CN104893709A - Surface treatment method for scintillator - Google Patents

Surface treatment method for scintillator Download PDF

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Publication number
CN104893709A
CN104893709A CN201510312884.9A CN201510312884A CN104893709A CN 104893709 A CN104893709 A CN 104893709A CN 201510312884 A CN201510312884 A CN 201510312884A CN 104893709 A CN104893709 A CN 104893709A
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Prior art keywords
scintillator
polystyrene microsphere
treatment method
surface treatment
monocrystalline silicon
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CN201510312884.9A
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Inventor
刘金良
刘波
朱智超
陈亮
欧阳晓平
程传伟
胡静
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Tongji University
Northwest Institute of Nuclear Technology
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Tongji University
Northwest Institute of Nuclear Technology
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Abstract

The invention discloses a surface treatment method for a scintillator to solve the technical problem that the existing scintillator is poor in time resolution capacity. The technical scheme is that the surface treatment method comprises the following steps: dripping a polystyrene microsphere-ethanol mixed solution to a treated monocrystalline silicon chip; and when the polystyrene microsphere-ethanol mixed solution is fully spread out on the monocrystalline silicon chip and water is completely volatilized, putting the monocrystalline silicon chip attached with polystyrene microspheres into deionized water, wherein the polystyrene microspheres are naturally arranged hexagonally under the action of molecular force. The polystyrene microsphere arrays floating on the surface of the deionized water are gently fished out by using the scintillator, and when the water is naturally evaporated, the polystyrene microsphere arrays are attached to the surface of the scintillator, and a protective layer is manufactured on the polystyrene microsphere arrays attached to the surface of the scintillator to ensure that the protective layer can be in the same shape with the polystyrene microsphere arrays. By adopting the surface treatment method disclosed by the invention, a polystyrene microsphere array photonic crystal structure is prepared on the surface of the scintillator by virtue of a self-assembly method, and the time resolution capacity of the scintillator is improved.

