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Journal Articles

Nature of the physicochemical process in water photolysis uncovered by a computer simulation

Kai, Takeshi; Toigawa, Tomohiro; Ukai, Masatoshi*; Fujii, Kentaro*; Watanabe, Ritsuko*; Yokoya, Akinari*

Journal of Chemical Physics, 158(16), p.164103_1 - 164103_8, 2023/04

New insight into water radiolysis and photolysis is indispensable in the dramatic progress of sciences and technologies in various research areas. In the radiation field, reactive hydrated electrons are considerably produced along radiation tracks. Although the formation results from a transient dynamic correlation between ejected electrons and water, the individual mechanisms of electron thermalization, delocalization, and polarization are unknown. Using a dynamic Monte Carlo code, we show herein that the ejected electrons are immediately delocalized by molecular excitations in parallel with phonon polarization and gradually thermalized by momentum transfer with an orientation polarization in a simultaneous manner. Our results show that these mechanisms heavily depend on the intermolecular vibration and rotation modes peculiar to water. We expect our approach to be a powerful technique for connecting physical and chemical processes in various solvents.

Journal Articles

A Significant role of non-thermal equilibrated electrons in the formation of deleterious complex DNA damage

Kai, Takeshi; Yokoya, Akinari*; Ukai, Masatoshi*; Fujii, Kentaro*; Toigawa, Tomohiro; Watanabe, Ritsuko*

Physical Chemistry Chemical Physics, 20(4), p.2838 - 2844, 2018/01

 Times Cited Count:19 Percentile:75.72(Chemistry, Physical)

It is thought that complex DNA damage which induces in radiation biological effects is formed at radiation track end. Thus, the earliest stage of water radiolysis at the electron track end was studied to predict DNA damage. These results indicate that DNA damage sites comprising multiple nucleobase lesions with a single strand breaks can therefore be formed by multiple collisions of the electrons within three base pairs (3bp) of a DNA strand. This multiple damage site cannot be processed by base excision repair enzymes. However, pre-hydrated electrons can also be produced resulting in an additional base lesion more than 3bp away from the multi-damage site. This clustered damage site may be finally converted into a double strand break (DSB) when base excision enzymes process the additional base lesions. These DSBs include another base lesion(s) at their termini that escape from the base excision process and which may result in biological effects such as mutation in surviving cells.

Journal Articles

Deceleration processes of secondary electrons produced by a high-energy Auger electron in a biological context

Kai, Takeshi; Yokoya, Akinari; Ukai, Masatoshi; Fujii, Kentaro; Watanabe, Ritsuko

International Journal of Radiation Biology, 92(11), p.654 - 659, 2016/11

 Times Cited Count:9 Percentile:68.73(Biology)

Journal Articles

Dynamic behavior of secondary electrons in liquid water at the earliest stage upon irradiation; Implications for DNA damage localization mechanism

Kai, Takeshi; Yokoya, Akinari*; Ukai, Masatoshi*; Fujii, Kentaro*; Watanabe, Ritsuko*

Journal of Physical Chemistry A, 120(42), p.8228 - 8233, 2016/10

 Times Cited Count:16 Percentile:61.15(Chemistry, Physical)

Low energy secondary electrons produced by an ionizing radiation in a living cell may involve in formation of complexed DNA damage. We performed theoretical study for numerical calculation of dynamic behavior of the electrons to imply a formation of radiation damage to DNA. The decelerating electrons are gradually attracted to their parent cations by the Coulombic force within hundreds of fs, and about 12.6 % of electrons are finally distributed within 2 nm from the cations. The collision fraction of the ionization and excitation within 1 nm from the cation was estimated to be about 40 %. From those analyses, we suggested a process of DNA damage that the secondary electrons may cause highly localized lesions around a cation in DNA molecule through additional dissociative electron transfer as well as the ionization or the excitation if the electrons are ejected from DNA. The localized damage may involve ultimately in biological effects such as cell death or mutation induction.

