CN106842384B - A kind of composite photonic crystal structure scintillator - Google Patents

A kind of composite photonic crystal structure scintillator Download PDF

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Publication number
CN106842384B
CN106842384B CN201710146652.XA CN201710146652A CN106842384B CN 106842384 B CN106842384 B CN 106842384B CN 201710146652 A CN201710146652 A CN 201710146652A CN 106842384 B CN106842384 B CN 106842384B
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layer
crystal structure
scintillator
photonic crystal
bullet
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CN106842384A (en
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刘波
程传伟
顾牡
陈鸿
张娟楠
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Tongji University
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    • GPHYSICS
    • G02OPTICS
    • G02BOPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B1/00Optical elements characterised by the material of which they are made; Optical coatings for optical elements
    • G02B1/10Optical coatings produced by application to, or surface treatment of, optical elements
    • G02B1/11Anti-reflection coatings
    • G02B1/118Anti-reflection coatings having sub-optical wavelength surface structures designed to provide an enhanced transmittance, e.g. moth-eye structures
    • GPHYSICS
    • G02OPTICS
    • G02BOPTICAL ELEMENTS, SYSTEMS OR APPARATUS
    • G02B1/00Optical elements characterised by the material of which they are made; Optical coatings for optical elements
    • G02B1/002Optical elements characterised by the material of which they are made; Optical coatings for optical elements made of materials engineered to provide properties not available in nature, e.g. metamaterials
    • G02B1/005Optical elements characterised by the material of which they are made; Optical coatings for optical elements made of materials engineered to provide properties not available in nature, e.g. metamaterials made of photonic crystals or photonic band gap materials

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  • Physics & Mathematics (AREA)
  • General Physics & Mathematics (AREA)
  • Optics & Photonics (AREA)
  • Chemical & Material Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Measurement Of Radiation (AREA)

Abstract

The present invention relates to a kind of composite photonic crystal structure scintillators, including scintillator substrate, the antireflection layer being arranged in scintillator substrate, the layer of photonic crystals being arranged on antireflection layer, antireflection layer by with graded index bullet or cone table constituted in periodic array or disordered array, layer of photonic crystals is the internal high refractive index material layer for forming periodical air hole.Compared with prior art, the present invention is be combined with each other using specific anti-reflection layer and layer of photonic crystals, Fresnel reflection and total internal reflection comprehensive consideration are overcome, the efficiency of light output is improved to greatest extent, used technical solution is easy to low cost and prepares large area sample, is conducive to practical application and popularization.

