Measurement of uranium isotope ratio by laser ablation absorption spectroscopy

Ye Hao; Huang Yin-Bo; Wang Chen; Liu Guo-Rong; Lu Xing-Ji; Cao Zhen-Song; Huang Yao; Qi Gang; Mei Hai-Ping

doi:10.7498/aps.70.20210193

Abstract

High precision measurement of uranium isotope ratio (²³⁵U/²³⁸U) has important application in the field of nuclear energy safety. In this paper, based on high sensitivity tunable absorption spectroscopy technology, combined with the sample processing method of pulsed laser ablation plasma, high-precision measurement of uranium ²³⁵U/²³⁸U isotope ratio in solid material is realized. In the experimental measurement, transitions near 394.4884 nm/394.4930 nm (vacuum) are selected as the ²³⁵U/²³⁸U analytical lines. The influence of buffer gas and its pressure on the persistence time of uranium atom in laser ablated plasma are studied in detail. The experimental results show that different buffer gases have different ability to restrict the movement of particles in the plasma, which leads to different longitudinal expansion velocity of the plasma (perpendicular to the surface of the sample), and increases the persistence time of uranium atoms in the laser beam. The effect of pressure change on plasma evolution can be reduced by adding buffer gas. When helium is used as the buffer gas, the persistence time of uranium atoms in the plasma is longer, which can improve the selection space of data acquisition delay. In the ablation environment with helium, the electron number density of laser ablated plasma is relatively low, which can reduce the influence of Stark broadening effect and obtain narrower absorption lines, which is more conducive to the measurement of uranium atomic absorption spectrum. In order to reduce the influence of Doppler shift effect on absorption spectrum measurement and avoid misjudgment in spectrum analysis, it is more appropriate to carry out experimental measurement after 3μs sampling delay. Through experiments, the optimal conditions for measuring atomic absorption spectrum of uranium are obtained. Under these conditions, five different samples with ²³⁵U content of 4.95%, 4.10%, 3.00%, 1.10% and 0.25% respectively are measured, and the high-resolution absorption spectrum signals of ²³⁵U and ²³⁸U are obtained. The absorption spectra of samples with different content are measured and statistically analyzed, the ²³⁵U absorption signal has high linearity, the fitting correlation coefficient can reach 0.989, and the limit of detection is 0.033% (3σ). The stability test of absorption spectrum signal shows that the relative standard deviation of ²³⁸U, ²³⁵U and ²³⁵U / ²³⁸U signals are 2.054%, 2.152% and 0.524% respectively. The wavelength scanning mode is superior to the fixed wavelength spectrum measurement, and the influence of the energy fluctuation between different ablation pulses on the spectrum measurement is weakened by the wavelength scanning mode to a certain extent. The results show that laser ablation combined with absorption spectroscopy technology is suitable for uranium isotope ratio analysis and has great potential applications in rapid isotope analysis of nuclear fuel.

Keywords:

PACS:

32.30.-r	(Atomic spectra)
32.10.Bi	(Atomic masses, mass spectra, abundances, and isotopes)
32.30.Jc	(Visible and ultraviolet spectra)

Authors and contacts

1.
Key Laboratory of Atmospheric Optics, Anhui Institute of Optics and Fine Mechanics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China
2.
Science Island Branch of Graduate School, University of Science and Technology of China, Hefei 230026, China
3.
Advanced Laser Technology Laboratory of Anhui Province, Hefei 230037, China
4.
Department of Radiochemistry, China Institute of Atomic Energy, Beijing 102413, China

Corresponding author: Cao Zhen-Song, zscao@aiofm.ac.cn

Funds: Project supported by the Strategic Priority Research Program of Chinese Academy of Sciences (Grant No. XDA17010104)

