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Ultrafast laser ablation coupled with optical emission spectroscopy is currently under development for standoff detection of elements and their isotopes for a wide range of application areas. In this work, we explore the role of ambient air pressure during the interaction of an ultrafast laser beam with two metallic targets (brass and uranium) with significantly different oxygen gas-phase reactivity. Plasma plumes were generated by focusing ∼800 nm, ∼35 fs pulses from an ultrafast laser system using a long focal length lens (f = 1 m). Two-dimensional spectral imaging was performed over the pressure range of 30 mTorr to 700 Torr air to evaluate emission dynamics, plasma chemistry, signal-to-background ratio, and characteristic parameters (i.e. excitation temperature, electron density). An increase in ambient air pressure during ultrafast laser ablation leads to plume confinement and subsequent changes in the emission dynamics due to plasma chemistry as well as changes in plasma generation conditions (i.e. focused fs laser ablation versus filament ablation). Ablation crater morphologies were also investigated via scanning electron microscopy. Results indicate atomic emission intensity and signal-to-background ratios peak at moderate pressure levels (∼50–100 Torr air) for both targets studied, although plasma chemistry influences uranium emission signatures. The emission features of the uranium plasma at pressures ≥10 Torr showed the presence of oxide molecules. We also find filament ablation leads to wider, more shallow craters compared to focused laser ablation. Our study provides unique insight into the interplay between plume dynamics, confinement, and plasma chemistry of fs laser-produced plasmas and how these phenomena evolve with changing ambient air pressure.

Tumor DNA sequencing data can be interpreted by computational methods that analyse genomic heterogeneity to infer evolutionary dynamics. A growing number of studies have used these approaches to link cancer evolution with clinical progression and response to therapy. Although the inference of tumor phylogenies is rapidly becoming standard practice in cancer genome analyses, standards for evaluating tumor phylogenies are lacking. To address this need, we systematically assess methods for reconstructing tumor sub-clonality. First, we elucidate the main algorithmic problems in subclonal reconstruction and develop quantitative metrics for evaluating them. Then we simulate realistic tumor genomes that harbor all known clonal and subclonal mutation types and processes. We benchmark 580 tumor reconstructions, varying tumor read-depth, tumour type, and somatic variant detection. Our analysis provides a baseline for the establishment of gold-standard methods to analyze tumor heterogeneity., Editors summary Methods for reconstructing tumor evolution are benchmarked in the DREAM Somatic Mutation Calling Tumour Heterogeneity Challenge using novel tools.

Laser induced breakdown spectroscopy is a promising, rapid analysis method for the detection and quantification of Li and its isotopes needed in geochemical, nuclear, and energy storage applications. However, spectral broadening in laser produced plasmas, presence of fine and hyperfine structures, and self-reversal effects make Li isotopic analysis via laser induced breakdown spectroscopy challenging. The present study explores the influence of Ar, N2, and He ambient gases over the pressure range of 0.05 - 100 Torr on line broadening and self-reversal of the Li I transition with the greatest isotopic shift in the VIS spectral region (i.e., ≈670.8 nm, ≈15.8 pm isotopic shift). We perform spatially and temporally resolved optical emission spectroscopy of plasmas produced via laser ablation of LiAlO2 substrates. Our results show that the self-reversal and linewidth is reduced at lower pressures for all gases, and using optimized plasma conditions with chemometric methods, the 6Li/7Li isotopic ratios can be predicted.

Gas-phase oxidation of uranium (U), plume chemistry, and the corresponding impact on optical emission features of the U plasma are investigated. Plasmas were produced via nanosecond laser ablation of a natural U target in a chamber where U oxidation was controlled by varying the oxygen partial pressure in an argon cover gas. Monochromatic imaging of U atoms and monoxide (UO) molecules was performed using narrow bandpass optical filters. Results reveal the spatio-temporal evolution of atomic and molecular species in the plasma. U oxides are found to be formed further from the target (in comparison to U atoms), where lower temperatures favor molecular recombination. Segregation between the distribution of U atoms and UO species is observed at later times of plasma evolution, and is more apparent at lower oxygen partial pressures. At higher oxygen partial pressures, significant variation in plume morphology is noticed for UO species, which can be attributed to the higher oxide (UxOy) formation further from the target. The monochromatic images of U atoms and UO molecules and corresponding spectral features at various oxygen partial pressures presented here provide unique insight into gas-phase, high-temperature U oxidation and chemistry, with implications for a wide range of nuclear applications, from stand-off detection of radioisotopes to forensics and safeguards.

