Structural investigation of simulated waste glass surface drained in operation confirmation test of 3rd TVF glass melter

Nagai, Takayuki; Hasegawa, Takehiko*

JAEA-Research 2023-008, 41 Pages, 2023/12

JAEA-Research-2023-008.pdf:7.52MB

To reduce the risks posed by stored the high-level radioactive liquid waste (HAW), Tokai Vitrification Facility (TVF) is working to produce the HAW into vitrified bodies. With the aim of steady vitrification of HAW in TVF, the vitrification technology section has manufactured a new 3rd melter with an improved bottom structure and is working to verify the performance of this melter. In this study, solidified glass samples were taken from simulated vitrified bodies produced by flowing molten glass during the bottom drain-out test in the operation confirmation of the TVF 3rd melter. And the properties of the surface layer and fracture surface of the vitrified bodies were evaluated by using Raman spectroscopy, synchrotron radiation XAFS measurement, and laser ablation inductively coupled plasma atomic emission spectroscopy (LA ICP-AES) analysis. As a result of measuring the surface layer and fracture surface of the solidified samples produced on an actual scale, a slight difference was confirmed between the properties of the surface layer and those of the fracture surface. Since the chemical composition of these simulated vitrified bodies does not contain platinum group elements, it is expected that the glass structure of solidified glass samples is different from that of the actual vitrified body. However, this sample measuring was a valuable opportunity to evaluate samples produced by using the direct energized joule heating method. The properties of cullet used the operation confirmation of the TVF 3rd melter and the cullet of another production lot were measured and analyzed in the same manner under the measuring conditions of solidified glass samples. As a result, it was confirmed that cullet with different producing histories have different glass structures even with the same chemical composition, and that differences in glass structures remain in the glass samples after melting these cullet.

Development of laser ablation absorption spectroscopy for nuclear fuel materials; Plume expansion behavior for refractory metals observed by laser-induced fluorescence imaging spectroscopy

Miyabe, Masabumi; Oba, Masaki; Akaoka, Katsuaki; Kato, Masaaki*; Hasegawa, Shuichi*; Wakaida, Ikuo

Applied Physics A, 126(3), p.213_1 - 213_10, 2020/03

AA2019-0700.pdf:2.82MB

https://doi.org/10.1007/s00339-020-3368-0

The dynamic behavior of an ablation plume in low pressure rare gas ambient was investigated with laser-induced fluorescence imaging spectroscopy for three refractory metals, i.e. titanium, zirconium and hafnium. A comparison of the plume expansion behaviors for the species of these elements revealed an atomic weight effect on the plume structure formation. A hemispherical thin layer and cavity structure reported previously for gadolinium were observed also for these elements. It was found that the plume size increases as well as the layer thickness decreases with increasing atomic weight. For ground state atoms of Ti, substantial amount of atoms were observed even at the center of the plume. Also, the persistence of the Ti atomic plume was as long as 300 s, which was significantly longer than the other species studied. Furthermore, the mass-dependent elemental separation was observed in the ablation plume produced from a multielement sample. These results suggest that the observed plume structure arises from the ion-electron recombination process and the recoil of the ablated species during the multiple collisions with gas atoms.

Laser ablation absorption spectroscopy for isotopic analysis of plutonium; Spectroscopic properties and analytical performance

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

https://doi.org/10.1016/j.sab.2017.05.008

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.

Observation of dynamics and modification of solid surface using a picosecond soft X-ray laser

Nishikino, Masaharu; Kawachi, Tetsuya; Hasegawa, Noboru; Ishino, Masahiko; Minami, Yasuo*; Suemoto, Toru*; Onishi, Naofumi*; Ito, Atsushi*; Sato, Katsutoshi*; Faenov, A.*; et al.

X-Ray Lasers and Coherent X-Ray Sources; Development and Applications XI (Proceedings of SPIE, Vol.9589), p.958902_1 - 958902_7, 2015/09

Ablation plume structure and dynamics in ambient gas observed by laser-induced fluorescence imaging spectroscopy

Miyabe, Masabumi; Oba, Masaki; Iimura, Hideki; Akaoka, Katsuaki; Khumaeni, A.*; Kato, Masaaki; Wakaida, Ikuo

Spectrochimica Acta, Part B, 110, p.101 - 117, 2015/08

AA2015-0183.pdf:3.11MB

https://doi.org/10.1016/j.sab.2015.06.004

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.

