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At least 91 records · Page 5

Real-time monitoring of trace noble gases using laser-induced breakdown spectroscopy—An investigation of the impact of bulk gas on plasma properties and sensitivity

The impact of Ar and He bulk gases on laser-induced breakdown spectroscopy (LIBS) real-time monitoring of trace Xe and Kr was assessed. LIBS is being developed as a monitoring tool for measuring noble gas transport in molten salt systems, in which traditional sensors may face challenges associated with radiation, corrosive materials, and/or mixed phases. The plasma temperature and electron densities of LIBS plasmas were measured in both static and various flowing Ar and He streams (0–5 L min −1 ). The use of an Ar bulk gas resulted in higher plasma temperature, greater electron densities by an order of magnitude, and extended plasma lifetime compared with when He bulk gas was used. Gas flow rate was found to have little impact on plasma temperature; however, its effect on electron density was significant, indicating the need to consider flow rate–specific models. Matrix effects on emission peaks were reported for both bulk gases. Due to these matrix effects, multivariate models were developed for Xe and Kr ranging from 0 to 700 ppm in both bulk gases. Although the predictive behavior was similar (root mean square error of prediction ranging from 11.1 to 20.6 ppm), the limits of detection were superior in He (Xe: 22.9 ppm, Kr: 30.4 ppm). Furthermore, these models were employed in demonstrative real-time tests (>1 h), which showed strong predictive precision (relative standard deviation <5 %) regardless of the bulk gas. Ultimately, this study provides a guide for the considerations required when developing gaseous LIBS models for real-time monitoring.

Gas flow effects↗

Creation of large temperature anisotropies in a laboratory plasma

Ion temperature anisotropy in an expanding magnetized plasma is investigated using laser induced fluorescence. Parallel and perpendicular ion velocity distribution functions (IVDFs) were measured simultaneously with high spatial resolution in the expanding plasma. Large ion temperature anisotropies (T ⊥i /T ∥i ~ 10) are observed in a conical region at the periphery of the expanding plasma plume. A simple 2D Boris stepper model that incorporates the measured electric field structure is able to reproduce the gross features of the measured perpendicular IVDFs. Here, a Nyquist stability analysis of the measured IVDFs suggests that multiple instabilities with k ⊥ρi ~ 1 and k ||ρi ~ 0.2 are likely to be excited in these plasmas.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A computational model for nanosecond pulse laser-plasma interactions

A multi-physics numerical model for laser-induced optical breakdown and laser-plasma interaction in a non-equilibrium gas is presented, accounting for: production of priming electrons via multi-photon ionization, energy absorption, cascade ionization, induced hydrodynamic response, and shock formation and propagation. The gas is governed by the Navier-Stokes equations, with non-equilibrium effects taken into account by means of a two-temperature model. The space-time dependence of the laser beam is modeled with a flux-tube formulation for the Radiative Transfer Equation. The flow governing equations are discretized in space using a second-order finite volume method. The semi-discrete equations are marched in time using an implicit-explicit (IMEX) dual time-stepping strategy, where diffusion and chemistry are solved implicitly, whereas convection is explicit. Application to a 20 ns long 50 mJ pulse laser-induced breakdown in quiescent O 2 shows the advantages of this temporal discretization during and just after the laser pulse, while a less-expensive symmetric Strang splitting (with implicit chemistry) is sufficient for the post-breakdown gas dynamics after ≃ 0.1 μs. The integrated model is shown to reproduce key features of corresponding experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Proton radiography inversions with source extraction and comparison to mesh methods

In this article, proton radiography is a central diagnostic technique for measuring electromagnetic (EM) fields in high-energy-density, laser-produced plasmas. In this technique, protons traverse the plasma where they accumulate small EM deflections which lead to variations in the proton fluence pattern on a detector. Path-integrated EM fields can then be extracted from the fluence image through an inversion process. In this work, experiments of laser-driven foils were conducted on the OMEGA laser and magnetic field reconstructions were performed using both “fluence-based” techniques and high-fidelity “mesh-based” methods. We implement nonzero boundary conditions into the inversion and show their importance by comparing against mesh measurements. Good agreement between the methods is found only when nonzero boundary conditions are used. We also introduce an approach to determine the unperturbed proton source profile, which is a required input in fluence reconstruction algorithms. In this approach, a fluence inversion is embedded inside of a mesh region, which provides overconstrained magnetic boundary conditions. A source profile is then iteratively optimized to satisfy the boundary information. This method substantially enhances the accuracy in recovering EM fields. Lastly, we propose a scheme to quantify uncertainty in the final inversion that is introduced through errors in the source retrieval.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Measurements of the Growth and Saturation of Electron Weibel Instability in Optical-Field Ionized Plasmas