Laser-induced breakdown spectroscopy is a promising method for rapidly measuring hydrogen and its isotopes, critical to a wide range of disciplines (e.g. nuclear energy, hydrogen storage). However, line broadening can hinder the ability to detect finely spaced isotopic shifts. Here, the effects of varying plasma generation conditions (nanosecond versus femtosecond laser ablation) and ambient environments (argon versus helium gas) on spectral features generated from Zircaloy-4 targets with varying hydrogen isotopic compositions were studied. Time-resolved 2D spectral imaging was employed to detail the spatial distribution of species throughout plasma evolution. Results highlight that hydrogen and deuterium isotopic shifts can be measured with minimal spectral broadening in a ∼ 10 Torr helium gas environment using ultrafast laser-produced plasmas.

We introduce a new, to the best of our knowledge, modality of dual-comb spectroscopy (DCS) that enables a simplified and powerful new approach for time-resolved measurements with increased acquisition rates. This “burst mode” form of DCS relies on the multiplexing of each probe pulse into a short train of pulses. With this approach we demonstrate a time-resolved series of absorption-based spectroscopic measurements of a laser-induced plasma using only a single laser ablation shot and identify 22 Nd lines not previously reported in the literature. The transmission spectra spanned 3.1 THz and were acquired at an effective acquisition rate of 25 kHz with 40 µs time resolution. This simple modification to ∼ 100 M H z level dual-comb systems provides a flexible approach for studying transient and low-duty-cycle events such as laser-induced plasmas, combustion, and explosive reactions.

Rapid and sensitive standoff measurement techniques are needed for detection of trace chemicals in outdoor plume releases, for example from industrial emissions, unintended chemical leaks or spills, burning of biomass materials, or chemical warfare attacks. Here, we present results from 235 m standoff detection of transient plumes for 5 gas-phase chemicals: Freon 152a (1,1-difluoroethane), Freon 134a (1,1,1,2-tetrafluoroethane), methanol (CH3OH), nitrous oxide (N2O), and ammonia (NH3). A swept-wavelength external cavity quantum cascade laser (ECQCL) measures infrared absorption spectra over the range 955-1195 cm−1 (8.37- 10.47 µm), from which chemical concentrations are determined via spectral fits. The fast 400 Hz scan rate of the swept-ECQCL enables measurement above the turbulence time-scales, reducing noise and allowing plume fluctuations to be measured. For high-speed plume detection, noise-equivalent column densities of 1-2 ppm*m are demonstrated with 2.5 ms time resolution, improving to 100-400 ppb*m with 100 ms averaging.

Laser ablation in conjunction with optical emission spectroscopy is a potential non-contact, stand-off 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 detection of materials. 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. Time-resolved, two-dimensional plume and spectral 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 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 component 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.

Oxygen present in the ambient gas medium may affect both laser-induced breakdown spectroscopy (LIBS) and laser-induced fluorescence (LIF) emission through a reduction of emission intensity and persistence. In this study, an evaluation is made on the role of oxygen in the ambient environment under atmospheric pressure conditions in LIBS and laser ablation (LA)-LIF emission. To generate plasmas, 1064 nm, 10 ns pulses were focused on an aluminum alloy sample. LIF was performed by frequency scanning a CW laser over the 396.15 nm (3s 2 4s 2 S 1/2 → 3s 2 3p 2 P° 3/2 ) Al I transition. Time-resolved emission and fluorescence signals were recorded to evaluate the variation in emission intensity caused by the presence of oxygen. The oxygen partial pressure ( p o ) in the atmospheric pressure environment using N 2 as the makeup gas was varied from 0 to 400 Torr O 2 . 2D–fluorescence spectroscopy images were obtained for various oxygen concentrations for simultaneous evaluation of the emission and excitation spectral features. Results showed that the presence of oxygen in the ambient environment reduces the persistence of the LIBS and LIF emission through an oxidation process that depletes the density of atomic species within the resulting laser-produced plasma (LPP) plume.