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References

[1]	Russo R E 1995 Appl. Spectrosc. 49 14 Google Scholar
[2]	Chichkov B N, Momma C, Nolte S, Alvensleben F, Tünnermann A 1996 Appl. Phys. A 63 109 Google Scholar
[3]	Russo R E, Mao X, Liu H, Gonzalez J, Mao S S 2002 Talanta 57 425 Google Scholar
[4]	Harilal S S, Brumfield B E, LaHaye N L, Hartig K C, Phillips M C 2018 Appl. Phys. Rev. 5 021301 Google Scholar
[5]	Miziolek A W, Palleschi V, Schechter I 2006 Crit. Rev. Anal. Chem. 27 257 Google Scholar
[6]	Harilal S S, Lahaye N L, Phillips M C 2017 Opt. Express. 25 2312 Google Scholar
[7]	Skrodzki P J, Shah N P, Taylor N, Hartig K C, Lahaye N L, Brumfield B E, Jovanovic I, Phillips M C, Harilal S S 2016 Spectrochim. Acta, Part B 122 112 Google Scholar
[8]	Smith C A, Martinez M A, Veirs D K, Cremers D A 2000 Spectrochim. Acta, Part B 57 929 Google Scholar
[9]	Cremers D A, Beddingfield A, Smithwick R, Chinni R C, Jones C R, Beardsley B, Karch L 2012 Appl. Spectrosc. 66 250 Google Scholar
[10]	Chan C Y, Choi I, Mao X, Zorba V, Lam O P, Shuh D K, Russo R E 2016 Spectrochim. Acta, Part B 122 31 Google Scholar
[11]	Phillips M C, Brumfield B E, Lahaye N, Harilal S S, Hartig K C, Jovanovic I 2017 Scie. Rep 7 3784 Google Scholar
[12]	Quentmeier A, Bolshov M, Niemax K 2001 Spectrochim. Acta, Part B 56 45 Google Scholar
[13]	Liu H, Quentmeier A, Niemax K 2002 Spectrochim. Acta, Part B 57 1611 Google Scholar
[14]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Ohba H 2013 Appl. Phys. A 112 87 Google Scholar
[15]	Miyabe M, Oba M, Jung K, Iimura H, Akaokaa K, Katoa M, Otobeb H, Khumaeni A, Wakaida I 2017 Spectrochim. Acta, Part B 134 42 Google Scholar
[16]	Taylor N R, Phillips M C 2014 Opt. lett. 39 594 Google Scholar
[17]	叶浩, 张骏昕, 梅海平, 黄尧, 袁子豪, 曹振松, 黄印博 2020 中国激光 47 299 Google Scholar Ye H, Zhang J X, Mei H P, Huang Y, Yuan Z H, Cao Z S, Huang Y B 2020 Chin. J. Lasers 47 299 Google Scholar
[18]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Wakaida I 2010 Appl. Phys. A 101 65 Google Scholar
[19]	Yan P, Luo W, Zhang J, Wang L 1992 Chin. J. Lasers 5 27
[20]	Kramida Y, Ralchenko J, Reader N A NIST Atomic Spectra Database, National Institute of Standards and Technology http://physics.nist.gov/asd [2021-01-25]
[21]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Wakaida I, Watanabe K 2009 4^th international conference on laser probing Nagoya, Japan, October 6–10, 2008 p30
[22]	Man B Y, Wang X T, Liu A H 1998 J. Appl. Phys. 83 3509 Google Scholar
[23]	张树东, 陈冠英, 刘亚楠, 董晨钟 2002 原子核物理评论 19 206 Google Scholar Zhang S D, Chen G Y, Liu Y N, Dong C Z 2002 Nucl. Phys. Rev. 19 206 Google Scholar

Cited By

期刊类型引用(3)

1.	齐刚，黄印博，凌菲彤，杨佳琦，黄俊，杨韬，张雷雷，卢兴吉，袁子豪，曹振松. 多微管阵列结构腔-原子吸收光谱测量Rb同位素比. 物理学报. 2023(05): 212-220 . 百度学术
2.	陈文婧，黄春平，刘丰刚，梁仁瑜，刘奋成，杨海欧. 激光立体成形和超声冲击混合制造Ti60合金的显微组织和性能（英文）. Transactions of Nonferrous Metals Society of China. 2023(11): 3319-3331 . 百度学术
3.	李耀宗，张小安，梁昌慧，周贤明，曾利霞，梅策香. 激光诱导Al表面等离子体温度的发射谱诊断. 原子与分子物理学报. 2022(06): 100-107 . 百度学术

其他类型引用(2)

图 1 LAAS测量原理示意图

Figure 1. Principle of LAAS.