The temporal evolution of the magnetic field associated with electron thermal Weibel instability in optical-field ionized plasmas is measured using ultrashort (1.8 ps), relativistic (45 MeV) electron bunches from a linear accelerator. The self-generated magnetic fields are found to self-organize into a quasistatic structure consistent with a helicoid topology within a few picoseconds and such a structure lasts for tens of picoseconds in underdense plasmas. Here, the measured growth rate agrees well with that predicted by the kinetic theory of plasmas taking into account collisions. Magnetic trapping is identified as the dominant saturation mechanism.

Electric & magnetic plasma measurements↗

Formation of collisionless shocks driven by strongly magnetized relativistic electrons in the laboratory

In experiments performed with the OMEGA EP laser system, proton deflectometry captured magnetic field dynamics consistent with collisionless shock formation driven by strongly magnetized relativistic electrons. During laser-foil interactions, shocks can form as relativistic electrons and strong surface magnetic fields generated by a short-pulse laser impinge on a cooler plasma produced by a longer-pulse laser. Three-dimensional particle-in-cell simulations reproduce the magnetic draping and fast formation speeds measured in the experiment and reveal that this relativistic-electron-driven shock forms at an interface that is unstable to shear and streaming instabilities. The simulation results provide insight into the microphysics that may influence high-energy shocks observed in extreme astrophysical environments. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Structure of Self-Generated Magnetic Fields in Laser-Solid Interaction from Proton Tomography

Self-generated magnetic fields in laser-solid interactions are experimentally characterized to reveal the 3D location and local field strength, rather than path-integrated quantities, using multi-view proton radiography and tomographic inversion. We infer magnetic fields that extend several millimeters off the target into the hot, rarefied corona, sufficient to strongly magnetize the plasma (Ω e τ e ≫ 1). The data are compared to MHD simulations incorporating recent improvements in modeling magnetic field generation and transport; the volume-averaged coronal field strength and magnetic flux agree to within 25% using a model with magnetic re-localization of transport, although the near-target morphology is not reproduced. This work demonstrates tomographic proton radiography as a valuable tool for investigating magnetic fields in laser-produced plasmas.

High-energy-density plasmas↗

OH density and water vapor concentration gradients during plasma-droplet interactions

Plasma-droplet interactions significantly promote the reactivity transfer of gas phase species from the plasma to the liquid phase. Nonetheless, experimental studies on the impact of droplet evaporation on reactive species generation in such systems remain scarce. We report the spatial distribution of water vapor and OH radical densities around a droplet (∼41 μm in diameter) in He and He-Ar plasma using laser-induced fluorescence. The results reveal a significant gradient in both water vapor and OH radical concentrations near the droplets. Mutiple droplets present in the plasma can lead to a significant accumulation of water vapor and even local quenching of the discharge. The findings are critical for developing a quantitative understanding of plasma-liquid interactions for a broad range of plasma-enabled applications in the liquid phase often involving OH radicals.

42 ENGINEERING↗

Preheat effects in laser-driven Rayleigh–Taylor instability experiments at intensities greater than $10^{15}$ $\textrm{W}$ $\textrm{cm}^{-2}$ at OMEGA EP and the NIF

The propagation of high-energy X-rays or hot electrons have the potential to alter the initial conditions in experimental target designs, especially at material interfaces, for laser-driven inertial confinement fusion (ICF) and high-energy density (HED) experimental platforms. Hot-electron preheat can drastically modify the initial conditions of experimental targets used to study the deceleration-stage Rayleigh–Taylor instability (RTI) both with and without applied magnetic fields. Therefore, it is necessary to understand and quantify the impact of hot-electron preheat. The hydrodynamic (HD) capabilities in the Ares code are used to study the effects varying levels of preheat can have on RTI evolution. The experimental and computational studies presented in this work demonstrate that at high laser intensities of around or greater than 10 15 W cm −2 , there is hot-electron generation from laser plasma instabilities which induces substantial preheat and impacts the morphology of RTI evolution and even inhibits the intended RTI growth such that it is not observable experimentally. The necessity of better quantifying hot-electron induced preheat and mitigating its impact on such high-intensity direct-drive laser experiments in the future is discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Spatial profile of argon (1s 5 ) metastables in an electron beam generated plasma