We investigate the oxidation of uranium (U) species, the physical conditions leading to uranium monoxide (UO) formation and the interplay between plume hydrodynamics and plasma chemistry in a laser-produced U plasma. Plasmas are produced by ablation of metallic U using nanosecond laser pulses. An ambient gas environment with varying oxygen partial pressures in 100 Torr inert Ar gas is used for controlling the plasma oxidation chemistry. Optical emission spectroscopic analysis of U atomic and monoxide species shows a reduction in the emission intensity and persistence with increasing oxygen partial pressure. Spectral modelling is used for identifying the physical conditions in the plasma that favor UO formation. The optimal temperature for UO formation is found to be in the temperature range of ∼1500-5000 K. The spectrally integrated and spectrally filtered (monochromatic) imaging of U atomic and molecular species reveals the evolutionary paths of various species in the plasma. Our results also highlight that oxidation in U plasmas predominantly occurs at the cooler periphery and is delayed with respect to plasma formation, and the dissipation of molecular species strongly depends on oxygen partial pressure.

This study employs laser ablation (LA) to investigate mechanisms for U optical signal variation under various environmental conditions during laser absorption spectroscopy (LAS) and optical emission spectroscopy (OES). Potential mechanisms explored for signal quenching related to ambient conditions include plasma chemistry (e.g., uranium oxide formation), ambient gas confinement effects, and other collisional interactions between plasma constituents and the ambient gas. LA-LAS studies show that the persistence of the U ground state population is significantly reduced in the presence of air ambient compared to nitrogen. LA-OES yields congested spectra from which the U I 356.18 nm transition is prominent and serves as the basis for signal tracking. LA-OES signal and persistence vary negligibly between the test gases (air and N 2 ), unlike the LA-LAS results. The plume hydrodynamic features and plume fundamental properties showed similar results in both air and nitrogen ambient. Investigation of U oxide formation in the laser-produced plasma suggests that low U concentration in a sample hinders consistent detection of UO molecular spectra.

A swept-wavelength external cavity quantum cascade laser (ECQCL) is used to perform standoff detection of combustion gases in a plume generated from an outdoor high-explosive (HE) open detonation. The swept-ECQCL system was located at a standoff distance of 830 m from a 41 kg charge of LX-14 (polymer-bonded high explosive) and was used to measure the infrared transmission/absorption through the post-detonation plume as it propagated through the beam path. The swept-ECQCL was operated continuously to record broadband absorption spectra at a 200 Hz rate over a spectral range from 2050 to 2230 cm−1 (4.48–4.88 μm). Fitting of measured spectra was used to determine time-resolved column densities of CO, CO2, H2O, and N2O. Analysis of visible video imagery was used to provide timing correlations and to estimate plume dimensions, from which gas mixing ratios were estimated. Measured emission factors and modified combustion efficiency show good agreement with previously reported values.

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 plasmas were produced during ns laser ablation on a natural U metal target which contains 0.73% 235U. Our results show that isotopic shifts between 238U and 235U are entangled with hyperfine structures of 235U. Measurements obtained using laser-induced fluorescence are affected by the high absorbance of 238U. Time-resolved laser absorption spectroscopy is carried out for evaluating the optical absorption and estimating the hyperfine constants.

Uranium, because of its pyrophoricity, oxidizes rapidly in an oxygen-containing high-temperature environment. However, so far, the identification of uranium oxide (UO) emission from a laser-produced plasma system is limited to a spectral feature around 593.55 nm. The aim of this study is to elucidate UO emission features in the visible spectral regime from uranium plasmas generated in an environment with varying oxygen concentrations. The plasmas are produced by focusing nanosecond laser pulses on a uranium metal target in a controlled ambient environment. Space- and time-resolved optical emission spectroscopic investigations are used for isolating UO molecular emission structures from crowded U atomic line emission. Our studies highlight that the emission from a U plasma, even in the presence of trace oxygen is accompanied by a strong background-like emission with partially resolved bands from uranium monoxide and higher oxides. We also report several UO spectral emission bands in the visible spectral region.

