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Journal Articles

Rapid multi-nuclide identification method by simultaneous $$beta$$, $$gamma$$, and X-ray spectrum analysis

Oshima, Masumi*; Goto, Jun*; Hayakawa, Takehito*; Asai, Masato; Kin, Tadahiro*; Shinohara, Hirofumi*

Isotope News, (790), p.19 - 23, 2023/12

When analyzing samples that contain many radionuclides at various concentrations, such as radioactive waste or fuel debris, it is difficult to apply general spectrum analysis methods and is necessary to chemically separate each nuclide before quantifying it. The chemical separation is especially essential for analysis using a liquid scintillation counter (LSC). In this report, the authors explain the newly developed spectral determination method (SDM) in which the entire spectrum is fitted to quantify radioactivity of nuclides mixed in a sample. By applying the SDM to $$beta$$- and X-ray spectrum measured by LSC and $$gamma$$-ray spectrum measured by Ge detector simultaneously, the authors demonstrated that radioactivity of 40 radionuclides mixed in a sample at concentrations varying by two orders could be quantified, which is useful to simplify chemical separation process in radionuclide quantification.

Journal Articles

The Role of collision ionization of K-shell ions in nonequilibrium plasmas produced by the action of super strong, ultrashort PW-class laser pulses on micron-scale argon clusters with intensity up to 5 $$times$$ 10$$^{21}$$ W/cm$$^{2}$$

Skobelev, I. Yu.*; Ryazantsev, S. N.*; Kulikov, R. K.*; Sedov, M. V.*; Filippov, E. D.*; Pikuz, S. A.*; Asai, Takafumi*; Kanasaki, Masato*; Yamauchi, Tomoya*; Jinno, Satoshi; et al.

Photonics (Internet), 10(11), p.1250_1 - 1250_11, 2023/11

 Times Cited Count:0 Percentile:0(Optics)

It is challenging to clearly distinguish the impacts of the optical field and collisional ionization in the evolution of the charge state of a plasma produced when matter interacts with high-intensity laser pulses. In this work, time-dependent calculations of plasma kinetics are used to show that it is possible only when low-density gaseous targets with sufficiently small clusters are used. In the case of Ar plasma, the upper limit of the cluster radius was estimated to be $$R_0 = 0.1 mu$$m.

Journal Articles

New $$K$$ isomers in $$^{248}$$Cf

Orlandi, R.; Makii, Hiroyuki; Nishio, Katsuhisa; Hirose, Kentaro; Asai, Masato; Tsukada, Kazuaki; Sato, Tetsuya; Ito, Yuta; Suzaki, Fumi; Nagame, Yuichiro*; et al.

Physical Review C, 106(6), p.064301_1 - 064301_11, 2022/12

 Times Cited Count:1 Percentile:33.4(Physics, Nuclear)

Journal Articles

On the adsorption and reactivity of element 114, flerovium

Yakushev, A.*; Lens, L.*; D$"u$llmann, Ch. E.*; Khuyagbaatar, J.*; J$"a$ger, E.*; Krier, J.*; Runke, J.*; Albers, H. M.*; Asai, Masato; Block, M.*; et al.

Frontiers in Chemistry (Internet), 10, p.976635_1 - 976635_11, 2022/08

 Times Cited Count:9 Percentile:79.28(Chemistry, Multidisciplinary)

Flerovium (Fl, element 114) is the heaviest element chemically studied so far. The first chemical experiment on Fl suggested that Fl is a noble-gas-like element, while the second studies suggested that Fl has a volatile-metal-like character. To obtain more reliable conclusion, we performed further experimental studies on Fl adsorption behavior on Si oxide and gold surfaces. The present results suggest that Fl is highly volatile and less reactive than the volatile metal, Hg, but has higher reactivity than the noble gas, Rn.

