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Optical spectroscopic tools for standoff uranium detection

Rapid and standoff analysis of uranium is important for many applications. We present the recent advances in standoff detection of uranium using emission and laser-induced fluorescence spectroscopy in conjunction with ultrafast laser filament ablation-based solid sampling.

(020.3260) Isotope shifts, (140.3440) Laser-induce↗

Hyperfine structures and isotopic shifts of uranium transitions using tunable laser spectroscopy of laser ablation plumes

We report isotopic shifts and hyperfine structures of selected U transitions employing tunable spectroscopy viz: laser-induced fluorescence and laser absorption spectroscopy of laser ablation plumes. The laser-produced plasmas were produced during ns laser ablation on a natural U metal which contains 0.7% 235U. Our results show that isotopic shifts between 238U and 235U are entangled with hyperfine structures of 235U. The isotopic ratio obtained using laser-induced fluorescence is affected by optical saturation effect. Time-resolved laser absorption spectroscopy is carried out for evaluating the optical absorption and estimating the hyperfine constants.

(020.3260) Isotope shifts↗

Laser ablation spectrometry for studies of uranium plasmas, reactor monitoring, and spent fuel safety

Nuclear security is one of the defining challenges of our time. Nuclear threats range from deliberate dispersal of radioactive material to contaminate the vital infrastructure to diversion and smuggling of special nuclear material for clandestine nuclear programs and nuclear terrorism, respectively. There is an associated need to develop and sustain the nuclear forensics capabilities, which requires the understanding of complex processes that occur in plasmas of nuclear materials. The area of nuclear safety has seen a resurgence of public interest, and there is a concomitant need to safely store used nuclear fuel and detect structural material failure in nuclear power systems, especially in innovative reactor designs envisioned for future adoption. Laser-produced plasmas are complicated extreme environments that can generate intense and rich, highly specific signatures of nuclear and radiological materials, which can then be explored in a wide range of applications. They include interdiction and rapid detection of nuclear materials, including their isotopic composition, detection over long distances, laboratory simulation of weapons effects, monitoring the condition of structural materials in dry cask storage containers, and novel instrumentation for nuclear power systems. We present a compilation of recent representative examples of the application of laser spectroscopy, and laser-induced breakdown spectroscopy in particular, to nuclear safety and security problems. A case is made that spectroscopic techniques based on laser-produced plasmas offer complementary, and sometimes unique, capabilities that motivate the continued exploration of their efficient production and understanding of the signatures they produce

(020.3260) Isotope shifts, (140.3440) Laser-induce↗

Spectro-temporal comparisons of optical emission, absorption, and laser-induced fluorescence for characterizing ns and fs laser-produced plasmas

We performed simultaneous measurement of absorption, emission, and laser-induced fluorescence spectroscopic signatures for determining nanosecond and femtosecond laser-produced plasma’s physical properties throughout its lifecycle. Plasmas are produced by focusing either ~6 ns, 1064 nm pulses from an Nd:YAG or ~35 fs, ~800 nm pulses from a Ti:Sapphire laser on an Inconel target that contains Al as a minor alloying addition. A continuous-wave narrowband tunable laser was used for performing absorption and fluorescence spectroscopy while a fast-gated detection system was used for emission spectroscopy. The temporal evolution of emission, fluorescence, and absorbance of Al transitions are compared for both ns and fs laser-produced plasms. Time-resolved absorbance was also used for evaluating linewidth, lineshape, temperature, and column-averaged atomic number density at late times of ns and fs plasma evolution. Our results demonstrate that lower and excited-state populations of fs laser produced plasmas are short-lived in comparison to those in ns plasmas. The lower state population is observed to reach a maximum value earlier in time for the fs plasma versus the ns plasma, while the kinetic temperature for the ns plasma was higher than for the fs plasma at most times of the plasma evolution.