Journal Articles

Demonstration result of sample assay system equipped alternative He-3 detectors

Tanigawa, Masafumi; Mukai, Yasunobu; Tobita, Hiroshi; Kurata, Noritaka*; Kobayashi, Nozomi*; Takase, Misao*; Makino, Risa; Ozu, Akira; Nakamura, Hironobu; Kurita, Tsutomu; et al.

56th Annual Meeting of the Institute of Nuclear Materials Management (INMM 2015), Vol.1, p.693 - 701, 2016/00

no abstracts in English

Journal Articles

Development of sample assay system equipped with $$^{3}$$He Alternative Neutron Detectors (ASAS), 1; Design and fabrication of ASAS detector

Ozu, Akira; Tobita, Hiroshi; Kureta, Masatoshi; Tanigawa, Masafumi; Mukai, Yasunobu; Nakamichi, Hideo; Nakamura, Hironobu; Kurita, Tsutomu; Seya, Michio

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-36-Kai Nenji Taikai Rombunshu (Internet), 9 Pages, 2015/12

Against the background of the serious shortage of $$^{3}$$He gas, the Japan Atomic Energy Agency (JAEA) has newly developed an alternative ZnS ceramic scintillation neutron detector for the safeguards, with the support of the government (MEXT). A demonstrator of plutonium inventory sample assay system (ASAS) has been also developed as an alternative HLNCC (High Level Neutron Coincidence Counter). The results from numerical simulations using Monte-Carlo code MCNPX showed that the fundamental performances of ASAS equipped with the 24 alternative neutron detectors, such as neutron detection efficiency and die-away time, equal to or higher than those of conventional HLNCC could be obtained. Here we present the inner mechanical structure of ASAS, together with the results of the simulating design.

Journal Articles

Development of sample assay system equipped with $$^{3}$$He Alternative Neutron Detectors (ASAS), 2; Results of ASAS measurement test

Tanigawa, Masafumi; Mukai, Yasunobu; Kurita, Tsutomu; Makino, Risa; Nakamura, Hironobu; Tobita, Hiroshi; Ozu, Akira; Kureta, Masatoshi; Seya, Michio

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-36-Kai Nenji Taikai Rombunshu (Internet), 9 Pages, 2015/12

Against the background of the serious shortage of $$^{3}$$He gas, design and development of a new detector equipped ZnS/$$^{10}$$B$$_{2}$$O$$_{3}$$ ceramic scintillation neutron detectors in JAEA, with the support of the government (the Ministry of Education, Culture, Sports, Science & Technology). The design of the alternative $$^{3}$$He detector is referred from INVS (INVentory Sample assay system (HLNCC (High Level Neutron Coincidence Counter) type)) which is being used for the verification of MOX powder etc. and is named it as ASAS (Alternative Sample Assay System). In order to prove the Pu quantitative performance as an alternative technology, several measurement tests and comparison test with INVS were conducted using ASAS. In these tests, evaluation of fundamental performance (counting efficiency and die-away time) and uncertainty evaluations were implemented. As a result, although fundamental performance of ASAS was not achieved to the one of INVS, we could confirm that ASAS has almost the same Pu quantitative performance including measurement uncertainty as that of INVS.

Journal Articles

Thermal equilibrium and prehydration processes of electrons injected into liquid water calculated by dynamic Monte Carlo method

Kai, Takeshi; Yokoya, Akinari; Ukai, Masatoshi*; Fujii, Kentaro; Watanabe, Ritsuko

Radiation Physics and Chemistry, 115, p.1 - 5, 2015/10

 Times Cited Count:29 Percentile:94.36(Chemistry, Physical)

Role of secondary electrons on DNA damage have not been understood sufficiently because there still exists a lack of study for thermalization process of an electron in liquid phase. We calculated thermalization lengths and spatial distributions of an electron in liquid water using cross sections for rotation and phonon excitations in a liquid phase. Obtained thermalization lengths are in good agreement with experimental results reported by literatures. Thermalization time was also estimated from time evolution of spatial distributions of the incident electron to be hundreds femtoseconds. From these results, we predict that thermalization and pre-hydration of electron might progress simultaneously. These electrons possibly cause damage in biological molecules in a cell. Particularly severe types of DNA damage consisting of proximately located multiple lesions are potentially induced by reaction of DNA with the thermalized electrons by dissociative electron transfer.