Dual-comb spectroscopy has become a powerful spectroscopic technique in applications that rely on its broad spectral coverage combined with high frequency resolution capabilities. Experiments to date have primarily focused on detection and analysis of multiple gas species under semi-static conditions, with applications ranging from environmental monitoring of greenhouse gases to high-resolution molecular spectroscopy. Here, we utilize dual-comb spectroscopy to demonstrate broadband, high-resolution, and time-resolved measurements in a laser-induced plasma. As a demonstration, we simultaneously detect trace amounts of Rb and K in solid samples with a single laser ablation shot, with transitions separated by over 6 THz (13 nm) and spectral resolution sufficient to resolve isotopic and ground state hyperfine splittings of the Rb D2 line. This new spectroscopic approach offers the broad spectral coverage found in the powerful techniques of laser-induced breakdown spectroscopy (LIBS) while providing the high-resolution and accuracy of cw laser-based spectroscopies., Dual-comb spectroscopy has become a valuable tool for broadband high-resolution measurements. Here Bergevin et al. apply this technique to a laser-induced plasma detecting different species in a solid sample with a spectral resolution sufficient to resolve hyperfine splitting of the Rb D2 line.

We report the use of laser-induced fluorescence (LIF) of laser ablation (LA) plumes for standoff applications. The standoff analysis of Al, as major and minor species in samples, is performed in a nanosecond laser-produced plasma created at a distance of ∼10 m. The LIF of LA plumes is carried out by resonantly exciting an Al transition at 394.4 nm (S1/22−P1/22) using a continuous wave (cw) tunable laser and by collecting the direct-line fluorescence signal at 396.15 nm. The spectral resolution of LIF is obtained by scanning the cw tunable LIF laser across the selected Al transition. Our results highlight that LIF provides enhanced signal intensity, emission persistence, and spectral resolution when compared to thermally excited emission.

Laser-induced plasma spectroscopy provides much impetus as a nuclear forensics tool because of its capability of standoff detection and real-time analysis. However, special nuclear materials like U, Pu, etc. provide very crowded spectra and, when combined with shifts and broadening of spectral lines caused by ambient atmospheric operation, generate a complex plasma spectroscopy system. We explored the spatio-temporal evolution of excited U species in a laser ablation plume under various ambient pressure conditions. Plasmas were generated using 1064 nm, 6 ns pulses from a Nd:YAG laser on a U containing glass matrix target. The role of air ambient pressure on U line intensities, signal-to-background ratios, and linewidths were investigated. Spatially and temporally resolved optical time-of-flight emission spectroscopy of excited uranium atoms were used for studying the expansion hydrodynamics and the persistence of U species in the plume. Our results showed that U emission linewidths increased with pressure due to increased Stark broadening; however, the broadening was less than that for Ca. A comparison with U emission features in the presence of an inert gas showed the persistence of U species in plasmas in ambient air is significantly reduced; this could be due to oxide and other reactive species formation.

We investigated the expansion dynamics of laser-produced plasmas expanding into an axial magnetic field. Plasmas were generated by focusing 1.064 μm Nd:YAG laser pulses onto a planar tin target in vacuum and allowed to expand into a 0.5 T magnetic field where the field lines were aligned along the plume expansion direction. Gated images employing an intensified charge-coupled device showed focusing of the plasma plume, which were also compared with results, obtained using particle-in-cell modeling methods. The estimated density and temperature of the plasma plumes employing emission spectroscopy revealed significant changes in the presence and absence of the 0.5 T magnetic field. In the presence of the field, the electron temperature is increased with distance from the target, while the density showed opposite effects.

