CN107356954A - A kind of photonic crystal scintillation component to be lighted with directionality - Google Patents

A kind of photonic crystal scintillation component to be lighted with directionality Download PDF

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Publication number
CN107356954A
CN107356954A CN201710493560.9A CN201710493560A CN107356954A CN 107356954 A CN107356954 A CN 107356954A CN 201710493560 A CN201710493560 A CN 201710493560A CN 107356954 A CN107356954 A CN 107356954A
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photonic crystal
lighted
layers
scintillator
directionality
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刘波
程传伟
顾牡
陈鸿
陈亮
刘金良
欧阳晓平
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Tongji University
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Tongji University
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Priority to PCT/CN2017/115411 priority patent/WO2019000849A1/en
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    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16Measuring radiation intensity
    • G01T1/20Measuring radiation intensity with scintillation detectors
    • G01T1/202Measuring radiation intensity with scintillation detectors the detector being a crystal
    • G01T1/2023Selection of materials

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  • Chemical & Material Sciences (AREA)
  • Crystallography & Structural Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Health & Medical Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Physics & Mathematics (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Molecular Biology (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Measurement Of Radiation (AREA)
  • Luminescent Compositions (AREA)

Abstract

The present invention relates to a kind of photonic crystal scintillation component to be lighted with directionality, including substrate, be disposed thereon layer of photonic crystals, with the conformal Si layers of photonic crystal, be wrapped in the scintillator layers of Si layers outer surface.Compared with prior art, the present invention is using the lattice constant of fixed photonic crystal, and by changing regulation and control of the thickness realization of Si conforma layers to different emission wavelength scintillator light emission directions, method is easy.

