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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,495 records · Page 83
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Comb-assisted subkilohertz linewidth quantum cascade laser for high-precision mid-infrared spectroscopy

We report on the linewidth narrowing of a room-temperature mid-infrared quantum cascade laser by phase-locking to a difference-frequency-generated radiation referenced to an optical frequency comb synthesizer. A locking bandwidth of 250 kHz, with a residual rms phase-noise of 0.56 rad, has been achieved. The laser linewidth is narrowed by more than 2 orders of magnitude below 1 kHz, and its frequency is stabilized with an absolute traceability of 2 Multiplication-Sign 10{sup -12}. This source has allowed the measurement of the absolute frequency of a CO{sub 2} molecular transition with an uncertainty of about 1 kHz.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

ElementLIBS User's Guide: An operational aid for use and development

Laser-Induced Breakdown Spectroscopy or LIBS is a rapid, in-situ analytical technique where a laser of known energy is pulsed at the surface of an analyte. The laser pulse rapidly heats a localized area to many thousand degrees Kelvin, ablating part of the analyte and turning it into a plasma. As the plasma cools, excited atoms return to a ground state with known emission energies. This emitted energy is captured by various spectrometers and provides a spectrum of the emitted energies and intensities. This spectrum can be analyzed to provide the elemental composition of a sample by using known emission lines and relative abundance. ElementLIBS was developed for the SciAps hand-held LIBS model Z300 but will work with any model that provides a LIBS spectrum of similar resolution. The Z300 has an integrated resolution of 1/30 nm with a range of approximately 180nm – 960nm, providing an output spectrum of 23431 pixels across three spectrometers. These criteria are only provided as a reference, as the software was designed to work with any size spectrum, provided the input file is of the correct format and the models were developed using the same framework. If spectra of varying dimensions are used, the software will fail without warning and unusual events could occur.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Measuring the Surface Photovoltage of a Schottky Barrier under Intense Light Conditions: Zn/p-Si(100) by Laser Time-Resolved Extreme Ultraviolet Photoelectron Spectroscopy

A metal-semiconductor heterojunction is investigated by Auger and photoelectron spectroscopy to characterize the structural and electronic properties of the metallic film and to obtain the time-resolved electronic response induced by femtosecond laser excitation of the semiconductor material. The 3.5 monolayer (ML) Zn films deposited on p-type Si(100) at liquid nitrogen temperature grows in a layer-by-layer fashion. Electronic structure measurements by extreme ultraviolet (XUV) photoelectron spectroscopy indicate that the films are metallic in nature, creating a Schottky barrier at the 3.5 ML Zn/p-Si(100) interface. Utilizing a 35 fs, 800 nm pump pulse at a pump intensity of (2.5-6) × 10 9 W/cm 2 to excite the Si and a time-delayed extreme ultraviolet pulse to probe the Zn, we observed large transient surface photovoltage shifts of 0.3-2.2 eV at carrier densities of (1.5-4.5) × 10 20 cm -3 . Three shifts are determined the Zn 3d core level, the photoemission onset, and the metallic Fermi level. The photovoltages increase with laser excitation intensity, and the Zn 3d core level exhibits the largest binding energy shifts due to pronounced screening of the core level. The large observed shifts are rationalized on the basis of the energetics of band flattening and carrier accumulation in the metallic layer of the Zn/p-Si(100) heterojunction at high carrier densities. The observed carrier recombination dynamics are biexponential in character, with similar time constants for both the Zn 3d and photoemission onset binding energy shifts. The Zn 3d core level shifts are also found to be sensitive to the electron temperature. These results show that core-level photoemission can be used to monitor valence electron dynamics, allowing separation of charge dynamics in heterojunctions and solids composed of multiple elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Uncertainty of Integrated Intensity Following Line Profile Fitting of Multiline Spectra

A novel method of determining the total uncertainty in the integrated intensity of fitted emission lines in multi-peaked emission spectra is presented. The proposed method does not require an assumption of the type of line profile to be specified. The absolute difference between a fit and measured spectrum defines the uncertainty of the integrated signal intensity and is subsequently decomposed to determine the uncertainty of each peak in multi-line fits. Decomposition relies on tabulating a weighting factor which describes how each peak contributes to the total integral uncertainty. Applications of this method to quantitative approaches in laser-induced breakdown spectroscopy analysis are described.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Combination of atomic lines and molecular bands for uranium optical isotopic analysis in laser induced plasma spectrometry