Description

A kind of composite photonic crystal structure scintillator
Technical field
The invention belongs to nuclear radiation detection fields, more particularly, to a kind of composite photonic crystal structure scintillator.
Background technology
Nuclear radiation detection is answered in high-energy physics experiment, nuclear physics experiment, nuclear medicine, cosmic-ray detection, synchrotron radiation Play an important roll with, weapon research, anti-terrorism safety check, nuclear emergency disposition etc., many is related to national security wherein containing With the great demand of large scientific facilities.Nuclear radiation detection includes that (such as electronics, proton, α particles, fission are broken to various charged particles Piece), neutral particle (such as neutron) and high-energy photon (such as X-ray and gamma-rays) carry out time resolution, energy resolution, spatial discrimination It is measured with particle discrimination.Scintillation detector is due to efficient, sensitive volume is big etc. in numerous nuclear radiation detection devices Advantage becomes one of most popular detection method.
The basic principle of scintillation detector is interacted by nuclear radiation and scintillator, and scintillator absorbs radiating particle Visible light-black light transmitting (being referred to as flashing) is generated after energy, flashing is received by photoelectric devices such as photomultipliers Collect and be converted into electric signal, recorded by electronic system, can realize the detection to radiation.Flashing process includes radiation grain Sub- energy conversion, secondary electron excitation, electron thermalization, centre of luminescence excitation and light emitting, entire scitillation process contain radiation The information of particle, therefore the cognition to radiation can be realized to the inverting of passage of scintillation light.
In practical application, the efficiency for the detector that the light output of scintillator directly determines, light output is by the intrinsic of scintillator Photoyield and light extraction efficiency codetermine, and the intrinsic photoyield of major part commercial scintillators used at present is all passed through crystal and given birth to The abundant of long technology optimizes close to ideal value.But due to the refractive index of most of scintillator it is larger (generally between 1.8 to 2.2 it Between), passage of scintillation light is smaller at the inner total reflection angle that exit facet is formed, and causing most of passage of scintillation light to be limited in inside scintillator can not Outgoing, other than inner total reflection, at the interface of scintillation crystal, there is also Fresnel reflections, can equally be limited due to the effect of reflection The output of passage of scintillation light, thus while many scintillators maintain high internal quantum efficiency, but since inner total reflection and Fresnel are anti- The collective effect penetrated, a large amount of scintillation photons, which cannot be introduced into detection system, becomes effective passage of scintillation light, therefore how to extract this part Being limited in the light inside scintillator seems particularly significant.
Application No. is the Chinese patents of 201410496266X to disclose using photon crystal structure realization scintillator light output The raising of efficiency uses photon crystal structure in the invention, the raising of light output is realized by the method for reducing inner total reflection, But Fresnel reflection is not acted on, efficiency improves limited.Paper (Enhanced light extraction of Bi3Ge4O12scintillator by graded-refractiveindexantireflection coatingsFei Tong, Bo Liu, Hong Chen, Zhichao Zhu, and Mu Gu, Appl.Phys.Lett.103,071907 (2013)) In the elimination that Fresnel reflection how is realized using the multilayer film that graded index is constituted illustrated, but the structure is to inner total reflection Cut little ice, efficiency improve it is limited, while the graded index multilayer film for preparing of the sol-gel method that is used in paper its Refractive index size is more difficult to control, and dissolving each other between multilayer film can also limit the application of this method.Lacking one kind at present can be simultaneously The technical solution for reducing Fresnel reflection and inner total reflection realizes greatly improving for scintillator light output.
Invention content
Luxuriant and rich with fragrance alunite is solved it is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide a kind of simultaneously You reflect with scintillation photons caused by total internal reflection by sunken effect, and the composite photonic crystal structure for improving the light output of scintillator is dodged Bright body.
The purpose of the present invention can be achieved through the following technical solutions:
A kind of composite photonic crystal structure scintillator, including scintillator substrate, the antireflective that is arranged in scintillator substrate Layer, the layer of photonic crystals being arranged on antireflection layer,
The antireflection layer by with graded index bullet or cone table be in periodic array or disordered array structure At the layer of photonic crystals is the internal high refractive index material layer for forming periodical air hole.
The bottom edge length of the bullet is between λ/30 and λ/10, and base angle is between 20-60 degree, each bullet Between mean gap be less than λ/30, wherein λ be flashing centre wavelength.
The bottom edge of the cone table and the length of top margin between λ/30 and λ/10, base angle between 20-60 degree, Mean gap between each cone table is less than λ/30, and wherein λ is the centre wavelength of flashing.
The effect of anti-reflection layer is to reduce and eliminate Fresnel reflection, and graded index may be used in the elimination of Fresnel reflection Method, what this patent used belongs to sub-wavelength structure anti-reflection, and the scale of each bullet or cone table is much smaller than wavelength, then When light wave meets with it, what is experienced is mean refractive index effect, and mean refractive index size is from bullet or cone table and its The weighted average of surrounding air, therefore gradually increasing with height, mean refractive index continuously decreases.It is this gradually reduce it is more slow Slowly, then Fresnel reflection eliminate it is more, when using bullet when, the refractive index of top has had already decreased to 1, with air roll over It is completely the same to penetrate rate.In view of the influence of preparation condition, cone table is also feasible technical solution.
