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At least 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2017

Standoff Detection of Uranium and its Isotopes by Femtosecond Filament Laser Ablation Molecular Isotopic Spectrometry

The ability to perform not only elementally but also isotopically sensitive detection and analysis at standoff distances is important for remote sensing applications in diverse ares, such as nuclear nonproliferation, environmental monitoring, geophysics, and planetary science. We demonstrate isotopically sensitive real-time standoff detection of uranium by the use of femtosecond filament-induced laser ablation molecular isotopic spectrometry. A uranium oxide molecular emission isotope shift of 0.05 ± 0.007 nm is reported at 593.6 nm. We implement both spectroscopic and acoustic diagnostics to characterize the properties of uranium plasma generated at different filament- uranium interaction points. The resulting uranium oxide emission exhibits a nearly constant signal-to-background ratio over the length of the filament, unlike the uranium atomic and ionic emission, for which the signal-to-background ratio varies significantly along the filament propagation. This is explained by the different rates of increase of plasma density and uranium oxide density along the filament length resulting from spectral and temporal evolution of the filament along its propagation. Lastly, the results provide a basis for the optimal use of filaments for standoff detection and analysis of uranium isotopes and indicate the potential of the technique for a wider range of remote sensing applications that require isotopic sensitivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Laser-ablation sampling for inductively coupled plasma distance-of-flight mass spectrometry

An inductively coupled plasma distance-of-flight mass spectrometer (ICP-DOFMS) has been coupled with laser-ablation (LA) sample introduction for the elemental analysis of solids. ICP-DOFMS is well suited for the analysis of laser-generated aerosols because it offers both high-speed mass analysis and simultaneous multi-elemental detection. Here, we evaluate the analytical performance of the LA-ICP-DOFMS instrument, equipped with a microchannel plate-based imaging detector, for the measurement of steady-state LA signals, as well as transient signals produced from single LA events. Steady-state detection limits are 1 mg g1, and absolute single-pulse LA detection limits are 200 fg for uranium; the system is shown capable of performing time-resolved single-pulse LA analysis. By leveraging the benefits of simultaneous multi-elemental detection, we also attain a good shot-to-shot reproducibility of 6% relative standard deviation (RSD) and isotope-ratio precision of 0.3% RSD with a 10 s integration time.

Gundlach-Graham, Alexander W.↗
DOE OSTI2017

Characterization of extreme ultraviolet laser ablation mass spectrometry for actinide trace analysis and nanoscale isotopic imaging

The purpose of this research was to characterize Extreme Ultraviolet Time-of-Flight (EUV TOF) Laser Ablation Mass Spectrometry for high spatial resolution elemental and isotopic analysis. We compare EUV TOF results with Secondary Ionization Mass Spectrometry (SIMS) to orient the EUV TOF method within the overall field of analytical mass spectrometry. Using the well-characterized NIST 61x glasses, we show that the EUV ionization approach produces relatively few molecular ion interferences in comparison to TOF SIMS. We demonstrate that the ratio of element ion to element oxide ion is adjustable with EUV laser pulse energy and that the EUV TOF instrument has a sample utilization efficiency of 0.014%. The EUV TOF system also achieves a lateral resolution of 80 nm and we demonstrate this lateral resolution with isotopic imaging of closely spaced particles or uranium isotopic standard materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Gas-phase oxidation and nanoparticle formation in multi-element laser ablation plumes

The evolution from gas-phase oxidation to nanoparticle and agglomerate formation was studied in nanosecond laser-produced plasmas of a multi-principal element alloy target in air. Here gas-phase oxidation of plasma species was monitored in situ via optical emission spectroscopy, while a custom-built single particle mass spectrometer was used to measure size and compositions of agglomerated nanoparticles formed in laser ablation plumes. Ex situ analysis employing transmission electron microscopy was used to study nanoparticle morphology, crystal structure, and element distribution at the nanoscale. Emission spectra indicate that gas-phase oxidation of elements in the alloy target are formed at varying times during plume evolution, and mass spectrometry results indicate fractal agglomerates contain all principal alloying elements and their oxides. Finally, electron microscopy characterization illustrates that these agglomerates consist of multiple material types: sub-10 nm diameter amorphous, multi-element nanoparticles, ≈10–30 nm diameter Ti-rich crystalline oxide nanoparticles, and ejected base material. Results highlight that the multi-component target composition impacts molecular formation in the gas phase and the morphology, composition, and structure of nanoparticles and agglomerates formed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Informing air–carbon ablation modeling with theoretical calculations of atomic oxygen and nitrogen interacting with carbon surfaces