Journal Articles

Demonstration result of sample assay system equipped alternative He-3 detectors

Nakamura, Hironobu; Mukai, Yasunobu; Tobita, Hiroshi; Nakamichi, Hideo; Ozu, Akira; Kureta, Masatoshi; Kurita, Tsutomu; Seya, Michio

Proceedings of 37th ESARDA Annual Meeting (Internet), p.45 - 53, 2015/08

JAEA conducted an R&D project to develop a new type of neutron detector using ZnS/$$^{10}$$B$$_{2}$$O$$_{3}$$ ceramic scintillator (as an alternative neutron detector to He-3) with support of Japanese government. The design of the JAEAs alternative system (ASAS: Alternative Sample Assay System using ceramic scintillator tubes) refers basically to the INVS (INVentory Sample assay system) which is the passive type of neutron assay system equipped total 18 He-3 tubes and capable of measuring the small amount of Pu in the MOX powder or Pu nitrate solution in a vial for nuclear material accountancy and safeguards verification. In order to prove the alternative technology and the performance instead of He-3 detector, and to establish Pu measurement capability, JAEA developed and fabricated ASAS equipped 24 alternative ceramic scintillator tubes (which is equivalent to the same counting efficiency of INVS) and demonstrated. The demonstration activity implemented the confirmation of reproducibility about sample positioning, optimization of detector parameters, counting statistical uncertainty, stability check and figure of merit (FOM) using Cf check source and actual MOX powder in PCDF (Plutonium Conversion Development Facility). In addition, performance comparison between the current INVS and the ASAS was also implemented. In this paper, we present demonstration results with design information with Monte-Carlo simulation code (MCNP).

Journal Articles

Nitrogen K-edge X-ray absorption near edge structure of pyrimidine-containing nucleotides in aqueous solution

Shimada, Hiroyuki*; Minami, Hirotake*; Okuizumi, Naoto*; Sakuma, Ichiro*; Ukai, Masatoshi*; Fujii, Kentaro; Yokoya, Akinari; Fukuda, Yoshihiro*; Saito, Yuji

Journal of Chemical Physics, 142(17), p.175102_1 - 175102_9, 2015/05

AA2015-0073.pdf:1.15MB

 Times Cited Count:10 Percentile:38.84(Chemistry, Physical)

Journal Articles

Cross sections, stopping powers, and energy loss rates for rotational and phonon excitation processes in liquid water by electron impact

Kai, Takeshi; Yokoya, Akinari; Ukai, Masatoshi*; Watanabe, Ritsuko

Radiation Physics and Chemistry, 108, p.13 - 17, 2015/03

 Times Cited Count:22 Percentile:90.12(Chemistry, Physical)

Role of secondary electrons on DNA damage have not been understood sufficiently because there still exists a lack of cross section of rotational and phonon excitation in the liquid phase for precise simulation of the electron behavior. We calculated cross sections, stopping powers, and energy loss rates for the excitations in liquid water. The values for rotation are less by three orders of magnitude than those in the gas phase, while the values for phonon are close to those reported for amorphous ice. Thermalization process has so far been estimated from an assumption that the energy loss rates do not depend strongly on the energy below 1 eV. However, we found that the energy loss rates depend significantly on the energy. This fact indicates that the thermalization time will be longer than the previously estimated time, and we predict that thermalization process strongly involve in subsequent hydrated and chemical processes. The data set provide here is expected to useful to make the role of the secondary electrons on DNA damage much clear.

