WO2022030141A1 - Dispositif de conversion de rayonnement ionisant, son procédé de fabrication et procédé de détection de rayonnement ionisant - Google Patents

Dispositif de conversion de rayonnement ionisant, son procédé de fabrication et procédé de détection de rayonnement ionisant Download PDF

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Publication number
WO2022030141A1
WO2022030141A1 PCT/JP2021/024434 JP2021024434W WO2022030141A1 WO 2022030141 A1 WO2022030141 A1 WO 2022030141A1 JP 2021024434 W JP2021024434 W JP 2021024434W WO 2022030141 A1 WO2022030141 A1 WO 2022030141A1
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Prior art keywords
ionizing radiation
radiation conversion
conversion device
substrate
conversion unit
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PCT/JP2021/024434
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English (en)
Japanese (ja)
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幸広 金子
卓之 根上
太佑 松井
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パナソニックＩｐマネジメント株式会社
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Publication of WO2022030141A1 publication Critical patent/WO2022030141A1/fr

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    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00—Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/16—Measuring radiation intensity
    • G01T1/24—Measuring radiation intensity with semiconductor detectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/08—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof in which radiation controls flow of current through the device, e.g. photoresistors

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  • the present disclosure relates to an ionizing radiation conversion device, a method for manufacturing the same, and a method for detecting ionizing radiation.
  • Non-Patent Document 1 methyl ammonium iodide is used as a perovskite compound that converts X-rays into electric charges.
  • An object of the present disclosure is to provide an ionizing radiation conversion device having high sensitivity to ionizing radiation.
  • the ionizing radiation conversion device of the present disclosure is With a substrate and an ionizing radiation conversion layer located on the substrate, here,
  • the ionizing radiation conversion layer includes a first ionizing radiation conversion unit and an insulating unit.
  • the first ionizing radiation conversion unit contains a perovskite compound.
  • the present disclosure provides an ionizing radiation conversion device having high sensitivity to ionizing radiation.
  • FIG. 1A shows a cross-sectional view of the ionizing radiation conversion device 100 according to the first embodiment.
  • FIG. 1B shows a top view of the ionizing radiation conversion device 100 according to the first embodiment.
  • FIG. 2A shows a cross-sectional view of the ionizing radiation conversion device 200 according to the second embodiment.
  • FIG. 2B shows a top view of the ionizing radiation conversion device 200 according to the second embodiment.
  • FIG. 3 shows a cross-sectional view of the ionizing radiation conversion device 300 according to the second embodiment.
  • FIG. 4 shows a cross-sectional view of the ionizing radiation conversion device 400 according to the second embodiment.
  • FIG. 5 shows a cross-sectional view of the ionizing radiation conversion device 500 according to the third embodiment.
  • FIG. 1A shows a cross-sectional view of the ionizing radiation conversion device 100 according to the first embodiment.
  • FIG. 1B shows a top view of the ionizing radiation conversion device 100.
  • the ionizing radiation conversion device 100 includes a substrate 10 and an ionizing radiation conversion layer 60 located on the substrate 10.
  • the ionizing radiation conversion layer 60 includes a first ionizing radiation conversion unit 51 and an insulating unit 30.
  • the first ionizing radiation conversion unit 51 contains a perovskite compound.
  • the ionizing radiation conversion device 100 has high sensitivity to ionizing radiation. That is, the ionizing radiation conversion device 100 can efficiently convert ionizing radiation into an electric signal.
  • the ionizing radiation conversion device 100 can be used, for example, as an ionizing radiation detector, an image pickup device, or a dosimeter.
  • the perovskite compound has an excellent structure for converting light such as synchrotron radiation into electric charges. Further, the structure can contain an element having a large atomic number in order to further increase the sensitivity.
  • the insulating part eliminates the mixing of signals with the separated perovskite compounds. Further, in order to efficiently convert ionizing radiation into an electric signal, it is preferable that the ionizing radiation conversion layer has a thick film thickness. This is because when the film thickness is thin, a part of the ionizing radiation passes through the ionizing radiation conversion layer without being converted into an electric signal. On the other hand, when an attempt is made to make a thick perovskite compound from a liquid raw material, it is difficult to keep the liquid raw material on the substrate and it is difficult to form a thick film. Therefore, by providing the insulating portion, it becomes possible to keep the liquid raw material on the substrate. As a result, an ionizing radiation conversion layer having a film thickness capable of efficiently converting ionizing radiation into an electric signal can be realized.