To understand the gas–surface chemistry above the thermal protection system of a hypersonic vehicle, it is necessary to map out the kinetics of key elementary reaction steps. In this work, extensive periodic density functional theory (DFT) calculations are performed to elucidate the interaction of atomic oxygen and nitrogen with both the basal plane and edge sites of highly oriented pyrolytic graphite (HOPG). Reaction energies and barriers are determined for adsorption, desorption, diffusion, recombination, and several reactions. These DFT results are compared with the most recent finite-rate model for air–carbon ablation. Our DFT results corroborated some of the parameters used in the model but suggest that further refinement may be necessary for others. The calculations reported here will help to establish a predictive kinetic model for the complex reaction network present under hypersonic flight conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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 OSTI2012

Spatio-temporal mapping of ablated species in ultrafast laser-produced graphite plasmas

We studied the spatial and temporal distributions of ionic, neutral, and molecular species generated by femtosecond laser produced plasma under varying ambient nitrogen gas pressures. Plasmas were generated by irradiating planar graphite targets using 40 fs pulses of 800 nm radiation from a Ti:Sapphire laser. The results show that in the presence of an ambient gas, the molecular species spatial extension and lifetime are directly correlated to the evolution of excited ions. The present studies also provide valuable insights into the evolution history of various species and their excitation during ultrafast laser ablation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2012

Comparisons of NIF convergent ablation simulations with radiograph data

A technique for comparing simulation results directly with radiograph data from backlit capsule implosion experiments will be discussed. Forward Abel transforms are applied to the kappa*rho profiles of the simulation. These provide the transmission ratio (optical depth) profiles of the simulation. Gaussian and top hat blurs are applied to the simulated transmission ratio profiles in order to account for the motion blurring and imaging slit resolution of the experimental measurement. Comparisons between the simulated transmission ratios and the radiograph data lineouts are iterated until a reasonable backlighter profile is obtained. This backlighter profile is combined with the blurred, simulated transmission ratios to obtain simulated intensity profiles that can be directly compared with the radiograph data. Examples will be shown from recent convergent ablation (backlit implosion) experiments at the NIF.

Olson, R. E.↗
DOE OSTI2012

Design of a deuterium and tritium-ablator shock ignition target for the National Ignition Facility

Shock ignition presents a viable path to ignition and high gain on the National Ignition Facility (NIF). In this paper, we describe the development of the 1D design of 0.5 MJ class, all-deuterium and tritium (fuel and ablator) shock ignition target that should be reasonably robust to Rayleigh-Taylor fluid instabilities, mistiming, and hot electron preheat. The target assumes 'day one' NIF hardware and produces a yield of 31 MJ with reasonable allowances for laser backscatter, absorption efficiency, and polar drive power variation. The energetics of polar drive laser absorption require a beam configuration with half of the NIF quads dedicated to launching the ignitor shock, while the remaining quads drive the target compression. Hydrodynamic scaling of the target suggests that gains of 75 and yields 70 MJ may be possible.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Zinc oxide based diluted magnetic semiconductor nanoparticles: Synthesis by laser ablation in liquids, microstructural and optical properties

Nanoparticles of ZnO and ZnO doped with transition metals (Mn, Co) were synthesized by laser ablation in liquid medium. Scanning electron microscopy (SEM) showed formation of nanostructures with different shapes. Atomic force microscopy (AFM) gives information about surface morphology of the formed nanostructures. Absorption edge of ZnO, ZnO:Mn and ZnO:Co colloidal nanoparticles exhibits blue shift due to confinement effect. In photoluminescence spectra three peaks are attributed to the band-edge transitions and defect states. The Faraday rotation in ZnO:Mn nanoparticles gives evidence for paramagnetic behavior at room temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Investigation of optical limiting properties of Aluminium nanoparticles prepared by pulsed laser ablation in different carrier media

In this communication, we carried out the systematic investigation of nonlinear absorption and scattering properties of Aluminium nanoparticles (Al NPs) in various polar and non-polar solvents. Al NPs were synthesized with pulsed Nd:YAG laser operated at 1064 nm by ablating Al target in polar and non-polar liquid environment like chloroform, chlorobenzene, toluene, benzene, and carbon tetrachloride. Synthesized Al NPs colloids of various solvents differ in appearance and UV-Vis extinction spectra exhibit absorption in the UV region. The characterization of Al NPs performed by Transmission electron microscopy (TEM) studies reveal that NPs are made up of a well crystallized Al inner part (bright zone) embedded with an amorphous metal Al shell (dark region). Growth, aggregation, and precipitation mechanisms which influence the optical properties and stability of NPs are found to be related to the dipole moment of the surrounding liquid environment. The nonlinear absorption and scattering studies are performed by open aperture Z-scan technique with 532 nm under nanosecond pulse excitation. The Z-scan measurements are fitted theoretically to estimate both two-photon absorption (TPA) and nonlinear scattering (NLS) coefficients. In polar solvents like chlorobenzene, chloroform synthesized Al NPs exhibited higher TPA, NLS coefficient values, and lower optical limiting threshold values in comparison with partially polar solvent like toluene and non-polar solvents like benzene and carbontetrachloride. These results indicate the potential use of Al NPs as a versatile optical limiting material.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Femtosecond laser ablation dynamics of fused silica extracted from oscillation of time-resolved reflectivity

