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JAEA Reports

Development of rapid and sensitive radionuclide analysis method by simultaneous analysis of $$beta$$, $$gamma$$, and X-rays (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Japan Chemical Analysis Center*

JAEA-Review 2021-060, 105 Pages, 2022/03


The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2020. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2020, this report summarizes the research results of the "Development of rapid and sensitive radionuclide analysis method by simultaneous analysis of $$beta$$, $$gamma$$, and X-rays" conducted in FY2020. The present study aims to enable rapid analysis of radionuclides in fuel debris and waste, and develops the measurement system such as multiple $$gamma$$-ray detection method. We develop a spectral determination method (SDM method) for integrated analysis by constructing a spectral database for nuclides including $$beta$$-rays and X-rays by measurement using this system and radiation simulation calculation. This method enables simultaneous quantification of multiple nuclides and reduces the chemical separation process.

Journal Articles

${it In situ}$ spectrometry of terrestrial gamma rays using portable germanium detectors in area of 80 km radius around the Fukushima Daiichi Nuclear Power Plant

Mikami, Satoshi; Tanaka, Hiroyuki*; Okuda, Naotoshi*; Sakamoto, Ryuichi*; Ochi, Kotaro; Uno, Kiichiro*; Matsuda, Norihiro; Saito, Kimiaki

Nihon Genshiryoku Gakkai Wabun Rombunshi, 20(4), p.159 - 178, 2021/12

In order to know the background radiation level where the area affected by the Fukushima Daiichi Nuclear Power Plant accident in 2011, terrestrial gamma rays had been measured by using portable germanium detectors repeatedly from 2013 through 2019, at 370 locations within 80 km radius area centered on the Fukushima Daiichi Nuclear Power Plant. Radioactive concentrations of Uranium 238, Thorium 232, Potassium 40 and kerma rates in air due to terrestrial gamma rays were obtained at those locations based on the method of ICRU report 53. Averaged concentrations of $$^{238}$$U, $$^{232}$$Th and $$^{40}$$K were 18.8, 22.7, 428 Bq/kg, respectively, and kerma rate in air over the area was found to be 0.0402 $$mu$$Gy/h. The obtained kerma rates in air were compared to those reported in literatures. It was confirmed that the data were correlated with each other, and were agreed within the range of their uncertainty. This is because the kerma rate in air due to terrestrial gamma rays is depend on geology. The similar trend to previous findings was observed that the kerma rate in air at locations geologically classified as Mesozoic era, Granite and Rhyolite were statistically significantly higher than the others.

Journal Articles

Utilizing PUNITA experiments to evaluate fundamental delayed gamma-ray spectroscopy interrogation requirements for nuclear safeguards

Rodriguez, D.; Koizumi, Mitsuo; Rossi, F.; Seya, Michio; Takahashi, Tone; Bogucarska, T.*; Crochemore, J.-M.*; Pedersen, B.*; Takamine, Jun

Journal of Nuclear Science and Technology, 57(8), p.975 - 988, 2020/08

 Times Cited Count:3 Percentile:62.87(Nuclear Science & Technology)

Journal Articles

Delayed gamma-ray spectroscopy inverse Monte Carlo analysis method for nuclear safeguards nondestructive assay applications

Rodriguez, D.; Rossi, F.; Seya, Michio; Koizumi, Mitsuo

Proceedings of 2017 IEEE Nuclear Science Symposium and Medical Imaging Conference (NSS/MIC 2017) (Internet), 3 Pages, 2018/11

Journal Articles

$$gamma$$-ray pipe monitoring for comprehensive safeguards process monitoring of reprocessing facilities

Rodriguez, D.; Tanigawa, Masafumi; Mukai, Yasunobu; Isomae, Hidemi; Nakamura, Hironobu; Rossi, F.; Koizumi, Mitsuo; Seya, Michio

Proceedings of INMM 58th Annual Meeting (Internet), 9 Pages, 2017/07

Safegaurding nuclear material at reprocessing facilities utilizes sampling to verify the quantity and process monitoring to maintain continuity-of-knowledge to reduce re-verification. Solution Monitoring and Measurement Systems that determine the solution density and volume are installed at solution tanks, though this only provides indirect verification. To offset this safeguards limitation we propose measuring $$gamma$$ rays from solutions passing through the pipes and at the tanks to provide improved continuous monitoring and direct verification. This can provide both real-time flow measurements and Pu isotopic composition quantification through passive nondestructive assay. This concept was tested by recent experimental studies performed at the Japan Atomic Energy Agency's Plutonium Conversion Development Facility of flowing Pu-nitrate $$gamma$$ rays. This presentation will describe the concept details and analysis of using $$gamma$$ ray pipe monitoring as a capability for real-time safeguards verification.