The antireflection layer is prepared using self-assembled silicon dioxide microballoon, then utilizes fluorine-containing plasma etching Obtain bullet or cone table self-assembled monolayer array.
The layer of photonic crystals is TiO2Layer, in the TiO2Distribution is in the airport of single layer HCP structure in layer Hole.
The layer of photonic crystals is prepared using following methods:
1) self-assembling method is used to form single layer polystyrene microsphere array;
2) in its surface conformal deposited high refractive index TiO2Layer, deposition thickness is between 100-300nm;
3) method for using heating evaporation removes polystyrene microsphere, and obtaining has periodic air hole composition TiO2Layer photon crystal structure.
The period of the photonic crystal, i.e., the distance between adjacent airport hole central point between 0.8 λ and 2 λ, Wherein λ is the centre wavelength of flashing.
Layer of photonic crystals specifically may be used following methods and be prepared:
1. silicon chip is handled.The dodecane methylsulfuric acid sodium solution that mass fraction is 5% is prepared, by the silicon that thickness is 0.5mm Piece is put into the solution, is placed 12 hours.
2. preparing polystyrene microsphere (microsphere diameter 414nm) solution.The polystyrene for taking mass fraction to be 2.5% is micro- Ball solution and absolute ethyl alcohol, by 1:1 ratio mixing.
3. prepared polystyrene microsphere solution is dripped on processed silicon chip, it is waited for fully to be opened up on silicon chip It opens, and moisture is volatilized completely.
4. the silicon chip of attachment polystyrene microsphere is slowly put into deionized water, at this moment polystyrene microsphere swims in water On face, and form hexagonal array arrangement.
5. the sample for covering silica circular cone volume array with surface drags for the polystyrene microsphere array of floating from water It rises, after extra moisture is fallen after natural evaporation, scintillator layers surface is attached to polystyrene microsphere array.
6. coating TiO2Preparation.Using Three-dimensional atom layer deposition techniques, in polystyrene microsphere deposited over arrays TiO2 Layer, deposition thickness 200nm, operating temperature when deposition are 60 degrees Celsius.
350 degrees Celsius are slowly warming up to 7. sample is positioned in Muffle furnace, removes polystyrene microsphere, obtaining has week The TiO that the air hole of phase property is constituted2Layer photon crystal structure.
After eliminating the influence of Fresnel reflection as much as possible, passage of scintillation light encounters photon crystal structure, in photon crystalline substance Under the diffraction of body, by momentum in additional plane, effective extraction of total internal reflection light is realized.The photon that the application uses is brilliant Body structure is to eliminate the transconfiguration of polystyrene microsphere, and the purpose is to improve contrast (the i.e. air and TiO of refractive index2's Refringence, 2.8-1=1.8).If not removing polystyrene microsphere, refractive index contrast 2.8-1.5=1.3.Refraction The raising of rate contrast allow more multi-mode by local photonic crystal high refractive index layer, to improve the effect of light extraction Rate.
The scintillator substrate includes inorganic scintillator, plastic scintillant or glass scintillator.
Fresnel reflection and total internal reflection are that property is entirely different, but the reflex all being had an impact to light output.Disappear Except they also must be based on different physical principles and corresponding technical solution.What anti-reflection layer was eliminated is Fresnel reflection, is used Scheme be sub-wavelength constitute mean refractive index gradient mode, to reduce total internal reflection there is no any effect.And Photon crystal structure belongs to the photon structure of wavelength magnitude, and it is additional that significant diffraction effect causes it to generate total internal reflection photon Momentum in plane can be realized when the momentum meets into the condition of air and break to total internal reflection, and wavelength structure Photon crystal structure can not play a role for eliminating Fresnel reflection.
Compared with prior art, the present invention has the following advantages:
(1) the technical program is be combined with each other using specific anti-reflection layer and layer of photonic crystals, by Fresnel reflection and entirely interior Reflection, which is considered every possible angle, to be overcome, and improves the efficiency of light output to greatest extent;
(2) used technical solution is easy to low cost preparation large area sample, is conducive to practical application and popularization.
Description of the drawings
Fig. 1 is composite photonic crystal structure scintillator structural schematic diagram.
Fig. 2 is the relation schematic diagram of layer of photonic crystals and anti-reflection layer.
Fig. 3 is the structural schematic diagram of bullet or cone table in anti-reflection layer.
Fig. 4 is photon crystal structure schematic diagram.
Fig. 5 is the silica array SEM figures of bullet in embodiment 1.
Fig. 6 is sample and the luminescent spectrum when excitation of X-rays of contrast sample in embodiment 1.
In figure, 1 it is scintillator substrate, 2 is antireflection layer, 3 is layer of photonic crystals.
Specific implementation mode
The present invention is described in detail with specific embodiment below in conjunction with the accompanying drawings.Following embodiment will be helpful to this field Technical staff further understand the present invention, but the invention is not limited in any way.It should be pointed out that the general of this field For logical technical staff, without departing from the inventive concept of the premise, various modifications and improvements can be made.These are belonged to Protection scope of the present invention.
Embodiment 1
A kind of composite photonic crystal structure scintillator, including scintillator substrate, the antireflective that is arranged in scintillator substrate Layer, the layer of photonic crystals being arranged on antireflection layer.
