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WO2024173868A1 - Dispositif à base de pérovskite pour la détection de rayons gamma - Google Patents

Dispositif à base de pérovskite pour la détection de rayons gamma Download PDF

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Publication number
WO2024173868A1
WO2024173868A1 PCT/US2024/016268 US2024016268W WO2024173868A1 WO 2024173868 A1 WO2024173868 A1 WO 2024173868A1 US 2024016268 W US2024016268 W US 2024016268W WO 2024173868 A1 WO2024173868 A1 WO 2024173868A1
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Prior art keywords
perovskite material
perovskite
material layer
frequency downshifting
frequency
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PCT/US2024/016268
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English (en)
Inventor
Hendrik UTZAT
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University of California Berkeley
University of California San Diego UCSD
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University of California Berkeley
University of California San Diego UCSD
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    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B6/00—Apparatus or devices for radiation diagnosis; Apparatus or devices for radiation diagnosis combined with radiation therapy equipment
    • A61B6/02—Arrangements for diagnosis sequentially in different planes; Stereoscopic radiation diagnosis
    • A61B6/03—Computed tomography [CT]
    • A61B6/037—Emission tomography
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B6/00—Apparatus or devices for radiation diagnosis; Apparatus or devices for radiation diagnosis combined with radiation therapy equipment
    • A61B6/42—Arrangements for detecting radiation specially adapted for radiation diagnosis
    • A61B6/4208—Arrangements for detecting radiation specially adapted for radiation diagnosis characterised by using a particular type of detector
    • A61B6/4258—Arrangements for detecting radiation specially adapted for radiation diagnosis characterised by using a particular type of detector for detecting non x-ray radiation, e.g. gamma radiation
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
    • C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
    • C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
    • C09K11/66—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing germanium, tin or lead
    • 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
    • G01T1/20—Measuring radiation intensity with scintillation detectors
    • G01T1/202—Measuring radiation intensity with scintillation detectors the detector being a crystal
    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01T—MEASUREMENT OF NUCLEAR OR X-RADIATION
    • G01T1/00—Measuring X-radiation, gamma radiation, corpuscular radiation, or cosmic radiation
    • G01T1/29—Measurement performed on radiation beams, e.g. position or section of the beam; Measurement of spatial distribution of radiation
    • G01T1/2914—Measurement of spatial distribution of radiation
    • G01T1/2985—In depth localisation, e.g. using positron emitters; Tomographic imaging (longitudinal and transverse section imaging; apparatus for radiation diagnosis sequentially in different planes, steroscopic radiation diagnosis)
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y15/00—Nanotechnology for interacting, sensing or actuating, e.g. quantum dots as markers in protein assays or molecular motors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y20/00—Nanooptics, e.g. quantum optics or photonic crystals