  • ionizing radiation means ⁇ ray, ⁇ ray, neutron beam, proton beam, X-ray, or ⁇ ray.
  • the ionizing radiation conversion device 100 may further include a read-out circuit that reads out the electric charge.
  • the readout circuit is electrically connected to the ionizing radiation conversion device 100.
  • the readout circuit may be located inside the substrate 10 or may be located outside the substrate 10.
  • the substrate 10 is, for example, a glass substrate or a plastic substrate (including a plastic film).
  • the ionizing radiation conversion device 100 may further include a first pixel electrode 21.
  • the first pixel electrode 21 is located between the substrate 10 and the first ionizing radiation conversion unit 51. By providing the pixel electrodes, it is possible to separate each pixel and take out an electric signal.
  • the mechanism by which the ionizing radiation incident on the ionizing radiation conversion device 100 is converted into an electric signal will be explained.
  • the incident ionizing radiation is converted into an electric signal by the first ionizing radiation conversion unit 51 according to its intensity.
  • the intensity of the converted electrical signal is read out by, for example, a reading circuit electrically connected to the ionizing radiation conversion device 100.
  • the "perovskite compound” is a compound represented by ABX 3 or an analog thereof.
  • the compound represented by ABX 3 is, for example, BaTiO 3 , MgSiO 3 , CsPbI 3 , CsPbBr 3 or (CH 3 NH 3 ) PbI 3 .
  • the analog of the compound represented by ABX 3 has the following structure (i) or (ii).
  • (I) In the compound represented by ABX 3 the structure in which the A site, the B site, or a part of the X site is deleted (for example, (CH 3 NH 3 ) 3 Bi 2 I 9 ).
  • (Ii) In the compound represented by ABX 3 the structure in which the A site, the B site, or the X site is composed of a material having a plurality of different valences (for example, Cs (Ag 0.5 Bi 0.5 ) I 3 ).
  • the perovskite compound contained in the first ionizing radiation conversion unit 51 may contain two or more types of cations and monovalent anions.
  • the perovskite compound may substantially consist of two or more cations and one or more monovalent anions.
  • a perovskite compound is substantially composed of two or more cations and one or more monovalent anions" means that two or more cations are used with respect to the total amount of substance of all the elements constituting the perovskite compound. And it means that the total amount of substance of one or more monovalent anions is 90 mol% or more.
  • the perovskite compound may consist of two or more cations and one or more monovalent anions.
  • the two or more cations may contain at least one selected from the group consisting of Pb 2+ , Sn 2+ , Ge 2+ , and Bi 3+ .
  • the monovalent anion is, for example, a halogen anion or a composite anion.
  • halogen anions are fluorine, chlorine, bromine, or iodine.
  • composite anions are SCN-, NO 3- , or HCOO- .
  • the perovskite compound is, for example, a compound represented by the chemical formula ABX 3 (A is a monovalent cation, B is a divalent cation, and X is a halogen anion).
  • A is an organic cation or an alkali metal cation.
  • organic cations are methylammonium cations (ie CH 3 NH 3+ ), formamidinium cations (ie NH 2 CHNH 2 + ), phenylethylammonium cations (ie C 6 H 5 C 2 H 4 NH 3 ) . + ), Or a guanidinium cation (ie, CH 6 N 3 + ).
  • alkali metal cations examples include cesium cations (ie, Cs + ) or rubidium cations (ie, Rb + ).
  • A may contain, for example, at least one selected from the group consisting of Cs + , formamidinium cations, and methylammonium cations.
  • A may be a mixture of the above-mentioned plurality of organic cations.
  • A may be a mixture of at least one of the above-mentioned organic cations and at least one of the metal cations.
  • B is, for example, a divalent cation of Group 13 to Group 15 elements.
  • B may contain a Pb cation (ie, Pb 2+ ) or a Sn cation (ie, Sn 2+ ).
  • Perovskite compounds include, for example, CH 3 NH 3 PbI 3 , CH 3 CH 2 NH 3 PbI 3 , HC (NH 2 ) 2 PbI 3 , CH 3 NH 3 PbBr 3 , CH 3 NH 3 Cl 3 , CsPbI 3 , or CsPbBr. It is 3 .
  • the insulating portion 30 is made of an insulating material.
  • the insulating material may be an organic insulating material or an inorganic insulating material.
  • organic insulating materials are epoxy resins, silicone resins, or polyimides.
  • inorganic insulating materials are silicon oxide, silicon nitride, silicon nitride, hafnium oxide, aluminum oxide, and tantalum oxide. Silicon oxide is suitable from the viewpoint of processability, stability, and insulation.