The scintillator substrate that the present embodiment uses is surface 10X20mm2, thickness is (Lu, the Y) of 1mm2SiO5:Ce flickers are brilliant Body, glow peak are about 420nm, and the preparation of anti-reflection layer uses the silicon dioxide microsphere of a diameter of 40nm.By self assembling process, It obtains scintillator surface and covers silicon dioxide microsphere periodic array.Sample is then put into plasma chamber, is evacuated down to 1x10- 6Torr then uses CF4And O2Mixed gas (wherein O2Content be 15%) generate plasma bombardment sample surfaces 300 seconds, the silica array of bullet is obtained, electromicroscopic photograph is as shown in Figure 5.Photonic crystal preparation process is as follows, 1. silicon Piece processing.The dodecane methylsulfuric acid sodium solution that mass fraction is 5% is prepared, the silicon chip that thickness is 0.5mm is put into the solution In, it places 12 hours.2. preparing polystyrene microsphere (microsphere diameter 414nm) solution.It is 2.5% polyphenyl to take mass fraction Ethylene microspheres solution and absolute ethyl alcohol, by 1:1 ratio mixing.3. prepared polystyrene microsphere solution is dripped to processing On the silicon chip crossed, it is waited for be sufficiently spread out on silicon chip, and moisture is volatilized completely.4. the silicon chip of attachment polystyrene microsphere It is slowly put into deionized water, at this moment polystyrene microsphere is swum on the water surface, and forms hexagonal array arrangement.5. being covered with surface The sample of lid silica circular cone volume array picks up the polystyrene microsphere array of floating from water, and it is extra to wait for that natural evaporation is fallen Moisture after, scintillator layers surface i.e. be attached to polystyrene microsphere array.6. coating TiO2Preparation.Using Three-dimensional atom Layer deposition techniques, in polystyrene microsphere deposited over arrays TiO2Layer, deposition thickness 200nm, operating temperature when deposition are 60 degrees Celsius.350 degrees Celsius are slowly warming up to 7. sample is positioned in Muffle furnace, polystyrene microsphere is removed, is had The TiO that periodic air hole is constituted2Layer photon crystal structure.
In order to compare general effect, it is prepared for respectively containing only anti-reflection layer (reference sample 1) and containing only layer of photonic crystals (reference Sample 2) sample, and carry out contrast test.
Fig. 6 is illustrated under excitation of X-rays, the luminescent spectrum of sample, the results showed that includes anti-reflection layer and layer of photonic crystals Shining for sample is all significantly increased than only having the sample of anti-reflection layer and only layer of photonic crystals in entire luminescent spectrum section.
Embodiment 2
A kind of composite photonic crystal structure scintillator, structure is as shown in Figure 1, including scintillator substrate 1, be arranged in flicker Antireflection layer 2 in body substrate 1, the layer of photonic crystals 3 being arranged on antireflection layer 2.
Scintillator substrate 1 is using inorganic scintillator.Antireflection layer 2 is by bullet or frustum with graded index Body is constituted in periodic array, and layer of photonic crystals 3 is the internal high refractive index material layer for forming periodical air hole, and structure is such as Shown in Fig. 2.
For the size a1, b1, b2 of each bullet or cone table between λ/30 and λ/10, wherein λ is flashing Centre wavelength.The angles Θ are between 20-60 degree, as shown in Figure 3.Mean gap between bullet or cone table is less than λ/30. Using bullet in the present embodiment, a length of λ/30 in bottom surface, the angles Θ are 60 °.
Antireflection layer 2 is prepared using self-assembled silicon dioxide microballoon, is then obtained using fluorine-containing plasma etching Bullet or cone table self-assembled monolayer array.
Layer of photonic crystals is TiO2Layer, in the TiO2Distribution is in the air hole of single layer HCP structure, knot in layer Structure is as shown in Figure 4.Layer of photonic crystals is prepared using following methods:
1) self-assembling method is used to form single layer polystyrene microsphere array;
2) in its surface conformal deposited high refractive index TiO2Layer, deposition thickness 100nm;
3) method for using heating evaporation removes polystyrene microsphere, and obtaining has periodic air hole composition TiO2Layer photon crystal structure, the distance between period, that is, adjacent airport hole central point of photonic crystal are 0.8 λ, and wherein λ is The centre wavelength of flashing.
Embodiment 3
A kind of composite photonic crystal structure scintillator, including scintillator substrate, the antireflective that is arranged in scintillator substrate Layer, the layer of photonic crystals being arranged on antireflection layer.
Scintillator substrate is using plastic scintillant.Antireflection layer is by the cone table with graded index in period battle array Row are constituted, and the length on the bottom edge of cone table is λ/10, and the length of top margin is λ/30, and base angle is 20 degree, flat between each cone table Equal gap is less than λ/30, and wherein λ is the centre wavelength of flashing.
Antireflection layer 2 is prepared using self-assembled silicon dioxide microballoon, is then obtained using fluorine-containing plasma etching Bullet or cone table self-assembled monolayer array.
Layer of photonic crystals is that the internal periodicity air hole that formed is TiO2Layer, in the TiO2Distribution is in single layer six in layer The air hole of angle close-packed structure, layer of photonic crystals are prepared using following methods:
1) self-assembling method is used to form single layer polystyrene microsphere array;
2) in its surface conformal deposited high refractive index TiO2Layer, deposition thickness 300nm;
3) method for using heating evaporation removes polystyrene microsphere, and obtaining has periodic air hole composition TiO2Layer photon crystal structure, the distance between period, that is, adjacent airport hole central point of photonic crystal are 1.2 λ, and wherein λ is The centre wavelength of flashing.
Specific embodiments of the present invention are described above.It is to be appreciated that the invention is not limited in above-mentioned Particular implementation, those skilled in the art can make various deformations or amendments within the scope of the claims, this not shadow Ring the substantive content of the present invention.

