CN110068854A - A kind of scintillation component with nested type micro-sphere array photon structure surface - Google Patents

A kind of scintillation component with nested type micro-sphere array photon structure surface Download PDF

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Publication number
CN110068854A
CN110068854A CN201910233857.0A CN201910233857A CN110068854A CN 110068854 A CN110068854 A CN 110068854A CN 201910233857 A CN201910233857 A CN 201910233857A CN 110068854 A CN110068854 A CN 110068854A
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scintillator
sphere array
micro
array
sphere
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CN110068854B (en
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刘波
袁荻
程传伟
顾牡
张娟楠
陈鸿
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Tongji University
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Tongji University
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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
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16Measuring radiation intensity
    • G01T1/24Measuring radiation intensity with semiconductor detectors
    • GPHYSICS
    • G01MEASURING; TESTING
    • G01TMEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T7/00Details of radiation-measuring instruments

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  • 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 scintillation components with nested type micro-sphere array photon structure surface, including scintillator, it is arranged in the large scale micro-sphere array of scintillator upper surface, is deposited on the conforma layer of large scale micro-sphere array upper surface, the small size micro-sphere array being arranged on transparent material.Compared with prior art, photon structure of the invention can increase substantially the light extraction efficiency of scintillator, and may be implemented to produce in batches.

