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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.
Kai, Takeshi; Yokoya, Akinari*; Fujii, Kentaro*; Watanabe, Ritsuko*
Hoshasen Kagaku (Internet), (106), p.21 - 29, 2018/11
It is thought to that the biological effects such as cell death or mutation are induced by complex DNA damage which are formed by several damage sites within a few nm. As the prediction of complex DNA damage at an electron track end, we report our outcomes. These results indicate that DNA damage sites comprising multiple nucleobase lesions with a single strand breaks can be formed by multiple collisions of the electrons within 1 nm. This multiple damage site cannot be processed by base excision repair enzymes. Pre-hydrated electrons can also be produced resulting in an additional base lesion over a few nm from the multi-damage site. This clustered damage site may be finally converted into a double strand break. These DSBs include another base lesion(s) at their termini that escape from the base excision process and which may result in biological effect. Our simulation is useful to reveal phenomena involved in radiation physico-chemistry as well as the DNA damage prediction.
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：22 Percentile：75.15(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.
Watanabe, Ritsuko*; Kai, Takeshi; Hattori, Yuya*
Radioisotopes, 66(11), p.525 - 530, 2017/11
To understand the mechanisms of radiation biological effects, modeling and simulation studies are important. In particular, simulation approach is powerful tool to evaluate modeling of mechanisms and the relationship among experimental results in different spatial scale of biological systems such as DNA molecular and cell. This article summarizes our approach to evaluate radiation action on DNA and cells by combination of knowledge in radiation physics, chemistry and biology. It contains newly theoretical approach to estimate physico-chemical process of DNA damage induction in addition to typical method of DNA damage prediction. Outline of the mathematical model for dynamics of DNA damage and cellular response is also presented.
Kai, Takeshi; Yokoya, Akinari*; Fujii, Kentaro*; Watanabe, Ritsuko*
Yodenshi Kagaku, (8), p.11 - 17, 2017/03
It is thought to that the biological effects such as cell death or mutation are induced by complex DNA damage which are formed by several damage sites within a few nm. We calculated dynamic behavior of secondary electrons produced by primary electron and positon of high energy in water whose composition ratio is similar to biological context. The secondary electrons induce the ionization or electronic excitation near the parent cations. The decelerated electrons about 10% are distributed to their parent cations by the attractive Coulombic force. From the results, we predicted the following formation mechanism for the complex DNA damage. The electrons ejected from DNA could induce the ionization or the electronic excitation within the DNA. The electrons attracted by the Coulombic force are pre-hydrated in water layer of the DNA. The pre-hydrated electrons could induce to the DNA damage by dissociative electron transfer. As the results, the complex DNA damage with 1 nm could be formed by the interaction of not only the primary electron or positon but also the secondary electrons.
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：18 Percentile：62.79(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.
Kai, Takeshi; Yokoya, Akinari*; Fujii, Kentaro*; Watanabe, Ritsuko*
Hoshasen Kagaku (Internet), (102), p.49 - 56, 2016/00
Behavior analysis of low energy electrons in liquid water provides the fundamentals for successive radiation chemistry, and it makes analysis of DNA damage implication involved in the electrons possible. We have progressed theoretical studies for radiation physicochemical process of water to clear the role of secondary electrons damage to DNA. The process has included many unknown factors for the DNA damage so far. We implied a newly formation process of unrepair DNA damage produced by the secondary electrons. We report our outcomes separately in three manuscripts entitled "Recent progress of radiation physicochemical process (first, second, third parts)". In this second part, we show calculated results of thermalization lengths and times of electrons in water to verify a dynamic Monte Carlo code developed in this study. From the calculated results, we also report our prediction, which are different from previous one, for thermalization and pre-hydration processes.
Yokoya, Akinari; Fujii, Kentaro; Ushigome, Takeshi; Shikazono, Naoya; Urushibara, Ayumi; Watanabe, Ritsuko
Radiation Protection Dosimetry, 122(1-4), p.86 - 88, 2006/12
Times Cited Count：11 Percentile：60.27(Environmental Sciences)We have studied yields of DNA damages induced by soft X-rays obtained from a conventional soft X-ray machine in a LET region between 
-rays and ultrasoft X-rays. Practically soft X-rays with a broad energy spectrum emitted from a target of heavy metal, such as tungsten, have been widely used not only for radiobiological experiments but also for medical application such as mammography. Radiation weighting factors for these soft X-rays have been assigned to be 1 by ICRP. However, the fraction of a large number of low energy photons in the spectrum (below several tens keV) provided by bremsstrahlung is expected to be more effective for DNA damage induction than -rays since low energy photo- and Auger electrons predominantly ejected in consequence of a photoelectric effect can produce dense clusters of ionization/excitation on DNA molecules. We have examined the yield of DNA strand breaks induced by white soft X-rays (150 kVp, tungsten target). Yields of base lesions revealed by base excision repair enzymes will be also presented.
Yokoya, Akinari; Shikazono, Naoya; Urushibara, Ayumi; Fujii, Kentaro; Akamatsu, Ken; Watanabe, Ritsuko
Hoshasen Seibutsu Kenkyu, 40(2), p.168 - 184, 2005/06
Ionizing radiation causes modifications in a DNA molecule depending on the characteristic tack-structure in which two or more isolated lesions arise in a few nm scale (1 or 2 helical turn of DNA), known as "clustered DNA damage". These clustered DNA damages could be distinct from those by reactive oxygen species (ROS) endogenously induced on their severity of induction of biological effects such as mutation. However, the studies on the nature and repair mechanism of clustered DNA damage have still been behind because of the technical difficulties on determination of the chemical structure and yield. This article reviews some experimental evidences of the clustered DNA damages in this research field, as well as our recent progress on the studies on the clustered DNA damages using both molecular biological techniques and synchrotron spectroscopic method.