Definitions

  • the present disclosure provides nanophotonic frequency downshifting systems and devices.
  • the systems and devices are particularly useful for Positron Emission Tomography (PET) imaging applications.
  • PET Positron Emission Tomography
  • PET uses radioisotopes as tracers of metabolic function in a non-invasive biomedical imaging technology.
  • PET is a powerful tool both in biomedical research and clinical patient care, particularly in the diagnosis of cancer, search of metastases, cancer treatment monitoring, the diagnosis of diffuse diseases causing dementia, or metabolic blood-flow imaging (as discussed in Gambhir, S. S. (2002), “Molecular imaging of cancer with positron emission tomography,” Nat. Rev. Cancer 2, 683-693; Drzezga, A., Bischof, G. N., Giehl, K. & van Eimeren, T.
  • Radioisotopes are administered prior to a scan, for example 18 F-containing chemicals, that, during radioactive decay, simultaneously emit two highly energetic gamma photons in opposite directions (as discussed in Almuhaideb, A., Papathanasiou, N. & Bomanji, (2011), J. 18F-FDGPET/CT imaging in oncology, Ann. Saudi Med. 31, 3-13).
  • FIG. 1A illustrates the principle of time-of-flight PET highlighting the need for high time-resolution detectors.
  • a detector array 100 is configured to detect gamma photons (e.g., 102 and 104) from tracer decay 106.
  • a pair of highly energetic gamma photons e.g., 102 and 104 emitted in opposite directions from tracer decay 106.
  • Two detector units (DI and D2) in the detector array 100 which corresponds to a line-of-response (LOR) 108, detect the pair of gamma photons (102 and 104), respectively.
  • LOR line-of-response
  • the present embodiments provide novel nanophotonic frequency downshifting devices and methods and systems incorporating the same.
  • the nanophotonic frequency downshifting devices are particularly useful in PET imaging systems and applications.
  • the present embodiments provide devices that enable the fast (down to 10 picoseconds) downshifting of single gamma- and X-ray photons to visible photons that can subsequently be detected with high timing-resolution visible single-photon detectors.
  • devices include nanoparticles of lead-halide perovskites that efficiently absorb gamma and X-ray photons, and re-emit the energy with tunable color and with high speed and efficiency.
  • the nanoparticles are integrated with nanophotonic metasurfaces to accelerate the emission further, thus enabling ultrafast gamma-ray downshifting.
  • the devices can easily be integrated with existing visible single-photon detector technologies to sensitize them for high-energy radiation.
  • the devices have immediate applications as detectors in positron-emission tomography (PET) scanners with an order of magnitude reduced cost and increased performance in efficiency and speed.
  • PET positron-emission tomography
  • the present embodiments advantageously provide advances in PET detector technologies that will have a multiplicative impact.
  • the higher efficiency and timing resolution not only enable higher spatial resolution to, for example, identify and localize small metastases, but also drastically reduce the PET system capital cost and operational cost via a reduction in the needed radiotracer. The latter will further de-risk PET for elderly patient populations.
  • a frequency downshifting device e.g., nanophotonic frequency downshifting, device.
  • the device comprises a perovskite material layer, wherein gamma radiation impinging on a first surface of the perovskite material layer is converted to visible radiation within the perovskite material layer, wherein at least a portion of the visible radiation is emitted from a second surface of the perovskite material layer opposite the first surface; and a visible light detector configured to detect visible radiation and located proximal to the second surface of the perovskite material layer.
  • the device further comprises a periodic array structure located between the perovskite material layer and the visible light detector, the periodic array structure including an array of nanoscale structural elements.
  • each nanoscale structural element in the periodic array structure comprises a dielectric material or a metal.
  • the array of nanoscale structural elements includes an array of nanopillars, half-spheres, spheres, and/or rectangle-shaped features or other gaps with the function of enhancing the electric field.
  • the periodic array structure comprises a material selected from GaN, silicon, lithium niobate, diamond, titanium dioxide, aluminium, or a Noble metal.
  • the periodic array structure includes an array of Au nanopillars.
  • the perovskite material layer comprises a leadhalide perovskite material.
  • the lead-halide perovskite material is a perovskite having a structure of CsPbX3, FAPbX3, or MAPbX3.
  • MA comprises methylammonium
  • FA comprises the formamidinium ion
  • X comprises one of I, Cl, Br or a mixture thereof, or similar compositions replacing lead with tin (Sn).
  • the perovskite material layer comprises a perovskite nanocrystal material.
  • the perovskite material layer comprises a bulk perovskite material.
  • the perovskite material layer comprises perovskite sheets or platelets.
  • the visible light detector comprises a photonmultiplier tube, a silicon single-photon detector or a superconducting nanowire single-photon detector.
  • the visible light detector comprises an array detector.
  • the device further comprises a fiber optic cable optically connected between the periodic array structure and the visible light detector.
  • the device further comprises a source of gamma radiation or other high-energy radiation.
  • a Positron-Emission Tomography (PET) device comprising a plurality of nanophotonic frequency downshifting devices disclosed herein is provided.
  • a method of timing the arrival of gamma radiation photons with one or multiple nanophotonic frequency downshifting devices as substantially described herein is provided.
  • a method of using the arrival time information of gamma photons for image reconstruction with one or multiple nanophotonic frequency downshifting devices as substantially described herein is provided.
  • a system, apparatus, and non-transitory computer-readable medium are provided to facilitate methods disclosed herein.
  • FIG. 1A illustrates the principle of time-of-flight Positron Emission Tomography (PET) highlighting the need for high time-resolution detectors.
  • PET Positron Emission Tomography
  • FIG. IB illustrates a nanophotonic hybrid downshifting device based on perovskite nanocrystals, according to an embodiment.