Description

The surface treatment method of scintillator
Technical field
The present invention relates to a kind of surface treatment method, particularly relate to a kind of surface treatment method of scintillator.
Background technology
In radiation detection field, scintillator refer to the radiation effect such as ray or particle after can produce the material of fluorescence.Popular says, scintillator function is exactly energy transformation radiation be deposited on wherein is that fluorescent photon discharges.Scintillation detector is generally made up of scintillator and photodetector, and the energy transformation that wherein scintillator makes radiation deposit is fluorescent photon, and photodetector detection scintillator fluorescence is also converted into electrical signal output, thus realizes the detection to radiation.The information such as kind, time, energy, position, momentum of radiation field particle can be obtained from the electrical signal that photodetector exports.Therefore, scintillation detector is widely used in the fields such as ground nuclear radiation detection, space dosimetry and particle physics experiment.
The temporal resolution performance of scintillation detector to the measuring accuracy of many parameters, detection efficiency and detector is closely related.As flight time-positron emission tomography (TOF-PET) device to produce the right due in of gamma-ray photon time difference by measuring positron annihilation determines to bury in oblivion position occurs.The temporal resolution of TOF-PET detector is higher, and it is less that it determines to meet event time window width, and the random signals probability of random occurrence is lower, determine to bury in oblivion precision that position occurs and signal to noise ratio also higher.In neutron time of flight method (nTOF), the time of flying over one section of specific range by measuring neutron determines neutron energy.Neutron energy differentiates the rootmean-square positive correlation of differentiating with detection time, and the neutron energy of the better then measuring result of detector temporal resolution is differentiated higher.And for example, in Short-lived radionuclide research, the time response of detector faster, higher decaying phenomenon and the Physical Mechanism being more conducive to observational study short-lived nuclide of temporal resolution.
Under the detector timing properties b of scintillation detector depends primarily on scintillator fluorescence, unit time inherent photodetector time level generates photoelectronic quantity.Through theory deduction and experimental verification, numerically scintillator temporal resolution Δ t square be proportional to scintillator τ fall time, be inversely proportional to the photoelectron number N of photodetector detection pe, namely Δ t numerical value is less, and the time resolution of scintillation detector is higher.Therefore, reduce scintillator fall time, improve the time resolution that photoelectron quantity that photodetector measures can improve scintillation detector.
Normally, scintillator determines primarily of the de excitation process of excited state fall time, and the photoelectron number of photodetector detection then determines primarily of the luminescence yield of scintillator and the spectral response of photomultiplier.For reality photodetector these be also subject to photon total reflection and crystal photon shooting angle distribution impact.On the one hand, the specific refraction of scintillator is all greater than 1 usually.Be connected on interface at scintillator with photodetector, the fluorescence only having input angle to be less than the interface angle of total reflection could enter photodetector smoothly and be detected, and the fluorescence that input angle is greater than the angle of total reflection is reflected back transmission and multiple reflections in crystal on interface.These multiple reflections exercising results are: (1) fluorescent photon needs to transmit farther light path in scintillator, which increases the temporal dispersion that photodetector measures fluorescent photon; (2) more photon and scintillator effect and by scintillator own absorption, reduce the photoelectron quantity that photodetector measures.On the other hand, the scintillator fluorescence that radiation sedimentary energy inspires is launched from energy deposition o'clock to 4 π space uniforms, is an individual light sources when scintillator is luminous.Scintillator is connected on interface with photodetector, emergent light within the scope of-90 ° ~ 90 °, have distribution.The fluorescence of wide-angle outgoing arrives the temporal dispersion of photodetector time level more greatly, and the probability be detected is lower.
Photonic crystal is that a class has the engineer of periodic dielectric structures and the crystal of manufacture on optics yardstick.Similar with the modulation of semiconductor lattice to electron wave function, photonic crystal can be used for modulating the photon with respective wavelength.If make the special photon crystal structure of one deck in scintillator surface, make blinking more intensively go out to shoot out sooner by the modulation of photonic crystal, then can improve scintillator time resolution.Document 1 " a kind of highlight extract efficiency scintillator utilizing surface photon structure to realize " (Chinese patent, application number 201410496266.X) in, disclose a kind of polyphenyl micro-sphere array photon crystal structure with scintillator surface that formed, result shows the light extraction efficiency that this arrangement enhances scintillator, confirms the modulating action of photonic crystal to blinking.
