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DOE OSTI2026

A lumped particle direct simulation Monte-Carlo method combined with the collisional-radiative model for simulations of non-equilibrium laser-induced plasma plumes

Collisional plasma plumes induced by laser irradiation of material targets exhibit large variations in local density as well as ionization and excitation states, making purely hydrodynamic or kinetic simulations inaccurate or infeasible. To address this challenge and capture non-equilibrium effects in laser-induced plasma plumes at arbitrary degrees of ionization, we develop a hybrid computational approach that combines the kinetic direct simulation Monte Carlo (DSMC) method with a collisional-radiative model (CRM). This ℓDSMC-CRM approach utilizes a lumped particle method to represent minor fractions of excited ions in particle-based simulations and a special coarse-graining technique for atomic spectra and photoionization rates, ensuring numerical convergence at reduced computational cost. The hybrid approach is applied to simulate spatially homogeneous relaxation as well as one- and two-dimensional expansions of plasma plumes induced by irradiation of a copper target by a nanosecond laser pulse in a vacuum or background gas. The comparison with an equilibrium model, where local Saha-Boltzmann equilibrium is enforced, shows that the non-equilibrium effects play a dominant role. The equilibrium model can fail to predict the flow structure and strongly underestimate the degree of absorption of laser radiation by the plume. The ℓDSMC-CRM approach is validated against experimental data demonstrating reasonable agreement with the experimental electron density and temperature, while the equilibrium model is found to dramatically underestimate electron density and temperature. The flexibility of the ℓDSMC-CRM approach allows for its seamless integration into existing DSMC frameworks, making it a valuable tool for high-fidelity plasma modeling in laser-material interactions, laser-based manufacturing, and beyond.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2025

Effects of non-equilibrium ionization and excitation on radiation absorption in plasma plumes induced by ablation of metal targets with nanosecond laser pulses

Ionization and radiation absorption in nanosecond laser-induced plasma plumes are routinely modeled using the Saha–Boltzmann equilibrium ionization model (EQM). However, the equilibrium assumption can be inaccurate during the laser pulse when non-equilibrium effects significantly impact radiation absorption. In the present work, the EQM and non-equilibrium collisional-radiative model (CRM) are compared to reveal the effect of plasma non-equilibrium on radiation absorption in non-homogeneous plumes and degree of plasma shielding. Simulations of plume expansion induced by irradiation of a copper target in 1 atm argon background gas with a 10 ns Gaussian pulse at a fluence from 8 Jcm −2 to 14 Jcm −2 are performed with a hybrid computational model that couples a lumped particle direct simulation Monte Carlo method with either CRM or EQM. The simulations show that the EQM strongly underestimates the effects of ionization and radiation absorption compared to CRM and, contrary to the CRM, predict strong ionization of the background gas. The differences between the models are explained by the qualitatively different coupling between plume expansion and dynamics of ionization and exitation processes in the CRM and EQM under conditions when the characteristic times for most radiation- and electron-induced processes are longer than the pulse duration. The CRM-based predictions are also found to agree much better with available experimental data. In conclusion, these results indicate that the model of Saha–Boltzmann equilibrium cannot be used for reliable prediction of the degree of plasma shielding in plumes induced by nanosecond laser pulses or for processing results of spectroscopic measurements at early stages of expansion of such plumes.

Physics - Plasma physics↗

DOE OSTI2021

NO PLIF flow visualization and time-resolved temperature distributions in laser induced breakdown plumes

NO planar laser induced fluorescence (PLIF) is used to obtain images of laser-induced breakdown plasma plumes in NO-seeded nitrogen and dry air at near atmospheric pressure. Single-shot PLIF-images show that the plume development 5–50 μs after the breakdown pulse is fairly reproducible shot-to-shot, although the plume becomes increasingly stochastic on longer timescales, 100–500 μs. The stochastic behavior of the plume is quantified using probability distributions of the loci of the plume boundary. Analysis of the single-shot images indicates that the mixing of the plume with ambient gas on sub-ms time scale is insignificant. The induced flow velocity in the plume is fairly low, up to 30 m s –1 , suggesting that laser breakdowns are ineffective for mixing enhancement in high speed flows. The ensemble-averaged PLIF images indicate the evolution of the plume from an initially elongated shape to near-spherical to toroidal shape, with a subsequent radial expansion and formation of an axial jet in the center. Temperature distributions in the plume in air are obtained from the NO PLIF images, using two rotational transitions in the NO(X, v' = 0 → A, v'' = 0) band, J'' = 6.5 and 12.5 of the Q R 12 + Q 2 branch. The results indicate that the temperature in the plume remains high, above 1000 K, for approximately 100 μs, after which it decays gradually, to below 500 K at 500 μs. The residual NO fraction in the plume is ~0.1%, indicating that repetitive laser-assisted ignition may result in significant NO-generation. Furthermore, these measured temperature and velocity distributions can be used for detailed validation of kinetic models of laser-induced breakdown and assessment of their predictive capability.