Journal Articles

Dynamics of low-energy electrons in liquid water with consideration of Coulomb interaction with positively charged water molecules induced by electron collision

Kai, Takeshi; Yokoya, Akinari; Ukai, Masatoshi*; Fujii, Kentaro; Higuchi, Mariko; Watanabe, Ritsuko

Radiation Physics and Chemistry, 102, p.16 - 22, 2014/09

 Times Cited Count:21 Percentile:86.56(Chemistry, Physical)

no abstracts in English

Journal Articles

Nitrogen K-edge X-ray absorption near edge structure (XANES) spectra of purine-containing nucleotides in aqueous solution

Shimada, Hiroyuki*; Fukao, Taishi*; Minami, Hirotake*; Ukai, Masatoshi*; Fujii, Kentaro; Yokoya, Akinari; Fukuda, Yoshihiro*; Saito, Yuji

Journal of Chemical Physics, 141(5), p.055102_1 - 055102_8, 2014/08

 Times Cited Count:15 Percentile:54.25(Chemistry, Physical)

Journal Articles

Development and demonstration of a Pu NDA system using ZnS/$$^{10}$$B$$_{2}$$O$$_{3}$$ ceramic scintillator detectors

Nakamura, Hironobu; Ozu, Akira; Kobayashi, Nozomi*; Mukai, Yasunobu; Sakasai, Kaoru; Nakamura, Tatsuya; Soyama, Kazuhiko; Kureta, Masatoshi; Kurita, Tsutomu; Seya, Michio

Proceedings of INMM 55th Annual Meeting (Internet), 9 Pages, 2014/07

To establish an alternative technique of He-3 neutron detector that is used for nuclear material accountancy and safeguards, we have started an R&D project to develop a new type of neutron detector (Pu NDA system) using ZnS/$$^{10}$$B$$_{2}$$O$$_{3}$$ ceramic scintillator with support of Japanese government. The design of the alternative system (ASAS: Alternative Sample Assay System) is basically referenced from INVS (INVentory Sample assay system) which is passive neutron assay system of plutonium and has total 18 He-3 tubes (about 42% of counting efficiency), and the small amount of Pu in the MOX powder or Pu nitrate solution in a vial can be measured. In order to establish the technology and performance after the fabrication of the new detector progresses, we are planning to conduct demonstration activity in the early 2015 experimentally. The demonstration activity implements the confirmation of reproducibility about sample positioning, optimization of detector parameters, counting statistical uncertainty, stability (temperature and $$gamma$$-ray change) check and figure of merit (FOM) using check source and actual MOX powder. In addition to that, performance comparison between current INVS and the ASAS are also conducted. In this paper, we present some analytical study results using a Monte-Carlo simulation code (MCNP), entire ASAS design and demonstration plan to prove technology and performance.

Journal Articles

Localization of DNA damage induced by inner-shell ionization

Yokoya, Akinari; Ukai, Masatoshi*; Oka, Toshitaka*; Kai, Takeshi; Watanabe, Ritsuko; Fujii, Kentaro

Shototsu, 11(2), p.33 - 39, 2014/03

no abstracts in English

Journal Articles

Structural changes of nucleic acid base in aqueous solution as observed in X-ray absorption near edge structure (XANES)

Shimada, Hiroyuki*; Fukao, Taishi*; Minami, Hirotake*; Ukai, Masatoshi*; Fujii, Kentaro; Yokoya, Akinari; Fukuda, Yoshihiro*; Saito, Yuji

Chemical Physics Letters, 591, p.137 - 141, 2014/01

 Times Cited Count:8 Percentile:33.58(Chemistry, Physical)

Journal Articles

Unpaired electron species in thin films of calf-thymus DNA molecules induced by nitrogen and oxygen K-shell photoabsorption

Oka, Toshitaka; Yokoya, Akinari; Fujii, Kentaro; Fukuda, Yoshihiro; Ukai, Masatoshi*

Physical Review Letters, 109(21), p.213001_1 - 213001_5, 2012/11

 Times Cited Count:12 Percentile:59.83(Physics, Multidisciplinary)

no abstracts in English

Journal Articles

Demonstration plan of Pu NDA system using ZnS ceramic scintillator

Nakamura, Hironobu; Kureta, Masatoshi; Ozu, Akira; Soyama, Kazuhiko; Nakamura, Tatsuya; Mukai, Yasunobu; Seya, Michio