Femtosecond laser ablation dynamics of fused silica is examined via time-resolved reflectivity measurements. After optical breakdown was caused by irradiation of a pump pulse with fluence F{sub pump} = 3.3–14.9 J/cm{sup 2}, the reflectivity oscillated with a period of 63 ± 2 ps for a wavelength λ = 795 nm. The period was reduced by half for λ = 398 nm. We ascribe the oscillation to the interference between the probe pulses reflected from the front and rear surfaces of the photo-excited molten fused silica layer. The time-resolved reflectivity agrees closely with a model comprising a photo-excited layer which expands due to the formation of voids, and then separates into two parts, one of which is left on the sample surface and the other separated as a molten thin layer from the surface by the spallation mechanism. Such oscillations were not observed in the reflectivity of soda-lime glass. Whether the reflectivity oscillates or not probably depends on the layer viscosity while in a molten state. Since viscosity of the molten fused silica is several orders of magnitude higher than that of the soda-lime glass at the same temperature, fused silica forms a molten thin layer that reflects the probe pulse, whereas the soda-lime glass is fragmented into clusters.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Direct periodic patterning of GaN-based light-emitting diodes by three-beam interference laser ablation

We report on the direct patterning of two-dimensional periodic structures in GaN-based light-emitting diodes (LEDs) through laser interference ablation for the fast and reliable fabrication of periodic micro- and nano-structures aimed at enhancing light output. Holes arranged in a two-dimensional hexagonal lattice array having an opening size of 500 nm, depth of 50 nm, and a periodicity of 1 μm were directly formed by three-beam laser interference without photolithography or electron-beam lithography processes. The laser-patterned LEDs exhibit an enhancement in light output power of 20% compared to conventional LEDs having a flat top surface without degradation of electrical and optical properties of the top p-GaN layer and the active region, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Indirect-drive ablative Rayleigh-Taylor growth experiments on the Shenguang-II laser facility

In this research, a series of single-mode, indirect-drive, ablative Rayleigh-Taylor (RT) instability experiments performed on the Shenguang-II laser facility [X. T. He and W. Y. Zhang, Eur. Phys. J. D 44, 227 (2007)] using planar target is reported. The simulation results from the one-dimensional hydrocode for the planar foil trajectory experiment indicate that the energy flux at the hohlraum wall is obviously less than that at the laser entrance hole. Furthermore, the non-Planckian spectra of x-ray source can strikingly affect the dynamics of the foil flight and the perturbation growth. Clear images recorded by an x-ray framing camera for the RT growth initiated by small- and large-amplitude perturbations are obtained. The observed onset of harmonic generation and transition from linear to nonlinear growth regime is well predicted by two-dimensional hydrocode simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Pulsed laser generation of ultrasound in a metal plate between the melting and ablation thresholds

The generation of ultrasound in a metal plate exposed to nanosecond pulsed laser heating, sufficient to cause melting but not ablation, is treated. Consideration is given to the spatial and temporal profiles of the laser pulse, penetration of the laser beam into the sample, the evolution of the melt pool, and thermal conduction in the melt and surrounding solid. The excitation of the ultrasound takes place over a few nanoseconds, and occurs predominantly within the thermal diffusion length of a micron or so beneath the surface. Because of this, the output of the thermal simulations can be represented as axially symmetric transient radial and normal surface force distributions. The epicentral displacement response at the opposite surface to these forces is obtained by two methods, the one based on the elastodynamic Green’s functions for plate geometry determined by the Cagniard generalized ray method, and the other using a finite element numerical method. The two approaches are in very close agreement. Numerical simulations are reported of the epicentral displacement response of a 3.12mm thick tungsten plate irradiated with a 4 ns pulsed laser beam with Gaussian spatial profile, at intensities below and above the melt threshold. Comparison is made between results obtained using available temperature dependent thermophysical data, and room temperature materials constants except near the melting point.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Laser-ablated loading of solid target through foams of overcritical density

The main objective of the work is to study the conversion of the laser pulse energy into the energy of the hydrodynamic motion of matter in a solid target following the initial absorption of laser radiation in a layer of porous material. Results of experiments on plane massive aluminum targets, coated with a layer of porous plastic with density greater than the critical density of the plasma created, are presented. Experiments were carried out on the laser installation ABC of the Research Center ENEA-Frascati; the targets were irradiated by a beam of the fundamental harmonic of Nd-laser radiation with an energy of about 50 kJ, intensity of 10{sup 13 }W/cm{sup 2}, and 3 ns duration. The experimental method consisted in measuring the volume of the craters created on the aluminum surface behind various thicknesses and densities of the porous absorber of laser radiation. On the basis of these measurements and of an advanced analytical model, quantitative conclusions are made on how the efficiency of laser energy transfer to the solid part of the target (laser-ablated loading) depends on thickness and density of the porous absorber.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