Electron beams with an applied magnetic field generate a secondary cold plasma with a selective chemical composition, featuring low-energy ions and metastable species in the discharge periphery, ideal for low-damage plasma treatment of material substrates. In this work, we studied the plasma generated by an e-beam using a 4 kV voltage in a pure argon gas environment under a magnetic field of 150 G and in the pressure range of 25–90 mTorr. We measured the absolute spatial density profile of argon (1 s 5 ) metastables in an electron beam generated plasma by laser-induced fluorescence and found it to be of the order of 10 16 m −3 . The electron temperature and the electron density measured by a Langmuir probe were of the order of 10 16 m −3 and less than an eV respectively. Electron-impact quenching was identified as a significant loss mechanism for the Ar(1s 5 ) state, leading to the saturation of the metastable density at higher pressures. Outside the primary ionization region, the spatial distribution of argon metastables followed a linear diffusion profile, indicating negligible additional production in those regions.

EEDF↗

Comparison of laser-produced plasma spatio-temporal electron density evolution measured using interferometry with simulation results

Due to the difficulties associated with experimental measurements of laser-produced plasma (LPP) properties during the earliest stages of plasma evolution, radiation hydrodynamic codes are often used. However, although these codes have been extensively validated in the higher intensity regimes, validation at low to moderate intensities has been limited. In this study, the spatio-temporal electron density evolution in an LPP generated at moderate laser intensities and at various laser wavelengths was validated against the FLASH code for times up to 20 ns. The LPP was generated by focusing the fundamental and various harmonics radiation (1064, 532, and 266 nm) from a 6 ns full width half maximum Nd:YAG laser, at a laser intensity of 10 GW cm -2 , onto a copper target. The spatio-temporal density evolution of the expanding plasma was analyzed using Nomarski interferometry. Experimental measurements were found to be consistent with FLASH simulations, and the dependence of electron densities on wavelength was found to be in agreement with analytical models, varying as n e ∝ λ -0.7 . However, slight differences were noted in the widths and shape functions of the experimental and simulated electron density profiles.

2D fast imaging↗

Filament-induced breakdown spectroscopy with structured beams

Filament-induced ablation represents an attractive scheme for long-range material identification via optical spectroscopy. However, the delivery of laser energy to the target can be severely hindered by the stochastic nature of multiple-filamentation, ionization of ambient gas, and atmospheric turbulence. In order to mitigate some of these adverse effects, we examine the utility of beam shaping for femtosecond filament-induced breakdown spectroscopy with Gaussian and structured (Laguerre-Gaussian, Airy, and Bessel-Gaussian) beams in the nonlinear regime. Interaction of filaments with copper, zinc, and brass targets was studied by recording axially-resolved broadband emission from the filament-induced plasma. The laser-solid coupling efficacy was assessed by inferring thermodynamic parameters such as excitation temperature and electron density. While under our experimental conditions the ablation rate with Gaussian- and Laguerre-Gaussian beams is found to be similar, the Airy and Bessel-Gaussian beams offer the advantage of longitudinally extended working zones. These results provide insights into potential benefits of structuring ultrafast laser beams for standoff sensing applications.

47 OTHER INSTRUMENTATION↗

Unraveling Nonequilibrium Generation of Atomic Nitrogen and Hydrogen in Plasma-Aided Ammonia Synthesis

In this study, nonequilibrium generation of atomic nitrogen and hydrogen governing ammonia production both in the gas phase and on the catalyst surface is critical to plasma-aided ammonia synthesis. Here, this work studies the nonequilibrium generation of atomic nitrogen and hydrogen with a focus on the kinetic role of vibrational energy transfer of hydrogen molecules in plasma-aided ammonia synthesis. By combining two-photon absorption laser-induced fluorescence measurements and plasma kinetic modeling, we found that plasma not only generates ammonia but also produces critical H, N, and NH radicals via both electron impact and vibrational energy transfer excitations. The vibrational energy transfer from the excited hydrogen H 2 (v = 1) to higher vibrational levels H 2 (v = 2–3) via the V–V exchange (H 2 (v)–H 2 (v)) and V–V' exchange (N 2 (v)–H 2 (v)) significantly enhances the H and NH production and then promotes the coupling between N and NH for ammonia synthesis both in the gas phase and on the catalyst surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Enhancing analytical merits of laser-induced breakdown spectroscopy of hydrogen isotopes using an orthogonal double-pulsing scheme