Kaku Busshitsu Kanri Gakkai (INMM) Nihon Shibu Dai-33-Kai Nenji Taikai Rombunshu (Internet), 8 Pages, 2012/10

To establish an alternative technique of $$^{3}$$He neutron detector as a safeguards application, we have started an R&D project to develop a new type of neutron detector (Pu NDA) using ZnS ceramic scintillator with support of Japanese government. The detector design is basically referenced from PCDF-PCAS (Plutonium Canister Assay System) which has total 22 $$^{3}$$He tubes and is used for a MOX canister measurement. In order to prove the technology and performance after the fabrication, we are planning to conduct 2 stage of demonstration activity. The first stage of demonstration implements the confirmation of flatness response profile for vertical axis, determination of detector parameters and basic performance comparison using Cf source and MOX powder around June 2013. After some modification will have completed, the second stage of demonstration activity will be conducted around December 2013. During the activity, we plan to perform the performance comparison between current PCAS and the new Pu NDA regarding Pu mass and counting statistics. It is expected that the new Pu NDA proves good performance for establishment of alternative technology instead of $$^{3}$$He neutron detector.

Journal Articles

Demonstration plan of Pu NDA system using ZnS ceramic scintillator

Nakamura, Hironobu; Kureta, Masatoshi; Ozu, Akira; Soyama, Kazuhiko; Nakamura, Tatsuya; Mukai, Yasunobu; Seya, Michio

Proceedings of INMM 53rd Annual Meeting (CD-ROM), 6 Pages, 2012/07

To establish an alternative technique of $$^{3}$$He neutron detector that is used for nuclear material accountancy and safeguards, we have started an R&D project to develop a new type of neutron detector (Pu NDA system) using ZnS ceramic scintillator with support of Japanese government. The design of the alternative system is basically referenced from PCDF-PCAS (Plutonium Canister Assay System) which can measure up to 5 kg Pu mass in a MOX canister. In order to prove the technology and performance after the fabrication of the new detector progresses, we are planning to conduct 2 stage of demonstration activity in the near future experimentally. The first stage of demonstration activity implements the confirmation of flatness response profile for vertical axis, integrity check of detector parameters and basic performance comparison between calculated and measured using MOX powder around June 2013. After some modification and upgrade will have completed, we will conduct second stage of demonstration activity around December 2013. During the activity, we plan to perform the performance comparison between current PCAS and the new Pu NDA related to the counting statistics.

JAEA Reports

Conceptual design of multipurpose compact research reactor; Annual report FY2010 (Joint research)

Imaizumi, Tomomi; Miyauchi, Masaru; Ito, Masayasu; Watahiki, Shunsuke; Nagata, Hiroshi; Hanakawa, Hiroki; Naka, Michihiro; Kawamata, Kazuo; Yamaura, Takayuki; Ide, Hiroshi; et al.

JAEA-Technology 2011-031, 123 Pages, 2012/01

JAEA-Technology-2011-031.pdf:16.08MB

The number of research reactors in the world is decreasing because of their aging. However, the planning to introduce the nuclear power plants is increasing in Asian countries. In these Asian countries, the key issue is the human resource development for operation and management of nuclear power plants after constructed them, and also the necessity of research reactor, which is used for lifetime extension of LWRs, progress of the science and technology, expansion of industry use, human resources training and so on, is increasing. From above backgrounds, the Neutron Irradiation and Testing Reactor Center began to discuss basic concept of a multipurpose low-power research reactor for education and training, etc. This design study is expected to contribute not only to design tool improvement and human resources development in the Neutron Irradiation and Testing Reactor Center but also to maintain and upgrade the technology on research reactors in nuclear power-related companies. This report treats the activities of the working group from July 2010 to June 2011 on the multipurpose low-power research reactor in the Neutron Irradiation and Testing Reactor Center and nuclear power-related companies.

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