We have investigated the effects of helium ion irradiation energy and sample temperature on the performance of grain boundaries as helium sinks in ultrafine grained and nanocrystalline tungsten. Irradiations were performed at displacement and non-displacement energies and at temperatures above and below that required for vacancy migration. Microstructural investigations were performed using Transmission Electron Microscopy (TEM) combined with either in-situ or ex-situ ion irradiation. Under helium irradiation at an energy which does not cause atomic displacements in tungsten (70 eV), regardless of temperature and thus vacancy migration conditions, bubbles were uniformly distributed with no preferential bubble formation on grain boundaries. At energies that can cause displacements, bubbles were observed to be preferentially formed on the grain boundaries only at high temperatures where vacancy migration occurs. Under these conditions, the decoration of grain boundaries with large facetted bubbles occurred on nanocrystalline grains with dimensions less than 60 nm. We discuss the importance of vacancy supply and the formation and migration of radiation-induced defects on the performance of grain boundaries as helium sinks and the resulting irradiation tolerance of ultrafine grained and nanocrystalline tungsten to bubble formation.

Plasma facing components for future fusion applications will experience helium- and neutron-induced structural damage. Direct observation of the in-situ dynamic response of such components during particle beam exposure assists in fundamental understanding of the physical phenomena that give rise to their irradiation resistance. We investigated the response of ultrafine and nanocrystalline-grained tungsten to 3 MeV heavy ion irradiations (Si{sup 2} {sup +}, Cu{sup 3} {sup +} and W{sup 4} {sup +}) for the simulation of neutron-induced damage through transmutation reactions via in-situ ion irradiation–transmission electron microscopy experiments. Defect densities as a function of irradiation dose (displacement per atom) and fluence were studied. Four stages of defect densities evolution were observed, as a function of irradiation dose: 1) increase in defect density at lower doses, 2) higher defect production rate at the intermediate doses (before saturation), 3) reaching the maximum value, and 4) drop of the defect density in the case of W{sup 4} {sup +}, possibly due to defect coalescence and grain boundary absorption of small defect clusters. The effect of grain size on defect densities was investigated and found that defect densities were independent of grain size in the ultrafine and nanocrystalline region (60–400 nm). These results were comparedmore » to other heavy ion irradiation studies of structural materials. - Graphical abstract: Bright-field TEM micrographs and defect densities of UF and NC tungsten grains irradiated with a) Si{sup +} {sup 2} at 1.03 dpa: 1) 140 nm — 7.2 × 10{sup −} {sup 3} defects/nm{sup 2}, 2) 122 nm — 6.9 × 10{sup −} {sup 3} defects/nm{sup 2}, 3) 63 nm — 4.7 × 10{sup −} {sup 3} defects/nm{sup 2}, and 4) 367 nm — 6.4 × 10{sup −} {sup 3} defects/nm{sup 2}; b) Cu{sup +} {sup 3} to 3.79 dpa: 1) 228 nm — 4.3 × 10{sup −} {sup 3} defects/nm{sup 2}; 2) 202 nm — 5.9 × 10{sup −} {sup 3} defects/nm{sup 2}; and 3) 137 nm — 6.1 × 10{sup −} {sup 3} defects/nm{sup 2}; and c) W{sup +} {sup 4} to 5.72 dpa: 1) 372 nm — 2.3 × 10{sup −} {sup 3} defects/nm{sup 2} and 2) 128 nm — 4.5 × 10{sup −} {sup 3} defects/nm{sup 2}. - Highlights: • Heavy ion irradiations were performed on UF and NC grained tungsten. • Irradiations were performed with 3 MeV (Si{sup 2} {sup +}, Cu{sup 3} {sup +} and W{sup 4} {sup +}) ions at RT. • Defect density vs. dpa demonstrated four different stages in the case of W{sup 4} {sup +} irradiation. • Defect coalescence and absorption by the grain boundaries were observed after a dose of 3 dpa during W{sup 4} {sup +} irradiation. • No correlation existed between the grain width and the defect density for the UF and NC region.« less