(280.4788) Optical Sensing, (300.2140) Emission Sp↗

Analysis of hydrogen and lithium isotopes using Laser-Induced Breakdown Spectroscopy

The detection and quantification of hydrogen (1,2,3H) and lithium (6,7Li) isotopes are critical to several energy and defense application areas, including hydrogen storage, nuclear forensics, and safeguards/non-proliferation. In this context, laser-induced breakdown spectroscopy (LIBS) is very promising and it comes with certain advantages such as rapid detection, and standoff capability. Although LIBS provides experimental simplicity and is capable of detecting all elements in the periodic table in any phase (solid, liquid, or gas), there exist certain challenges for isotopic analyses of H and Li due to spectral broadening, the presence of closely spaced fine and hyperfine structures, and line distortion effects (e.g., self-absorption and self-reversal) present in laser-produced plasmas. This article reports recent developments in H and Li isotopic analysis using LIBS, and existing challenges.

(020.3260) Isotope shifts, (140.3440) Laser-induce↗

Spatiotemporal evolution of emission and absorption signatures in a laser-produced plasma

Here we report spatiotemporal evolution of emission and absorption signatures of Al species in a nanosecond (ns) laser-produced plasma (LPP). The plasmas were generated from an Inconel target, which contained ~0:4 wt. % Al, using 1064 nm, ≈6 ns full width half maximum pulses from an Nd:YAG laser at an Ar cover gas pressure of ≈34 Torr. The temporal distributions of the Al I (394.4 nm) transition were collected from various spatial points within the plasma employing time-of-flight (TOF) emission and laser absorption spectroscopy, and they provide kinetics of the excited state and ground state population of the selected transition. The emission and absorption signatures showed multiple peaks in their temporal profiles, although they appeared at different spatial locations and times after the plasma onset. The absorption temporal profiles showed an early time signature representing shock wave propagation into the ambient gas. We also used emission and absorption spectral features for measuring various physical properties of the plasma. The absorption spectral profiles are utilized for measuring linewidths, column density, and kinetic temperature, while emission spectra were used to measure excitation temperature. A comparison between excitation and kinetic temperature was made at various spatial points in the plasma. Our results highlight that the TOF measurements provide a resourceful tool for showing the spatiotemporal LPP dynamics with higher spatial and temporal resolution than is possible with spectral measurements but are difficult to interpret without additional information on excitation temperatures and linewidths. The combination of absorption and emission TOF and spectral measurements thus provides a more complete picture of LPP spatiotemporal dynamics than is possible using any one technique alone.

(140.3440) Laser-induced breakdown, (280.4788) Opt↗

Expansion dynamics and chemistry evolution in ultrafast laser filament produced plasmas

Laser ablation in conjunction with optical emission spectroscopy is a potential non-contact, standoff detection method for all elements in the periodic table and certain isotopes such as radionuclides. Currently, significant development efforts are on-going to use ultrafast laser filaments for remote sensing. The application of filaments is of particular interest in extending the range of stand-off capability associated with elemental and isotopic detection via laser-induced breakdown spectroscopy. In this study, we characterize the expansion dynamics and chemical evolution of filament-produced uranium (U) plasmas. Laser filaments are generated in the laboratory by loosely focusing 35 femtosecond (fs), 6 milli Joule (mJ) pulses in air. Two-dimensional spectrally-integrated and time-resolved imaging was performed to study hydrodynamics and evolution of U atomic and UO molecular emission in filament-produced U plasmas. Our results highlight that filament ablation of U plasmas gives a cylindrical plasma plume morphology with an appearance of plume splitting into slow and fast moving components at later times of its evolution. Emission from the slow-moving region shows no distinct spectral features (i.e. broadband-like) and is contributed in part by nanoparticles generated during ultrafast laser ablation. Additionally, we find U atoms and U oxide molecules (i.e. UO, UxOy) co-exist in the filament produced plasma, which can be attributed to the generation of low-temperature plasma conditions during filament ablation

(140.3440) Laser-induced breakdown, (280.5395) Pla↗