Description

A kind of photonic crystal scintillation component to be lighted with directionality
Technical field
The invention belongs to nuclear radiation detection field, more particularly, to a kind of photonic crystal scintillator to be lighted with directionality Device, the structural scintillator improve the collection effect of scintillation photons by strengthening its emission effciency in normal direction Rate and sensitivity and the signal to noise ratio for lifting detection system.
Background technology
Scintillation detecter system is very important spoke in high-energy physics experiment, nuclear physics experiment and nuclear medicine imaging system Measurement apparatus is penetrated, the Core Feature material in the device is exactly scintillator.Scintillator is by absorbing high-energy ray and being converted The detection to ray is realized for the mode of visible ray.Scintillator film has important application in imaging field, but film The luminous spatial distribution with Lambertian of scintillator, is not orientated specifically, in most scintillography system, only Passage of scintillation light near normal direction can be collected by photoelectric device, therefore regulate and control scintillator film as much as possible along normal side It is most important for the efficiency for improving detection system to transmitting.
Photonic crystal can be used for regulating and controlling the light emission direction of scintillator, such as the A of patent CN 105204191 and CN 105204114 A disclose the directionality regulation and control scintillator film of photonic crystal realization.Plastic scintillant and quantum dot scintillator The method of spin coating can be used to prepare, but their launch wavelength is often due to the difference of the condition prepared causes in lighting The difference of cardiac wave length, such as the emission wavelength peak of plastic scintillant are usually located at 420-500nm scopes, quantum dot scintillator Launch wavelength may be typically located at 450-550nm scopes by the regulation and control of quantum dot size size.
Usual photonic crystal is that strong wavelength relies on for luminous regulation and control, so if needing different transmitting light Need to design the photonic crystal of different lattice constants during the scintillator of spectrum, when preparing photonic crystal for large area, can use Nanometer embossing, nanometer embossing need realization to prepare template, once template prepares, its lattice constant is just fixed Get off, therefore according to the A of patent CN 105204191 and the A of CN 105204114 method, the tune to be lighted for different wave length Control then needs the template of different lattice constants, that is, adds cost, is also unfavorable for batch and prepares.How in fixed photonic crystal Lattice constant on the basis of can also adapt to the regulation and control of different emission simultaneously, this is that technology now urgently to be resolved hurrily is asked Topic.
The content of the invention
It is an object of the present invention to overcome the above-mentioned drawbacks of the prior art and provide a kind of fixed lattice constant, The scintillation component that there is directionality to launch of suitable different emission is obtained with reference to last handling process.
The purpose of the present invention can be achieved through the following technical solutions:
A kind of photonic crystal scintillation component to be lighted with directionality, including substrate, the photonic crystal that is disposed thereon Layer and the conformal Si layers of photonic crystal, the scintillator layers for being wrapped in Si layers outer surface.
Described substrate uses transparent material, includes but is not limited to quartz, sapphire or glass.
Described layer of photonic crystals is the array that hexagonal pillar cell is formed, between two neighboring pillar cell away from From for 600 ± 20nm, 300 ± 10nm of diameter of pillar cell, 300 ± 10nm of height.
Described pillar cell is directly that of avoiding biography using the photoresist structure of solidification using the benefit of solidification photoresist Caused structural damage during pattern transfer in system technology, particularly with the sample preparation of large area (cm size), pattern transfer Loss it is more serious.Preparation method is preferably nano impression.Being mainly in view of nano impression can quickly and easily prepare The photon crystal structure in big face, template may be reused, and improve efficiency.
Described Si layers are wrapped in the upper surface of the substrate between layer of photonic crystals outer surface and each pillar cell, and thickness is 5-20nm.The selection of specific thickness needs to use computer simulation, finite time-domain difference (FDTD) method or rigorous coupled wave side Method (RCWA) so that it is determined that thickness have optimal enhancing effect in the normal direction at luminescence peak.The reason for selecting Si It is that Si has big refractive index (4-5) in 400-600nm scopes, generally it is much larger than the refractive index of transparent oxide material.Fig. 2 shows Transmission, reflection and the absorption in the normal direction of the thick Si of 20nm simulation are shown.Wherein reflection comes from Fresnel reflection. Need to pay close attention to absorptivity again.Because as a rule Si is opaque material in visual field, and application herein needs it most Possible low absorption.Found by studying, when its thickness is less than below 20nm, its influence for absorbing for passage of scintillation light can neglect Slightly.Si has a very high refractive index, therefore can be significantly improved in the photon crystal surface of low-refraction by conformal one layer of Si The refractive index contrast of whole photon crystal structure, so as to improve its regulating effect.On the other hand, when changing its thickness, its institute Respective change can occur for corresponding dispersion relation, cause the wavelength of dispersion formant to produce movement, so as to be provided for wavelength tuning control Physical basis.When the lattice constant of fixed photonic crystal, only by changing the thickness of Si conforma layers, it is possible to easily regulate and control not With the scintillator of launch wavelength, this is a kind of very easy method, because the thickness for changing Si in preparation process is very easy.