DownLoad: Full-Size Img PowerPoint

图 2 LAAS实验装置简图

Figure 2. Schematic diagram of the experimental setup of LAAS.

DownLoad: Full-Size Img PowerPoint

图 3 (a)等离子体透过率测量; (b)实验测量的²³⁵U/ ²³⁸U吸收光谱

Figure 3. (a) Plasma transmittance measurement; (b) measured absorption spectrum of ²³⁵U/ ²³⁸U.

DownLoad: Full-Size Img PowerPoint

图 4 不同环境气体下测量结果比较(Air, He, Ar, N₂)

Figure 4. Comparison of measurement results under different ambient gases (Air, He, Ar, N₂).

DownLoad: Full-Size Img PowerPoint

图 5 不同烧蚀环境下等离子体持续时间随样品池内压力的变化

Figure 5. The persistence of ablation plasma changes with pressure.

DownLoad: Full-Size Img PowerPoint

图 6 等离子体膨胀简易模型示意图

Figure 6. Simple model of plasma expansion.

DownLoad: Full-Size Img PowerPoint

图 7 不同采样延时的²³⁸U吸收光谱

Figure 7. Absorption spectra with different sampling delays.

DownLoad: Full-Size Img PowerPoint

图 8 不同含量样品²³⁵U/²³⁸U吸收光谱

Figure 8. ²³⁵U/²³⁸U absorption spectra of samples with different concentration.

DownLoad: Full-Size Img PowerPoint

图 9 不同含量样品²³⁵U/²³⁸U吸收光谱及Voigt线型拟合光谱, 拟合曲线下部为拟合残差图

Figure 9. ²³⁵U/²³⁸U absorption spectra and Voigt fitting spectra of samples with different concentration, the lower part of the fitted curve is the fitted residual graph.

DownLoad: Full-Size Img PowerPoint

图 10 ²³⁵U丰度与吸收强度的定标曲线

Figure 10. Calibration curve of ²³⁵U abundance and absorption intensity.

DownLoad: Full-Size Img PowerPoint

图 11 1.10%样品²³⁵U/²³⁸U吸收光谱及Voigt线型拟合光谱

Figure 11. ²³⁵U/²³⁸U absorption spectrum and Voigt fitting spectrum of 1.10% sample.

DownLoad: Full-Size Img PowerPoint

图 12 ²³⁵U/²³⁸U吸收光谱信号稳定性研究

Figure 12. Study on the stability of ²³⁵U/²³⁸U absorption spectrum signal.

DownLoad: Full-Size Img PowerPoint

表 1 LAAS实验装置关键器件参数

Table 1. Key device parameters of LAAS experimental device.

实验装置关键器件	参数
探测激光器	线宽100 kHz
烧蚀激光器	波长1064 nm, 脉宽8 ns, 重复频率1—20 Hz, 单脉冲能量最大为200 mJ, 能量稳定性 ≤ 1%
带通滤光片	Semrock, 中心波长λ = 395 nm, 带宽Δλ = 11 nm
陷波滤光片	Thorlabs, 中心波长λ = 1064 nm, 带宽Δλ = 44 nm
光电探测器	Thorlabs, 探测带宽150 MHz