The laser ablation of materials induced by an ultrashort femtosecond pulse is a complex phenomenon, which depends on both the material properties and the properties of the laser pulse. A combination of molecular dynamics (MD) and momentum scaling model (MSM) methods is applied to a large atomic system to study the process of ultrafast laser-material interactions, behavior of matter in a highly nonequilibrium state, material disintegration, and formation of nanoclusters (NCs). Laser pulses with several fluences in the range from $500\phantom{\rule{0.16em}{0ex}}\mathrm{J}/{\mathrm{m}}^{2}$ to $5000\phantom{\rule{0.16em}{0ex}}\mathrm{J}/{\mathrm{m}}^{2}$ interacting with a large system of aluminum atoms are simulated. The response of Al to laser energy deposition is investigated within the finite-size laser spot. It is found that the shape of the plasma plume is dynamically changing during expansion. At several tens of picoseconds it can be characterized as a long hollow ellipsoid surrounded by Al atoms and NCs. The time evolution of NCs in the plume is investigated. The collisions between single Al atoms and generated NCs and fragmentation of large NCs determine the fractions of different-size NCs in the plume. The MD-MSM simulations show that laser fluence greatly affects the size distribution of NCs, their polar angles, and magnitude and direction vectors of NC velocities. These results and predictions are consistent, in many aspects, with the experimental data and previous MD simulations.

We report on the observation of uranium monoxide (UO) emission following fs laser ablation (LA) of a uranium metal sample. The formation and evolution of the molecular emission is studied under various ambient air pressures. Observation of UO emission spectra at a rarefied residual air pressure of ~1 Torr indicates that the UO molecule is readily formed in the expanding plasma with trace concentrations of oxygen present within the vacuum chamber. The persistence of the UO emission exceeded that of the atomic emission; however, the molecular emission was delayed in time compared to the atomic emission due to the necessary cooling and expansion of the plasma before the UO molecules can form.

Recent results using nanosecond and femtosecond laser ablation combined with tunable laser absorption and fluorescence spectroscopy show the potential for rapid standoff characterization of uranium isotopes in solid samples at atmospheric pressure.

In this work we study the effectiveness of long-wavelength heating in double pulse (DP) LIBS, quantitatively comparing figures of merit with those from traditional single pulse (SP) LIBS. The first laser pulse serves as the source of sample ablation, creating an aerosol-like plume that is subsequently reheated by the second laser pulse. At power densities used, the long-wavelength CO2 laser pulse does not ablate any of the solid sample in the atmospheric conditions investigated, meaning plasma emission and enhanced signal can be entirely attributed to the reheated plume rather than increased sample ablation. The signal discrimination was improved significantly using long-wavelength DP-LIBS. For bulk elemental analysis, DP-LIBS provided maximum enhancements of about 14 and 15 times for S/N and S/B, respectively, compared to SP-LIBS using the same quantity of ablated sample. For trace elemental analysis, maximum enhancements of about 7 and 4 times for S/N and S/B, respectively, were observed. These improvements are attributed to effective coupling between the second heating pulse and expanding plume and more efficient excitation of plume species than from the single pulse alone. Most significant improvements were observed in the case of low prepulse energy and minimal sample ablation. While bulk elemental analysis observed improvements for all prepulse energies studied, trace element discrimination only significantly improved for the lowest prepulse energy studied.

Infrared laser absorption spectroscopy provides a powerful tool for probing physical and chemical properties of high-explosive detonations. A broadly tunable swept-wavelength external cavity quantum cascade laser operating in the mid-wave infrared (MWIR) spectral region is used to measure transmission through explosive fireballs generated from 14 g charges of 4 different explosive types detonated in an enclosed chamber. Analysis of time-resolved transmission and emission at a 2 μs sampling rate shows the evolution of fireball infrared opacity in the first 10 ms after detonation. Broadband high-resolution absorption spectra acquired over the spectral range of 2050–2300 cm−1 (4.35–4.88 μm) at a 100 Hz rate are used to measure properties of fireball evolution over longer time scales out to 100 s. Path-integrated concentrations of combustion products CO, CO2, H2O, and N2O are measured and show evolutions over multiple time scales and significant differences between explosive types. Spectral analysis is used to characterize gas temperature and to measure broadband attenuation from absorption and scattering of particulates. Analysis of the results provides information on the MWIR optical properties, gaseous detonation/combustion products, and particulates throughout the explosive process including initial detonation, fireball expansion and cooling, and diffusive mixing in the chamber.

