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 · Thu Aug 02 00:00:00 EDT 2018 · Scientific Reports

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

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

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

Grant/Contract Number:: NA0000979; NA0002534; NA0003180

OSTI ID:: 1500001

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

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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