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Miyabe, Masabumi; Oba, Masaki; Jung, K.; Iimura, Hideki; Akaoka, Katsuaki; Kato, Masaaki; Otobe, Haruyoshi; Khumaeni, A.*; Wakaida, Ikuo
Spectrochimica Acta, Part B, 134, p.42 - 51, 2017/08
Times Cited Count：30 Percentile：91.46(Spectroscopy)Spectroscopic properties of atomic species of plutonium were investigated by combining laser ablation and resonance absorption techniques for the analysis of a plutonium oxide sample. For 17 transitions of Pu atoms and ions, the absorbance, isotope shift, and hyperfine splitting were determined via Voigt profile fitting of the recorded absorption spectra. Three transitions were selected as candidates for analytical use. Using these transitions, we investigated the analytical performance that was attainable and determined a correlation coefficient R2 between the absorbance and plutonium concentration of 0.9999, a limit of detection of 30-130 ppm, and a relative standard deviation of approximately 6% for an abundance of 
Pu of 2.4%. These results demonstrate that laser ablation absorption spectroscopy is applicable to the remote isotopic analysis of highly radioactive nuclear fuels and waste materials containing multiple actinide elements.
Miyabe, Masabumi; Oba, Masaki; Iimura, Hideki; Akaoka, Katsuaki; Khumaeni, A.*; Kato, Masaaki; Wakaida, Ikuo
Spectrochimica Acta, Part B, 110, p.101 - 117, 2015/08
Times Cited Count：25 Percentile：82.1(Spectroscopy)The dynamic behavior of an ablation plume in ambient gas has been investigated by laser-induced fluorescence imaging spectroscopy. The second harmonic beam from an Nd:YAG laser (0.5-6J/cm
) was focused on a sintered oxide pellet or a metal chip of gadolinium. The produced plume was subsequently intersected with a sheet-shaped UV beam from a dye laser so that time-resolved fluorescence images were acquired with an intensified CCD camera at various delay times. The obtained cross-sectional images of the plume indicate that the ablated ground state atoms and ions of gadolinium accumulate in a hemispherical contact layer between the plume and the ambient gas, and a cavity containing a smaller density of ablated species is formed near the center of the plume. At earlier expansion stage, another luminous component also expands in the cavity so that it coalesces into the hemispherical layer. The splitting and coalescence for atomic plume occur later than those for ionic plume. Furthermore, the hemispherical layer of neutral atoms appears later than that of ions; however, the locations of the layers are nearly identical. This coincidence of the appearance locations of the layers strongly suggests that the neutral atoms in the hemispherical layer are produced as a consequence of three-body recombination of ions through collisions with gas atoms. The obtained knowledge regarding plume expansion dynamics and detailed plume structure is useful for optimizing the experimental conditions for ablation-based spectroscopic analysis.
Khumaeni, A.; Tampo, Motonobu; Akaoka, Katsuaki; Miyabe, Masabumi; Wakaida, Ikuo
Optics Express (Internet), 21(24), p.29755 - 29768, 2013/12
Times Cited Count：51 Percentile：91.11(Optics)Intensified microwave coupled by a loop antenna (diameter of 3 mm) has been employed to enhance the laser-induced breakdown spectroscopy (LIBS) emission. In this method, a laser plasma was induced on Gd
O
sample at a reduced pressure by focusing a pulsed Nd:YAG laser (532 nm, 10 ns, 5 mJ) at a local point, at which electromagnetic field was produced by introducing microwave radiation using loop antenna. The plasma emission was significantly enhanced by absorbing the microwave radiation, resulting in high-temperature plasma and long-lifetime plasma emission. By using this method, the enhancement of Gd lines was up to 32 times, depending upon the emission lines observed. A linear calibration curve of Ca contained in the GdO sample was made. The detection limit of Ca was approximately 2 mg/kg. This present method is very useful for identification of trace elements in nuclear fuel and radioactive materials.