  • the insulating portion 30 may contain at least one selected from the group consisting of epoxy resin, silicon resin, and polyimide.
  • the insulating portion 30 may be provided along the end portion of the substrate 10.
  • the insulating portion 30 may be provided so as to surround each pixel electrode.
  • the ionizing radiation conversion device 100 may be composed of a single pixel or may be composed of a plurality of pixels.
  • the ionizing radiation conversion device 100 may further include an electrode layer 40.
  • the ionizing radiation conversion layer 60 is located between the substrate 10 and the electrode layer 40.
  • the electrode layer 40 may be divided into pixels.
  • the electrode layer 40 is made of a conductive material.
  • the conductive material may or may not be transparent.
  • An example of a transparent conductive material is a metal oxide.
  • An example of the metal oxide is (I) Indium-tin composite oxide, (Ii) Antimony-doped tin oxide, (Iii) Fluorine-doped tin oxide, (Iv) zinc oxide doped with at least one element selected from the group consisting of boron, aluminum, gallium, and indium, or (v) a complex thereof.
  • non-transparent conductive materials are platinum, gold, silver, copper, aluminum, rhodium, indium, titanium, iron, nickel, tin, zinc, or alloys containing any of these, or conductive carbon materials. be.
  • the ionizing radiation conversion layer 60 may have a thickness of 0.1 micrometer or more. As a result, the ionizing radiation conversion device 100 has high sensitivity.
  • the ionizing radiation conversion layer 60 may have a thickness of, for example, 0.1 micrometer or more and 1 cm or less. Desirably, it may have a thickness of 100 micrometers or more and 1 mm or less.
  • the first ionizing radiation conversion unit 51 may contain 30 mol% or more of the perovskite compound. Desirably, the first ionizing radiation conversion unit 51 may contain 80 mol% or more of the perovskite compound.
  • the first ionizing radiation conversion unit 51 may be composed of only a perovskite compound.
  • FIG. 2A shows a cross-sectional view of the ionizing radiation conversion device 200 according to the second embodiment.
  • FIG. 2B shows a top view of the ionizing radiation conversion device 200.
  • the ionizing radiation conversion layer 60 includes not only the first ionizing radiation conversion unit 51 but also the second ionizing radiation conversion unit 52.
  • the first ionizing radiation conversion unit 51, the second ionizing radiation conversion unit 52, and the insulating unit 30 are all located on the substrate 10. Further, at least a part of the insulating portion 30 is located between the first ionizing radiation conversion unit 51 and the second ionizing radiation conversion unit 52.
  • the second ionizing radiation conversion unit 52 may contain a perovskite compound. The perovskite compound is as described in the first embodiment.
  • the first ionizing radiation conversion unit 51 may be separated from the second ionizing radiation conversion unit 52. That is, the first ionizing radiation conversion unit 51 may not be in contact with the second ionizing radiation conversion unit 52. According to the above configuration, it is possible to prevent mixed loading of signals on the separated pixels.
  • the insulating portion 30 may be located between the first pixel electrode 51 and the second pixel electrode 52, and the second pixel electrode 52 may be separated from the first pixel electrode 51. According to the above configuration, it is possible to prevent mixed loading of signals on the separated pixels.
  • FIG. 3 shows a cross-sectional view of the ionizing radiation conversion device 300 according to the second embodiment.
  • the ionizing radiation conversion device 300 includes not only the first pixel electrode 21 but also the second pixel electrode 22.
  • the first pixel electrode 21 and the second pixel electrode 22 are both located between the substrate 10 and the first ionizing radiation conversion unit 51.
  • the first pixel electrode 21 is not in contact with the second pixel electrode 22. According to the above configuration, the patterning of the insulating portion 30 can be increased, so that the process of forming the insulating portion 30 becomes simple.
  • FIG. 4 shows a cross-sectional view of the ionizing radiation conversion device 400 according to the second embodiment.
  • the ionizing radiation conversion layer 60 includes not only the first ionizing radiation conversion layer 51 but also the second ionizing radiation conversion layer 52.
  • the first pixel electrode 21 is located between the substrate 10 and the first ionizing radiation conversion unit 51, and is located between the substrate 10 and the second ionizing radiation conversion unit 52. That is, the insulating portion 30 separates one pixel into a plurality of. According to the above configuration, it is possible to stably form an ionizing radiation conversion unit made of a perovskite compound even when the pixel is large.
  • FIG. 5 shows a cross-sectional view of the ionizing radiation conversion device 500 according to the third embodiment.