Document 2 " P.Lecoq, E.Auffray A.Knapitsch.How photonic crystals can improve the timing resoultion of scintillators.IEEE Transcations on Nuclear Science.2013; 60 (3), 1653 ~ 1657 ", in, disclose a kind of technology of traditional electron beam lithography that adopts and make the method for photonic crystal in scintillator surface.The photon crystal structure that the method makes improves scintillator time resolution.But adopt conditional electronic bundle lithographic method cost very high, and small area flicker body (1 ~ 2mm can only be used for 2size) process, which has limited the practical application of the method.
On the other hand, there is the preparation method of many new photon crystal micro-balls and microspheres solution in recent years.Document 3 " a kind of preparation method of ionic gel photonic crystal " (Chinese patent, application number 201410467443.1) in, the photonic crystal arrays suspension configured and polyvinyl alcohol solution are mixed, form gel photonic crystal precursor solution, then photonic crystal template is immersed in photonic crystal precursor solution, makes photonic crystal by gel polymerisation.Document 4 " a kind of photon crystal micro-ball, its preparation method and application " (Chinese patent, application number 201410391225.4) in, provide the method preparing photon crystal micro-ball, its photonic crystal is made up of kernel and polymer shell, can be used for biomolecule detection and coding.In document 5 " a kind of preparation method of photonic crystal hydrogel of chemically crosslinked of Color tunable " (Chinese patent, application number 201410056696.X), describe a kind of by two kinds of monomer structure polymerizations, make the method for photonic crystal hydrogel solution.In these patents, although finally all made microballoon or micro-sphere array, do not find that the photonic crystal utilizing self-assembly microspheres array to form is for scintillator surface so far, obtained the report that temporal resolution improves.
Summary of the invention
In order to overcome the deficiency of existing scintillator time resolution difference, the invention provides a kind of surface treatment method of scintillator.The method will prepare polystyrene microsphere-alcohol mixed solution and drip on treated monocrystalline silicon piece, treat that polystyrene microsphere-alcohol mixed solution fully launches on monocrystalline silicon piece, and moisture is volatilized completely, the monocrystalline silicon piece being attached with polystyrene microsphere is put into deionized water, and under molecular force effect, polystyrene microsphere becomes sexangle to arrange naturally.Pending scintillator is utilized to be picked up gently by the polystyrene microsphere array swimming in deionized water surface; after moisture spontaneous evaporation, namely polystyrene microsphere array is attached to scintillator surface; the polystyrene microsphere array of scintillator surface attachment makes layer protective layer, makes protective layer can be conformal with micro-sphere array.The present invention prepares polystyrene microsphere array photon crystal structure by self-assembling method in scintillator surface, due to the coupling of polystyrene microsphere array structure photonic crystal and scintillator fluorescence, significantly improve the light output of scintillator, shorten rise time and the fall time of scintillator luminescence simultaneously, improve the time resolution of scintillator.
The technical solution adopted for the present invention to solve the technical problems is: a kind of surface treatment method of scintillator, is characterized in adopting following steps:
Step one, get massfraction is 2 ~ 2.5%, diameter is 450 ~ 500nm polystyrene microsphere solution and dehydrated alcohol, be mixed to form polystyrene microsphere-alcohol mixed solution according to volume ratio 1:0.1 ~ 1:1.0 ratio.
Step 2, the polystyrene microsphere-alcohol mixed solution prepared dripped on the monocrystalline silicon piece after soaking for 9 ~ 10 hours in the dodecane methylsulfuric acid sodium solution of 5%, wait for that polystyrene microsphere-ethanolic soln fully launches on monocrystalline silicon piece, and moisture is volatilized completely.
Step 3, attachment polystyrene microsphere monocrystalline silicon piece slowly put into deionized water, at this moment polystyrene microsphere swims on the water surface, and self-assembling formation hexagonal array arrangement.
Step 4, scintillator is put into water gently, utilize scintillator end face to be picked up by the polystyrene microsphere array of deionized water surface flotation, after moisture spontaneous evaporation, namely the polystyrene microsphere array of scintillator surface attachment forms photon crystal structure.
Step 5, employing ald, Deposition of protective layer on the polystyrene microsphere photonic crystal of scintillator surface attachment, during Deposition of protective layer, the temperature of sediment chamber is 60 degrees Celsius.
Described scintillator is any one of silicic acid lutetium yttrium or yttrium aluminum garnet.
The diameter of described polystyrene microsphere is preferably identical with scintillator peak luminous wavelength.
Described protective layer material is TiO 2, ZnO, Al 2o 3or adamantine any one.
The invention has the beneficial effects as follows: the method will prepare polystyrene microsphere-alcohol mixed solution and drip on treated monocrystalline silicon piece, treat that polystyrene microsphere-alcohol mixed solution fully launches on monocrystalline silicon piece, and moisture is volatilized completely, the monocrystalline silicon piece being attached with polystyrene microsphere is put into deionized water, and under molecular force effect, polystyrene microsphere becomes sexangle to arrange naturally.Pending scintillator is utilized to be picked up gently by the polystyrene microsphere array swimming in deionized water surface; after moisture spontaneous evaporation, namely polystyrene microsphere array is attached to scintillator surface; the polystyrene microsphere array of scintillator surface attachment makes layer protective layer, makes protective layer can be conformal with micro-sphere array.The present invention prepares polystyrene microsphere array photon crystal structure by self-assembling method in scintillator surface, due to the coupling of polystyrene microsphere array structure photonic crystal and scintillator fluorescence, significantly improve the light output of scintillator, shorten rise time and the fall time of scintillator luminescence simultaneously, improve the time resolution of scintillator.After tested, the scintillator after the inventive method process, its temporal resolution half-width comparatively prior art reduces 11.9 ~ 17.6%.
