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Title: Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging

Abstract

We have developed ultra-fast cerium-coped lutetium-iodide (LuI{sub 3}:Ce) films thermally evaporated as polycrystalline, structured scintillator using hot wall epitaxy (HWE) method. The films have shown a 13 ns decay compared to the 28 ns reported for crystals. The fast speed coupled with its high density (∼5.6 g/cm{sup 3}), high effective atomic number (59.7), and the fact that it can be vapor deposited in a columnar form makes LuI{sub 3}:Ce an attractive candidate for high frame rate, high-resolution, hard X-ray imaging. In crystal form, LuI{sub 3}:Ce has demonstrated bright (>100,000 photons/MeV) green (540 nm) emission, which is well matched to commercial CCD/CMOS sensors and is critical for maintaining high signal to noise ratio in light starved applications. Here, we report on the scintillation properties of films and those for corresponding crystalline material. The vapor grown films were integrated into a high-speed CMOS imager to demonstrate high-speed radiography capability. The films were also tested at Advanced Photon Source, Argonne National Laboratory beamline 1-ID under hard X-ray irradiation. The data show a factor of four higher efficiency than the reference LuAG:Ce scintillators, high image quality, and linearity of scintillation response over a wide energy range. The films were employed to perform hard X-raymore » microtomography, the results of which will also be discussed.« less

Authors:
; ; ; ;  [1]; ; ; ; ;  [2]
  1. Radiation Monitoring Devices, Inc., Watertown, MA 02472 (United States)
  2. Advanced Photon Source, Argonne National Laboratory, Argonne, IL 60439 (United States)
Publication Date:
OSTI Identifier:
22608417
Resource Type:
Journal Article
Resource Relation:
Journal Name: AIP Conference Proceedings; Journal Volume: 1741; Journal Issue: 1; Conference: SRI2015: 12. international conference on synchrotron radiation instrumentation, New York, NY (United States), 6-10 Jul 2015; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY; ADVANCED PHOTON SOURCE; ANL; ATOMIC NUMBER; CERIUM ADDITIONS; CHARGE-COUPLED DEVICES; EMISSION; EPITAXY; FILMS; HARD X RADIATION; IRRADIATION; LUTETIUM IODIDES; NOISE; PHOSPHORS; POLYCRYSTALS; RESOLUTION; SCINTILLATIONS; SENSORS; SIGNAL-TO-NOISE RATIO