Khumaeni, A.; Tampo, Motonobu; Akaoka, Katsuaki; Miyabe, Masabumi; Wakaida, Ikuo
no journal, ,
A novel method for the analysis of nuclear elements such as uranium and plutonium in the next generation nuclear fuel cycle system was developed by utilizing microwave enhanced laser induced plasma spectroscopy (MELIPS). In this study, a Nd YAG laser was focused on a material target by using plano convex lens with a 200 mm focal length to induce a micro plasma. The plasma contains ablated material due to the ablation of the sample. The pulsed microwave generated by a magnetron through the antenna in the mesh chamber was then supplied to the micro plasma to enhance the plasma emission. The sample used in the study was gadolinium oxide pellet as a simulated fuel pellet. The result certified that the plasma lifetime was extent several hundreds of microsecond when the pulsed microwave was applied. The emission spectrum of Gd using standard LIPS (without microwave) was compared with MELIPS method. The spectrum of Gd was drastically enhanced by using MELIPS.
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Oba, Hironori; Otobe, Haruyoshi; Maruyama, Yoichiro; Kato, Masaaki; Khumaeni, A.; Tampo, Motonobu
no journal, ,
In decommissioning of nuclear power plant especially in damaged core, development of onsite remote diagnostic methods will be strongly required for planning and the view point of the safeguard. We are now developing the remote diagnostic technique for simultaneous analysis of element and isotope ratio by the combination of laser induced breakdown spectroscopy (LIBS) and ablation resonance absorption spectroscopy. For the development of diagnostic technique, microwave assisted LIBS was studied and enhancement of emission intensity was obtained. For liquid phase sample, ultra-thin laminate flow as the target was accomplished high sensitivity. For onsite diagnostic, Optical Fiber LIBS Probe is now under construction. For analytical development, basic database of optical emission of nuclear fuel materials are indispensable for the analysis of the complex spectra. To obtain emission spectra from MOX sample, we have constructed the remote diagnostic setup in the globe box.
Khumaeni, A.; Akaoka, Katsuaki; Maruyama, Yoichiro; Miyabe, Masabumi; Wakaida, Ikuo
no journal, ,
Laser-induced breakdown spectroscopy has been employed for the analysis of nuclear materials. However, this method has several drawbacks including low sensitivity. To increase the sensitivity, we have developed a novel method by utilizing microwave-assisted laser-induced breakdown spectroscopy. In order to improve the ability for practical application, the emission characteristics of microwave-assisted laser plasma such as plasma lifetime, plasma temperature, and atomic distributions in the plasma region are investigated. And by using this method, the enhancement up to approximately 200 times will be demonstrated in Ca oxide sample.
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Oba, Hironori; Otobe, Haruyoshi; Maruyama, Yoichiro; Kato, Masaaki; Khumaeni, A.; Tampo, Motonobu*; Shimizu, Osamu
no journal, ,
The background and recent results of the R&D titled of "Development of laser remote analysis for next generation nuclear fuel and applied study by MOX sample" entrusted to Japan Atomic Energy Agency by the Ministry of Education, Culture, Sports, Science and Technology of Japan (MEXT) will be summarized as the first speaker of the series lecture consist with four titles. We had developed the laser remote spectroscopy system in the glove box at NUCEF facility in JAEA, and applied to oxide samples of Pu, U and Pu mixed in U. For elemental analysis, quantitative determination by Laser Induced Breakdown Spectroscopy will be demonstrated. For isotopic analysis, isotope ratio of 
Pu and Pu will be quantitatively determined in U oxide base matrix by ablation resonance absorption spectroscopy. Application for the molten debris in the accident of Fukushima power plant will be also discussed.