Claims (8)

1. a kind of composite photonic crystal structure scintillator, including scintillator substrate, be arranged in scintillator substrate antireflection layer, The layer of photonic crystals being arranged on antireflection layer, which is characterized in that
The antireflection layer by with graded index bullet or cone table constituted in periodic array or disordered array, institute The layer of photonic crystals stated is the internal high refractive index material layer for forming periodical air hole.
2. a kind of composite photonic crystal structure scintillator according to claim 1, which is characterized in that the bullet Bottom edge length between λ/30 and λ/10, base angle between 20-60 degree, mean gap between each bullet be less than λ/ 30, wherein λ are the centre wavelength of flashing.
3. a kind of composite photonic crystal structure scintillator according to claim 1, which is characterized in that the cone table The length of bottom edge and top margin is between λ/30 and λ/10, and base angle is between 20-60 degree, the mean gap between each cone table Less than λ/30, wherein λ is the centre wavelength of flashing.
4. a kind of composite photonic crystal structure scintillator according to claim 1, which is characterized in that the antireflection layer It is prepared using self-assembled silicon dioxide microballoon, then obtains bullet or cone table from group using fluorine-containing plasma etching Fill monolayer array.
5. a kind of composite photonic crystal structure scintillator according to claim 1, which is characterized in that the photonic crystal Layer is TiO2Layer, in the TiO2Distribution is in the air hole of single layer HCP structure in layer.
6. a kind of composite photonic crystal structure scintillator according to claim 5, which is characterized in that the photonic crystal Layer is prepared using following methods:
1) self-assembling method is used to form single layer polystyrene microsphere array;
2) in its surface conformal deposited high refractive index TiO2Layer, deposition thickness is between 100-300nm;
3) method for using heating evaporation removes polystyrene microsphere, obtains the TiO that there is periodic air hole to constitute2Layer Photon crystal structure.
7. a kind of composite photonic crystal structure scintillator according to claim 6, which is characterized in that in adjacent airport hole For the distance between heart point between 0.8 λ and 2 λ, wherein λ is the centre wavelength of flashing.
8. a kind of composite photonic crystal structure scintillator according to claim 1, which is characterized in that the scintillator base Bottom is inorganic scintillator, plastic scintillant or glass scintillator.
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CN108152851B (en) * 2017-11-27 2020-11-20 中核控制系统工程有限公司 Fast and slow neutron composite detector
CN108387923B (en) * 2018-03-15 2023-10-20 西北核技术研究所 Packaged scintillator with photonic crystal layer and scintillation detector
CN108761517B (en) * 2018-04-19 2021-09-03 同济大学 Built-in photonic crystal scintillator
CN218037369U (en) * 2022-03-25 2022-12-13 北京滨松光子技术股份有限公司 Scintillation crystal array, detector and medical imaging equipment

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