42 ENGINEERING↗

DOE OSTI2022

The influence of particle size on the fluid dynamics of a laser-induced plasma

The interaction of a laser-induced shock wave with nanoparticles and microparticles of aluminum oxide is investigated through experiments and modeling. The chemistry and physics of the interaction between the particles and plasma generated from laser ablation shows similarities and discrete differences for the two particle sizes. For both particle sizes, early stage (< 10 μs) ionization was dominant and evidenced by higher concentrations of Al II. While both sizes exhibit ionization over the same duration, the intensity of emission was greater for nanoparticles indicating greater concentrations of ionized species. Moreover, the dispersion of species was notably more elongated for microparticles while radial dispersion was more pronounced for nanoparticles with elevated drag forces. At later stages (i.e., > 10 μs), oxidation reactions were dominant for both particle sizes, but the same distinctions in flow field were observed and attributed to particle drag. In all stages of interaction, microparticles expand axially with less drag that suppresses their radial expansion. As a result, the dispersion of reactive species was mapped over an up to 80% larger area for nanoparticles relative to microparticles. Results shown here can be applied toward advancing experimental diagnostics and particle-shock wave modeling and simulation efforts for energetic materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Sodium tracer measurements of an expanded dense aluminum plasma from e-beam isochoric heating

Spatially and temporally resolved visible absorption spectroscopy is performed on sodium D-lines present as surface contaminants on an expanded dense aluminum plasma plume. An 80-ns FWHM, intense, relativistic electron beam deposits 5.4 J into a 100- μ m-thick Al foil, which isochorically heats and subsequently hydrodynamically expands the material through the warm dense matter state and into a classical-like plasma state, with a coupling parameter of approximately 0.2 and a degeneracy parameter of approximately 270. The Na contamination, carried along with the expanding plume, shows saturated absorption features in the dense Al continuum for λ > 450 nm. X-ray photoelectron spectroscopy and laser-induced breakdown spectroscopy confirm Na is a surface contaminant with an atomic concentration of ~ 0.1 % when interrogating identical foil samples. Additioanlly, a spectroscopic-quality radiation transport model is used to post-process 2D hydrodynamic simulations to interpret the plasma conditions based on the measured Na 3p-3s doublet line profiles. A sodium number density of 3 × 10 15 cm -3 best matches the experimental spectra, which originate from a dense surface plasma with n e = 3.0 ± 0.8 × 10 18 cm -3 .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Spatiotemporal characterization of cerium monoxide in laser ablation plasmas using spectrally-resolved fast-gated imaging

The impact of oxidation chemistry on the emission characteristics and spatial structure of laser-produced Ce metal plasmas was investigated using laser-induced breakdown spectroscopy (LIBS) and time-resolved fast-gated imaging employing narrowband optical filters. Images of the plasma emission show that CeO coexists with atomic species in the periphery and vortex ring of the plasma plume. Image processing was also applied to combine independent monochromatic images of the plasma emission into a single merged image, culminating in a timelapse on the spatiotemporal evolution of atomic and molecular species within the plasma plume. The formation of CeO species was observed to proceed faster for plasmas generated in atmospheres containing larger concentrations of oxygen based on ratios of CeO-to-atomic emission intensities. Furthermore, these same ratios were shown to plateau and decrease at later times (≥25 μs), potentially indicating the depletion of CeO number densities in the plasma as the monoxide undergoes reactions to form higher polyatomic oxides. Altogether, these results provide fundamental insights into the chemical dynamics and intermixing between plasma-gas species in laser ablation cerium plasmas, advancing our understanding on optical signatures of nuclear-relevant materials to enable in-field measurement capabilities.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Expansion dynamics of femtosecond laser-induced plasmas: Influence of thermophysical plasma properties