Journal Articles

Effects of $$gamma$$-ray polarization in NRF-based nondestructive assay of nuclear materials

Omer, M.; Hajima, Ryoichi*; Shizuma, Toshiyuki*; Koizumi, Mitsuo

Proceedings of INMM 58th Annual Meeting (Internet), 7 Pages, 2017/07

Nuclear resonance fluorescence (NRF) is a process in which the electric and/or the magnetic dipole excitations of the nucleus take place. Since these excitations are unique signatures of each nucleus, the NRF provides a practical tool for a non-destructive detection and assay of nuclear materials. Using a polarized $$gamma$$-ray beam, distinguishing the nature of the excitation is straightforward. At a scattering angle of 90$$^{circ}$$, the electric dipole excitations are radiated normal to the polarization plane whereas the magnetic dipole excitations are radiated in the same plane as the incident beam polarization. By contrast, other $$gamma$$-ray interactions with the atom may exhibit different responses regarding the polarization of the incident beam. For example, the elastic scattering is expected to give approximately 60% lower yield in the direction of the incident beam polarization than the other direction. This fact significantly affects the sensitivity of the NRF technique because it is not possible to separate the NRF and the elastic scattering on the basis of the photon energy. We report the results of a photon scattering experiment on $$^{238}$$U using a 100% linearly polarized $$gamma$$-ray beam with an energy of 2.04 MeV. We demonstrate how the elastic scattering responds to the polarization of the incident beam. Accordingly, we are able to resolve the effects of the polarization of incident photon in an NRF measurement.

Journal Articles

Gamma radiation resistance of spin Seebeck devices

Yagmur, A.*; Uchida, Kenichi*; Ihara, Kazuki*; Ioka, Ikuo; Kikkawa, Takashi*; Ono, Madoka*; Endo, Junichi*; Kashiwagi, Kimiaki*; Nakashima, Tetsuya*; Kirihara, Akihiro*; et al.

Applied Physics Letters, 109(24), p.243902_1 - 243902_4, 2016/12

 Times Cited Count:2 Percentile:12.91(Physics, Applied)

Thermoelectric devices based on the spin Seebeck effect (SSE) were irradiated with gamma ($$gamma$$) rays with the total dose of around 3$$times$$10$$^{5}$$ Gy in order to investigate the $$gamma$$-radiation resistance of the devices. To demonstrate this, Pt/Ni$$_{0.2}$$Zn$$_{0.3}$$Fe$$_{2.5}$$O$$_{4}$$/Glass and Pt/Bi$$_{0.1}$$Y$$_{2.9}$$Fe$$_{5}$$O$$_{12}$$/Gd$$_{3}$$Ga$$_{5}$$O$$_{12}$$ SSE devices were used. We confirmed that the thermoelectric, magnetic, and structural properties of the SSE devices are not affected by the $$gamma$$-ray irradiation. This result demonstrates that SSE devices are applicable to thermoelectric generation even in high radiation environments.

Journal Articles

Simulation of the elastic scattering contributions to the NRF-based nondestructive assay of nuclear materials

Omer, M.; Hajima, Ryoichi*; Angell, C.*; Shizuma, Toshiyuki*; Hayakawa, Takehito*; Seya, Michio; Koizumi, Mitsuo