  • FIG. 2A illustrates a scintillation PET detector device architecture, according to an embodiment.
  • FIG. 2B demonstrates the high-resolution PET detection capabilities achievable using the exemplary scintillation PET device as depicted in FIG. 2A.
  • FIG. 3 is a block diagram of an exemplary process, according to one or more embodiments of the present disclosure.
  • the disclosed devices advantageously possess an order of magnitude enhanced timing resolution and detection efficiency, and at least an order of magnitude reduced cost compared to the prior, state-of-the-art detection devices.
  • a device works by downshifting a high energy gamma photon emitted from PET radiotracer contrast agents to a lower-energy visible photon that can subsequently be detected with existing fast detector technology (e.g., as depicted in FIG. 2A).
  • the device includes a hybrid optoelectronic slab that integrates nanometer-sized semiconductor crystals of lead-halide perovskites (perovskite quantum dots or nanoplatelets) with photonically active nanostructured surfaces (metasurfaces) located atop a detector, e.g., any known detector of visible single photons such as a photon-multiplier tube, a silicon single-photon detector or super-conducting nanowire single-photon detector, as well as arrays of these detectors in pixels of single-photon cameras.
  • a detector e.g., any known detector of visible single photons such as a photon-multiplier tube, a silicon single-photon detector or super-conducting nanowire single-photon detector, as well as arrays of these detectors in pixels of single-photon cameras.
  • the present embodiments combine three recent developments: i) the measurement of ultrafast photon emission from lead-halide perovskites at low temperature, ii) the realization that the proven properties of perovskite semiconductors as gamma-ray absorbers should be transferable to positron-emission tomography, and iii) the use of photonic metasurfaces in PET to accelerate the emission of visible photons from scintillator materials, thus reducing the timing uncertainty in the transduction of gamma to visible photons.
  • Each of these advances is individually and independently novel and useful, and their multiplicative advantages will improve virtually all relevant performance and cost parameters of PET detectors by orders of magnitude.
  • FIG. IB is a schematic illustrating an exemplary nanophotonic hybrid downshifting device, according to an embodiment.
  • a nanophotonic hybrid downshifting device 150 includes various components, including a frequency downshifter 152, a photonic accelerator 154, sensing elements (e.g., optical fiber 156, optical detector 158), and/or other suitable components.
  • the frequency downshifter 152 includes perovskite nanocrystal structures 162, such as perovskite nanocrystals, which may lead to a reduction in the frequency of received gamma photons (e g., 160).
  • the photonic accelerator 154 may incorporate various suitable layers, materials, and/or photonic structures tailored to perform functions such as amplifying, modulating, or manipulating the downshifted signal (e g., the downshifted photons 164) in various ways.
  • the output of the photonic accelerator 154 may be captured by suitable optical components, such as a sensing element(s) that is connected to a single-photon detector 158 via an optical fiber 156.
  • the nanophotonic frequency downshifting device 150 includes a perovskite material layer (e.g., 152) that acts as a gamma-to- visible conversion or downshifter layer.
  • Gamma radiation e.g., 160
  • the visible radiation e.g., 164
  • FIG. 2A is a schematic illustrating an exemplary scintillation PET device, according to an embodiment.
  • the scintillation PET device 200 comprises various components, including a photon transducer 210, a photonic accelerator 220, and a photon detector 230.
  • the photon transducer 210 may include a layer made of perovskite nanoplatelets 218. Additionally, the layer of the photon transducer 210 may be patterned, for example, with an array of through holes, as illustrated in FIG. 2A.
  • the photonic accelerator 220 may be constructed utilizing a metasurface design.
  • the photon detector 230 may include silicon single-photon detector.
  • a nanophotonic frequency downshifting device e.g., the scintillation PET device 200
  • a perovskite photon transducer layer 210 that acts as a gamma-to-visible conversion or downshifter layer. Similar to the nanophotonic hybrid downshifting device 150 depicted in FIG.
  • gamma radiation e.g., incident gamma photon 21
  • visible radiation e.g., downconverted visible photon 216
  • FIG. 2B demonstrates the high-resolution PET detection capabilities achievable using the exemplary scintillation PET device 200 as depicted in FIG. 2A. As shown in FIG. 2B, the number of photon counts (in arbitrary units) reaches its peak at approximately zero time difference (T in nanoseconds).
  • one or more visible light detectors are located proximal to the second surface of the perovskite material layer 152 in FIG. IB, or the perovskite photon transducer layer 210 in FIG. 2A.
  • the detector(s) may include any detector capable of detecting visible single photons such as a photon-multiplier tube, a silicon single-photon detector or super-conducting nanowire single-photon detector.
  • the nanophotonic frequency downshifting device may include a fiber optic cable, or other light guiding device or elements, optically connected between the periodic array structure and the visible light detector to guide or deliver the visible photons to the visible light detector(s) (e.g., as depicted in FIG. IB).
  • the nanophotonic frequency downshifting device includes a periodic array structure, or metasurface photonic accelerator structure, located between the perovskite material layer and the visible light detector (e.g., as depicted in FIG. 2A).
  • the periodic array structure may include an array of nanoscale structural elements, or metasurfaces, configured to enhance the light field as will be discussed in more detail below.
  • the perovskite material layer includes a lead-halide perovskite, e.g., chemical formula CsPbX3.
  • lead-halide perovskite materials include perovskite materials having a structure of CsPbX3, FAPbX3, or MAPbX3, wherein MA comprises methylammonium, FA comprises the formamidinium ion, and X comprises one of I, Cl, Br or a mixture thereof.
  • the perovskite material may include a perovskite nanocrystal material or a bulk perovskite material.