Through computer simulation on experimentally acquired optical spectra, uranium isotopic analysis by laser ablation molecular isotopic spectrometry and laser induced breakdown spectroscopy were studied. The use of only one spectral feature, either the strong UO band at 593.55 nm or the nearby U I 593.382 nm line, are similar in precisions (~ 1.5% in absolute 235 U abundances). Precision improves to 0.72% with the use of a group of U atomic lines from 591.6 to 596.5 nm. The use of both molecular bands and atomic lines further advances the precision to 0.42% and compares well with the U II 424.437 nm single-line benchmark (0.48% precision).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2015

Optical feedback cavity-enhanced absorption spectroscopy with a 3.24 μm interband cascade laser

The development of interband cascade lasers (ICLs) has made the strong C-H transitions in the 3 μm spectral region increasingly accessible. We present the demonstration of a single mode distributed feedback ICL coupled to a V-shaped optical cavity in an optical feedback cavity-enhanced absorption spectroscopy (OF-CEAS) experiment. We achieved a minimum detectable absorption coefficient, α{sub min}, of (7.1±0.2)×10{sup −8} cm{sup −1} for a spectrum of CH{sub 4} at 3.24 μm with a two second acquisition time (100 scans averaged). This corresponds to a detection limit of 3 ppb CH{sub 4} at atmospheric pressure, which is comparable to previously reported OF-CEAS instruments with diode lasers or quantum cascade lasers. The ability to frequency lock an ICL source in the important 3 μm region to an optical cavity holds great promise for future spectroscopic applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Enhanced sensitivity for electron affinity measurements of rare elements

The electron affinity (EA), the energy released when a neutral atom binds an additional electron, is a fundamental property of atoms that is governed by electron-electron correlations and is strongly related to an element’s chemical reactivity. However, conventional techniques for EA determination lack the experimental sensitivity to probe very scarce samples. As a result, the EA for the heaviest elements of the periodic table is entirely uncharted. Here, we present a novel technique to determine EAs through Laser Photodetachment Threshold Spectroscopy, performed in an electrostatic ion beam trap to increase the samples’ exposure to laser photons and, thus, improve the experimental signal sensitivity by three orders of magnitude. Moreover, the additional exposure time allows the use of lower-power continuous-wave narrow-band lasers that reduce uncertainties associated with broadening effects induced by the laser bandwidth. By applying this technique, we measure the EA of 35 Cl to be 3.612720(44) eV, achieving state-of-the-art precision while employing five orders of magnitude fewer anions. The demonstrated sensitivity paves the way for systematic EA measurements across isotopic chains - including isotope shifts and hyperfine splittings - and ultimately for the first direct determination of electron affinities in superheavy elements.

Maier, F. M. [Univ. of Greifswald (Germany); Europ↗
NASA NTRS1994

Spaceborne Photonics Institute

This report describes in chronological detail the development of the Spaceborne Photonics Institute as a sustained research effort at Hampton University in the area of optical physics. This provided the research expertise to initiate a PhD program in Physics. Research was carried out in the areas of: (1) modelling of spaceborne solid state laser systems; (2) amplified spontaneous emission in solar pumped iodine lasers; (3) closely simulated AM0 CW solar pumped iodine laser and repeatedly short pulsed iodine laser oscillator; (4) a materials spectroscopy and growth program; and (5) laser induced fluorescence and atomic and molecular spectroscopy.

Venable, D. D.↗
DOE OSTI2014

Infrared laser induced plasma diagnostics of silver target

In the present work, the optical emission spectra of silver (Ag) plasma have been recorded and analyzed using the laser induced breakdown spectroscopy technique. The emission line intensities and plasma parameters were investigated as a function of lens to sample distance, laser irradiance, and distance from the target surface. The electron number density (n{sub e}) and electron temperature (T{sub e}) were determined using the Stark broadened line profile and Boltzmann plot method, respectively. A gradual increase in the spectral line intensities and the plasma parameters, n{sub e} from 2.89 × 10{sup 17} to 3.92 × 10{sup 17 }cm{sup −3} and T{sub e} from 4662 to 8967 K, was observed as the laser irradiance was increased 2.29 × 10{sup 10}–1.06 × 10{sup 11} W cm{sup −2}. The spatial variations in n{sub e} and T{sub e} were investigated from 0 to 5.25 mm from the target surface, yielding the electron number density from 4.78 × 10{sup 17} to 1.72 × 10{sup 17 }cm{sup −3} and electron temperature as 9869–3789 K. In addition, the emission intensities and the plasma parameters of silver were investigated by varying the ambient pressure from 0.36 to 1000 mbars.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Control of Charge Transfer in C60–ZnO Composite Under the Influence of UV Laser Radiation by the Methods of Raman Spectroscopy and Photoluminescence