Described scintillator layers are prepared using the method for spin coating, from plastic scintillant or quantum dot scintillator.
Preferably, plastic scintillant is polymethylstyrene or polymethyl methacrylate or polyphenyl second including plastic matrix P-terphenyl (C is adulterated in alkene18H14) or PBD (C20H14N2O luminous agent and POPOP (C) are used as20H14N2O2) or BBO (C24H18NO) it is used as Wavelength shifter;
Preferably, quantum dot scintillator is CdSe/ZnS, CdTe/ZnS or CdTe/CdS including nuclear shell structure quantum point.
The height of described scintillator layers is 500-3000nm, and this has highly taken into account the tune of total luminous efficiency and directionality Control effect.
Compared with prior art, the present invention has advantages below:
(1) generally photonic crystal can be used for regulating and controlling the directionality transmitting of scintillator, but conventional method needs to change lattice Constant is to adapt to the demand of different emission.The present invention is conformal by changing Si using the lattice constant for fixing photonic crystal The thickness of layer realizes the regulation and control to different emission wavelength scintillator light emission directions, method simplicity.
(2) Si has very high refractive index in visual field, when its is conformal when on photonic crystal, has very high refractive index Contrast, this can greatly enhance the coupling of photonic crystal and the centre of luminescence, obtain the directionality regulation and control significantly increased.But body material Si has serious absorption to visible ray, and by substantial amounts of experimental studies have found that when Si thickness is less than 20nm, it is to flicker The luminous absorption of body can be ignored, final to determine that Si thickness degree is 5-20nm.
(3) present invention directly make use of the photonic crystal of the photoresist structure without pattern transfer, using nano impression side Prepared by method, template can be reused, and is easy to cheap extensive preparation.
(4) present invention can greatly improve the collection efficiency to scintillation photons of detector, and then improve nuclear radiation detection Efficiency.
Brief description of the drawings
Fig. 1 is the structural representation of photonic crystal scintillator;
Fig. 2 is transmission, reflection and the absorption spectrum of 20nm thickness of silicon in embodiment 1;
Fig. 3 is the electron micrograph of embodiment 1;
Fig. 4 is the simulation of the emission spectra of the normal direction different-thickness Si layers of embodiment 1;
Fig. 5 is the dispersion relation of embodiment 1;
Fig. 6 is the varied angle luminescent spectrum of embodiment 1;
Fig. 7 is the varied angle luminous intensity of the wavelength integration of embodiment 1 compared with structureless reference sample;
Fig. 8 is the varied angle luminous intensity of the wavelength integration of embodiment 2 compared with structureless reference sample.
In figure, 1- substrates, 2- layer of photonic crystals, 3-Si layers, 4- scintillator layers.
Embodiment
The present invention is described in detail with specific embodiment below in conjunction with the accompanying drawings.Following examples will be helpful to this area Technical staff further understand the present invention, but the invention is not limited in any way.It should be pointed out that to the general of this area 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 photonic crystal scintillation component to be lighted with directionality, its structure is as shown in figure 1, including substrate 1, arrangement Layer of photonic crystals 2 and the conformal Si layers 3 of photonic crystal thereon, the scintillator layers 4 for being wrapped in the outer surface of Si layers 3.
In the present embodiment, the quartz glass of 1mm thickness is chosen as substrate, using standard nanometer embossing on its surface Prepare photon crystal structure.Using commercialized Si material patterns, size is 1 inch, and surface texture is the photon in hexagonal cycle Crystal column, lattice parameter 600nm, pillar diameter 300nm, pillar height 300nm.Carry out turning over system using PDMS soft templates, After release treatment is carried out to silicon template, PDMS is coated onto silicon template surface, after PDMS solidifications, there is complementary pore structure Hexagonal periodic array formd on PDMS surfaces, then the PDMS of solidification is removed from silicon masterplate, the template of reprinting of formation can For directly imprinting photonic crystal.In one layer of PMMA photoresist (n=1.5) of quartz substrate surface spin coating, the PDMS moulds that will be reprinted Plate is impressed on PMMA photoresists, then makes photoetching adhesive curing with ultraviolet light irradiation.PDMS templates are removed, photonic crystal is made Get ready, the layer of photonic crystals of the final photoresist structure for obtaining the solidification consistent with formwork structure.Its ESEM such as Fig. 3 institutes Show.Scintillator uses CdSe/ZnS quantum dots, and its luminous peak wavelength is located at 540nm.In order to determine the suitable of Si conforma layers Thickness, we are simulated using RCWA methods, and what Fig. 4 was represented is anti-when Si thickness is respectively 5,10,15 and 20nm Spectrum is penetrated, reflectance spectrum reflects the optical dispersion relation of photon structure, and peak band corresponding to reflectance spectrum is the spectral position of luminescence enhancement, Its complete dispersion relation is as shown in Figure 5.It will be seen that when Si thickness increase, its peak value moves to long wave direction. For the present embodiment, when thickness is 20nm, corresponding peak is 540nm.20nm is prepared using standard magnetically controlled sputter method The conforma layer of thickness is on photon crystal structure.