Journal Articles

Application of a novel gas phase synthesis approach to carbonyl complexes of accelerator-produced 5d transition metals

G$"o$tz, M.*; Yakushev, A.*; G$"o$tz, S.*; Di Nitto, A.*; D$"u$llmann, Ch. E.*; Asai, Masato; Kindler, B.*; Krier, J.*; Lommel, B.*; Nagame, Yuichiro*; et al.

Radiochimica Acta, 110(2), p.75 - 86, 2022/02

 Times Cited Count:2 Percentile:31.78(Chemistry, Inorganic & Nuclear)

The study of volatile superheavy element carbonyl complexes requires more efficient methods because the yield of transactinide elements decreases with increasing atomic number. This is achieved by using a newly developed double chamber system to separate the recoil chamber and the reaction one, thereby avoiding the decomposition of reactive molecules by the projectile ion beam, which hinders the synthesis of carbonyl complexes. The feasibility of this method was verified by synthesizing 5d metal short-lived isotopes as homologous element isotopes of the light transactinide elements Sg, Bh, Hs, and Mt at the Japan Atomic Energy Agency tandem accelerator and conducting model experiments.

Journal Articles

Chemical characterization of a volatile dubnium compound, DbOCl$$_3$$

Chiera, N. M.*; Sato, Tetsuya; Eichler, R.*; Tomitsuka, Tomohiro; Asai, Masato; Adachi, Sadia*; Dressler, R.*; Hirose, Kentaro; Inoue, Hiroki*; Ito, Yuta; et al.

Angewandte Chemie; International Edition, 60(33), p.17871 - 17874, 2021/08

 Times Cited Count:2 Percentile:14.88(Chemistry, Multidisciplinary)

The formation and the chemical characterization of single atoms of dubnium (Db, element 105), in the form of its volatile oxychloride, was investigated using the on-line gas phase chromatography technique, in the temperature range 350 - 600 $$^circ$$C. Under the exact same chemical conditions, comparative studies with the lighter homologs of group-5 in the Periodic Table clearly indicate the volatility sequence being NbOCl$$_3 > $$ TaOCl$$_3 geq$$ DbOCl$$_3$$. From the obtained experimental results, thermochemical data for DbOCl$$_3$$ were derived. The present study delivers reliable experimental information for theoretical calculations on the chemical properties of transactinides.

Journal Articles

Measurement of double-differential thick-target neutron yields of the C($$d,n$$) reaction at 12, 20, and 30 MeV

Patwary, M. K. A*; Kin, Tadahiro*; Aoki, Katsumi*; Yoshinami, Kosuke*; Yamaguchi, Masaya*; Watanabe, Yukinobu*; Tsukada, Kazuaki; Sato, Nozomi*; Asai, Masato; Sato, Tetsuya; et al.

Journal of Nuclear Science and Technology, 58(2), p.252 - 258, 2021/02

 Times Cited Count:0 Percentile:0.01(Nuclear Science & Technology)

While designing deuteron accelerator neutron sources for radioisotopes production, nuclear data for light elements such as Li, Be, and C have been systematically measured in the deuteron energy range from a few MeV to around 50 MeV. Currently, the experimental data available on double-differential thick-target neutron yields (DDTTNYs) is insufficient, especially for deuteron energies between 18 and 33 MeV. In this study, we measured the DDTTNYs of ($$d,n$$) reactions on $$^{rm nat}$$C target for incident deuteron energies of 12, 20, and 30 MeV using the multiple-foils activation method to improve nuclear data insufficiency. We applied the GRAVEL code for the unfolding process to derive the DDTTNYs. The results were compared with the calculation by DEURACS. The present data were also used to confirm the systematics of the differential neutron yields at 0$$^{circ}$$ and total neutron yield per incident deuteron in the wide range of deuteron energy.

Journal Articles

Search for elements 119 and 120

Khuyagbaatar, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; Asai, Masato; Block, M.*; Boll, R. A.*; Brand, H.*; Cox, D. M.*; et al.