Raman and photoluminescence spectra of nanostructured ZnO films with adsorbed C60 molecules were studied. The possibility of intensive C60–ZnO electronic coupling forming in this composite was investigated. It is shown that such an electron coupling can be significantly enhanced by irradiating the composite with high intensity UV laser radiation (λ = 325 nm).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Laser Wavelength and Argon Ambient Gas Pressure Effects on Metallic Plasma Emission

The effects of laser wavelength and argon ambient gas pressure on ionic and atomic emission from aluminum and copper metal plasmas has been studied. The plasmas were generated using metal targets excited with a Q-switched Nd:YAG laser operating at the first fundamental (1064 nm), second (532 nm), third (355 nm), and fourth harmonics (266 nm) with repetition rate up to 10 Hz. The spectroscopic analysis of the plasma plume emission revealed that the intensities and signal-to-noise (S/N) ratio of various neutral and ion spectral lines, small components, and trace impurities increase sharply when the fourth laser harmonic is used at a wavelength of 266 nm. Based on LTE assumption, the electron excitation temperature (T{sub e}) and electron number density (N{sub e}) of the produced plasma have been estimated from the Boltzmann plot using neutral spectral lines of Al I at 256.8, 257.5, 309.3, and 396.15 nm and Cu I at 427.58, 510.59, 570.07, and 578.58 nm and from Stark broadening width profile of Al II at 281.6 nm and Cu I at 324.75 nm, respectively. The variations of T{sub e}, N{sub e}, and emission intensities of metals as a function of laser irradiance of different laser wavelengths at 1064, 532, 355, and 266 nm were studied. The effect of the argon ambient gas pressure on the plasma parameters was also studied. The diagnostics of the produced metal plasma was undertaken using laser induced breakdown spectroscopy (LIBS).

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

Metalloprotein structures at ambient conditions and in real-time: biological crystallography and spectroscopy using X-ray free electron lasers

We have studied the structure of enzymes and the chemistry at the catalytic sites, intensively and have acquired an understanding of the atomic-scale chemistry which requires a new approach beyond steady state X-ray crystallography and X-ray spectroscopy at cryogenic temperatures. Following the dynamic changes in the geometric and electronic structure of metallo-enzymes at ambient conditions, while overcoming the severe X-ray-induced changes to the redox active catalytic center, is key for deriving reaction mechanisms. Such studies become possible by the intense and ultra-short femtosecond (fs) X-ray pulses from an X-ray free electron laser (XFEL) by acquiring a signal before the sample is destroyed. Our review describes the recent and pioneering uses of XFELs to study the protein structure and dynamics of metallo-enzymes using crystallography and scattering, as well as the chemical structure and dynamics of the catalytic complexes (charge, spin, and covalency) using spectroscopy during the reaction to understand the electron-transfer processes and elucidate the mechanism.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

The Effect of Intensity Fluctuations on Sequential X-ray Photon Correlation Spectroscopy at the X-ray Free Electron Laser Facilities

How materials evolve at thermal equilibrium and under external excitations at small length and time scales is crucial to the understanding and control of material properties. X-ray photon correlation spectroscopy (XPCS) at X-ray free electron laser (XFEL) facilities can in principle capture dynamics of materials that are substantially faster than a millisecond. However, the analysis and interpretation of XPCS data is hindered by the strongly fluctuating X-ray intensity from XFELs. Here we examine the impact of pulse-to-pulse intensity fluctuations on sequential XPCS analysis. We show that the conventional XPCS analysis can still faithfully capture the characteristic time scales, but with substantial decrease in the signal-to-noise ratio of the g2 function and increase in the uncertainties of the extracted time constants. We also demonstrate protocols for improving the signal-to-noise ratio and reducing the uncertainties.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Spectral emission characteristics near 646 nm and plasma properties of laser-induced plasma of gaseous uranium hexafluoride

