CN110068854B - Scintillator device with nested microsphere array photon structure surface - Google Patents
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- G01T1/16—Measuring radiation intensity
- G01T1/20—Measuring radiation intensity with scintillation detectors
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- G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
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Abstract
The invention relates to a scintillator device with a nested microsphere array photon structure surface, which comprises a scintillator, a large-size microsphere array arranged on the upper surface of the scintillator, a conformal layer deposited on the upper surface of the large-size microsphere array, and a small-size microsphere array arranged on a transparent material. Compared with the prior art, the photon structure can greatly improve the light emitting efficiency of the scintillator and realize mass production.
Description
Technical Field
The invention belongs to the field of nuclear radiation detection, and particularly relates to a scintillator device with a nested microsphere array photon structure surface, wherein the structural scintillator can obviously improve the light output of the scintillator in a radiation detector, so that the sensitivity and the signal to noise ratio of a detection system are improved.
Background
The scintillator is a functional material for absorbing high-energy particles or high-energy rays and converting the high-energy particles or high-energy rays into visible light, and the visible light emitted by the scintillator, namely the scintillation light, is received by a subsequent photoelectric detection device such as a photomultiplier tube, a photodiode and a CCD device, so that the detection of the high-energy particles or the high-energy rays is realized, the scintillator is a core component in a scintillation detection system, and the luminous characteristic of the scintillator directly determines the performance of the detection system. Scintillation detection systems play an increasingly important role in high-energy physics experiments, nuclear weapon experimental diagnostics, nuclear medicine imaging, cosmic ray detection and security inspection, and are responsible for irreplaceable functions.
However, most scintillators have refractive indices between 1.5 and 2.5, and high refractive indices result in total internal reflection of the luminescence inside the scintillator, and the efficiency of light output is greatly limited. Thus reducing the sensitivity and signal-to-noise ratio of the detection system. The scintillator light output efficiency can be improved to a certain extent by adopting the photon artificial microstructure method, and the method has important application in the radiation detection field. Chinese patent CN104280761a, for example, discloses a method for preparing photonic crystal structures by microsphere self-assembly for achieving an improvement in scintillation light output efficiency. However, the regulation effect of the microsphere array with a single structure size on the scintillator is limited, and the photon structure must be improved in order to further improve the light output efficiency.
Disclosure of Invention
It is an object of the present invention to overcome the above-mentioned drawbacks of the prior art by providing a scintillator device with a nested microsphere array photon structured surface with improved light output efficiency.
The aim of the invention can be achieved by the following technical scheme:
a scintillator device having a nested microsphere array photonic structure surface, comprising
The light source of the scintillator is arranged on the surface of the substrate,
a large-sized microsphere array disposed on an upper surface of the scintillator,
a conformal layer deposited on the upper surface of the array of large-sized microspheres,
an array of small-sized microspheres disposed on a transparent material.
The scintillator comprises a plastic scintillator, a glass scintillator, a ZnO scintillator, lu 2 SiO 5 Ce scintillator, (Lu, Y) 2 SiO 5 Ce scintillator, bi 4 Ge 3 O 12 Scintillator, Y 3 Al 5 O 12 Ce scintillator, csI: tl scintillator, naI: tl scintillator or PbWO 4 A scintillator.
The large-size microsphere array is an array formed by polystyrene microspheres with the size of 2-10 micrometers, and the polystyrene microspheres are prepared into an array with a single-layer hexagonal close-packed structure through self-assembly. The size of the polystyrene microsphere is firstly far greater than the light-emitting wavelength of the scintillator, and when 2 microns (which is about 4 times of the light-emitting wavelength) is selected, part of light can be firstly introduced into the large-size microsphere by a geometrical optics method, so that a foundation is laid for the subsequent extraction of the small-size microsphere. The upper limit of 10 μm is because of the limitation of the preparation of the polystyrene microsphere self-assembly method, and the larger-sized spheres are difficult to self-assemble into a periodic array structure.