Proceedings of INMM 57th Annual Meeting (Internet), 9 Pages, 2016/07

Isotope-specific $$gamma$$-rays emitted in the nuclear resonance fluorescence (NRF) process provide a good technique for a non-destructive detection and assay of nuclear materials. We are developing technologies relevant to $$gamma$$-ray nondestructive detection and assay utilizing NRF. A Monte Carlo code to simulate NRF process is necessary for design and evaluation of NDA systems. We are developing NRFGeant4, a Geant4-based simulation code, for this purpose. In NRF experiments, highly-enriched targets are generally used such that the NRF signals are dominant and easily measured. In contrast, a real situation may involve very small contents of isotopes of interest. This results in a difficulty in measuring NRF signals because of the interference with other interactions, e.g. elastic scattering. For example, a typical nuclear fuel pellet contains about 90% of $$^{238}$$U as a host material and less than 1% of $$^{239}$$Pu as an isotope of interest. When measuring NRF of $$^{239}$$Pu, there would be a huge background coming from the elastic scattering of $$^{238}$$U. Therefore, an estimation of the elastic scattering with the host material is essential for precise determination of isotope of interest. Satisfying estimation of elastic scattering is currently not available except for some calculations. In the present study, we upgrade our simulation code to include the calculation of elastic scattering events.

Journal Articles

Measurement of the $$^{77}$$Se($$gamma$$, n) cross section and uncertainty evaluation of the $$^{79}$$Se(n, $$gamma$$) cross section

Kitatani, Fumito; Harada, Hideo; Goko, Shinji*; Iwamoto, Nobuyuki; Utsunomiya, Hiroaki*; Akimune, Hidetoshi*; Toyokawa, Hiroyuki*; Yamada, Kawakatsu*; Igashira, Masayuki*

Journal of Nuclear Science and Technology, 53(4), p.475 - 485, 2016/04

 Times Cited Count:2 Percentile:25.63(Nuclear Science & Technology)

Journal Articles

Recovery of the electrical characteristics of SiC-MOSFETs irradiated with gamma-rays by thermal treatments

Yokoseki, Takashi; Abe, Hiroshi; Makino, Takahiro; Onoda, Shinobu; Tanaka, Yuki*; Kandori, Mikio*; Yoshie, Toru*; Hijikata, Yasuto*; Oshima, Takeshi

Materials Science Forum, 821-823, p.705 - 708, 2015/07

Journal Articles

Mechanical properties of organic materials used in superconducting magnets irradiated by gamma rays at liquid nitrogen temperature

Nakamoto, Tatsushi*; Idesaki, Akira; Morishita, Norio; Ito, Hisayoshi; Kamiya, Tomihiro; Kimura, Nobuhiro*; Makida, Yasuhiro*; Ogitsu, Toru*; Ohata, Hirokatsu*; Yamamoto, Akira*

AIP Conference Proceedings 824, p.225 - 232, 2006/03

Radiation resistance with respect to mechanical properties of organic materials used in the superconducting magnets for the 50 GeV - 750 kW proton beam line for the J-PARC neutrino experiment was studied. Specimens cooled at liquid nitrogen temperature of 77 K were irradiated by gamma rays beyond 10 MGy. The flexural strength of glass-fiber reinforced plastics (GFRPs), the tear strength of polyimide films and the tensile lap-shear strength of adhesive films were evaluated. It was verified that the organic materials used in the superconducting magnet have a sufficient radiation resistance, and the degradation of their mechanical properties after 10 years operation was estimated to be negligible.

Journal Articles

LaCl$$_{3}$$(Ce) scintillation detector applications for environmental $$gamma$$-ray measurements of low to high dose rates

Tsutsumi, Masahiro; Tanimura, Yoshihiko

Nuclear Instruments and Methods in Physics Research A, 557(2), p.554 - 560, 2006/02

 Times Cited Count:12 Percentile:65.95(Instruments & Instrumentation)

A new cerium-doped LaCl$$_{3}$$(Ce) scintillator is evaluated with respect to the application in environmental $$gamma$$-ray dosimetry and spectrometry. The scintillator is very attractive for $$gamma$$-ray spectrometry in the case of high count rate, because it has excellent energy resolution and fast decay time. The performance characteristics of a scintillator with a 25.4 mm $$times$$ 25.4 mm LaCl$$_{3}$$(Ce) crystal are studied and compared to those of a NaI(Tl) scintillator with the same size crystal. Acquired pulse-height spectra are converted to dose rates by using the G(E) function method. Though the LaCl$$_{3}$$(Ce) crystal itself produces a rather high background in the crystal itself, the scintillator provides good energy information and dose-rate readings from low to high-level (several mGy/h) by subtracting the self-background. The properties of LaCl$$_{3}$$(Ce) scintillator suggest that the scintillator could be a promising candidate for monitoring at high-dose levels as in emergencies, as well as at ordinary levels of background radiation.