This study investigates the expansion dynamics of femtosecond laser-induced plasmas, emphasizing the impact of plasma thermophysical properties and ambient gas composition. Through shadowgraphy experiments and multiphase computational fluid dynamics (CFD) simulations, the influence of parameters such as heat capacity, molecular weight, and thermal conductivity on plume morphology, shockwave evolution, and energy dissipation mechanisms is examined. A mixture multiphase model is implemented to capture the interaction between the plasma and the surrounding gas. Simulation results reveal that plasma expansion is strongly inertia-driven. Results show that differences in plasma properties and ambient conditions affect the shape and temperature distribution of the expanding plume. The early-stage dynamics are primarily dictated by pressure forces, whereas thermal and viscous effects play a growing role in the plume's behavior during later stages of expansion. The CFD findings show the necessity of accurate initial condition characterization, including crater geometry and plasma pressure and temperature, for reliable modeling of plasma evolution in laser ablation processes.

CFD modeling↗

DOE OSTI2020

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↗

DOE OSTI2024

Impact of target-derived and ambient oxygen on gas-phase oxidation in laser ablation plumes

Gas-phase oxidation in a laser-produced plasma is significantly influenced by the availability of oxygen in and around the plume. In this study, we investigate the role of target-derived and ambient oxygen on AlO formation in plasmas generated from aluminum (Al) and Al 2 O 3 targets in air and argon, respectively. Our results highlight that gas-phase oxidation occurs early during the evolution of Al 2 O 3 plasmas in argon, in contrast to Al plasmas in air, where the initial exclusion of oxygen from the plume delays the chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Spatiotemporal Plasma-Particle Characterization of Dry Aerosols Using Nanosecond, Femtosecond, and Filament Laser-Produced Plasmas

The ability to rapidly characterize dry aerosols in air using laser-induced breakdown spectroscopy (LIBS) with femtosecond laser pulses promises advancement towards real-time atmospheric sampling and standoff capabilities. Of particular interest is the ability to apply LIBS in the context of low-particle loaded environments where discrete particle interactions must be observed within the sampling volume of the laser-produced plasma (LPP). In this study, dry nanoparticles in suspension are generated from a standard solution and sampled in air using Q-switched nanosecond (ns-) pulses, short-focus (SF) femtosecond (fs-) pulses, and filaments. Short time-gated plasma images are captured to observe spatially and temporally varying discrete plasma-particle interactions, which is shown to influence early air breakdown behavior and subsequent plasma evolution. Along with images, photo-multiplier tube (PMT) measurements are conducted where strong spatiotemporal dependencies are exhibited by the collected emission signal on particle proximity and plasma expansion behavior. Finally, conditional analysis is performed on LIBS measurements to determine associated sampling probabilities and filter out spectra with poor or absent emission peaks with an adaptive threshold algorithm.

42 ENGINEERING↗

DOE OSTI2020

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↗

DOE OSTI2025

Detection limits for laser absorption spectroscopy of Li in laser ablation plumes

A high-sensitivity laser absorption spectroscopy (LAS) method is demonstrated for rapid and non-contact analysis of Li in solids. Glass samples with Li concentrations ranging from 1-500 ppm by mass are ablated in 5 Torr air, and time-resolved Li atomic absorption is measured using a tunable laser near 671 nm. Significant improvements in analytical performance over prior laser-induced breakdown techniques are demonstrated. Here, a single-shot limit of detection (LOD) of 180 ppb is shown for fixed wavelength operation, improving to 6 ppb with averaging over 1000 ablation shots (100 s acquisition time). Isotope-resolved Li absorption spectra are measured with a 17 ppb LOD in 40 s. Methods for optimizing LOD based on noise/averaging properties of LAS experiments in LA plumes are discussed.