Physical Review C, 102(6), p.064602_1 - 064602_9, 2020/12

 Times Cited Count:43 Percentile:98.01(Physics, Nuclear)

A search for production of the superheavy elements with atomic numbers 119 and 120 was performed in the $$^{50}$$Ti+$$^{249}$$Bk and $$^{50}$$Ti+$$^{249}$$Cf fusion-evaporation reactions, respectively, at the gas-filled recoil separator TASCA. Over four months of irradiation, neither was detected at cross-section sensitivity levels of 65 and 200 fb, respectively. The non-observation of elements 119 and 120 is discussed within the concept of fusion-evaporation reactions including various theoretical predictions on the fission-barrier heights of superheavy nuclei in the region of the island of stability.

Journal Articles

Study of charged particle activation analysis, 2; Determination of boron concentration in human blood samples

Ikebe, Yurie*; Oshima, Masumi*; Bamba, Shigeru*; Asai, Masato; Tsukada, Kazuaki; Sato, Tetsuya; Toyoshima, Atsushi*; Bi, C.*; Seto, Hirofumi*; Amano, Hikaru*; et al.

Applied Radiation and Isotopes, 164, p.109106_1 - 109106_7, 2020/10

 Times Cited Count:2 Percentile:24.28(Chemistry, Inorganic & Nuclear)

Boron Neutron Capture Therapy (BNCT) is a radiotherapy for the treatment of intractable cancer. In BNCT precise determination of $$^{10}$$B concentration in whole blood sample before neutron irradiation is crucial for control of the neutron irradiation time and the neutron dosimetry. We have applied the Charged Particle Activation Analysis (CPAA) to non-destructive and accurate determination of $$^{10}$$B concentration in whole blood sample. The experiment was performed at JAEA Tandem Accelerator using an 8 MeV proton beam. The 478 keV $$gamma$$ ray of $$^{7}$$Be produced in the $$^{10}$$B(p,$$alpha$$)$$^{7}$$Be reaction was used to quantify the $$^{10}$$B, and $$gamma$$ rays of $$^{56}$$Co originating from the reaction with Fe in blood was used to normalize the $$gamma$$-ray intensity. The results demonstrated that the present CPAA method can be applied to the determination of the $$^{10}$$B concentration in the blood sample.

Journal Articles

True coincidence summing correction for cylindrical volume samples in $$gamma$$-ray spectrometry

Yamada, Takashi*; Asai, Masato; Yonezawa, Chushiro*; Kakita, Kazutoshi*; Hirai, Shoji*

Radioisotopes, 69(9), p.287 - 297, 2020/09

We have confirmed that the commercially available Japanese "standard" gamma-ray analysis programs do not consider the effect of sample volume in calculating true coincidence summing (TCS) corrections, which results in underestimation of $$^{134}$$Cs radioactivity in cylindrical volume samples. In this work, we have developed and examined a practical TCS correction method for general Ge detectors which consider the effect of sample volume properly, and have confirmed that this method can reduce the $$^{134}$$Cs radioactivity underestimation to less than 1%.

Journal Articles

First online operation of TRIGA-TRAP

Grund, J.*; Asai, Masato; Blaum, K.*; Block, M.*; Chenmarev, S.*; D$"u$llmann, Ch. E.*; Eberhardt, K.*; Lohse, S.*; Nagame, Yuichiro*; Nagy, Sz.*; et al.

Nuclear Instruments and Methods in Physics Research A, 972, p.164013_1 - 164013_8, 2020/08

 Times Cited Count:6 Percentile:60.71(Instruments & Instrumentation)

We report on the successful coupling of the Penning-trap mass spectrometry setup TRIGA-TRAP to the research reactor TRIGA Mainz. This offers the possibility to perform direct high-precision mass measurements of short-lived nuclei produced in neutron-induced fission of a $$^{235}$$U target located near the reactor core. An aerosol-based gas-jet system is used for efficient transport of short-lived neutron-rich nuclei from the target chamber to a surface ion source. In conjunction with new ion optics and extended beam monitoring capabilities, the experimental setup has been fully commissioned. The design of the surface ion source, efficiency studies and first results are presented.