  • the ionizing radiation conversion device 500 a part of the first ionizing radiation conversion unit 51 is separated by the insulating unit 30.
  • the ionizing radiation conversion device 500 has a configuration in which at least a part of the insulating portion 30 is located between the substrate 10 and the first ionizing radiation conversion unit 51. According to the above configuration, when the electrodes 40 are formed on the ionizing radiation conversion layer 60 in the same plane, they can be formed without interruption.
  • the perovskite compound may be used as a scintillator.
  • the same effect can be obtained by arranging an element such as a photodiode that converts light into an electric signal between the first ionizing radiation conversion unit 51 and the substrate 10.
  • the first pixel electrode 21 and the electrode layer 40 may not be provided.
  • the ionizing radiation conversion device of the present disclosure may be used in combination with a lens or the like.
  • the method for manufacturing the ionizing radiation conversion device is as follows: a first step of preparing the substrate 10, a second step of forming the insulating portion 30 on the substrate 10, and forming a first ionizing radiation converting portion 51 containing a perovskite compound on the substrate 10.
  • the third step is included.
  • the third step is executed after the second step.
  • the substrate 10 is prepared.
  • the substrate 10 may have a readout circuit.
  • the pixel pitch is, for example, 125 micrometers.
  • the insulating portion 30 is formed on the substrate 10.
  • the insulating portion 30 is formed by applying a silicon oxide film by a coating method and patterning by etching.
  • the first pixel electrode 21 is formed on the substrate 10 before or after the second step.
  • the first ionizing radiation conversion unit 51 containing the perovskite compound is formed on the substrate 10.
  • the ionizing radiation conversion layer 60 is formed.
  • raw materials are prepared so that the perovskite compound has a desired composition.
  • the raw material of the perovskite compound is dissolved in a solvent to obtain a precursor solution of the first ionizing radiation conversion unit 51.
  • this precursor solution By applying this precursor solution to the region on the substrate 10 and surrounded by the insulating portion 30, the first ionizing radiation conversion portion 51 is formed.
  • the third step will be described.
  • raw materials for the perovskite compound for example, 0.92 mol / L PbI 2 , 0.17 mol / L PbBr 2 , 0.83 mol / L formamidinium iodide, 0.17 mol / L methylammonium bromide, and CsI of 0.05 mol / L is prepared. These materials are dissolved in a mixed solvent of dimethyl sulfoxide and N, N-dimethylformamide. As a result, a precursor solution of the first ionizing radiation conversion unit 51 containing the perovskite compound is obtained.
  • the mixing ratio of dimethyl sulfoxide and N, N-dimethylformamide is, for example, 1: 4 (volume ratio).
  • the first ionizing radiation conversion unit 51 is formed by applying the precursor solution to the region surrounded by the insulating unit 30 by, for example, an inkjet method.
  • the first ionizing radiation conversion unit 51 may be formed from a solution containing a raw material and a solvent for the perovskite compound. Due to the presence of the insulating portion 30, the first ionizing radiation converting portion 51 is stably formed even when a liquid perovskite compound precursor is used.
  • the electrode layer 40 is formed on the ionizing radiation conversion layer 60.
  • the electrode layer 40 made of gold is formed by a thin-film deposition method.
  • the method for detecting ionizing radiation of the present disclosure is a method of detecting ionizing radiation using the above-mentioned ionizing radiation conversion device of the present disclosure.
  • the method for detecting ionizing radiation of the present disclosure includes, for example, a substrate 10 and an ionizing radiation conversion layer 60 located on the substrate 10, where the ionizing radiation conversion layer 60 includes a first ionizing radiation conversion unit 51 and an insulating unit. 30 is included, and the first ionizing radiation conversion unit 51 uses an ionizing radiation conversion device 100 containing a perovskite compound.
  • the charge or light generated by irradiating the perovskite compound with ionizing radiation is detected by the ionizing radiation conversion device 100.
  • the ionizing radiation conversion device used may be an ionizing radiation conversion device 200, 300, 400, or 500.
  • the ionizing radiation conversion device is applied as an element for converting ionizing radiation into an electric signal.
  • the ionizing radiation conversion device of the present disclosure is utilized in, for example, an ionizing radiation detector.
  • Substrate 21 1st pixel electrode 22 2nd pixel electrode 30 Insulation unit 40 Electrode layer 51 1st ionizing radiation conversion unit 52 2nd ionizing radiation conversion unit 60 Ionizing radiation conversion layer 100, 200, 300, 400, 500 Ionizing radiation conversion device