  • Lead-halide perovskites are solution-processed semiconductors that are particularly useful in many optoelectronic technologies, e.g., using nanoscale structures of lead-halide perovskite, so called quantum dots, as ultrafast and near unity-efficient single-photon emitters (as discussed in Hendrik, U. et al. (2019), “Coherent single-photon emission from colloidal lead halide perovskite quantum dots,” Science (80). 363, 1068-1072; Becker, M. A. et al. (2018), “Bright triplet excitons in caesium lead halide perovskites,” Nature 553, 189-193).
  • perovskite quantum dots when cooled to cryogenic temperatures, perovskite quantum dots will radiate photons one to two orders of magnitude faster than most other emissive materials (200 picoseconds , 95% efficiency, see, Utzat, Science, 2019).
  • embodiments herein harness this ultrafast emission of perovskite nanostructures in a fast-scintillating material in PET.
  • the high atomic weight of lead endows perovskites with an unprecedented stopping power for high-energy radiation which has very recently been harnessed in record-breaking detectivities of bulk thin-film perovskite X-ray detectors (as discussed in Chen, Q. et al.
  • Downshifting is a two-step process. First, a gamma-photon, or other high energy photon, is absorbed in the perovskite, which creates a high-energy excitation which is quickly losing its energy to form a lower-energy excitation. Second, the lower-energy excitation subsequently emits a photon with energies in the visible spectral range. The second process is many orders of magnitude slower than the first process and limits the overall downshifting speed. Although the emission performance of the perovskite nanoplatelets is already better than established scintillator materials (200-500ps, 1-2% efficiency), in an embodiment, the performance may be further improved by using photonic acceleration of the perovskite emission.
  • a thin film of perovskite nanoplatelets may be integrated with nanostructured semiconductor surfaces, the so called metasurfaces.
  • These metasurfaces may include periodic arrays of nanoscale dielectric structures that enhance the light field between them for certain frequencies, akin to the structured color effect of a butterfly wing.
  • the oscillation of the electrons in the perovskite material and the photons on the metasurface will mutually reinforce, resonantly accelerating the emission of visible photons.
  • each nanoscale structural element in the periodic array structure may include a dielectric material or a metal.
  • the array of nanoscale structural elements may include an array of nanopillars, half-spheres, spheres, and/or rectangle-shaped features.
  • the periodic array structure may include a material selected from GaN, silicon, lithium niobate, diamond, titanium dioxide, aluminium, or a Noble metal.
  • the periodic array structure may include an array of Au nanopillars.
  • the ink-like form of chemically-made perovskite nanoplatelets may be used to enable the straightforward integration of perovskite materials with photonic metasurfaces of gallium nitride (GaN), a material with minimal absorption losses in the spectral region of perovskite emission.
  • Initial calculations of the perovskite-metasurface reveal acceleration factors of up to ⁇ 20, and thus a possible total downshifting time of as low at 10 picoseconds.
  • a Positron-Emission Tomography (PET) device that includes one or a plurality of nanophotonic frequency downshifting devices as described herein. Using such a device or similar device enables methods of detecting or imaging objects, such as objects or patients containing radioisotopes as tracers. Objects with other sources of radiation may be imaged using devices according to embodiments herein.
  • PET Positron-Emission Tomography
  • methods of timing the arrival of gamma radiation photons are enabled using one or multiple nanophotonic frequency downshifting device embodiments as described herein.
  • methods of using the arrival time information of gamma photons for image reconstruction are enabled using one or multiple nanophotonic frequency downshifting devices as described herein.
  • FIG. 3 is a block diagram of an exemplary process, according to one or more embodiments of the present disclosure.
  • the process 300 may be performed by a PET system incorporating a nanophotonic frequency downshifting device provided herein, such as the device 150 as depicted in FIG. IB and/or the device 200 as demonstrated in FIG. 2A.
  • a computing system may be utilized to perform various suitable operations, such as generating a power spectrum, conducting further data analysis, etc.
  • the computing system may be integrated in or connected to the PET system.
  • the PET system receives a plurality of first photons of a first energy.
  • the plurality of first photons may be gamma radiation of a high energy.
  • the gamma radiation may impinge on a first surface of a perovskite material / transducer layer in the nanophotonic frequency downshifting device.
  • the PET system obtains a plurality of second photons of a second energy based on the plurality of first photons.
  • the gamma radiation is converted to visible radiation within the perovskite material / transducer layer.
  • at least a portion of the visible radiation may be emitted from a second surface of the perovskite material / transducer layer opposite the first surface.
  • the PET system generates, based on the plurality of second photons, a spectrum by correlating pairs of second photons of the plurality of second photons.
  • a visible light detector in the PET system may be configured to detect visible radiation.
  • the visible light detector may be located proximal to the second surface of the perovskite material / transducer layer.
  • the correlation of the second photon pairs may be indicated by power intensity (e.g., corresponding to the photon counts).
  • a computing system comprising one or more processors, may be employed to facilitate the described functions.
  • a “computer-readable medium” includes one or more of any suitable media for storing the executable instructions of a computer program such that the instruction execution machine, system, apparatus, or device may read (or fetch) the instructions from the computer-readable medium and execute the instructions for carrying out the described embodiments.
  • Suitable storage formats include one or more of an electronic, magnetic, optical, and electromagnetic format.
  • a non-exhaustive list of conventional exemplary computer-readable medium includes: a portable computer diskette; a random-access memory (RAM); a read-only memory (ROM); an erasable programmable read only memory (EPROM); a flash memory device; and optical storage devices, including a portable compact disc (CD), a portable digital video disc (DVD), and the like.

