure 5 As shown;
[0044] II. Testing: During testing, ensure that the testing environment is free from interference from ultraviolet and visible light signals. Place the hybrid sensing probe and optical signal collection device in the environment where the X-ray dose needs to be tested. Set the optical collection integration time to 1000ms. Collect the fluorescence intensity I3 at 486nm and the ultraviolet fluorescence intensity I4 at 300nm respectively. Calculate the intensity ratio LIR = I4 / I3 from the obtained data. Compare the intensity ratio LIR with the standard curve to obtain the real-time dose rate value.
[0045] The ratio-type radiation sensing device with nonlinear response to dose rate in this embodiment uses the ratio of fluorescence intensity of two nanocrystals as the detection signal. The ratio method can automatically cancel common interference factors such as probe concentration fluctuations, detection system efficiency drift, and probe wear changes, eliminating the need for frequent external calibration, significantly improving detection accuracy, and achieving high-precision self-calibration detection.
[0046] The ratiometric radiation sensing device with nonlinear dose rate response in Embodiment 1 can achieve accurate detection over a wide range of 1.86~14.95 Gy / s. Furthermore, at low dose rates of 0~1.86 mGy / s, the signal intensity is increased by extending the integration time of the optical signal collection module (e.g., adjusting it to 5000 ms). Simultaneously, piecewise fitting is performed in the low-dose region to further improve the relative sensitivity in this area, achieving a relative sensitivity of 17.71%. This satisfies various detection scenarios from low to high dose rates without requiring replacement of the sensing probe or adjustment of the device structure.
[0047] The ratiometric radiation sensing device with nonlinear response to dose rate in this embodiment uses two types of nanocrystals prepared by thermal decomposition. The hybrid sensing probe is made by mechanical mixing and pressing, which does not require complex thin film deposition or device integration processes. It has high production efficiency and can mass-produce probes of different specifications (such as changing the mold diameter to 5mm or 20mm and the thickness to 1mm or 3mm) to adapt to different application scenarios, which is conducive to standardization and promotion.
Claims
1. A ratiometric radiation sensing device with a nonlinear response to dose rate, characterized in that, This ratiometric radiation sensing device includes an X-ray excitation module, a hybrid sensing probe, and a light signal collection module; wherein the hybrid sensing probe is a disc pressed from a uniform mixture of NaLuF4:3Pr,5Er nanocrystals and NaLuF4:3Ce nanocrystals; wherein, in the NaLuF4:3Pr,5Er nanocrystals, Pr... 3+ The molar concentration of doping is 3%, Er 3+ The molar concentration of the doping is 5%; in the NaLuF4:3Ce nanocrystals, Ce 3+ The molar concentration of the doping is 3%.
2. The ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1, characterized in that, The diameter of the disc is 5-12 mm and the thickness is 1-3 mm.
3. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The NaLuF4:3Pr,5Er nanocrystalline material is prepared using NaLuF4 as a matrix through a combination of thermal decomposition and hot injection technology.
4. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The NaLuF4:3Ce nanocrystalline material is prepared using NaLuF4 as a matrix via thermal decomposition.
5. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The mass ratio of NaLuF4:3Pr,5Er nanocrystals to NaLuF4:3Ce nanocrystals is 1:(0.9~1.1).
6. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The compression is performed using an electric tablet press at a pressure of 60-65 MPa for 1-3 minutes.
7. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The X-ray excitation module is an adjustable dose rate X-ray source used to emit stable X-rays to the hybrid sensing probe to excite the characteristic scintillation fluorescence of two nanocrystals, NaLuF4:3Pr,5Er and NaLuF4:3Ce.
8. A ratiometric radiation sensing device with nonlinear response to dose rate according to claim 1 or 2, characterized in that, The optical signal collection module can detect the 486nm characteristic fluorescence of NaLuF4:3Pr,5Er nanocrystals and the 270~340nm characteristic fluorescence of NaLuF4:3Ce nanocrystals.
9. A method of using the ratiometric radiation sensing device with nonlinear response to dose rate as described in claim 1, characterized in that, This method is performed in the following steps: I. Standard Curve Measurement of Ratio-Type Radiation Sensing Device: Turn on the X-ray excitation source and preheat to ensure stable dose rate output; place the standard radiation dosimeter at the X-ray irradiation position, calibrate the actual output dose rate of the X-ray excitation source, set different dose rates respectively, and test the fluorescence intensity I1 at 480~490nm and the ultraviolet fluorescence intensity I2 at 270~340nm of the hybrid sensing probe under different dose rates and in an environment without ultraviolet and visible light signal interference, and calculate the luminous intensity ratio I2 / I1. Plot I2 / I1 as the ordinate and the corresponding dose rate as the abscissa to obtain the standard curve; II. Testing: During testing, ensure that the testing environment is free from interference from ultraviolet and visible light signals. Place the hybrid sensing probe and optical signal collection device in the environment where the X-ray dose needs to be tested. Set the optical collection integration time and collect the fluorescence intensity I3 at 480~490nm and the ultraviolet fluorescence intensity I4 at 270~340nm respectively. Calculate the fluorescence intensity ratio LIR = I4 / I3 from the obtained data. Compare the fluorescence intensity ratio LIR with the standard curve to obtain the real-time dose rate value.
10. A method of using a ratiometric radiation sensing device with nonlinear response to dose rate according to claim 9, characterized in that, The light collection integration time is 1000~5000ms.