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Abstract

Le dispositif de conversion de rayonnement ionisant (100) selon la présente invention comprend un substrat (10) et une couche de conversion de rayonnement ionisant (60) positionnée sur le substrat (10). La couche de conversion de rayonnement ionisant (60) comprend une première partie de conversion de rayonnement ionisant (51) et une partie d'isolation (30). La première partie de conversion de rayonnement ionisant (51) contient un composé de pérovskite.
PCT/JP2021/024434 2020-08-06 2021-06-29 Dispositif de conversion de rayonnement ionisant, son procédé de fabrication et procédé de détection de rayonnement ionisant WO2022030141A1 (fr)

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JP2020134151A JP2023127001A (ja) 2020-08-06 2020-08-06 電離放射線変換デバイス、その製造方法、および電離放射線の検出方法
JP2020-134151 2020-08-06

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2017536698A (ja) * 2014-12-11 2017-12-07 ジーメンス ヘルスケア ゲゼルシャフト ミット ベシュレンクテル ハフツングＳｉｅｍｅｎｓ Ｈｅａｌｔｈｃａｒｅ ＧｍｂＨ ペロブスカイト結晶を含有する検出層
WO2018003328A1 (fr) * 2016-06-30 2018-01-04 浜松ホトニクス株式会社 Détecteur de rayonnement et son procédé de fabrication
JP2019520565A (ja) * 2016-06-08 2019-07-18 コーニンクレッカ フィリップス エヌ ヴェＫｏｎｉｎｋｌｉｊｋｅ Ｐｈｉｌｉｐｓ Ｎ．Ｖ． 位相コントラスト撮像及び／又は暗視野撮像のための分析格子
WO2020085214A1 (fr) * 2018-10-25 2020-04-30 株式会社 東芝 Détecteur de rayonnement de type à comptage de photons et dispositif de détection d'examen de rayonnement l'utilisant
US20200225367A1 (en) * 2017-09-29 2020-07-16 Northwestern University Thick alkali metal halide perovskite films for low dose flat panel x-ray imagers

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2017536698A (ja) * 2014-12-11 2017-12-07 ジーメンス ヘルスケア ゲゼルシャフト ミット ベシュレンクテル ハフツングＳｉｅｍｅｎｓ Ｈｅａｌｔｈｃａｒｅ ＧｍｂＨ ペロブスカイト結晶を含有する検出層
JP2019520565A (ja) * 2016-06-08 2019-07-18 コーニンクレッカ フィリップス エヌ ヴェＫｏｎｉｎｋｌｉｊｋｅ Ｐｈｉｌｉｐｓ Ｎ．Ｖ． 位相コントラスト撮像及び／又は暗視野撮像のための分析格子
WO2018003328A1 (fr) * 2016-06-30 2018-01-04 浜松ホトニクス株式会社 Détecteur de rayonnement et son procédé de fabrication
US20200225367A1 (en) * 2017-09-29 2020-07-16 Northwestern University Thick alkali metal halide perovskite films for low dose flat panel x-ray imagers
WO2020085214A1 (fr) * 2018-10-25 2020-04-30 株式会社 東芝 Détecteur de rayonnement de type à comptage de photons et dispositif de détection d'examen de rayonnement l'utilisant

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