Citation Formats

Marton, Zsolt, E-mail: zmarton@rmdinc.com, Miller, Stuart R., Ovechkina, Elena, Singh, Bipin, Nagarkar, Vivek V., Kenesei, Peter, Moore, Matthew D., Woods, Russell, Almer, Jonathan D., and Miceli, Antonino. Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging. United States: N. p., 2016. Web. doi:10.1063/1.4952907.
Marton, Zsolt, E-mail: zmarton@rmdinc.com, Miller, Stuart R., Ovechkina, Elena, Singh, Bipin, Nagarkar, Vivek V., Kenesei, Peter, Moore, Matthew D., Woods, Russell, Almer, Jonathan D., & Miceli, Antonino. Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging. United States. doi:10.1063/1.4952907.
Marton, Zsolt, E-mail: zmarton@rmdinc.com, Miller, Stuart R., Ovechkina, Elena, Singh, Bipin, Nagarkar, Vivek V., Kenesei, Peter, Moore, Matthew D., Woods, Russell, Almer, Jonathan D., and Miceli, Antonino. Wed . "Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging". United States. doi:10.1063/1.4952907.
@article{osti_22608417,
title = {Ultra-fast LuI{sub 3}:Ce scintillators for hard x-ray imaging},
author = {Marton, Zsolt, E-mail: zmarton@rmdinc.com and Miller, Stuart R. and Ovechkina, Elena and Singh, Bipin and Nagarkar, Vivek V. and Kenesei, Peter and Moore, Matthew D. and Woods, Russell and Almer, Jonathan D. and Miceli, Antonino},
abstractNote = {We have developed ultra-fast cerium-coped lutetium-iodide (LuI{sub 3}:Ce) films thermally evaporated as polycrystalline, structured scintillator using hot wall epitaxy (HWE) method. The films have shown a 13 ns decay compared to the 28 ns reported for crystals. The fast speed coupled with its high density (∼5.6 g/cm{sup 3}), high effective atomic number (59.7), and the fact that it can be vapor deposited in a columnar form makes LuI{sub 3}:Ce an attractive candidate for high frame rate, high-resolution, hard X-ray imaging. In crystal form, LuI{sub 3}:Ce has demonstrated bright (>100,000 photons/MeV) green (540 nm) emission, which is well matched to commercial CCD/CMOS sensors and is critical for maintaining high signal to noise ratio in light starved applications. Here, we report on the scintillation properties of films and those for corresponding crystalline material. The vapor grown films were integrated into a high-speed CMOS imager to demonstrate high-speed radiography capability. The films were also tested at Advanced Photon Source, Argonne National Laboratory beamline 1-ID under hard X-ray irradiation. The data show a factor of four higher efficiency than the reference LuAG:Ce scintillators, high image quality, and linearity of scintillation response over a wide energy range. The films were employed to perform hard X-ray microtomography, the results of which will also be discussed.},
doi = {10.1063/1.4952907},
journal = {AIP Conference Proceedings},
number = 1,
volume = 1741,
place = {United States},
year = {Wed Jul 27 00:00:00 EDT 2016},
month = {Wed Jul 27 00:00:00 EDT 2016}
}
  • Here, we report the scintillation properties of LaBr{sub 3-x}I{sub x}:5%Ce{sup 3+} with four different compositions of x, i.e., x=0.75, 1.5, 2, and 2.25. Radioluminescence spectra reveal a shift of the emission wavelength with the LaBr{sub 3} to LaI{sub 3} ratio. LaBr{sub 1.5}I{sub 1.5}:5%Ce{sup 3+} shows the highest scintillation light yield of 58 000 photons/MeV, whereas LaBr{sub 0.75}I{sub 2.25}:5%Ce{sup 3+} shows the fastest scintillation decay time of 12 ns under 662 keV {gamma}-ray excitation. This decay time is faster than that of 16 ns in LaBr{sub 3}:Ce{sup 3+}. The temperature dependence of radioluminescence spectra is presented. The structures and lattice parametersmore » of the materials were determined from powder x-ray diffraction.« less
  • Highlights: • Single crystalline films of Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12} garnets at x = 0 ÷ 3.0 were grown by LPE method onto YAG substrates. • Lattice constant of Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12}:Ce film and the misfit m between films and YAG substrate changed linearly with increasing of Gd content. • Effective Gd{sup 3+}–Ce{sup 3+} energy transfer occurs in the Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12}:Ce films. • Best scintillation light yield is observed in the Lu{sub 3}Al{sub 5}O{sub 12}:Ce and Lu{sub 2.4}Gd{sub 0.6}Al{sub 5}O{sub 12}:Ce films. • Increase of the Gd content in x = 1.5–2.5 range resultsmore » in decreasing the scintillation LY of Lu{sub 3−x}Gd{sub x}Al{sub 5}O{sub 12}:Ce films. - Abstract: The work is related to the growth of scintillators based on the single crystalline films (SCF) of Ce{sup 3+} doped Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12} mixed rare-earth garnets by Liquid Phase Epitaxy (LPE) method. We have shown, that full set of Lu{sub 3−}Gd{sub x}Al{sub 5}O{sub 12} SCFs with x values ranging from 0 to 3.0 can be successfully crystallized by the LPE method onto Y{sub 3}Al{sub 5}O{sub 12} (YAG) substrates from the melt-solutions based on PbO-B{sub 2}O{sub 3} flux. The absorption, X-ray excited luminescence, photoluminescence, thermoluminescence and light yield measurements, the latter under excitation by α-particles of {sup 239}Pu and {sup 241}Am radioisotopes, were applied for their characterization.« less
  • In the context of research on U/minor actinides for nuclear fuel reprocessing in the transmutation process, developments are first studied with surrogates containing uranium and lanthanides to facilitate testing. The tests consist of precipitating and calcining a hydrazinium uranium/cerium oxalate. The structure of this oxalate had not been previously determined, but was necessary to validate the physicochemical mechanisms involved. The present study, firstly demonstrates the structural similarity of the U/Ce oxalate phase (N{sub 2}H{sub 5},H){sub 2.9}U{sub 1.1}Ce{sub 0.9}(C{sub 2}O{sub 4}){sub 5}·10H{sub 2}O, synthesized using a vortex precipitator for continuous synthesis of actinide oxalates, with previously known oxalates, crystallizing in P6{submore » 3}/mmc symmetry, obtained by more classical methods. This fast precipitation process induces massive nucleation of fine powders. Their structural and microstructural determination confirms that the raw and dried phases belong to the same structural family as (NH{sub 4}){sub 2}U{sub 2}(C{sub 2}O{sub 4}){sub 5}·0.7H{sub 2}O whose structure was described by Chapelet-Arab in P6{sub 3}/mmc symmetry, using single crystal data. However, they present an extended disorder inside the tunnels of the structure, even after drying at 100 °C, between water and hydrazinium ions. This disorder is directly related to the fast vortex method. This structure determination can be used as a basis for further semi-quantitative analysis on the U/minor actinides products formed under various experimental conditions. - Highlights: • Uranium cerium oxalate precipitate characterization by X-ray powder diffraction. • Morphology characterization by SEM analysis. • Structure determination by unit cell Rietveld refinement.« less
  • The authors have investigated changes in the electronic structures of digitally controlled La{sub 0.6}Sr{sub 0.4}MnO{sub 3} (LSMO) layers sandwiched between SrTiO{sub 3} as a function of LSMO layer thickness in terms of hard x-ray photoemission spectroscopy (HX-PES). The HX-PES spectra show the evolution of Mn 3d derived states near the Fermi level and the occurrence of metal-insulator transition at 8 ML. The detailed analysis for the thickness dependent HX-PES spectra reveals the existence of the less conducting and nonmagnetic transition layer with a film thickness of about 4 ML in the interface region owing to significant interaction through the interface.
  • Investigations of radioluminescence saturation in monocrystalline cerium doped yttrium aluminum garnet (Ce:YAG) exposed to intense extreme ultraviolet (XUV), soft X-ray and X-ray radiation delivered from three free-electron lasers are described in this article. The measurements were performed with wavelengths of 98, 25.6, 13.5 and 0.15 nm. We have found that saturation of the photon yield occurs at an excitation level of 2.0 x 10 20 eV/cm 3 resulting in an emission of 1.5 x 10 18 visible photons per cubic centimeter. This number is much smaller than the concentration of Ce3+ in the scintillator that was equal to 2 xmore » 10 20 cm –3. Because the internal radiance efficiency η does not depend strongly on the irradiating photon energy, i.e., η ≈0.035 ± 0.015 in the range 10 to 100 000 eV, the results presented here could be used to predict saturation effects in scintillator slabs placed in imaging systems of bright XUV, X-ray and particle beams. In conclusion, the saturation of the Ce 3+ emission is explained by mutual quenching of excitons created at high densities, preceding the stage of energy transfer to the Ce 3+ ions.« less