Journal Articles

New excited 2$$^+$$ and 3$$^-$$ two-proton states in $$_{84}^{210}$$Po$$_{126}$$ populated by two-proton transfer

Dupont, E.*; Astier, A.*; Petrache, C. M.*; Lv, B. F.*; Deloncle, I.*; Kiener, J.*; Orlandi, R.; Makii, Hiroyuki; Nishio, Katsuhisa; Hirose, Kentaro; et al.

Physical Review C, 101(1), p.014309_1 - 014309_6, 2020/01

 Times Cited Count:1 Percentile:13.56(Physics, Nuclear)

Journal Articles

Sensitivity of charged particle activation analysis for long-lived radioactive nuclide determination

Oshima, Masumi*; Yamaguchi, Yurie*; Asai, Masato; Tsukada, Kazuaki; Goto, Jun*; Bamba, Shigeru*; Bi, C.*; Morimoto, Takao*

Journal of Nuclear Science and Technology, 56(9-10), p.866 - 872, 2019/09

 Times Cited Count:1 Percentile:11.15(Nuclear Science & Technology)

Sensitivity of charged particle activation analysis with 8 MeV proton beam was studied for determination of 35 long-lived radioactive nuclides. Reaction cross sections for those nuclides were estimated with ALICE-91 code and isomer yield ratios were estimated from those of neighboring isotopes by taking into account their spins and parities. It was found that the proposed charged particle activation analysis should show high sensitivity for the determination of several hardly measurable nuclides with long half-lives such as $$^{135}$$Cs, $$^{244}$$Pu, $$^{129}$$I, $$^{126}$$Sn, $$^{93}$$Mo, $$^{107}$$Pd, $$^{236}$$U, $$^{248}$$Cm, and $$^{237}$$Np.

Journal Articles

Search for $$alpha$$ decay of $$^{104}$$Te with a novel recoil-decay scintillation detector

Xiao, Y.*; Go, S.*; Grzywacz, R.*; Orlandi, R.; Andreyev, A. N.; Asai, Masato; Bentley, M. A.*; de Angelis, G.*; Gross, C. J.*; Hausladen, P.*; et al.

Physical Review C, 100(3), p.034315_1 - 034315_8, 2019/09

 Times Cited Count:16 Percentile:84.48(Physics, Nuclear)

Journal Articles

Optimization of an isothermal gas-chromatographic setup for the chemical exploration of dubnium (Db, Z = 105) oxychlorides

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Ito, Yuta; Shirai, Kaori*; Suzuki, Hayato; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; et al.

Journal of Radioanalytical and Nuclear Chemistry, 320(3), p.633 - 642, 2019/06

 Times Cited Count:1 Percentile:11.15(Chemistry, Analytical)

An isothermal gas-chromatographic (IGC) device has been developed and tested for on-line gas phase studies of volatile oxychlorides of short-lived group-5 transition metals. Radioisotopes of niobium and tantalum, produced in nuclear fusion evaporation reactions, are directly flushed into the IGC setup by an inert gas-jet. Oxychloride compounds are formed by the addition of SOCl$$_2$$ and O$$_2$$. Parameters influencing the formation and transport of NbOCl$$_3$$ and TaOCl$$_3$$ are investigated. For nuclides with half-lives ($$t_{1/2}$$) of about 30 s, an overall efficiency of 7% is obtained, rendering the IGC setup suitable for the chemical exploration of $$^{262}$$Db($$t_{1/2}$$ = 34s).

Journal Articles

Fusion reaction $$^{48}$$Ca+$$^{249}$$Bk leading to formation of the element Ts (Z=117)

Khuyagbaatar, J.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Ackermann, D.*; Andersson, L.-L.*; Asai, Masato; Block, M.*; Boll, R. A.*; Brand, H.*; Cox, D. M.*; et al.