Description

A kind of scintillation component with nested type micro-sphere array photon structure surface
Technical field
The invention belongs to nuclear radiation detection fields, and in particular to a kind of with nested type micro-sphere array photon structure surface Scintillation component, which will significantly improve the light output of scintillator in radiation detector, and then is promoted and visited The sensitivity of examining system and signal-to-noise ratio.
Background technique
Scintillator is a kind of absorption high energy particle or high-energy ray and it is made to be converted into the functional material of visible light, scintillator The visible light launched, is also scintillation light, by subsequent Electro-Optical Sensor Set such as photomultiplier tube, photodiode and CCD device It receives, to realize the detection of high energy particle or high-energy ray, scintillator is the core component in scintillation detecter system, scintillator The characteristics of luminescence directly determine the performance of detection system.Scintillation detecter system is in high-energy physics experiment, nuclear physics experiment, nuclear weapon It is played an increasingly important role in device laboratory diagnosis, nuclear medicine, cosmic ray detection and safety check, being responsible for can not replace The function in generation.
However the refractive index of most of scintillator, between 1.5-2.5, high refractive index leads to shining inside scintillator It is accordingly totally internally reflected, the efficiency of light output is limited significantly.Therefore sensitivity and the signal-to-noise ratio of detection system are reduced.Using photon The method of artificial micro-structure can obtain a degree of raising of scintillator light output efficiency, have in radiation detection field important Using.Such as Chinese patent CN104280761A discloses a kind of method using microballoon self assembly and prepares photon crystal structure, For realizing the raising of flashing light output efficiency.But the micro-sphere array of this single structure size is to the regulating effect of scintillator It is limited, photon structure must be improved in order to further improve the efficiency of light output.
Summary 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 raising light outputs to imitate The scintillation component with nested type micro-sphere array photon structure surface of rate.
The purpose of the present invention can be achieved through the following technical solutions:
A kind of scintillation component with nested type micro-sphere array photon structure surface, including
Scintillator,
It is arranged in the large scale micro-sphere array of scintillator upper surface,
It is deposited on the conforma layer of large scale micro-sphere array upper surface,
The small size micro-sphere array being arranged on transparent material.
The scintillator includes plastic scintillant, glass scintillator, ZnO scintillator, Lu2SiO5: Ce scintillator, (Lu, Y)2SiO5: Ce scintillator, Bi4Ge3O12Scintillator, Y3Al5O12: Ce scintillator, CsI:Tl scintillator, NaI:Tl scintillator or PbWO4 Scintillator.
The large scale micro-sphere array is the array that polystyrene microsphere of the size between 2-10 microns is constituted, polyphenyl Ethylene microballoon prepares the array of single layer HCP structure through self assembly.The size of polystyrene microsphere first must be remote Greater than scintillator emission wavelength, when choosing 2 microns (being almost 4 times of emission wavelength), which can pass through geometric optics Method part light is first introduced into the large scale microballoon, lay the foundation for the extraction of subsequent small size microballoon.10 microns as upper Limit is the limitation because of the preparation of this polystyrene microsphere self-assembling method, and larger sized ball is difficult self assembly and goes out periodic array Structure.
The conforma layer is not deliquesce and transparent material layer in scintillator light emitting region, the material of conforma layer include TiO2、ZnO、Al2O3Or SiO2, with a thickness of 10-50 nanometers, prepared using Atomic layer deposition method, be deposited on large scale microballoon battle array The upper surface of column, the effect of this layer are to realize the good fixation of large scale micro-sphere array below, too thin not have fixation Effect, the too thick pattern for destroying surface gradually becomes a planar structure, to influence between big microballoon and minimicrosphere Coupling, therefore determine that 10-50 nanometers are a suitable scales by a large number of experiments.
The small size micro-sphere array is polystyrene microsphere array of the size between 0.3-1 microns, and small size is micro- Ball is embedded in the large scale micro-sphere array surface for being covered with conforma layer using self-assembling method.The effect of small size microballoon is to pass through The method of near-field coupling comes out the light extraction in big microballoon, the enhancing of light output efficiency is obtained, according to the basic of near-field coupling The regular size range mainly covers the range of scintillator emission wavelength, more appropriate by the range for choosing 0.3-1 microns.It is poly- Phenylethylene micro ball is too large or too small all to reduce coupling efficiency, or even the effect of near-field coupling is not achieved.
It can be by scintillator by the nesting type structure that large scale micro-sphere array, conforma layer, small size micro-sphere array are formed Interior lights first pass through large scale micro-sphere array and the special contact of scintillator surface is distributed, will be more using the principle of geometric optics Scintillation light be directed in big micro-sphere array, the size of the big microballoon much larger than flashing wavelength (generally between 0.4-0.6 Micron) therefore meet geometric optical theory.Light inside big microballoon can be passed through by the minimicrosphere array that its surface is adhered to again The mode of near field diffraction pattern is extracted, and generates effective outgoing.The diameter of minimicrosphere close to scintillator emission wavelength range, when When it interacts with scintillation light, there is significant near field diffraction pattern effect, this diffraction benefit may finally realize having for far field Effect reflection, the i.e. raising of light output efficiency.
Compared with prior art, the invention has the following advantages that
1, the light extraction efficiency of scintillator can be increased substantially using this photon structure.
2, the scintillator structure of the easily prepared large area of structure preparation method, therefore can satisfy most of detection systems Batch production is realized in requirement for scintillator.
Detailed description of the invention
Fig. 1 is the structural schematic diagram of the scintillation component with nested type micro-sphere array photon structure surface;
Fig. 2 is sweeping for the scintillation component with nested type micro-sphere array photon structure surface that embodiment 1 is prepared Retouch electron microscope picture;
Fig. 3 is that the scintillation component with nested type micro-sphere array photon structure surface that embodiment 1 is prepared is penetrated in X Emission spectrum under line excitation.
In figure, 1- scintillator, 2- large scale micro-sphere array, 3- conforma layer, 4- small size micro-sphere array.
Specific embodiment
The present invention is described in detail combined with specific embodiments below.Following embodiment will be helpful to the technology of this field Personnel further understand the present invention, but the invention is not limited in any way.It should be pointed out that the ordinary skill of this field For personnel, without departing from the inventive concept of the premise, various modifications and improvements can be made.These belong to the present invention Protection scope.
Embodiment 1
A kind of scintillation component with nested type micro-sphere array photon structure surface, including scintillator, are arranged in flashing The large scale micro-sphere array of body upper surface, is deposited on the conforma layer of large scale micro-sphere array upper surface, is arranged on transparent material Small size micro-sphere array.