The conformal layer is a material layer which is not deliquescent and transparent in the light emitting range of the scintillator, and the material of the conformal layer comprises TiO 2 、ZnO、Al 2 O 3 Or SiO 2 The thickness is 10-50 nanometers, the preparation is carried out by adopting an atomic layer deposition method, the atomic layer deposition method is deposited on the upper surface of a large-size microsphere array, the layer has the function of realizing good fixation of the large-size microsphere array below the atomic layer deposition method, the effect of being too thin to play a role of fixation is achieved, the appearance of the damaged surface is too thick, and the damaged surface gradually becomes a planar structure, so that the coupling between the large microsphere and the small microsphere is influenced, and therefore, the atomic layer deposition method is proved to be a proper scale through a large number of experiments.
The small-size microsphere array is a polystyrene microsphere array with the size of 0.3-1 micron, and the small-size microspheres are inlaid on the surface of the large-size microsphere array covered with the conformal layer by adopting a self-assembly method. The small-size microsphere has the function of extracting light in the large microsphere through a near-field coupling method to obtain enhancement of light output efficiency, the size range mainly covers the range of the scintillator emission wavelength according to the basic rule of near-field coupling, and the range of 0.3-1 micron is selected to be more suitable. The polystyrene microsphere is too large or too small, which can reduce coupling efficiency and even cannot achieve the effect of near-field coupling.
The nested structure formed by the large-size microsphere array, the conformal layer and the small-size microsphere array can lead the light inside the scintillator to be distributed through the special contact between the large-size microsphere array and the surface of the scintillator, and more scintillation light is guided into the large-size microsphere array by utilizing the principle of geometrical optics, and the size of the large-size microsphere is far greater than the wavelength (usually between 0.4 and 0.6 microns) of scintillation luminescence, so that the geometrical optics principle is satisfied. Light inside the large microsphere can be extracted again by the array of small microspheres attached to the surface of the large microsphere by means of near field diffraction, resulting in efficient exit. The diameter of the small microsphere is close to the luminous wavelength range of the scintillator, when the small microsphere interacts with the scintillation light, the small microsphere has obvious near-field diffraction effect, and the diffraction effect can finally realize effective reflection of a far field, namely the improvement of light output efficiency.
Compared with the prior art, the invention has the following advantages:
1. the photon structure can greatly improve the light-emitting efficiency of the scintillator.
2. The structure preparation method is easy to prepare a scintillator structure with a large area, so that the requirements of most detection systems on the scintillator can be met, and mass production is realized.
Drawings
FIG. 1 is a schematic structural diagram of a scintillator device having a nested microsphere array photonic structure surface;
FIG. 2 is a scanning electron microscope image of a scintillator device having a nested microsphere array photonic structure surface prepared in example 1;
fig. 3 is an emission spectrum of the scintillator device with the surface of the nested microsphere array photonic structure prepared in example 1 under X-ray excitation.
In the figure, 1-scintillator, 2-large-sized microsphere array, 3-conformal layer, 4-small-sized microsphere array.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the present invention, but are not intended to limit the invention in any way. It should be noted that variations and modifications could be made by those skilled in the art without departing from the inventive concept. These are all within the scope of the present invention.
Example 1
A scintillator device having a nested microsphere array photonic structure surface includes a scintillator, a large-sized microsphere array disposed on an upper surface of the scintillator, a conformal layer deposited on the upper surface of the large-sized microsphere array, and a small-sized microsphere array disposed on a transparent material.
The scintillator used in this example was a ZnO scintillator, and the large-size microsphere array was an array of 2 μm polystyrene microspheres, which were self-assembled to obtain a monolayer hexagonal close-packed structure array. The conformal layer is a material layer which is not deliquescent and transparent in the light emitting range of the scintillator, the material of the conformal layer used in the embodiment is ZnO, the thickness is 20 nanometers, the material is prepared by adopting an atomic layer deposition method, the material is deposited on the upper surface of the large-size microsphere array, and the function of the material layer is to realize good fixation of the large-size microsphere array below the material layer. The small-size microsphere array is a polystyrene microsphere array with the size of 0.5 microns, and the small-size microspheres are inlaid on the surface of the large-size microsphere array covered with the conformal layer by adopting a self-assembly method.
Example 2
A scintillator device having a nested microsphere array photonic structure surface includes a scintillator, a large-sized microsphere array disposed on an upper surface of the scintillator, a conformal layer deposited on the upper surface of the large-sized microsphere array, and a small-sized microsphere array disposed on a transparent material.