Oil-soluble CdSe/ZnS QDs are dissolved in toluene (concentration 5mg/ml), in order to improve the stickiness of solution, add Enter a certain amount of polystyrene and it is completely dissolved (concentration of polystyrene is 250mg/ml in solution).By the uniform of preparation Transparent solution is spun on photon crystal structure, after toluene volatilizees, CdSe/ZnS QDs quality in the film formed Fraction is about 2wt%.Using the oil-soluble quantum dot for being dissolved in toluene, preparation process adds to control viscosity to be easy to spin coating preparation Enter appropriate polystyrene.On the quantum dot solution spin coating prepared and the photon crystal structure prepared, treat that solvent is done The luminous layer film being embedded in structural material can be obtained after dry.For the effect of display structure regulation and control, we are using same The method of sample is prepared for the reference sample of structureless quantum dot scintillator layers on quartz substrate.
The test of luminescent properties is carried out to the sample prepared.Sample is positioned in test rotatable and with graduated On specimen holder, its emission spectra to angle change is measured under the exciting of X ray.As shown in Figure 6, the results showed that it is in normal side Tropism has significant humidification.Fig. 7 be wavelength integration varied angle luminous intensity with structureless reference sample compared with, tie Fruit shows that structured sample enhances about 4 times than structureless sample in the normal direction, and launch angle concentrates on strongly Normal direction.
Embodiment 2
The present embodiment is located at 420nm plastic scintillant by emission peak wavelength is regulated and controled.Scintillator is configured to polystyrene Middle doping luminous agent such as p-terphenyl (C18H14) and Wavelength shifter such as POPOP (C20H14N2O2), its emission center wavelength is 420nm. Using the photonic crystal for adapting to substrate and the photoresist structure of solidification in the same manner as in Example 1, the thickness selection of Si layers is 5nm.Fig. 8 is the varied angle luminous intensity of wavelength integration compared with structureless reference sample, the results showed that structured sample About 3.4 times are enhanced than structureless sample in the normal direction, launch angle concentrates on normal direction strongly.
Embodiment 3
A kind of photonic crystal scintillation component to be lighted with directionality, including substrate, the photonic crystal that is disposed thereon Layer and the conformal Si layers of photonic crystal, the scintillator layers for being wrapped in Si layers outer surface.
Substrate uses transparent material, and quartz is used in the present embodiment.Layer of photonic crystals is formed for hexagonal pillar cell The distance between array, two neighboring pillar cell be 600nm, the diameter 300nm of pillar cell, height 300nm.Above-mentioned post Shape unit is prepared using the photoresist structure of solidification using nano impression.Si layers be wrapped in layer of photonic crystals outer surface and The upper surface of substrate between each pillar cell.Thickness is 5nm.The thickness is calculated through finite time-domain difference (FDTD) method Machine simulates to obtain, it is desirable to can have optimal enhancing effect in the normal direction at luminescence peak.Scintillator layers use spin coating Method be prepared, select plastic scintillant in the present embodiment, plastic matrix is that luminous agent pair is adulterated in polymethylstyrene Terphenyl (C18H14) and Wavelength shifter POPOP (C20H14N2O2).The height of scintillator layers is 500nm, can take into account total luminous efficiency With the regulating effect of directionality.
Embodiment 4
A kind of photonic crystal scintillation component to be lighted with directionality, including substrate, the photonic crystal that is disposed thereon Layer and the conformal Si layers of photonic crystal, the scintillator layers for being wrapped in Si layers outer surface.
Substrate uses transparent material, and quartz is used in the present embodiment.Layer of photonic crystals is formed for hexagonal pillar cell The distance between array, two neighboring pillar cell be 580nm, the diameter 290nm of pillar cell, height 310nm.Above-mentioned post Shape unit is prepared using the photoresist structure of solidification using nano impression.Si layers be wrapped in layer of photonic crystals outer surface and The upper surface of substrate between each pillar cell.Thickness is 10nm.The thickness is calculated through rigorous coupled-wave method (RCWA) Machine simulates to obtain, it is desirable to can have optimal enhancing effect in the normal direction at luminescence peak.Scintillator layers use spin coating Method be prepared, CdSe/ZnS quantum dot scintillators are selected in the present embodiment, the height of scintillator layers is 1000nm, can Take into account the regulating effect of total luminous efficiency and directionality.
Embodiment 5
A kind of photonic crystal scintillation component to be lighted with directionality, including substrate, the photonic crystal that is disposed thereon Layer and the conformal Si layers of photonic crystal, the scintillator layers for being wrapped in Si layers outer surface.
Substrate uses transparent material, and quartz is used in the present embodiment.Layer of photonic crystals is formed for hexagonal pillar cell The distance between array, two neighboring pillar cell be 620nm, the diameter 310nm of pillar cell, height 290nm.Above-mentioned post Shape unit is prepared using the photoresist structure of solidification using nano impression.Si layers be wrapped in layer of photonic crystals outer surface and The upper surface of substrate between each pillar cell.Thickness is 20nm.The thickness is calculated through rigorous coupled-wave method (RCWA) Machine simulates to obtain, it is desirable to can have optimal enhancing effect in the normal direction at luminescence peak.Scintillator layers use spin coating Method be prepared, CdTe/CdS quantum dot scintillators are selected in the present embodiment, the height of scintillator layers is 3000nm, can Take into account the regulating effect of total luminous efficiency and directionality.
The specific embodiment of the present invention is 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 (10)