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Abstract

L'invention concerne un dispositif de rétrogradation de la fréquence. Le dispositif comprend une couche de matériau pérovskite, le rayonnement gamma frappant une première surface de la couche de matériau pérovskite étant converti en rayonnement visible à l'intérieur de la couche de matériau pérovskite, au moins une partie du rayonnement visible étant émise par une deuxième surface de la couche de matériau pérovskite opposée à la première surface ; et un détecteur de lumière visible configuré pour détecter le rayonnement visible et situé à proximité de la deuxième surface de la couche de matériau pérovskite.
PCT/US2024/016268 2023-02-16 2024-02-16 Dispositif à base de pérovskite pour la détection de rayons gamma Ceased WO2024173868A1 (fr)

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Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20060202125A1 (en) * 2005-03-14 2006-09-14 Avraham Suhami Radiation detectors
US20100261263A1 (en) * 2009-03-18 2010-10-14 Duke University Up and down conversion systems for production of emitted light from various energy sources
KR20170067815A (ko) * 2014-10-07 2017-06-16 버터플라이 네트워크, 인크. 초음파 신호 처리 회로와 관련 장치 및 방법
US20200323711A1 (en) * 2010-08-06 2020-10-15 Immunolight, Llc Color enhancement utilizing up converters and/or down converters
KR20210011667A (ko) * 2019-07-23 2021-02-02 고려대학교 산학협력단 자가 발전형 페로브스카이트 x선 검출기

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20060202125A1 (en) * 2005-03-14 2006-09-14 Avraham Suhami Radiation detectors
US20100261263A1 (en) * 2009-03-18 2010-10-14 Duke University Up and down conversion systems for production of emitted light from various energy sources
US20200323711A1 (en) * 2010-08-06 2020-10-15 Immunolight, Llc Color enhancement utilizing up converters and/or down converters
KR20170067815A (ko) * 2014-10-07 2017-06-16 버터플라이 네트워크, 인크. 초음파 신호 처리 회로와 관련 장치 및 방법
KR20210011667A (ko) * 2019-07-23 2021-02-02 고려대학교 산학협력단 자가 발전형 페로브스카이트 x선 검출기

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