We present a detailed investigation of the temporal evolution of line and continuum emissions in laser-induced breakdown spectroscopy (LIBS) of gaseous uranium hexafluoride (UF 6 ), focusing on the spectral region near 646 nm. Spectral emission features, signal-to-background ratios (SBRs) of selected uranium lines, and spectral linewidths were examined under varying UF 6 pressures (15–60 Torr) and laser pulse energies (10–60 mJ). Higher pressures and pulse energies enhanced continuum emission and reduced SBRs but did not cause significant spectral congestion. Additional studies with the use of different laser systems, including nanosecond-pulsed Nd:YAG lasers (at fundamental and various harmonics) and a femtosecond-pulsed Ti:sapphire laser, revealed long-lived plasma continua in all cases. This persistent continuum is attributed to a pseudo-continuum from overlapping molecular emissions, as its intensity scales linearly with electron number density, deviating from the expected quadratic dependence of classical ion–electron interactions for free-free and free-bound continuum emission. Based on plasma persistence time, SBR, U II/U I intensity ratios, and electronic excitation temperature, no fundamental advantage was found for femtosecond-pulsed lasers over conventional nanosecond-pulsed ones for UF 6 enrichment assay with direct LIBS measurement.

Laser-induced breakdown spectroscopy↗
DOE OSTI2018

Final Scientific/Technical Report, Multi-Sensor Inspection and Robotic Systems for Dry Storage Casks

Once removed from service, fuel rod assemblies are cooled in a pool and then placed in dry storage until they can be transported to a repository for disposal. The extended duration that used nuclear fuel spends in dry storage makes it prudent to be able to nondestructively inspect the dry storage casks. The degradation mechanisms of most concern are chloride-induced stress corrosion cracking of the stainless steel canister that confines the spent fuel and distributed cracking of the concrete in the overpack structure. Multi-sensor inspection and robotic systems were researched, developed, built, and tested. One system operates completely outside the cask to inspect the concrete. The other system, known as the PRINSE system, for Proactive Robotic Inspection of Nuclear Storage Enclosures, enters the cask through an outlet vent and navigates around the outer surface of the stainless steel canister. The PRINSE system delivers sensors for: (i) real-time characterization of the canister surface in order to assess whether chlorides are present, (ii) detecting the presence of cracks using shear-horizontal ultrasonic guided waves, (iii) measuring the temperature of the canister surface, and (iv) a gamma radiation counter. The four sensing modalities are applicable to any cask containing a stainless steel canister, however the robotic delivery system is designed specifically for Holtec’s HI-STORM family of casks. Horizontal axis casks have exposed concrete surfaces. A fully contactless air-coupled scanning ultrasonic test platform and a frequency-wavenumber domain data analysis method are used for these concrete structures. Analysis, numerical simulation and experimental results demonstrate that distributed cracks in concrete can be detected and cracked regions localized within a scanned region of concrete. Vertical axis casks (like the HI-STORM family) have steel-clad concrete overpacks. In a separate effort, a semi-coupled test platform and a guided wave attenuation-based data analysis method are used for disbond detection. Analysis, numerical simulation and experimental results show that the bonding conditions of steel-concrete interfaces can be quantitatively characterized using the guided wave signal analysis scheme. The PRINSE system is designed for vertical axis dry storage casks, specifically the HI-STORM family. The double pulse laser-induced breakdown spectroscopy (LIBS) system takes advantage of an optical fiber to deliver intense light to the canister surface that enables surface composition characterization in-situ in real time. Chlorine concentrations as low as 10 mg/m2 were detected on stainless steel. Additionally, a simpler laser setup was created to detect sodium as a surrogate for chlorine, and sodium was detectable when the chlorine concentration was as low as 0.5 mg/m2. The electromagnetic acoustic transducers (EMATs) enable detection of stress corrosion cracks. The EMATs generate shear-horizontal waves that propagate around the canister and are reflected by cracks enabling 100% of the canister weld lines to be inspected. The EMAT-based crack detection system was tested at the Pacific Northwest National Laboratory on a canister containing blind defects and was shown to detect the crack sizes it was designed to detect. The PRINSE system is a novel marsupial robot. The command center and winch outside the cask control the delivery arm and train of cars that traverse the outside of the canister from the cask ventilation system. The sensors are housed in the cargo bays of three cars that comprise the train, which is lowered to the bottom of the canister by the winch. Encoders on the winch enable the sensors to be delivered to a prescribed location, e.g., for re-inspection of a problem area. The PRINSE system does not mar the canister surface, can be extracted manually in the case of a power failure, and is designed for an elevated temperature and gamma radiation environment, although not all components of the prototype are made from the final materials. The PRINSE system was tested on a full canister that was placed inside a HI-STORM cask at the Holtec Manufacturing Division. It was also demonstrated on a full-height mockup at Penn State to a live audience.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Selective reflection of laser radiation from submicron layers of Rb and Cs atomic vapors: Applications in atomic spectroscopy

