Tritiated water detection in the 2.17 μM spectral region by cavity ring down spectroscopy

被引:10
作者
Bray, C. [1 ]
Pailloux, A. [2 ]
Plumeri, S. [3 ]
机构
[1] CEA, DEN, DPC, F-91191 Gif Sur Yvette, France
[2] CEA, DAM, DIF, F-91297 Arpajon, France
[3] Andra, F-92298 Chatenay Malabry, France
关键词
Nuclear waste containers; Infrared molecular spectroscopy; Continuous wave cavity ringdown spectroscopy (CRDS); Radionuclide; HTO; Tritium detection; VARIATIONAL CALCULATIONS; ABSORPTION-SPECTROSCOPY; CW-CRDS; CM(-1); BAND; HTO; SENSITIVITY; INTENSITIES; TRITIUM;
D O I
10.1016/j.nima.2015.03.064
中图分类号
TH7 [仪器、仪表];
学科分类号
0804 ; 080401 ; 081102 ;
摘要
Nuclear waste containers are intended to be stored in dedicated disposal sites. For the inside and environmental safety of the disposal sites, the tiny outgassing rates leaking out the containers are measured. Presently, the radioactive HT gas is measured by liquid scintillation. However an alternative method-cavity ring down spectroscopy, an isotopically selective laser technique based on molecular spectroscopy is currently developed and evaluated for tritium measurement in its oxidized form, HTO. Applying this method, the number density of the gaseous HTO sample hold in the optical cavity cell, is derived from the laser beam absorption by vibrational symmetric stretching 2 nu(1) (R) HTO lines in the 4590 and 4600 cm(-1) spectral range. To ensure a future accurate HTO measurement, the theoretical line intensities are confronted to the experiment: two tritiated water standards are measured with a dedicated CRDS set-up. Compared to the theoretical database, the line positions are correct (-0.067 to -0.128 cm(-1)), their relative intensities are in agreement with the database, but their absolute intensities are 20% weaker. Among the seven intense lines, the 4596.485 cm(-1) line (intensity 8.22 10(-22) cm/molecule) and the 4592.407 cm(-1) line (intensity 9.83 10(-22) cm/molecule) are isolated and intense for a sensitive detection. The HTO detection limit with the present set-up is 3 kBq (10 min), equivalent to 1.8 10(12) molecules in the 111 cm(3) CRDS cell. This detection limit could be improved by a factor 3 by reducing the detection noise. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:43 / 49
页数:7
相关论文
共 25 条
[1]  
[Anonymous], 2012, 467VA
[2]  
[Anonymous], 2014, Handbook of Chemistry and Physics, V95th
[3]  
Berden G., 2009, Cavity Ring-Down Spectroscopy: Techniques and Applications
[4]   The 4-0 band of carbon monoxide by high sensitivity Cavity Ring Down spectroscopy near 8200 cm-1 [J].
Campargue, A. ;
Karlovets, E. V. ;
Kassi, S. .
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 2015, 154 :113-119
[5]   Detection and analysis of three highly excited vibrational bands of 16O3 by CW-CRDS near the dissociation threshold [J].
Campargue, A. ;
Kassi, S. ;
Mondelain, D. ;
Barbe, A. ;
Starikova, E. ;
De Backer, M. -R. ;
Tyuterev, Vl. G. .
JOURNAL OF QUANTITATIVE SPECTROSCOPY & RADIATIVE TRANSFER, 2015, 152 :84-93
[6]  
Cherrier P.P., 1984, MOL SPECTROSC, V103, P41
[7]   ANALYSIS OF THE V1 FUNDAMENTAL MODE OF HTO [J].
COPE, SD ;
RUSSELL, DK ;
FRY, HA ;
JONES, LH ;
BAREFIELD, JE .
JOURNAL OF MOLECULAR SPECTROSCOPY, 1988, 127 (02) :464-471
[8]   Analysis of a tritium enhanced water spectrum between 7200 and 7245 cm-1 using new variational calculations [J].
Down, Michael J. ;
Tennyson, Jonathan ;
Hara, Masanori ;
Hatano, Yuji ;
Kobayashi, Kaori .
JOURNAL OF MOLECULAR SPECTROSCOPY, 2013, 289 :35-40
[9]  
Fayt G., 1972, P ACAD SCI PARIS B, V275, P459
[10]   MILLIMETER-WAVELENGTH AND SUBMILLIMETER-WAVELENGTH SPECTRA AND MOLECULAR CONSTANTS OF HTO AND DTO [J].
HELMINGER, P ;
DELUCIA, FC ;
GORDY, W ;
STAATS, PA ;
MORGAN, HW .
PHYSICAL REVIEW A, 1974, 10 (04) :1072-1081