Watanabe, Ritsuko; Yokoya, Akinari; Fujii, Kentaro; Saito, Kimiaki
International Journal of Radiation Biology, 80(11-12), p.823 - 832, 2004/11
Times Cited Count：15 Percentile：68.2(Biology)no abstracts in English
Yokoya, Akinari; Takakura, Kaoru*; Watanabe, Ritsuko; Akamatsu, Ken*; Ito, Takashi*
Radiation Research, 162(4), p.469 - 473, 2004/10
Radicals induced in a single crystal of 5-bromouracil (BrUra) by synchrotron soft X-rays in the Br K-edge region (13.461-13482 keV) were investigated using the X-band EPR method. The crystal was irradiated at three peak energies in the absorption spectrum at room temperature or at 80K. A hydrogen abstraction radical derived from N1 atom of the pyrimidine ring was commonly observed for all of the energies used, though with some variation in quantity. Similar characteristics were also observed in the EPR signal for the off-K-edge low energy (13.42 keV) and when 
Co -ray irradiation was employed as the reference. When irradiated at 80K, a much larger exposure (roughly 10 times) of soft X-rays was needed to obtain the same signal intensity as that observed at room temperature. EPR signals were not detectable with g-irradiation at liquid nitrogen temperature.
Yokoya, Akinari; Takakura, Kaoru*; Watanabe, Ritsuko; Akamatsu, Ken*; Ito, Takashi*
Radiation Research, 162(4), p.469 - 473, 2004/10
Times Cited Count：3 Percentile：10.08(Biology)X-ray absorption spectra from single crystals of 5-Bromouracil were measured with the transmission mode in the energy range from 13.41 to 13.50 keV using the linearly polarized synchrotron radiation (SR). A characteristic resonance structure, consisting of four peaks, was recognized in the spectra in the Br K-edge region. The intensities of these peaks were strongly dependent on the crystal rotation about the normal of the crystal b-c plane, which was set perpendicular to the X-ray beam direction. (SR X-rays are polarized in the horizontal plane.) Molecular orbital calculations indicate that these resonance peaks are associated with the transitions from the 1s electron of Br to the Br-C molecular antibonding orbitals and to a shape resonance. The observed anisotropy of each photoabsorption peak might originate from the angular dependences of these molecular orbitals.
Masuko, Kenji*; Watanabe, Ritsuko; Kume, Etsuo
JAERI-Data/Code 2004-005, 72 Pages, 2004/03
JAERI-Data-Code-2004-005.pdf:10.48MB
no abstracts in English
Watanabe, Ritsuko; Nikjoo, H.*
International Journal of Radiation Biology, 78(11), p.953 - 966, 2002/11
Times Cited Count：39 Percentile：90.08(Biology)Incorporation of halogenated pyrimidines, iodo- and bromo-deoxyuridines (HP), into DNA is known to sensitize cells to radiation. The aim of this study is to estimate the enhancement of DNA strand break induced by low LET radiation in the presence of HP and examine source, complexity and clustering properties of damage that could provide correlation between DNA damage and lethality. Monte Carlo track structure methods were used to model the induction of strand breakage by X-ray photons. As a result, the increase of strand breaks due to Br/IdU incorporation could be explained by the mechanism of uracilyl radical production originated from e-aq and direct hits on bases. The significant contribution of electron migration along DNA within limited distance is shown. It is also shown that the incorporation of Br/IdU causes a spectral shift towards greater complexity of clustered DNA damage. Further, it has been supported that DSB is responsible for radiation-induced cell killing.
Watanabe, Ritsuko; Saito, Kimiaki
Radiation and Environmental Biophysics, 41(3), p.207 - 215, 2002/08
Times Cited Count：21 Percentile：51.29(Biology)no abstracts in English
Kai, Takeshi; Yokoya, Akinari*; Ukai, Masatoshi*; Fujii, Kentaro*; Watanabe, Ritsuko*; Yonetani, Yoshiteru*; Toigawa, Tomohiro; Sato, Tatsuhiko
no journal, ,
It is very important to study water radiolysis by electrons because the study are applied to fields involved in atomic industry and radiotherapy, the study is also useful to predict radiation damage to DNA in a living cell. In this study, we calculated deceleration process of secondary electrons produced by ionization at a primary electron track end, at which a primary and secondary electrons densely deposit those energies to water, to understand the earliest process of water radiolysis. From the results, the secondary electrons distributed 10 nm from parent cations at 300 fs, and the mean energy of the electrons reached 0.7 eV. At this timescale, we indicated that the energy distribution shows the non-equilibrium state strongly, and fraction of the electrons energy below 0.1 eV is more than 10
. The results may indicate a new insight of the formation of prehydrated electrons due to the extremely low energy electrons.
Kai, Takeshi; Toigawa, Tomohiro; Ukai, Masatoshi*; Fujii, Kentaro*; Watanabe, Ritsuko*; Yokoya, Akinari*
no journal, ,
Fundamental studies of water radiolysis by radiation and laser irradiation are applied to atomic industry, and provide useful fundamental insights to understanding of radiation DNA damage. We developed a code to simulate dynamic behavior of electrons produced in water by energy deposition at energies, also performed theoretical study for the behaviors. The spatial probability distributions of the electrons depend on the deposition energies, also show the exponential or Gaussian types. We also show calculated results of energy probability distributions of the electrons. We found that the distributions below 100 meV are gradually close to Maxwell distribution with the temporal evolution, while the distributions above 100 meV not depend on the temporal evolution due to effect of Coulombic field of the parent cation. The findings provide significant insights to a connection radiation physics and radiation chemistry.
