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

Abstract

Uranyl fluoride (UO 2F 2) 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 UO 2F 2 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 UO 2F 2. We demonstrate that ultrafast laser filamentation coupled with LIF extends the capabilities of standard LIF to enable remote detection of UO 2F 2. 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 UO 2F 2 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 × 10 4 s -1 and discuss the characteristicsmore » 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 × 10 11 W cm -2 is promising for the application of this technique in remote sensing.« less

Authors:
 [1];  [1];  [1];  [2];  [2];  [3];  [2];  [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States). Dept. of Nuclear Engineering and Radiological Sciences. Center for Ultrafast Optical Science
  2. Univ. of Nevada, Las Vegas, NV (United States). Dept. of Chemistry
  3. Univ. of Michigan, Ann Arbor, MI (United States). Center for Ultrafast Optical Science
Publication Date:
Research Org.:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation (NA-20)
OSTI Identifier:
1500001
Grant/Contract Number:  
NA0000979; NA0002534; NA0003180
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; fluorescence spectroscopy; nonlinear optics; ultrafast lasers

Citation Formats

Skrodzki, P. J., Burger, M., Finney, L. A., Poineau, F., Balasekaran, S. M., Nees, J., Czerwinski, K. R., and Jovanovic, I. Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride. United States: N. p., 2018. Web. doi:10.1038/s41598-018-29814-8.
Skrodzki, P. J., Burger, M., Finney, L. A., Poineau, F., Balasekaran, S. M., Nees, J., Czerwinski, K. R., & Jovanovic, I. Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride. United States. doi:10.1038/s41598-018-29814-8.
Skrodzki, P. J., Burger, M., Finney, L. A., Poineau, F., Balasekaran, S. M., Nees, J., Czerwinski, K. R., and Jovanovic, I. Thu . "Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride". United States. doi:10.1038/s41598-018-29814-8. https://www.osti.gov/servlets/purl/1500001.
@article{osti_1500001,
title = {Ultrafast Laser Filament-induced Fluorescence Spectroscopy of Uranyl Fluoride},
author = {Skrodzki, P. J. and Burger, M. and Finney, L. A. and Poineau, F. and Balasekaran, S. M. and Nees, J. and Czerwinski, K. R. and Jovanovic, I.},
abstractNote = {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.},
doi = {10.1038/s41598-018-29814-8},
journal = {Scientific Reports},
number = ,
volume = 8,
place = {United States},
year = {2018},
month = {8}
}

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Figures / Tables:

Figure 1 Figure 1: Measured absorption spectrum of UO2F2 in solution using UV/VIS spectrophotometer (green); incident laser spectrum (blue).

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