Physical Review C, 99(5), p.054306_1 - 054306_16, 2019/05

AA2019-0039.pdf:5.03MB

 Times Cited Count:23 Percentile:90.91(Physics, Nuclear)

We have performed an experiment to synthesize the element 117 (Ts) with the $$^{48}$$Ca+$$^{249}$$Bk fusion reaction. Four $$alpha$$-decay chains attributed to the element 117 were observed. Two of them were long decay chains which can be assigned to the one originating from the $$alpha$$ decay of $$^{294}$$Ts. The other two were short decay chains which are consistent with the one originating from the $$alpha$$ decay of $$^{293}$$Ts. We have compared the present results with the literature data, and found that our present results mostly confirmed the literature data, leading to the firm confirmation of the synthesis of the element 117.

Journal Articles

Formation and thermochemical properties of oxychlorides of niobium (Nb) and tantalum (Ta); Towards the gas-phase investigation of dubnium (Db) oxychloride

Chiera, N. M.; Sato, Tetsuya; Tomitsuka, Tomohiro; Asai, Masato; Suzuki, Hayato*; Tokoi, Katsuyuki; Toyoshima, Atsushi; Tsukada, Kazuaki; Nagame, Yuichiro

Inorganica Chimica Acta, 486, p.361 - 366, 2019/02

 Times Cited Count:3 Percentile:18.6(Chemistry, Inorganic & Nuclear)

The formation of NbOCl$$_3$$ and TaOCl$$_3$$ and their adsorption behavior on quartz surfaces was explored by applying an isothermal gas-chromatographic method. Trace amounts of short-lived Nb and Ta isotopes were used. Adsorption enthalpy values ($$Delta H_{rm ads}$$) at zero surface coverage of -$$Delta H_{rm ads}$$(NbOCl$$_3$$) = 102 $$pm$$ 4 kJ/mol and -$$Delta H_{rm ads}$$(TaOCl$$_3$$) = 128 $$pm$$ 5 kJ/mol were determined by analyzing the chromatographic behavior of the Nb andTa complexes with a Monte-Carlo simulation method based on an adsorption-desorption kinetic model.By applying an empirical correlation, the experimental $$Delta H_{rm ads}$$ values were successively related to the macroscopic standard sublimation enthalpy, $$Delta H^circ _{rm subl}$$, as a measure of the volatility of each substance. The inferred sublimation enthalpies are in agreement with tabulated thermochemical values. Thus, the linear empirical correlation between $$Delta H_{rm ads}$$ and $$Delta H^circ _{rm subl}$$ for metal-oxychlorides was updated with the inclusion of the present data. According to the predicted $$Delta H^circ _{rm subl}$$(DbOCl$$_3$$), a $$Delta H_{rm ads}$$(DbOCl$$_3$$) value of 135 $$pm$$ 2 kJ/mol was extrapolated. The future accomplishment of comparative studies with DbOCl$$_3$$ under the same experimental conditions will provide valuable information on the volatility trend in Group-5 elements, together with an indication on the magnitude of relativistic effects on the electronic structure of dubnium.

Journal Articles

Electron-tracking Compton camera imaging of technetium-95m

Hatsukawa, Yuichi*; Hayakawa, Takehito*; Tsukada, Kazuaki; Hashimoto, Kazuyuki*; Sato, Tetsuya; Asai, Masato; Toyoshima, Atsushi; Tanimori, Toru*; Sonoda, Shinya*; Kabuki, Shigeto*; et al.