1. a kind of photonic crystal scintillation component to be lighted with directionality, it is characterised in that including substrate, be disposed thereon Layer of photonic crystals and the conformal Si layers of photonic crystal, the scintillator layers for being wrapped in Si layers outer surface.
A kind of 2. photonic crystal scintillation component to be lighted with directionality according to claim 1, it is characterised in that institute The substrate stated uses transparent material, includes but is not limited to quartz, sapphire or glass.
A kind of 3. photonic crystal scintillation component to be lighted with directionality according to claim 1, it is characterised in that institute The layer of photonic crystals stated be the distance between the array, two neighboring pillar cell that hexagonal pillar cell is formed be 600 ± 20nm, 300 ± 10nm of diameter of pillar cell, 300 ± 10nm of height.
A kind of 4. photonic crystal scintillation component to be lighted with directionality according to claim 3, it is characterised in that institute The pillar cell stated is prepared using the photoresist structure of solidification using nano impression.
A kind of 5. photonic crystal scintillation component to be lighted with directionality according to claim 3, it is characterised in that institute The Si layers stated are wrapped in the upper surface of the substrate between layer of photonic crystals outer surface and each pillar cell.
A kind of 6. photonic crystal scintillation component to be lighted with directionality according to claim 5, it is characterised in that institute The thickness for the Si layers stated is 5-20nm.
A kind of 7. photonic crystal scintillation component to be lighted with directionality according to claim 6, it is characterised in that institute The thickness for the Si layers stated is simulated through finite time-domain difference (FDTD) method or rigorous coupled-wave method (RCWA), makes determination Thickness has optimal enhancing effect in the normal direction at luminescence peak.
A kind of 8. photonic crystal scintillation component to be lighted with directionality according to claim 1, it is characterised in that institute The scintillator layers stated are prepared using the method for spin coating, from plastic scintillant or quantum dot scintillator.
A kind of 9. photonic crystal scintillation component to be lighted with directionality according to claim 8, it is characterised in that
It is in polymethylstyrene or polymethyl methacrylate or polystyrene that described plastic scintillant, which includes plastic matrix, Adulterate p-terphenyl (C18H14) or PBD (C20H14N2O luminous agent and POPOP (C) are used as20H14N2O2) or BBO (C24H18NO) make For Wavelength shifter;
Quantum dot scintillator is CdSe/ZnS, CdTe/ZnS or CdTe/CdS including nuclear shell structure quantum point.
A kind of 10. photonic crystal scintillation component to be lighted with directionality according to claim 1, it is characterised in that The height of described scintillator layers is 500-3000nm.
CN201710493560.9A 2017-06-26 2017-06-26 A kind of photonic crystal scintillation component to be lighted with directionality Pending CN107356954A (en)

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PCT/CN2017/115411 WO2019000849A1 (en) 2017-06-26 2017-12-11 Photonic crystal scintillator device having directivity luminescence

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Application publication date: 20171117