Observation of the dependence on the fluence and materials in femto-second laser ablation process by using the soft X-ray laser probe

Hasegawa, Noboru; Tomita, Takuro*; Nishikino, Masaharu; Eyama, Tsuyoshi*; Kakimoto, Naoya*; Minami, Yasuo*; Baba, Motoyoshi*; Onishi, Naofumi*; Ito, Atsushi*; Kawachi, Tetsuya; et al.

JAEA-Conf 2015-001, p.17 - 20, 2015/07

https://jopss.jaea.go.jp/pdfdata/JAEA-Conf-2015-001.pdf#page=27

We have succeeded in simultaneous observation of the ablation front and the expansion front with thin filmy structure in the femto-second laser ablation process of a gold target by using the 13.9 nm soft X-ray probe (incident angle to the sample 70 deg) with soft X-ray interferometer. The dependence on the laser local fluence and materials was obtained by the comparison between gold and tungsten.

Observation of femtosecond laser ablation on Tungsten by using soft X-ray reflection and interference imaging

Nishikino, Masaharu; Hasegawa, Noboru; Tomita, Takuro*; Eyama, Tsuyoshi*; Kakimoto, Naoya*; Onishi, Naofumi*; Ito, Atsushi*; Baba, Motoyoshi*; Minami, Yasuo*; Kawachi, Tetsuya; et al.

Reza Gakkai Dai-471-Kai Kenkyukai Hokoku; Tanhacho Ryoshi Bimu Hassei To Sono Oyo, p.9 - 12, 2014/12

no abstracts in English

Spectroscopic study of reaction mechanism of laser-ablated silicon ions and neutrals with benzene molecules

Saeki, Morihisa; Oba, Hironori; Yokoyama, Atsushi

Journal of Physics; Conference Series, 59, p.732 - 735, 2007/00

https://doi.org/10.1088/1742-6596/59/1/156

We have performed laser ablation of silicon in neon gas and benzene vapor. The reaction mechanism of the ablated silicon atoms with the neon atoms and benzene molecules were investigated by space- and time-resolved emission spectroscopy. The ablation in the neon gas suggested that (1) the neutral neon atoms are excited to 2pn states lying in 18-19 eV and (2) the neutral neon atoms are excited by electronic-to-electronic and translational-to-electronic energy transfer from the silicon ions. In the ablation in the benzene vapor, we found that the benzene molecules are decomposed into C2 and CH radicals by the collision with the silicon atoms.

Laser ablation of silicon in neon gas; Study of excitation mechanism of neon neutrals by ablated silicon ions

Saeki, Morihisa; Hirata, Koichi*; Sakka, Tetsuo*; Oba, Hironori; Yokoyama, Atsushi

Journal of Applied Physics, 98(4), p.044912_1 - 044912_6, 2005/08

https://doi.org/10.1063/1.2008387

no abstracts in English

optical spectroscopy of ablation plume for preparations of nanostructured TiO thin films by pulsed laser deposition

Kitazawa, Shinichi

Japanese Journal of Applied Physics, Part 1, 43(9A), p.6335 - 6341, 2004/09

https://doi.org/10.1143/JJAP.43.6335

Nanostructured TiO thin films on -AlO (0001) substrates prepared by pulsed laser deposition (PLD) were analyzed and evaluated in terms of the buffer O gas pressure (0 - 80 Pa) dependencies by optical spectroscopy and surface morphology. Optical emission spectra of the ablation plume from Ti and TiO targets were measured in-situ. The contribution from TiO molecules was observed by narrow-band photometry. The surface morphology was observed by an atomic force microscope (AFM), revealing the pressure dependence of nanostructures. The crystallographic structures of prepared TiO thin films were observed by X-ray diffraction (XRD). The optically observed band-gaps of the prepared thin films show that the crystallographic structures are mixed crystals of rutile and anatase. Evaporated Ti particles combine with buffer O gas thereby producing TiO molecules, which affect the formation of nanostructures on TiO thin films.