Scintillator used in the present embodiment is ZnO scintillator, the polystyrene microsphere that large scale micro-sphere array is 2 microns The array of composition, polystyrene microsphere prepare the array of single layer HCP structure through self assembly.Conforma layer is not damp The material of solution and transparent material layer in scintillator light emitting region, conforma layer used in the present embodiment is ZnO, with a thickness of 20 Nanometer, is prepared using Atomic layer deposition method, is deposited on the upper surface of large scale micro-sphere array, and the effect of this layer is realized under it The good fixation of the large scale micro-sphere array in face.The polystyrene microsphere array that small size micro-sphere array is 0.5 micron of size is small Sized microspheres are embedded in the large scale micro-sphere array surface for being covered with conforma layer using self-assembling method.
Embodiment 2
A kind of scintillation component with nested type micro-sphere array photon structure surface, including scintillator, are arranged in flashing The large scale micro-sphere array of body upper surface, is deposited on the conforma layer of large scale micro-sphere array upper surface, is arranged on transparent material Small size micro-sphere array.
Scintillator used in the present embodiment is Y3Al5O12: Ce scintillator, the polyphenyl that large scale micro-sphere array is 5 microns The array that ethylene microballoon is constituted, polystyrene microsphere prepare the array of single layer HCP structure through self assembly.It is conformal Not deliquesce and transparent material layer in scintillator light emitting region, the material of conforma layer used in the present embodiment is layer SiO2, it with a thickness of 10 nanometers, is prepared using Atomic layer deposition method, is deposited on the upper surface of large scale micro-sphere array, this layer Effect is to realize the good fixation of large scale micro-sphere array below.The polyphenyl that small size micro-sphere array is 0.3 micron of size Ethylene micro-sphere array, small size microballoon are embedded in the large scale micro-sphere array surface for being covered with conforma layer using self-assembling method.
Embodiment 3
A kind of scintillation component with nested type micro-sphere array photon structure surface, including scintillator, are arranged in flashing The large scale micro-sphere array of body upper surface, is deposited on the conforma layer of large scale micro-sphere array upper surface, is arranged on transparent material Small size micro-sphere array.
Scintillator used in the present embodiment is PbWO4Scintillator, the polystyrene that large scale micro-sphere array is 10 microns The array that microballoon is constituted, polystyrene microsphere prepare the array of single layer HCP structure through self assembly.Conforma layer is It does not deliquesce and transparent material layer in scintillator light emitting region, the material of conforma layer used in the present embodiment is Al2O3, thick Degree is 50 nanometers, is prepared using Atomic layer deposition method, and the upper surface of large scale micro-sphere array is deposited on, and the effect of this layer is real The now good fixation of large scale micro-sphere array below.The polystyrene microsphere battle array that small size micro-sphere array is 1 micron of size Column, small size microballoon are embedded in the large scale micro-sphere array surface for being covered with conforma layer using self-assembling method.
It can be by scintillator by the nesting type structure that large scale micro-sphere array, conforma layer, small size micro-sphere array are formed Interior lights first pass through large scale micro-sphere array and the special contact of scintillator surface is distributed, will be more using the principle of geometric optics Scintillation light be directed in big micro-sphere array, the size of the big microballoon much larger than flashing wavelength (generally between 0.4-0.6 Micron) therefore meet geometric optical theory.Light inside big microballoon can be passed through by the minimicrosphere array that its surface is adhered to again The mode of near field diffraction pattern is extracted, and generates effective outgoing.The diameter of minimicrosphere close to scintillator emission wavelength range, when When it interacts with scintillation light, there is significant near field diffraction pattern effect, this diffraction benefit may finally realize having for far field Effect reflection, the i.e. raising of light output efficiency.
Embodiment 4
The scintillator substrate that this example uses is surface area for 20X20mm2, with a thickness of the Bi of 3mm4Ge3O12Scintillator.Big ruler 4.5 microns of the size of very little microballoon, 0.5 micron of the size of small size microballoon.Conforma layer is the TiO with a thickness of 10 nanometers2Layer.Flashing Body is bought from Shanghai Xi Kasi company.Microballoon is bought from Alfa Aesar company.
Preparation is divided into following steps:
(1) silicon wafer is handled, the dodecane methylsulfuric acid sodium solution that mass fraction is 5% is prepared, it is molten that silicon wafer is statically placed in this In liquid, place 24 hours or more.
(2) polystyrene microsphere solution is prepared, taking a certain amount of diameter is 4.5 microns of polystyrene microsphere solution (microballoon 2.5%) and dehydrated alcohol liquid quality fraction is, to be sufficiently mixed in the ratio ultrasound of 1:2, then taking a certain amount of diameter is 0.5 micro- The polystyrene microsphere solution (microspheres solution mass fraction is 2.5%) and dehydrated alcohol of rice, it is sufficiently mixed in the ratio ultrasound of 1:4 It closes.
(3) first the 4.5 micron polystyrene microspheres solution points prepared are dripped on the good silicon wafer of cleaning, drying, waits it It is sufficiently spread on silicon wafer and moisture volatilizees completely.
(4) silicon wafer that drop crosses microspheres solution is slowly put into deionized water, separates micro-sphere array with silicon wafer, floated On the water surface.
(5) micro-sphere array is picked up from water using the scintillator substrate cleaned up, waits its moisture evaporation, it is completely attached In scintillator surface, obtain the close heap micro-sphere array of single layer hexagonal being made of 4.5 microns of diameter of polystyrene microsphere.
(6) using technique for atomic layer deposition (device model Picosun SUNALE R-200) in microsphere surface conformal deposited One layer of TiO2, specific preparation flow is as follows: using titanium tetrachloride and water as the presoma of titanium and oxygen, reaction generates titanium dioxide Titanium is simultaneously deposited on sample surfaces.During deposition, the indoor temperature of reaction chamber and pressure be respectively set to 75 DEG C and 17hPa.In the deposition process of each atomic layer, presoma is first passed through with the pulse of 0.3s, after the reaction was completed in sample surfaces shape At the TiO of 0.08nm thickness2Conforma layer then passes to nitrogen wash chamber.Above step carries out 125 circulations, is prepared total With a thickness of the TiO of 10nm2Conforma layer.
(7) TiO will be passed through2The sample of conformal protection repeats above-mentioned experimental procedure and fishes for the microballoon that diameter is 0.5 micron, shape At array, the scintillation component on nested type micro-sphere array photon structure surface is finally obtained, structure is as shown in Figure 1, include dodging Bright body 1, the large scale micro-sphere array 2 for being arranged in 1 upper surface of scintillator, are made of 4.5 microns of polystyrene microsphere of size, sink The long-pending conforma layer 3 in 2 upper surface of large scale micro-sphere array, and it is embedded in 2 table of large scale micro-sphere array for being covered with conforma layer 3 The small size micro-sphere array 4 in face.
Fig. 2 is the scanning electron microscope diagram of sample, as the result is shown be that the surface of big ball covers small spherical structure, be institute The structure feature needed.Fig. 3 is the emission spectrum for the sample tested under excitation of X-rays, the results showed that has structure and does not tie When the reference sample of structure compares, about 3 times are increased at peak value, entire wavelength integral domain enhances 2.5 times, illustrates Remarkable result.
The above description of the embodiments is intended to facilitate ordinary skill in the art to understand and use the invention. Person skilled in the art obviously easily can make various modifications to these embodiments, and described herein general Principle is applied in other embodiments without having to go through creative labor.Therefore, the present invention is not limited to the above embodiments, ability Field technique personnel announcement according to the present invention, improvement and modification made without departing from the scope of the present invention all should be of the invention Within protection scope.

