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

Miyabe, Masabumi; Oba, Masaki; Jung, Kyunghun; Iimura, H.; Akaoka, Katsuaki; Kato, Masaaki; Otobe, Haruyoshi; Khumaeni, Ali; Wakaida, Ikuo

doi:10.1016/j.sab.2017.05.008

Cited by 32 publications

(21 citation statements)

References 38 publications

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“…Absorption spectroscopy using broadband incoherent sources and a dispersive spectrograph has been used for probing laser ablation plumes, but suffers the same limitations on spectral bandwidth and resolution as optical emission spectroscopy 10 . Tunable cw lasers provide a means to probe laser ablation plumes via laser absorption spectroscopy (LAS) [11][12][13][14][15][16] or laser-induced fluorescence (LIF) [15][16][17][18][19][20] . The spectral linewidths of cw lasers (<10 MHz) are much smaller than the intrinsic linewidths of most transitions.…”

Section: Resultsmentioning

confidence: 99%

Dual-Comb Spectroscopy of Laser-Induced Plasmas

Bergevin

Yeak

Brumfield

et al. 2017

Conference on Lasers and Electro-Optics

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Dual-comb spectroscopy has become a powerful spectroscopic technique in applications that rely on its broad spectral coverage combined with high frequency resolution capabilities. Experiments to date have primarily focused on detection and analysis of multiple gas species under semi-static conditions, with applications ranging from environmental monitoring of greenhouse gases to high-resolution molecular spectroscopy. Here, we utilize dual-comb spectroscopy to demonstrate broadband, high-resolution, and time-resolved measurements in a laser-induced plasma. As a demonstration, we simultaneously detect trace amounts of Rb and K in solid samples with a single laser ablation shot, with transitions separated by over 6 THz (13 nm) and spectral resolution sufficient to resolve isotopic and ground state hyperfine splittings of the Rb D 2 line. This new spectroscopic approach offers the broad spectral coverage found in the powerful techniques of laser-induced breakdown spectroscopy (LIBS) while providing the high-resolution and accuracy of cw laser-based spectroscopies.

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Section: Resultsmentioning

confidence: 99%

Dual-Comb Spectroscopy of Laser-Induced Plasmas

Bergevin

Yeak

Brumfield

et al. 2017

Conference on Lasers and Electro-Optics

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“…Measurements are conducted at a reduced-pressure environment and with a certain time delay (s timescale) after the laser fires. Under these conditions, gas-kinetic temperatures, which determine Doppler line broadening, are typically in the range of 350 K to 400 K [26,99]. The low-pressure and relatively low-temperature environment warrant a narrow spectral profile (compared to the magnitude of the isotopic shift) in the atomic transition, which in turn ensures that the 235 U and 238 U absorption profiles are baseline resolved and no further spectral deconvolution is needed.…”

Section: Laser Ablation Absorbance Ratio Spectrometry (Laars)mentioning

confidence: 99%

Scoping study to expedite development of a field deployable and portable instrument for UF6 enrichment assay

Chan¹,

Valentine²,

Russo³

2017

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The primary objective of the present study is to identity the most promising, viable technologies that are likely to culminate in an expedited development of the next-generation, field-deployable instrument for providing rapid, accurate, and precise enrichment assay of uranium hexafluoride (UF 6 ). UF 6 is typically involved, and is arguably the most important uranium compound, in uranium enrichment processes. As the first line of defense against proliferation, accurate analytical techniques to determine the uranium isotopic distribution in UF 6 are critical for materials verification, accounting, and safeguards at enrichment plants. As nuclear fuel cycle technology becomes more prevalent around the world, international nuclear safeguards and interest in UF 6 enrichment assay has been growing.At present, laboratory-based mass spectrometry (MS), which offers the highest attainable analytical accuracy and precision, is the technique of choice for the analysis of stable and longlived isotopes. Currently, the International Atomic Energy Agency (IAEA) monitors the production of enriched UF 6 at declared facilities by collecting a small amount (between 1 to 10 g) of gaseous UF 6 into a sample bottle, which is then shipped under chain of custody to a central laboratory (IAEA's Nuclear Materials Analysis Laboratory) for high-precision isotopic assay by MS. The logistics are cumbersome and new shipping regulations are making it more difficult to transport UF 6 . Furthermore, the analysis is costly, and results are not available for some time after sample collection. Hence, the IAEA is challenged to develop effective safeguards approaches at enrichment plants. In-field isotopic analysis of UF 6 has the potential to substantially reduce the time, logistics and expense of sample handling. However, current laboratory-based MS techniques require too much infrastructure and operator expertise for field deployment and operation. As outlined in the IAEA Department of Safeguards Long-Term R&D Plan, 2012-2023, one of the IAEA long-term R&D needs is to "develop tools and techniques to enable timely, potentially real-time, detection of HEU (Highly Enriched Uranium) production in LEU (Lowly Enriched Uranium) enrichment facilities" (Milestone 5.2). iv measurements that do not require the stated high accuracy or precision of the ITVs to which it was compared).The list presented below summarizes the outcome of the present study, and groups all reviewed techniques into "recommended", "promising", or "not recommended"; the "benchmark" techniques are also included and labeled as such. The list is presented in a highly abridged way such that only the final recommendations are given. The performance of a technique in the seven evaluation metrics and its ranking are summarized in Table 6.1, whereas short discussion and comments on the recommendation can be found in Section 6.2 of this report. Furthermore, comprehensive and in-depth reviews on the scientific principle of each technique, its instrument option, its limitations and main gaps betwe...

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“…published work in this area in 2017. 18 Doucet et al. 19 applied LIBS and chemometrics in 2011 to determine 235 U/ 238 U ratios for application in nuclear forensics.…”

Section: Introductionmentioning

confidence: 99%