Below in conjunction with the drawings and specific embodiments, the present invention is elaborated.
Accompanying drawing explanation
Fig. 1 is through the electron micrograph of the scintillator surface after the inventive method process.
Fig. 2 is through the scintillator time discrimination measurement Comparative result figure after the inventive method process.
Embodiment
Following examples are with reference to Fig. 1-2.
Embodiment 1.
The step of photonic crystal is made: (1) gets the polystyrene microsphere solution and dehydrated alcohol that massfraction is 2.5%, diameter is 500nm, is mixed to form the mixing solutions of polystyrene microsphere-ethanol in the ratio of 1:1 in silicic acid lutetium yttrium scintillator surface; (2) polystyrene microsphere-alcohol mixed solution prepared is dripped on the monocrystalline silicon piece after soaking for 10 hours in the dodecane methylsulfuric acid sodium solution of 5%, wait for that polystyrene microsphere ethanolic soln fully launches on silicon chip, and moisture is volatilized completely; (3) monocrystalline silicon piece of attachment polystyrene microsphere is slowly put into deionized water, at this moment polystyrene microsphere disengaging monocrystalline silicon piece swims in deionized water on the surface, and the arrangement of self-assembling formation hexagonal array; (4) Ф 10 × 10mm will be of a size of 3silicic acid lutetium yttrium scintillator puts into water gently, an one circular end face is utilized to be picked up by the polystyrene microsphere array of deionized water surface flotation, after moisture spontaneous evaporation, namely the polystyrene microsphere array of silicic acid lutetium yttrium scintillator surface attachment forms photon crystal structure; (5) adopt Atomic layer deposition method, polystyrene microsphere photonic crystal deposits one deck TiO 2as protective layer, during ald, the temperature of sediment chamber is 60 degrees Celsius, and the protective layer thickness of deposition is 60nm.
As can be seen from Figure 1, the scintillator surface after the inventive method process presents the photon crystal structure of hexagonal array arrangement.
As can be seen from Fig. 2 measuring result comparison diagram, do not have the silicic acid lutetium yttrium scintillator processed, after Gaussian function fitting, result shows that the whole width of its half eminence was 1.475 nanoseconds; Through the silicic acid lutetium yttrium scintillator of the inventive method process, Gaussian function fitting result shows that the whole width of its half eminence was 1.216 nanoseconds.Relative to the silicic acid lutetium yttrium scintillator not having to process, the temporal resolution half-width of the silicic acid lutetium yttrium scintillator after the inventive method process reduces 17.6%.
Embodiment 2.
The step of photonic crystal is made: (1) preparation polystyrene microsphere-alcohol mixed solution in yttrium aluminum garnet scintillator surface, get massfraction is 2%, diameter is 450nm polystyrene microsphere solution and dehydrated alcohol, be mixed to form the mixing solutions of polystyrene microsphere-ethanol in the ratio of 1:0.1; (2) polystyrene microsphere-alcohol mixed solution prepared is dripped on the monocrystalline silicon piece after soaking for 9 hours in the dodecane methylsulfuric acid sodium solution of 5%, wait for that polystyrene microsphere ethanolic soln fully launches on silicon chip, and moisture is volatilized completely; (3) monocrystalline silicon piece of attachment polystyrene microsphere is slowly put into deionized water, at this moment polystyrene microsphere swims on the water surface, and the arrangement of self-assembling formation hexagonal array; (4) Ф 20 × 20mm will be of a size of 3yttrium aluminum garnet scintillator put into water gently, an one circular end face is utilized to be picked up by the polystyrene microsphere array of deionized water surface flotation, after moisture spontaneous evaporation, namely the polystyrene microsphere array of yttrium aluminum garnet scintillator surface attachment forms photon crystal structure; (5) adopt technique for atomic layer deposition, polystyrene microsphere photonic crystal deposits layer of ZnO as protective layer, during ald, the temperature of sediment chamber is 60 degrees Celsius, and protective layer thickness is 55nm.
The diameter of polystyrene microsphere is preferably identical with scintillator peak luminous wavelength.Protective layer material is except TiO 2, outside ZnO, can also Al be used 2o 3or diamond.
To the yag crystal after the process of employing the inventive method and contrast crystal time resolved measurement result thereof be: the halfwidth that surface free crosses the yag crystal temporal resolution curve of process was 2.828 nanoseconds, yag crystal halfwidth after the inventive method process was 2.489 nanoseconds, and temporal resolution half-width reduces 11.9%.
This embodiment illustrates for different sorts and large-sized solid scintillator, after the inventive method process, the time resolution of scintillator can both be improved.Process for other types scintillator does not enumerate at this.

