Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride

Skrodzki, P. J.; Burger, M.; Finney, L. A.; Poineau, F.; Balasekaran, S. M.; Nees, J.; Czerwinski, K. R.; Jovanovic, I.

doi:10.1038/s41598-018-29814-8

Title: Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride

Journal Article · 02 August 2018 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-018-29814-8 · OSTI ID:1500001

Skrodzki, P. J. ^[1]; Burger, M. ^[2]; Finney, L. A. ^[2]; Poineau, F. ^[3]; Balasekaran, S. M. ^[3]; Nees, J. ^[4]; Czerwinski, K. R. ^[3]; Jovanovic, I. ^[2]

Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear Engineering and Radiological Sciences. Center for Ultrafast Optical Science; OSTI
Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear Engineering and Radiological Sciences. Center for Ultrafast Optical Science
Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry
Univ. of Michigan, Ann Arbor, MI (United States). Center for Ultrafast Optical Science

Uranyl fluoride (UO₂F₂) is a compound which forms in the reaction between water and uranium hexafluoride, a uranium containing gas widely used for uranium enrichment. Uranyl fluoride exhibits negligible natural background in atmosphere; as a result, its observation implies the presence and active operation of nearby enrichment facilities and could be used as a tracer for treaty verification technologies. Additionally, detection of UO₂F₂ has a potential application in guiding remediation efforts around enrichment facilities. Laser-induced fluorescence (LIF) has been proposed in the past as a viable technique for the detection and tracking of UO₂F₂. We demonstrate that ultrafast laser filamentation coupled with LIF extends the capabilities of standard LIF to enable remote detection of UO₂F₂. An intense femtosecond laser pulse propagated in air collapses into a plasma channel, referred to as a laser filament, allowing for the extended delivery of laser energy. We first investigate the luminescence of UO₂F₂ excited by the second harmonic of an ultrafast Ti:sapphire laser and subsequently excite it using the conical emission that accompanies ultrafast laser filamentation in air. We measure the decay rates spanning 4.3–5.6 × 10⁴ s^-1 and discuss the characteristics of the luminescence for both ultrafast- and filament-excitation. Larger decay rates than those observed using standard LIF are caused by a saturated component of prompt decay from annihilation of dense excited states upon excitation with an ultrafast source. The reproducibility of such decay rates for the given range of incident laser intensities 1.0–1.6 × 10¹¹ W cm^-2 is promising for the application of this technique in remote sensing.

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Research Organization:: Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20)

Grant/Contract Number:: NA0000979; NA0002534; NA0003180

OSTI ID:: 1500001

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Vol. 8; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Uranyl fluoride luminescence in acidic aqueous solutions Beitz, James V.; Williams, Clatyon W. Journal of Alloys and Compounds, Vol. 250, Issue 1-2 https://doi.org/10.1016/S0925-8388(96)02753-3	journal	March 1997
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Direct Uranium(VI) and Nitrate Determinations in Nuclear Reprocessing by Time-Resolved Laser-Induced Fluorescence Moulin, Christophe; Decambox, Pierre; Mauchien, Patrick Analytical Chemistry, Vol. 68, Issue 18 https://doi.org/10.1021/ac9602579	journal	January 1996
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Initial Analysis of the Detectability of UO ₂ F ₂ Aerosols Produced by UF ₆ Released from Uranium Conversion Plants Kemp, R. Scott Science & Global Security, Vol. 16, Issue 3 https://doi.org/10.1080/08929880802551172	journal	December 2008
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Non-linear effects accompanying terawatt laser-pulse in air and their applications Stelmaszczyk, Kamil; Rohwetter, Philipp; Ackermann, Roland SPIE Proceedings https://doi.org/10.1117/12.675772	conference	February 2012
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Conical emission from laser filaments and higher-order Kerr effect in air Béjot, P.; Kasparian, J. Optics Letters, Vol. 36, Issue 24 https://doi.org/10.1364/OL.36.004812	journal	January 2011
Time-Resolved Laser-Induced Fluorescence of Uranium(VI) Hydroxo-Complexes at Different Temperatures Eliet, Véronique; Grenthe, Ingmar; Bidoglio, Giovanni Applied Spectroscopy, Vol. 54, Issue 1 https://doi.org/10.1366/0003702001948178	journal	January 2000
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Uranium Determination by Remote Time-Resolved Laser-Induced Fluorescence Moulin, Christophe; Rougeault, Stephane; Hamon, Dominique Applied Spectroscopy, Vol. 47, Issue 12 https://doi.org/10.1366/0003702934066316	journal	December 1993
Speciation of Uranyl Species in Nitric Acid Medium by Time-Resolved Laser-Induced Fluorescence Couston, Laurent; Pouyat, Dominique; Moulin, Christophe Applied Spectroscopy, Vol. 49, Issue 3 https://doi.org/10.1366/0003702953963553	journal	March 1995
Time-Resolved Laser-Induced Fluorescence as a Unique Tool for Low-Level Uranium Speciation Moulin, Christophe; Laszak, Ivan; Moulin, Valérie Applied Spectroscopy, Vol. 52, Issue 4 https://doi.org/10.1366/0003702981944076	journal	April 1998
Time-Resolved Laser-Induced Spectrofluorometry of UO22+ in Nitric Acid Solutions. Preliminary Results for On-Line Uranium Monitoring Applications Deniau, H.; Decambox, P.; Mauchien, P. Radiochimica Acta, Vol. 61, Issue 1 https://doi.org/10.1524/ract.1993.61.1.23	journal	January 1993
Uranium(VI) Sulfate Complexation Studied by Time-Resolved Laser-Induced Fluorescence Spectroscopy (TRLFS) Geipel, G.; Brachmann, A.; Brendler, V. Radiochimica Acta, Vol. 75, Issue 4 https://doi.org/10.1524/ract.1996.75.4.199	journal	January 1996
Interaction of Uranium(VI) with Arsenate(V) in Aqueous Solution Studied by Time-Resolved Laser-Induced Fluorescence Spectroscopy (TRLFS) Rutsch, M.; Geipel, G.; Brendler, V. Radiochimica Acta, Vol. 86, Issue 3-4 https://doi.org/10.1524/ract.1999.86.34.135	journal	January 1999
Spectroscopic properties of uranium(VI) minerals studied by time-resolved laser-induced fluorescence spectroscopy (TRLFS) Geipel, Gerhard; Bernhard, G.; Rutsch, M. Radiochimica Acta, Vol. 88, Issue 9-11 https://doi.org/10.1524/ract.2000.88.9-11.757	journal	September 2000
Femtosecond Laser Filamentation for Atmospheric Sensing Xu, Huai Liang; Chin, See Leang Sensors, Vol. 11, Issue 1 https://doi.org/10.3390/s110100032	journal	December 2010
Conical emission from laser filaments and higher-order Kerr effect in air Béjot, P.; Kasparian, J. Figshare https://doi.org/10.6084/m9.figshare.c.3754370.v1	collection	January 2011

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36 MATERIALS SCIENCE
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Title: Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride

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