Khumaeni, A.; Wakaida, Ikuo
no journal, ,
Khumaeni, A.; Miyabe, Masabumi; Akaoka, Katsuaki; Wakaida, Ikuo
no journal, ,
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Khumaeni, A.; Oba, Hironori; Saeki, Morihisa; Ito, Chikara; Otobe, Haruyoshi; Kato, Masaaki
no journal, ,
In the next generation nuclear fuel cycle, low-decontaminated fuel with TRU will be strongly required, and convenience, quick analytical techniques will be necessary. Simultaneous analysis of element and isotope by the combination of Laser Induced Breakdown Spectroscopy (LIBS) and Ablation Resonance Absorption Spectroscopy was demonstrated. For elemental analysis, detection lower limit of 1000 ppm of Pu in U oxide and relative error under 5% have been obtained within 5 min. For isotope analysis, Pu and Pu have been observed completely separated, and detection lower limit of several 10 ppm and error under 1% have been accomplished. A simple antenna coupled microwave assisted LIBS was performed and the enhancement of emission intensity of several 10 times was demonstrated. For liquid sample, ultra-thin laminate flow as the laser focused target was accomplished high sensitivity of ppb. For in-situ monitoring, Optical Fiber LIBS Probe by radiation resistant optical fiber is under construction.
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Kato, Masaaki; Otobe, Haruyoshi; Oba, Hironori; Khumaeni, A.
no journal, ,
In Japan Atomic Energy Agency (JAEA), research and development of quick analysis for next-generation MOX fuel without chemical analysis and neutron measurement had been carried out as the entrusted project by MEXT, and basic performances by using un-irradiated MOX fuel were demonstrated. In elemental analysis by Laser Induced Breakdown Spectroscopy (LIBS) with high resolution spectrometer, relative error of 2.9% at 30% Pu and the detection lower limit of 2,500 ppm in U oxide were demonstrated with the operation time of 5 min.. In isotope ratio analysis by Ablation Resonance Absorption Spectroscopy, tunable semiconductor laser system was constructed, and the relative deviation less than 1% in the ratio of Pu/Pu and sensitivity of 30-100 ppm in U were also accomplished within 5min. operation. As for an analysis in liquid sample, ultra-thin laminate flow was experimented as LIBS target, and the sensitivity comparable to conventional ICP-AES was confirmed.
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Khumaeni, A.; Oba, Hironori; Ito, Chikara
no journal, ,
In the new concept of next generation nuclear fuel cycle for long lived radioactive waste disposal by use of Accelerator Driven Subcritical reactor (ADS Cycle) and by a fast breeder reactor (FBR Cycle), utilization of low-decontaminated fuel with TRU will be promoted. Simultaneous analysis of element and isotope by the combination of Laser Induced Breakdown Spectroscopy (LIBS) and Ablation Resonance Absorption Spectroscopy was demonstrated by MOX fuel. For elemental analysis, detection lower limit of 1000 ppm of Pu in U oxide and relative error under 5% have been obtained within 5 min. For isotope analysis, Pu and Pu have been observed separately, and detection lower limit of several 10 ppm and error under 1% have been accomplished. A simple antenna coupled microwave assisted LIBS was performed and the enhancement of emission intensity of several 10 times was demonstrated. For liquid sample, ultra-thin laminate flow as the laser focused target was accomplished high sensitivity of ppb. For in-situ monitoring, Optical Fiber LIBS Probe by radiation resistant optical fiber is under construction.
Wakaida, Ikuo; Akaoka, Katsuaki; Miyabe, Masabumi; Otobe, Haruyoshi; Khumaeni, A.; Kato, Masaaki
no journal, ,
Research and development of laser based quick analysis without chemical analysis and neutron measurement for next-generation Minor Actinide containing MOX fuel has been carried out, and the basic performances by using un-irradiated MOX fuel were demonstrated. The remote diagnostic technique for simultaneous analysis of element and isotope ratio by the combination of Laser Induced Breakdown Spectroscopy and Laser Ablation Resonance Absorption Spectroscopy are developed, and specialized glove box with auto and remote arraignment system had re-constructed. For elemental analysis, detection limit of thousand ppm of Pu in MOX and the relative error under 5% have been successfully obtained within 5 min. operation. For isotope analysis, U and Pu isotopes have been observed separately and quantitative analysis was applied. Detection limit of several ten ppm for specified isotope in MOX sample and quantitative error under 1% have been accomplished within 5 min. operation.