Accurate detection and quantification of hydrogen isotopes in solid materials are vital for diverse applications, including fusion energy, hydrogen storage, and tritium production. Laser-induced breakdown spectroscopy (LIBS) is a well established, rapid, standoff method for this purpose, but it faces challenges related to the analytical merits required for isotopic analyses. In this study, we enhance the analytical and detection capabilities of traditional single-pulse LIBS by implementing an orthogonal double pulsing approach, focusing on the analysis of a range of 2 H concentrations in Zircaloy-4 substrates (acting as a proxy for 3 H). The double-pulse experiments employed an orthogonal re-heating configuration with two nanosecond Nd:YAG lasers. We systematically evaluated critical parameters affecting the signal intensity in double-pulse LIBS, including interpulse delay, ambient gas pressure, and heating laser energy. Finally, our results demonstrate that employing an orthogonal double-pulse scheme significantly enhances 2 H α emission while minimizing line broadening and self-absorption, ultimately improving the technique’s analytical capabilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-resolved absorption spectroscopic characterization of ultrafast laser-produced plasmas under varying background pressures

Time-resolved tunable laser absorption spectroscopy is used to characterize the physical properties of ultrafast laser-produced plasmas. The plasmas were produced from an Inconel target, with = 0.4 wt. % Al, using ~ 35 fs, ~800 nm laser pulses at varying Ar background pressures from 1-100 Torr. The absorption spectrum of atomic Al is measured with high spectral and temporal resolution when the probe laser is stepped across the selected Al transition at 394.4 nm. Spectral fitting is used to infer linewidths, kinetic temperature, Al column density, and pressure broadening coefficient. The late time physical properties of plasmas are compared for various pressure levels. Our studies highlight that a significant lower state population exists even at early times of ultrafast laser-produced plasma evolution and lower state population persistence decreases with increasing ambient pressure. We also show that the fundamental optical properties, such as pressure-broadening, can be measured using ultrafast laser-produced plasmas combined with laser absorption spectroscopy.

laser absorption spectroscopy, laser produced plas↗

ATOMIC Simulations and Experimental Data for CaCO3 Mixtures

This data consists of simulations and experimental measurements of laser-induced breakdown spectroscopy (LIBS). The simulations are produced by ATOMIC, a general purpose plasma modeling and kinetics code that has been designed to compute emission (or absorption) spectra from plasmas [1] and are used to develop a statistical characterization of matrix effects. Our overall suite of simulations includes contains several sets of simulations: training and validation sets of simulations for three and four element mixtures of calcium, carbon, oxygen, and nitrogen (included to account for atmosphere) along with simulations of the individual elements. The 4-element simulations include the mixture of all four elements mentioned and for each of the four individual elements. The 3-element simulations include output for the mixture of calcium, carbon, oxygen and for these three individual elements. The training data were produced using a 600-run design, shown in Figure 1, that varies input parameters temperature (T), electron density (Ne), and proportion of the elements calcium, carbon, oxygen, and nitrogen (Ca; C; O; N) for the 4 element output. The 3-element output includes all parameters except for the proportion of nitrogen. The element proportions (all the variables but T and Ne) sum to one and are unused in the single-element simulations. The validation data was produced with a 80-run design shown in Figure 2. The training and validation simulation outputs for the 4-element simulations for the mixture and for the single element calcium are shown as sample simulations in Figures 3 and 4 respectively. The simulations produce spectra over a range of 190nm - 950nm that roughly mimics the range collected by the SciAps Z-300 LIBS instrument that was used for the experimental data. The measured spectra for a CaCO3 (which may include contribution from Earth's atmosphere) in the experiment is shown in in Figure 5. All files are kept in directories whose names indicate the elemental composition (CaCO3, Ca, C, O, or N), number of elements (3 or 4), and purpose (training, which is not labeled in the file name, or validation) with file names numbered to indicate the line in the design files used to produce the simulation. The designs are provided as text files with names indicating their purpose. The experimental data is provided as a CSV file. [1] J Colgan, EJ Judge, DP Kilcrease, and JE Barefield II. Ab-initio modeling of an iron laser-induced plasma: Comparison between theoretical and experimental atomic emission spectra. Spectrochimica Acta Part B: Atomic Spectroscopy, 97:65{73}, 2014.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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↗