The scintillator used in this example is Y 3 Al 5 O 12 The Ce scintillator, the large-size microsphere array is an array formed by polystyrene microspheres with the size of 5 microns, and the polystyrene microspheres are prepared into an array with a single-layer hexagonal close-packed structure through self-assembly. The conformal layer is a material layer which is not deliquescent and transparent in the light emitting range of the scintillator, and the material of the conformal layer used in the embodiment is SiO 2 The thickness is 10 nanometers, the preparation is carried out by adopting an atomic layer deposition method, the atomic layer deposition is deposited on the upper surface of the large-size microsphere array, and the layer has the function of realizing the good fixation of the large-size microsphere array below the atomic layer deposition. The small-size microsphere array is a polystyrene microsphere array with the size of 0.3 microns, and the small-size microspheres are inlaid on the surface of the large-size microsphere array covered with the conformal layer by adopting a self-assembly method.
Example 3
A scintillator device having a nested microsphere array photonic structure surface includes a scintillator, a large-sized microsphere array disposed on an upper surface of the scintillator, a conformal layer deposited on the upper surface of the large-sized microsphere array, and a small-sized microsphere array disposed on a transparent material.
The scintillator used in this example was PbWO 4 Scintillator, large-size microsphere array isAnd an array formed by 10 micrometers of polystyrene microspheres, wherein the polystyrene microspheres are prepared into an array with a single-layer hexagonal close-packed structure through self-assembly. The conformal layer is a material layer which is not deliquescent and transparent in the light emitting range of the scintillator, and the material of the conformal layer used in the embodiment is Al 2 O 3 The thickness is 50 nanometers, the preparation is carried out by adopting an atomic layer deposition method, the atomic layer deposition is deposited on the upper surface of the large-size microsphere array, and the layer has the function of realizing the good fixation of the large-size microsphere array below the atomic layer deposition. The small-size microsphere array is a polystyrene microsphere array with the size of 1 micrometer, and the small-size microspheres are inlaid on the surface of the large-size microsphere array covered with the conformal layer by adopting a self-assembly method.
The nested structure formed by the large-size microsphere array, the conformal layer and the small-size microsphere array can lead the light inside the scintillator to be distributed through the special contact between the large-size microsphere array and the surface of the scintillator, and more scintillation light is guided into the large-size microsphere array by utilizing the principle of geometrical optics, and the size of the large-size microsphere is far greater than the wavelength (usually between 0.4 and 0.6 microns) of scintillation luminescence, so that the geometrical optics principle is satisfied. Light inside the large microsphere can be extracted again by the array of small microspheres attached to the surface of the large microsphere by means of near field diffraction, resulting in efficient exit. The diameter of the small microsphere is close to the luminous wavelength range of the scintillator, when the small microsphere interacts with the scintillation light, the small microsphere has obvious near-field diffraction effect, and the diffraction effect can finally realize effective reflection of a far field, namely the improvement of light output efficiency.
Example 4
The scintillator substrate used in this example was 20X20mm in surface area 2 Bi with thickness of 3mm 4 Ge 3 O 12 A scintillator. The size of the large-size microspheres is 4.5 microns, and the size of the small-size microspheres is 0.5 microns. The conformal layer is TiO with the thickness of 10 nanometers 2 A layer. Scintillators were purchased from Shanghai Sikasi corporation. Microspheres were purchased from Alfa Aesar company.
The preparation method comprises the following steps:
(1) Treating a silicon wafer, preparing a sodium dodecyl methyl sulfate solution with the mass fraction of 5%, standing the silicon wafer in the solution for more than 24 hours.
(2) Preparing polystyrene microsphere solution, mixing a certain amount of polystyrene microsphere solution with the diameter of 4.5 micrometers (the mass fraction of the microsphere solution is 2.5%) with absolute ethyl alcohol by ultrasound according to the proportion of 1:2, and mixing a certain amount of polystyrene microsphere solution with the diameter of 0.5 micrometers (the mass fraction of the microsphere solution is 2.5%) with absolute ethyl alcohol by ultrasound according to the proportion of 1:4.
(3) The prepared 4.5-micrometer polystyrene microsphere solution is dripped onto the cleaned and dried silicon wafer, and the silicon wafer is waited for full diffusion and complete volatilization of water.