DownLoad: CSV

表 2 实验参数设置

Table 2. experimental parameter setting

实验参数	烧蚀激光能量/ mJ	采样延时/μs	缓冲气体	压力/kPa	扫描时间/s
数值	40	4	He	4	50

DownLoad: CSV

[1]	Russo R E 1995 Appl. Spectrosc. 49 14 Google Scholar
[2]	Chichkov B N, Momma C, Nolte S, Alvensleben F, Tünnermann A 1996 Appl. Phys. A 63 109 Google Scholar
[3]	Russo R E, Mao X, Liu H, Gonzalez J, Mao S S 2002 Talanta 57 425 Google Scholar
[4]	Harilal S S, Brumfield B E, LaHaye N L, Hartig K C, Phillips M C 2018 Appl. Phys. Rev. 5 021301 Google Scholar
[5]	Miziolek A W, Palleschi V, Schechter I 2006 Crit. Rev. Anal. Chem. 27 257 Google Scholar
[6]	Harilal S S, Lahaye N L, Phillips M C 2017 Opt. Express. 25 2312 Google Scholar
[7]	Skrodzki P J, Shah N P, Taylor N, Hartig K C, Lahaye N L, Brumfield B E, Jovanovic I, Phillips M C, Harilal S S 2016 Spectrochim. Acta, Part B 122 112 Google Scholar
[8]	Smith C A, Martinez M A, Veirs D K, Cremers D A 2000 Spectrochim. Acta, Part B 57 929 Google Scholar
[9]	Cremers D A, Beddingfield A, Smithwick R, Chinni R C, Jones C R, Beardsley B, Karch L 2012 Appl. Spectrosc. 66 250 Google Scholar
[10]	Chan C Y, Choi I, Mao X, Zorba V, Lam O P, Shuh D K, Russo R E 2016 Spectrochim. Acta, Part B 122 31 Google Scholar
[11]	Phillips M C, Brumfield B E, Lahaye N, Harilal S S, Hartig K C, Jovanovic I 2017 Scie. Rep 7 3784 Google Scholar
[12]	Quentmeier A, Bolshov M, Niemax K 2001 Spectrochim. Acta, Part B 56 45 Google Scholar
[13]	Liu H, Quentmeier A, Niemax K 2002 Spectrochim. Acta, Part B 57 1611 Google Scholar
[14]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Ohba H 2013 Appl. Phys. A 112 87 Google Scholar
[15]	Miyabe M, Oba M, Jung K, Iimura H, Akaokaa K, Katoa M, Otobeb H, Khumaeni A, Wakaida I 2017 Spectrochim. Acta, Part B 134 42 Google Scholar
[16]	Taylor N R, Phillips M C 2014 Opt. lett. 39 594 Google Scholar
[17]	叶浩, 张骏昕, 梅海平, 黄尧, 袁子豪, 曹振松, 黄印博 2020 中国激光 47 299 Google Scholar Ye H, Zhang J X, Mei H P, Huang Y, Yuan Z H, Cao Z S, Huang Y B 2020 Chin. J. Lasers 47 299 Google Scholar
[18]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Wakaida I 2010 Appl. Phys. A 101 65 Google Scholar
[19]	Yan P, Luo W, Zhang J, Wang L 1992 Chin. J. Lasers 5 27
[20]	Kramida Y, Ralchenko J, Reader N A NIST Atomic Spectra Database, National Institute of Standards and Technology http://physics.nist.gov/asd [2021-01-25]
[21]	Miyabe M, Oba M, Iimura H, Akaoka K, Maruyama Y, Wakaida I, Watanabe K 2009 4^th international conference on laser probing Nagoya, Japan, October 6–10, 2008 p30
[22]	Man B Y, Wang X T, Liu A H 1998 J. Appl. Phys. 83 3509 Google Scholar
[23]	张树东, 陈冠英, 刘亚楠, 董晨钟 2002 原子核物理评论 19 206 Google Scholar Zhang S D, Chen G Y, Liu Y N, Dong C Z 2002 Nucl. Phys. Rev. 19 206 Google Scholar

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期刊类型引用(3)

1.	齐刚，黄印博，凌菲彤，杨佳琦，黄俊，杨韬，张雷雷，卢兴吉，袁子豪，曹振松. 多微管阵列结构腔-原子吸收光谱测量Rb同位素比. 物理学报. 2023(05): 212-220 . 百度学术
2.	陈文婧，黄春平，刘丰刚，梁仁瑜，刘奋成，杨海欧. 激光立体成形和超声冲击混合制造Ti60合金的显微组织和性能（英文）. Transactions of Nonferrous Metals Society of China. 2023(11): 3319-3331 . 百度学术
3.	李耀宗，张小安，梁昌慧，周贤明，曾利霞，梅策香. 激光诱导Al表面等离子体温度的发射谱诊断. 原子与分子物理学报. 2022(06): 100-107 . 百度学术

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