Claims (4)

1. a surface treatment method for scintillator, is characterized in that comprising the following steps:
Step one, get massfraction is 2 ~ 2.5%, diameter is 450 ~ 500nm polystyrene microsphere solution and dehydrated alcohol, be mixed to form polystyrene microsphere-alcohol mixed solution according to volume ratio 1:0.1 ~ 1:1.0 ratio;
Step 2, the polystyrene microsphere-alcohol mixed solution prepared dripped on the monocrystalline silicon piece after soaking for 9 ~ 10 hours in the dodecane methylsulfuric acid sodium solution of 5%, wait for that polystyrene microsphere-ethanolic soln fully launches on monocrystalline silicon piece, and moisture is volatilized completely;
Step 3, attachment polystyrene microsphere monocrystalline silicon piece slowly put into deionized water, at this moment polystyrene microsphere swims on the water surface, and self-assembling formation hexagonal array arrangement;
Step 4, scintillator is put into water gently, utilize scintillator end face to be picked up by the polystyrene microsphere array of deionized water surface flotation, after moisture spontaneous evaporation, namely the polystyrene microsphere array of scintillator surface attachment forms photon crystal structure;
Step 5, employing ald, Deposition of protective layer on the polystyrene microsphere photonic crystal of scintillator surface attachment, during Deposition of protective layer, the temperature of sediment chamber is 60 degrees Celsius.
2. the surface treatment method of scintillator according to claim 1, its feature exists: described scintillator is any one of silicic acid lutetium yttrium or yttrium aluminum garnet.
3. the surface treatment method of scintillator according to claim 1, its feature exists: the diameter of described polystyrene microsphere is preferably identical with scintillator peak luminous wavelength.
4. the surface treatment method of scintillator according to claim 1, its feature exists: described protective layer material is TiO 2, ZnO, Al 2o 3or adamantine any one.
CN201510312884.9A 2015-06-09 2015-06-09 Surface treatment method for scintillator Pending CN104893709A (en)

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Cited By (5)

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Publication number Priority date Publication date Assignee Title
CN105350077A (en) * 2015-10-20 2016-02-24 同济大学 Preparation method of photonic crystal scintillator by using polymer template
CN105425266A (en) * 2015-11-03 2016-03-23 同济大学 Preparation method for photonic crystal plastic scintillator
CN106842370A (en) * 2016-12-21 2017-06-13 兰州空间技术物理研究所 A kind of method for improving inorganic scintillation crystal light output
CN110068854A (en) * 2019-03-26 2019-07-30 同济大学 A kind of scintillation component with nested type micro-sphere array photon structure surface
CN111519165A (en) * 2020-05-08 2020-08-11 清华大学 Deliquescent scintillator photonic crystal and preparation method thereof

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CN104262672A (en) * 2014-09-15 2015-01-07 上海第二工业大学 Preparation method of ionic gel photon crystal
CN104280761A (en) * 2014-09-25 2015-01-14 同济大学 High-light-extraction-efficiency scintillator realized by utilizing surface photon structure

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN105350077A (en) * 2015-10-20 2016-02-24 同济大学 Preparation method of photonic crystal scintillator by using polymer template
CN105425266A (en) * 2015-11-03 2016-03-23 同济大学 Preparation method for photonic crystal plastic scintillator
CN106842370A (en) * 2016-12-21 2017-06-13 兰州空间技术物理研究所 A kind of method for improving inorganic scintillation crystal light output
CN110068854A (en) * 2019-03-26 2019-07-30 同济大学 A kind of scintillation component with nested type micro-sphere array photon structure surface
CN110068854B (en) * 2019-03-26 2023-05-02 同济大学 Scintillator device with nested microsphere array photon structure surface
CN111519165A (en) * 2020-05-08 2020-08-11 清华大学 Deliquescent scintillator photonic crystal and preparation method thereof

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