This work reports the spatiotemporal diagnostics of uranium species in plasma plumes produced by nanosecond near-infrared laser pulses in a low-pressure environment. Spatially and temporally resolved emission spectroscopy experiments are combined with the modeling of uranium emission for investigating the dynamics of the plume. The Saha-Eggert equation and Boltzmann plots generated from numerous U I transitions are used to infer temperature. This work also reports the measurements of uranium Stark broadening parameters for U I 499.01 nm and U II 500.82 nm transitions. The Stark widths of select U transitions were measured by comparing their linewidths with the broadening of the O I 777.19 nm line. The electron density was found to be of the order of 1016 cm−3, while the temperature was found to be in the range of 3000–9000 K. In addition to enhancing the fundamental understanding of high-Z plasmas in reduced-pressure environments, the knowledge of Stark broadening parameters could improve the modeling capabilities and analytical performance of techniques that rely on emission plasma spectroscopy.

The dynamics of expansion, thermodynamics, and chemical reactions in laser-produced plasmas is of general interest for all laser ablation applications. This study investigates the complex morphology and behavior of reactive species in nanosecond laser-produced uranium plasmas. Comparing plasma morphology in various inert and reactive ambient gases provides information about the role of gas-phase chemistry in plume hydrodynamics. Background gases including nitrogen and argon foster collisional interactions leading to more significant plume confinement and the increase in persistence of uranium species. On the other hand, environments containing reactive gases such as oxygen promote chemical reactions between the plasma and ambient species. By comparing the expansion dynamics of uranium plumes in nitrogen, air, and argon, we discover that chemical reactions modify the hydrodynamics of the plume at later times of its evolution in the air background. Furthermore, we observe that varying the concentration of oxygen in the fill gas promotes different reaction pathways that lead to the formation of uranium oxides. The reaction pathways from atoms to diatomic to polyatomic molecules strongly vary with ambient oxygen concentration. Lower oxygen concentrations enhance the formation of uranium monoxide from atomic uranium, whereas higher oxygen concentrations tend to depopulate both atomic uranium and uranium monoxide concentrations through the formation of more complex uranium oxides.The dynamics of expansion, thermodynamics, and chemical reactions in laser-produced plasmas is of general interest for all laser ablation applications. This study investigates the complex morphology and behavior of reactive species in nanosecond laser-produced uranium plasmas. Comparing plasma morphology in various inert and reactive ambient gases provides information about the role of gas-phase chemistry in plume hydrodynamics. Background gases including nitrogen and argon foster collisional interactions leading to more significant plume confinement and the increase in persistence of uranium species. On the other hand, environments containing reactive gases such as oxygen promote chemical reactions between the plasma and ambient species. By comparing the expansion dynamics of uranium plumes in nitrogen, air, and argon, we discover that chemical reactions modify the hydrodynamics of the plume at later times of its evolution in the air background. Furthermore, we observe that varying the concentration of o...

We utilize time-resolved dual-comb spectroscopy to measure the temporal evolution of the population number densities and absorption excitation temperature of Fe in a laser-induced plasma. The spectra of three excited-state transitions of Fe around 533 nm are simultaneously measured at different time delays following laser ablation of a stainless steel sample. This Letter probes late-time behaviors of laser-induced ablation plumes during plasma cooling. The high spectral resolution and broad spectral coverage of the dual-comb technique, combined with the time-resolved measurement capability shown here, will aid in the characterization of laser induced plasmas, including species identification and molecule and particle formation that can occur at later times in the plasma evolution.

Filament-induced breakdown spectroscopy (FIBS) is an attractive remote detection approach that is potentially applicable to nuclear materials such as uranium (U). Simultaneous detection of atomic U and U monoxide features is demonstrated in a single laser shot with detection probabilities of 52.2% and 39.0%, respectively, and with a 1% false-alarm probability. It is shown that a nearly 100% detection probability can be reached with 1% false-alarm probability in ≲1 second when using an 80 Hz laser and data acquisition system. Atomic U and uranium oxide (UO) signal features are identifiable in the remote measurement with comparable signal-to-background ratios, suggesting that, despite being broader than the U I emission line, the UO band is also suitable for remote detection of U by FIBS.