Journal Articles

Time-dependence of differential G-values of OH radicals in water under Ne ion radiolysis

Taguchi, Mitsumasa; Kojima, Takuji

JAEA-Review 2005-001, TIARA Annual Report 2004, p.181 - 182, 2006/01

The yields of OH radicals in water containing phenol have been investigated for several ten MeV/n C ion and Ne ion having the same LET value, as a function of the residual ion energy at the specific depth in water. In this study, beside such energy dependence, the dependence of reaction time of OH radical yield was examined by changing the concentration of phenol as solute. The defferential G'-values of OH radicals, those G-values per kinetic energy of ions increase with specific energy of Ne ions. The G'-value just after irradiation(1.5ns) is relatively high but become lower with reaction time to be the value (2.7) obtained for $$^{60}$$Co $$gamma$$-rays. It suggests the diffusion behavior of OH radicals locally induced in water.

Journal Articles

Decomposition of ${it p}$-nonylphenols in water and elimination of their estrogen activities by $$^{60}$$Co $$gamma$$-ray irradiation

Kimura, Atsushi; Taguchi, Mitsumasa; Otani, Yoshimi*; Takigami, Machiko; Shimada, Yoshitaka*; Kojima, Takuji; Hiratsuka, Hiroshi*; Namba, Hideki

Radiation Physics and Chemistry, 75(1), p.61 - 69, 2006/01

 Times Cited Count:12 Percentile:65.95(Chemistry, Physical)

Decomposition of ${it p}$-Nonylphenols (NPs) in water at 1 $$mu$$mol dm$$^{-3}$$ was decreased exponentially with absorbed dose when NPs were irradiated by $$^{60}$$Co$$gamma$$-rays. Two products having molecular weight of 236, presumably OH adducts of NPs, were detected by LC-MS analyses. The elimination of estrogen activity of aqueous NPs solution including such irradiation products at 5000 Gy (J kg$$^{-1}$$) was confirmed by the yeast two hybrid assay. These results should expand the application of ionizing radiation to the treatment of NPs.

Journal Articles

Chain terminations in the decomposition reactions of chloroethylenes in air through the deposition of alkylperoxy radicals on the wall of an irradiation vessel

Hakoda, Teruyuki; Kojima, Takuji

Radiation Physics and Chemistry, 74(5), p.302 - 309, 2005/12

 Times Cited Count:0 Percentile:0.01(Chemistry, Physical)

no abstracts in English

JAEA Reports

Estimation methods of blood boron concentration and error evaluation during boron neutron capture therapy for malignant brain tumor

Shibata, Yasushi*; Yamamoto, Kazuyoshi; Matsumura, Akira*; Yamamoto, Tetsuya*; Hori, Naohiko; Kishi, Toshiaki; Kumada, Hiroaki; Akutsu, Hiroyoshi*; Yasuda, Susumu*; Nakai, Kei*; et al.

JAERI-Research 2005-009, 41 Pages, 2005/03


The measurement of neutron flux and boron concentration in the blood during medical irradiation is indispensable in order to evaluate the radiation in boron neutron capture therapy. It is, however, difficult to measure the blood boron concentration during neutron irradiation because access to the patient is limited. Therefore we prospectively investigated the predictability of blood boron concentrations using the data obtained at the first craniotomy after infusion of a low dosage of BSH. When the test could not be carried out, the blood boron concentration during irradiation was also predicted by using the 2-compartment model. If the final boron concentration after the end of the infusion is within 95% confidence interval of the prediction, direct prediction from biexponential fit will reduce the error of blood boron concentrations during irradiation to around 6%. If the final boron concentration at 6 or 9 hours after the end of infusion is out of 95% confidence interval of the prediction, proportional adjustment will reduce error and expected error after adjustment to around 12%.