We studied selective reflection (SR) of laser radiation from a window of a nanocell with thickness L ~ λ{sub 1,2}/2 filled with Rb and Cs atoms, where λ{sub 1} = 780 nm and λ{sub 2} = 852 nm are the wavelengths resonant with the D{sub 2} laser lines for Rb and Cs, respectively. It is demonstrated that the negative derivative of the SR signal profile for L > λ/2 changes to the positive one for L < λ/2. It is shown that the real-time formation of the SR signal profile derivative (SRD) with the spectral width 30–40 MHz and located at the atomic transition is, in particular, a convenient frequency marker of D{sub 2} transitions in Rb and Cs. The amplitudes of SRD signals are proportional to the atomic transition probabilities. A comparison with the known saturated absorption (SA) method demonstrated a number of advantages, such as the absence of cross-over resonances in the SRD spectrum, the simplicity of realization, a low required power, etc. An SRD frequency marker also operates in the presence of the Ne buffer gas at a pressure of 6 Torr, which allowed us to determine the Ne–Rb collisional broadening, whereas the SA method is already inapplicable at buffer gas pressures above 0.1 Torr. The realization simplicity makes the SRD method a convenient tool for atomic spectroscopy. Our theoretical model well describes the SRD signal.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Ultrafast Laser Welding and Terahertz Time-domain Spectroscopy of Soda Lime Silicate Glass

Joining and welding techniques of similar and dissimilar materials have reached their limits due to the inflexibility of adapting dielectric materials, e.g., glasses and ceramics, reproducibility for transparent materials, and cycle process time. The ability to join pieces of glasses using laser irradiation allows rapid processing of vacuum insulating glass (VIG) for a widening range of commercial energy-efficient applications. We have used a 1064-nm laser wavelength with 15 picoseconds pulse width and a 155-kHz repetition rate to weld commercial plate glass pieces. The welded samples were characterized via x-ray fluorescence (XRF), time-of-flight secondary ion mass spectrometry (TOF–SIMS), polarimetry, and terahertz time-domain spectroscopy (THz-TDS) to determine the integrity of the weld and chemical changes in the welded areas. Our data shows no significant changes in glass chemistry and structure on average over nano- to micro-scales occurred from the welding process within the limits of the characterization tools. Our results demonstrate successful welding of glass plates without significant changes in the glass chemistry, structure, or properties in the laser-modified region or strains in the bulk glass.

Matthies, Kathleen [ORNL] (ORCID:0009000213135441)↗
DOE OSTI2025

Comparison of atomized mass and crater volume in laser ablation

The extent and dynamics of laser ablation are typically studied using crater imaging or by invoking the relationship between atomic emission and the mass removed. The former is a static view of a dynamic process and requires the accumulation of multiple shots in one location. The latter is complex and not absolute without calibration of the optical system with a standard of spectral radiance. We measure the mass of the atomized plume by laser atomic-absorption spectroscopy at 2 µs without external mass calibration; mass uncertainty in laser-ablation atomic absorption spectroscopy (LA-AAS) results from uncertainties in line area fitting, tabulated oscillator strengths, and partition functions as well as a <10% underrepresentation of the mass due to treating the plasma as a single thermodynamic equilibrium. The LA-AAS-measured mass pertains to the atoms in the probed charge states and does not include condensed or molecular species. The ablation efficiency at 300 mbar of helium varies significantly between the two focusing conditions used. A comparison of crater-derived masses and LA-AAS masses suggests that more defocused ablation may result in significant redeposition of material in the crater, distorting the conclusions from drilling studies and crater imaging. More focused ablation conditions result in crater-derived masses that exceed those measured with LA-AAS and suggest melt expulsion or phase explosion.

Merten, Jonathan [Arkansas State University, Jones↗