(020.3260) Isotope shifts↗

DOE OSTI2023

Elemental fractionation in aerosol laser-induced breakdown spectroscopy with nanosecond and femtosecond laser ablation

For the purpose of realizing atmospheric radiation plume tracking, laser-induced breakdown spectroscopy (LIBS) was performed to characterize Cs atomic emissions from airborne nanoparticles in a binary particle matrix using nanosecond and femtosecond laser ablation. As a surrogate to multi-element nuclear fallout particulates, both Cs and Na solutions were mixed with Cu at a 1:1.45 M concentration ratio and aerosolized to study elemental fractionation in atomic emissions, revealing Na I resonance emissions are enhanced whereas Cs I resonance emissions are reduced with Cu present despite sharing similar electronic and chemical properties. Femtosecond laser ablation reduced elemental fractionation effects by more than 50% while retaining the same temporal fractionation trends for Cs and Na. The origin of elemental fractionation in aerosol LIBS was further investigated using Al and Ti aerosols which revealed that the particle matrix induces changes to the local plasma temperature, population of atomic states, and subsequent molecular association and emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Gas density structure of supersonic flows impinged on by thin blades for laser-plasma accelerator targets

Density transition injection is an effective technique for controllably loading electrons into a trapped phase for laser plasma accelerators. One common technique to achieve the required fluid structure is to impinge a thin blade on the plume of a supersonic nozzle. Density transitions induced in this way are often assumed to be bow shocks and therefore sharp, but simulations and fluorescence measurements presented in this work show that in many cases of interest, the density transition accessible to a laser propagating transverse to the shock is an intercepting shock, and therefore, shock thickness and density vary with pressure, laser height, and blade position. The fluid dynamics of a supersonic nozzle impinged on by a thin, flat object are explored through simulations and relevant features are verified via planar laser-induced fluorescence measurements. Overall, the implications of the results for tuning electron beam injectors in laser plasma accelerators are discussed.

42 ENGINEERING↗

DOE OSTI2021

Laser-induced fluorescence of filament-produced plasmas

Self-guided ultrafast laser filaments are a promising method for laser beam delivery and plasma generation for standoff and remote detection of elements and isotopes via filament-induced breakdown spectroscopy (FIBS). Yet, there are several challenges associated with the practical application of FIBS, including delivery of sufficient laser energy at the target for generating plasma with a copious amount of emission signals for obtaining a high signal-to-noise ratio. Here, in this study, we use laser-induced fluorescence (LIF) to boost the emission signal and reduce self-reversal in the spectral profiles. Ultrafast laser filaments were used to produce plasmas from an Al 6061 alloy target at various standoff distances from 1 to 10 m. For LIF emission enhancement, a narrow linewidth continuous-wave laser was used in resonance with a 394.40 nm Al I resonant transition, and the emission signal was monitored from the directly coupled transition at 396.15 nm. Emission signal features of Al I are significantly enhanced by resonant excitation. In addition, LIF of filament ablation plumes reduces the self-reversal features seen in the thermally excited spectral profiles. Time-resolved two-dimensional fluorescence spectroscopy was performed for evaluating the optical saturation effects, which are found to be non-negligible due to high Al atomic densities in the filament-produced plasmas.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Evolution and persistence of SiO emission in nanosecond laser ablation plumes

Analyzing laser-produced plasmas in a controlled oxygen-containing environment provides insight into the formation and evolution of molecular species through gas-phase oxidation. This study explores the role of ambient pressure and oxygen availability in forming SiO molecular species in laser ablation plumes. The self-emission emanating during the reactive ablation of Si targets was characterized by optical emission spectroscopy and optical time-of-flight techniques. Our results showed that the SiO species formation was greatly influenced by both the ambient pressure and oxygen availability. The intensity and the persistence of SiO emission bands are lower at higher oxygen concentrations, indicating they are depopulated by the formation of more complex silicon oxides. The oxygen partial pressure effects on plume chemistry showed that SiO formation is favored even with a minimal oxygen concentration in the environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Measurements of extended magnetic fields in laser-solid interaction

Magnetic fields generated from a laser-foil interaction are measured with high fidelity using a proton radiography scheme with x-ray fiducials. In contrast to prior findings under similar experimental conditions, this technique reveals the self-generated, Biermann-battery fields extend beyond the edge of the expanding plasma plume to a radius of over 3.5 mm by t = + 1.4 ns. An analysis of two monoenergetic proton populations confirms that proton deflection is dominated by magnetic fields far from the interaction ( > 2 mm) and electric fields are insignificant. The results are not captured in state-of-the-art magnetohydrodynamics simulations and suggest the need to consider additional physics mechanisms for the magnetic field generation and transport in laser-solid interactions. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