(4) Slowly putting the silicon chip dropping the microsphere solution into deionized water to separate the microsphere array from the silicon chip and float on the water surface.
(5) And (3) taking the microsphere array out of the water by using the cleaned scintillator substrate, and waiting for the water to volatilize and completely attaching the microsphere array to the surface of the scintillator to obtain the single-layer hexagonal close-packed microsphere array formed by the polystyrene microspheres with the diameters of 4.5 micrometers.
(6) Conformally depositing a layer of TiO on the microsphere surface by adopting an atomic layer deposition technology (equipment model Picosun SUNALE R-200) 2 The specific preparation process is as follows: titanium tetrachloride and water are used as precursors of titanium and oxygen, which react to form titanium dioxide and deposit on the sample surface. During deposition, the temperature and pressure in the reaction chamber were set at 75℃and 17hPa, respectively. In the deposition process of each atomic layer, a precursor is firstly introduced by a pulse of 0.3s, and TiO with the thickness of 0.08nm is formed on the surface of a sample after the reaction is completed 2 The conformal layer was then purged with nitrogen. The steps are circulated for 125 times to prepare the TiO with the total thickness of 10nm 2 And a conformal layer.
(7) Will pass through TiO 2 The sample with conformal protection is repeatedly subjected to the experimental steps to scoop out microspheres with the diameter of 0.5 micrometer to form an array, and finally the scintillator device with the surface of the photon structure of the nested microsphere array is obtained, the structure of the scintillator device is shown as figure 1, the scintillator device comprises a scintillator 1, a large-size microsphere array 2 arranged on the upper surface of the scintillator 1, the scintillator device consists of polystyrene microspheres with the size of 4.5 micrometers, a conformal layer 3 deposited on the upper surface of the large-size microsphere array 2 and embedded on a coverA small-sized microsphere array 4 having a surface of the large-sized microsphere array 2 with a conformal layer 3.
Fig. 2 is a scanning electron microscope image of a sample showing the surface of a large sphere covered with a small sphere structure, which is a desired structural feature. Fig. 3 is an emission spectrum of a sample tested under X-ray excitation, showing an increase of about 3 times at the peak and a 2.5 times increase of the entire wavelength integration region, showing a significant effect, when compared to a reference sample with and without structure.
The previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.
Claims (4)
1. A scintillator device having a surface of a nested microsphere array photonic structure, comprising
The light source of the scintillator is arranged on the surface of the substrate,
a large-sized microsphere array disposed on an upper surface of the scintillator,
a conformal layer deposited on the upper surface of the array of large-sized microspheres,
an array of small-sized microspheres disposed on a transparent material;
the scintillator comprises a plastic scintillator, a glass scintillator, a ZnO scintillator, lu 2 SiO 5 Ce scintillator, (Lu, Y) 2 SiO 5 Ce scintillator, bi 4 Ge 3 O 12 Scintillator, Y 3 Al 5 O 12 Ce scintillator, csI: tl scintillator, naI: tl scintillator or PbWO 4 A scintillator;
the large-size microsphere array is an array formed by polystyrene microspheres with the size of 2-10 micrometers;
the polystyrene microsphere is prepared into an array with a single-layer hexagonal close-packed structure through self-assembly;
the small-size microsphere array is a polystyrene microsphere array with the size of 0.3-1 micron;
the small-size microspheres are inlaid on the surface of the large-size microsphere array covered with the conformal layer by adopting a self-assembly method.
2. A scintillator device having a nested microsphere array photonic structure surface according to claim 1, wherein the conformal layer is a layer of material that is non-deliquescent and transparent over the scintillator's light emitting range.
3. A scintillator device having a nested microsphere array photonic structure surface according to claim 1 or 2, wherein the material of the conformal layer comprises TiO 2 、ZnO、Al 2 O 3 Or SiO 2 。
4. A scintillator device having a nested microsphere array photonic structure surface according to claim 1 or 2, wherein the conformal layer has a thickness of 10-50 nm.
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| KR100629866B1 (en) * | 2003-12-23 | 2006-09-29 | 엘지전자 주식회사 | Fabrication method of microlens array with controlled conic coefficient |
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| CN105223602A (en) * | 2014-05-28 | 2016-01-06 | 中国科学院宁波材料技术与工程研究所 | Ceramic flashing volume array and preparation method thereof |
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