Claims (9)

1. a kind of scintillation component with nested type micro-sphere array photon structure surface, which is characterized in that including scintillator,
It is arranged in the large scale micro-sphere array of scintillator upper surface,
It is deposited on the conforma layer of large scale micro-sphere array upper surface,
The small size micro-sphere array being arranged on transparent material.
2. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1, special Sign is that the scintillator includes plastic scintillant, glass scintillator, ZnO scintillator, Lu2SiO5: Ce scintillator, (Lu, Y)2SiO5: Ce scintillator, Bi4Ge3O12Scintillator, Y3Al5O12: Ce scintillator, CsI:Tl scintillator, NaI:Tl scintillator or PbWO4 Scintillator.
3. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1, special Sign is that the large scale micro-sphere array is the array that polystyrene microsphere of the size between 2-10 microns is constituted.
4. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 3, special Sign is that the polystyrene microsphere prepares the array of single layer HCP structure through self assembly.
5. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1, special Sign is, the conforma layer is not deliquesce and transparent material layer in scintillator light emitting region.
6. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1 or 5, It is characterized in that, the material of the conforma layer includes TiO2、ZnO、Al2O3Or SiO2
7. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1 or 5, Be characterized in that, the conforma layer with a thickness of 10-50 nanometers.
8. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 1, special Sign is that the small size micro-sphere array is polystyrene microsphere array of the size between 0.3-1 microns.
9. a kind of scintillation component with nested type micro-sphere array photon structure surface according to claim 8, special Sign is that small size microballoon is embedded in the large scale micro-sphere array surface for being covered with conforma layer using self-assembling method.
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Citations (9)

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CN104280761A (en) * 2014-09-25 2015-01-14 同济大学 High-light-extraction-efficiency scintillator realized by utilizing surface photon structure
CN104820233A (en) * 2015-05-15 2015-08-05 中国科学院高能物理研究所 Scintillator array structure, and neutron detector employing same
CN104893709A (en) * 2015-06-09 2015-09-09 西北核技术研究所 Surface treatment method for scintillator
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
CN105350077A (en) * 2015-10-20 2016-02-24 同济大学 Preparation method of photonic crystal scintillator by using polymer template
CN106206636A (en) * 2016-08-16 2016-12-07 京东方科技集团股份有限公司 A kind of X-ray detection panel and preparation method thereof
CN107703529A (en) * 2017-08-25 2018-02-16 中国工程物理研究院材料研究所 A kind of new beta-ray detection device
CN108415062A (en) * 2018-01-19 2018-08-17 同济大学 A kind of scintillation component with photon microstructure surface

Patent Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20070070507A1 (en) * 2003-12-23 2007-03-29 Young-Joo Yee Aspherical microlens arrays and fabrication method thereof and applications using the same
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
CN104280761A (en) * 2014-09-25 2015-01-14 同济大学 High-light-extraction-efficiency scintillator realized by utilizing surface photon structure
CN104820233A (en) * 2015-05-15 2015-08-05 中国科学院高能物理研究所 Scintillator array structure, and neutron detector employing same
CN104893709A (en) * 2015-06-09 2015-09-09 西北核技术研究所 Surface treatment method for scintillator
CN105350077A (en) * 2015-10-20 2016-02-24 同济大学 Preparation method of photonic crystal scintillator by using polymer template
CN106206636A (en) * 2016-08-16 2016-12-07 京东方科技集团股份有限公司 A kind of X-ray detection panel and preparation method thereof
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