PLOS ONE (Internet), 13(12), p.e0208909_1 - e0208909_12, 2018/12

AA2018-0639.pdf:2.39MB

 Times Cited Count:3 Percentile:30.05(Multidisciplinary Sciences)

Imaging of $$^{95m}$$Tc radioisotope was conducted using an electron tracking-Compton camera (ETCC). $$^{95m}$$Tc emits 204, 582, and 835 keV $$gamma$$ rays, and was produced in the $$^{95}$$Mo(p,n)$$^{95m}$$Tc reaction with a $$^{95}$$Mo-enriched target. The recycling of the $$^{95}$$Mo-enriched molybdenum trioxide was investigated, and the recycled yield of $$^{95}$$Mo was achieved to be 70% - 90%. The images were obtained with each of the three $$gamma$$ rays. Results showed that the spatial resolution increases with increasing $$gamma$$-ray energy, and suggested that the ETCC with high-energy $$gamma$$-ray emitters such as $$^{95m}$$Tc is useful for the medical imaging of deep tissue and organs in the human body.

Journal Articles

Online chemical adsorption studies of Hg, Tl, and Pb on SiO$$_{2}$$ and Au surfaces in preparation for chemical investigations on Cn, Nh, and Fl at TASCA

Lens, L.*; Yakushev, A.*; D$"u$llmann, Ch. E.*; Asai, Masato; Ballof, J.*; Block, M.*; David, H. M.*; Despotopulos, J.*; Di Nitto, A.*; Eberhardt, K.*; et al.

Radiochimica Acta, 106(12), p.949 - 962, 2018/12

AA2018-0417.pdf:0.99MB

 Times Cited Count:8 Percentile:62.99(Chemistry, Inorganic & Nuclear)

Online gas-solid adsorption studies with single atom quantities of Hg, Tl, and Pb on SiO$$_{2}$$ and Au surfaces were carried out using short-lived radioisotopes with half-lives in the range of 4-49 s. This is a model study to measure adsorption enthalpies of superheavy elements Cn, Nh, and Fl. The short-lived isotopes were produced and separated by the gas-filled recoil separator TASCA at GSI. The products were stopped in He gas, and flushed into gas chromatography columns made of Si detectors whose surfaces were covered by SiO$$_{2}$$ or Au. The short-lived Tl and Pb were successfully measured by the Si detectors with the SiO$$_{2}$$ surface at room temperature. On the other hand, the Hg did not adsorb on the SiO$$_{2}$$ surface, but adsorbed on the Au surface. The results demonstrated that the adsorption properties of short-lived Hg, Tl, and Pb could be studied with this setup, and that this method is applicable to the experiment for Cn, Nh, and Fl.

Journal Articles

First ionization potentials of Fm, Md, No, and Lr; Verification of filling-up of 5f electrons and confirmation of the actinide series

Sato, Tetsuya; Asai, Masato; Borschevsky, A.*; Beerwerth, R.*; Kaneya, Yusuke*; Makii, Hiroyuki; Mitsukai, Akina*; Nagame, Yuichiro; Osa, Akihiko; Toyoshima, Atsushi; et al.

Journal of the American Chemical Society, 140(44), p.14609 - 14613, 2018/11

 Times Cited Count:27 Percentile:69.46(Chemistry, Multidisciplinary)

The first ionization potential (IP$$_1$$) yields information on valence electronic structure of an atom. IP$$_1$$ values of heavy actinides beyond einsteinium (Es, Z = 99), however, have not been determined experimentally so far due to the difficulty in obtaining these elements on scales of more than one atom at a time. Recently, we successfully measured IP$$_1$$ of lawrencium (Lr, Z = 103) using a surface ionization method. The result suggests that Lr has a loosely-bound electron in the outermost orbital. In contrast to Lr, nobelium (No, Z = 102) is expected to have the highest IP$$_1$$ among the actinide elements owing to its full-filled 5f and the 7s orbitals. In the present study, we have successfully determined IP$$_1$$ values of No as well as fermium (Fm, Z = 100) and mendelevium (Md, Z = 101) using the surface ionization method. The obtained results indicate that the IP$$_1$$ value of heavy actinoids would increase monotonically with filling electrons up in the 5f orbital like heavy lanthanoids.

384 (Records 1-20 displayed on this page)