Journal Articles

Development of PVB film for low-dose dosimetry in radiation processing

Solomon, H. M.*; Kojima, Takuji

Nucleus, 33, p.16 - 20, 2005/00

Low-dose dosimeters were developed based on the mixture films of polyvinyl butyral (PVB) and the acid-sensitive dye leucomalachite green (LMG). Chloral hydrate (RX) was added to the mixture for enhancement of the radiation sensitivity of the film dosimeters. Different film dosimeter materials were prepared using 9.07 $$times$$ 10$$^{-5}$$mole LMG per one gram PVB with various RX:LMG molar concentration ratio. The dosimeter response, which is expressed in terms of change in absorbance at 628 nm per unit thickness, increased linearly with dose and RX concentration. The PVB-LMG dosimeter system, in which the ratio of RX concentration to that of LMG is higher than 10, show measurable dose range of 1-100 Gy for $$^{60}$$Co $$gamma$$-rays.

JAEA Reports

Development of elemental components in NDA systems for certifying radioactive wastes with the clearance level

Tsutsumi, Masahiro; Oishi, Tetsuya*; Yamasoto, Kotaro; Yoshida, Makoto

JAERI-Research 2004-021, 43 Pages, 2004/12


We have designed and developed a $$gamma$$ measurement system to certify radioactive wastes below the clearance level. By advancing non-destructive $$gamma$$-ray assay technology, it aims at quantitative determination of radionuclides contained in 200 litter drum/container wastes. Unlike the waste from a nuclear power plant, you have to assume that the waste originating from radioisotope usage and nuclear research laboratory have a variety of contents and a complex mixture of radionuclides, and furthermore the uniformity of activity concentration is unknown. To cope with the problems, we have developed the $$gamma$$-ray measuring instruments (units) with effective improvement of capability against each problem. They are (1) germanium $$gamma$$ spectrometry unit for enhanced peak identification, (2) positioning detection unit for positioning of $$gamma$$ interactions and (3)high-efficiency detection unit for separation of low-energy component. This report summarizes the direction of the clearance level measuring system and the three developed measuring units with their performances.

Journal Articles

Discrimination of neutrons and $$gamma$$ ray by a neutron detector comprising a superconducting tunnel junction on a single crystal of Li$$_{2}$$B$$_{4}$$O$$_{7}$$

Nakamura, Tatsuya; Katagiri, Masaki; Soyama, Kazuhiko; Ukibe, Masahiro*; Ikeuchi, Takashi*; Okubo, Masataka*

Nuclear Instruments and Methods in Physics Research A, 529(1-3), p.402 - 404, 2004/08

 Times Cited Count:8 Percentile:50.96(Instruments & Instrumentation)

We evaluated the neutron-$$gamma$$-rays discrimination of the neutron detector comprising a superconducting tunnel junction (STJ) on the single crystal of Li$$_{2}$$B$$_{4}$$O$$_{7}$$. The neutron detector was irradiated with X-rays, $$gamma$$-rays and neutrons, and the signal pulses were analyzed including pulse height distributions and rise times. It was found that the most of the signal pulses for the neutron-events exhibited slower rise times than those for X-rays and $$gamma$$-rays. This indicated the capability of neutron-$$gamma$$-rays discrimination of the detector using the differences in the decay time of the signal current.

Journal Articles

Dyed Polyvinyl Chloride films for use as high-dose routine dosimeters in radiation processing

Mai, H. H.*; Duong, N. D.*; Kojima, Takuji

Radiation Physics and Chemistry, 69(5), p.439 - 444, 2004/04

 Times Cited Count:19 Percentile:77.18(Chemistry, Physical)

Characteristics of the polyvinyl chloride films containing 0.11wt% of malachite green oxalate or 6GX-setoglausine with 100$$mu$$m in thickness were studied for use as routine dosimeters in radiation processing. These films show basically color bleaching under $$^{60}$$Co $$gamma$$-ray irradiation in a dose range of 5 to 50 kGy. The sensitivity of the dosimeters and the linearity of dose response curves are improved by adding 2.5% of chloral hydrate [CCl$$_3$$CH(OH)$$_2$$] and 0.15% hydroquinone [HOC$$_6$$H$$_4$$OH]. These additions extent the minimum dose limit to 1 kGy covering dosimetric quality assurance in radiation processing of food and healthcare products. The dose responses of both films at irradiation temperatures of 20-35$$^{circ}$$C are constant relative to those at 25$$^{circ}$$C, and the irradiation temperature coefficients for 35-55$$^{circ}$$C were estimated to be (0.43 $$pm$$ 0.01)%/ $$^{circ}$$C. The dosimeter characteristics are stable within 1% at 25$$^{circ}$$C before and 60 days after irradiation.

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