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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Extraction, Characterization, and Stability Studies of Bistriazinyl-Derived Carboxylic Acids

Separation of An(III) and Ln(III) ions will benefit the recycling of used nuclear fuel (UNF). For this purpose, many ligands have been tested over the years, and several separation processes have been successfully demonstrated on the laboratory scale. Current research aims at the development of new ligands that are built only with carbon, hydrogen, oxygen, and nitrogen (CHON), as they can be incinerated completely without secondary waste production. Here, we tested a new class of water-soluble ligands, the bistriazinyl-octa-carboxylic acids. One member, in particular, 2,6-bis-[5,6-di(3,4-dicarboxyphenyl)-1,2,4- triazin-3-yl]-pyridine (BTPOA), was found to be suitable for the selective separation of Am(III) and Cm(III) ions from Ln(III) ions and may act as a CHON alternative to its sulfonated analogue (SO 3 -Ph-BTP). BTPOA exhibited good extraction results and a high selectivity for Am(III) over Eu(III) ions. This ligand’s complexation of metal ions was further studied using potentiometric spectroscopy, as well as time-resolved laser-induced spectroscopy with Cm(III) and Eu(III) in aqueous HClO 4 and HNO 3 media. Conditional stability constants of each formed species were determined. In the HClO 4 system, Cm(III) formed three species (1:1, 1:2, and 1:3) through the stepwise addition of a single BTPOA molecule. On the other hand, in HNO 3 , Cm(III) formed two 1:2 complexes and one 1:3 complex, while the stepwise formation of three species was observed for Eu(III). The stability constants are comparable to the values for SO 3 -Ph-BTP. The radiolytic behavior of BTPOA was also investigated using electron pulse irradiation measurements to determine absolute rate coefficients (k) under ambient temperature conditions for the reaction of BTPOA with typical UNF reprocessing radical radiolysis products the hydrated electron (e aq − , k = (1.60 ± 0.02) × 10 10 M −1 s −1 ), the hydrogen atom (H • , k = (2.17 ± 0.03) × 10 9 M −1 s −1 ), and hydroxyl ( • OH, k = (6.95 ± 0.06) × 10 9 M −1 s −1 ) and nitrate (NO 3 • , k = (0.37 ± 0.02) × 10 7 M −1 s−1) radicals. These rate coefficients indicate that the radiolytic longevity of BTPOA should increase with HNO 3 concentration, owing to the consumption of e aq − /H • , by nitrate anions, and the replacement of • OH by the less reactive NO 3 • .

Diaz Gomez, Laura [Forschungszentrum Juelich (Germ↗
DOE OSTI2024

Time-Resolved Probing of the Iodobenzene C-Band Using XUV-Induced Electron Transfer Dynamics

Time-resolved extreme ultraviolet spectroscopy was used to investigate photodissociation within the iodobenzene C-band. The carbon–iodine bond of iodobenzene was photolyzed at 200 nm, and the ensuing dynamics were probed at 10.3 nm (120 eV) over a 4 ps range. Two product channels were observed and subsequently isolated by using a global fitting method. Their onset times and energetics were assigned to distinct electron transfer dynamics initiated following site-selective ionization of the iodine photoproducts, enabling the electronic states of the phenyl fragments to be identified using a classical over-the-barrier model for electron transfer. In combination with previous theoretical work, this allowed the corresponding neutral photochemistry to be assigned to (1) dissociation via the 7B2, 8A2, and 8B1 states to give ground-state phenyl, Ph(X), and spin–orbit excited iodine and (2) dissociation through the 7A1 and 8B2 states to give excited-state phenyl, Ph(A), and ground-state iodine. The branching ratio was determined to be 87 ± 4% Ph(X) and 13 ± 4% Ph(A). Similarly, the corresponding amount of energy deposited into the internal phenyl modes in these channels was determined to be 44 ± 10 and 65 ± 21%, respectively, and upper bounds to the channel rise times were found to be 114 ± 6 and 310 ± 60 fs.

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

Room temperature persisting surface charge carriers driven by intense terahertz electric fields in a topological insulator Bi 2 Se 3

Topologically protected surface current is highly promising for next-generation low-dissipation and disorder-tolerant quantum electronics and computing. Yet, electric transport from the co-existing bulk state dominates the responses of the Dirac surface state, especially at elevated temperatures relevant to technological applications. Here, we present an approach that convincingly showcases the generation, disentanglement, and precise control of enduring surface charge carriers on a topological insulator, Bi 2 Se 3 , with high bulk conductivity, all achieved at room temperature. By using pump–probe modulation spectroscopy under ultrabroadband driving tunable from 4 meV to 1.55 eV, we show the terahertz (THz) field-induced surface carriers by discovering their initial temporal responses dominant over high density trivial bulk carriers. Strikingly, the response of the induced surface carrier responses persists for more than ~5 ps and is enhanced by reducing pump photon energy. The dynamics and lifetime of the distinct surface response manifest themselves as the enhanced THz pump-induced THz transmission, which directly correlates with the transient negative THz conductivity. Increasing the THz driving field reduces the induced surface carrier lifetime and identifies, particularly, an optimal pump field of E s ~ 224 kV cm -1 for generating the dominant surface response relative to the bulk. This surface carrier dominant regime is suppressed by a joint effect of enhanced surface-bulk scattering and a more rapid saturation of surface excitation compared to the bulk that sets in above E s . The controllability of room temperature topologically surface carriers through pump photon energy offer compelling possibilities for extending this approach to other topological complex materials.

36 MATERIALS SCIENCE↗
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↗
NASA NTRS1981

Ambient ammonia measurements using laser photo-acoustic spectroscopy

Ammonia concentrations reached minimal levels (approximately 0.1 ppb) in early winter, followed by a sudden later winter increase. A direct relationship between ambient ammonia levels and air temperature was inferred from the data (linear correlation coefficient r=0.53). Ammonia concentrations were determined to be directly related to the absolute humidity of the air (r=0.72); a weaker relationship between ammonia concentrations and relative humidity was discovered (r=0.37). The data also indicated that ammonia levels were generally higher within continental air masses than those of maritime origin. Soil parameters such as pH and moisture content were found to have a major bearing on the release of gaseous ammonia from soils in the region.

Aldridge, M. D., III↗
NASA NTRS1982

High resolution atmospheric spectroscopy using a diode laser heterodyne spectrometer

Ultrahigh resolution (0.007 per cm) atmospheric solar absorption spectra that have been obtained from a tunable infrared heterodyne radiometer are discussed. The radiometer was developed for ground based observations in the 8-12 micron region, and tunability is achieved through the use of Pb-salt semiconductor laser local oscillators. Spectra have been obtained in a piecewise fashion from 9.1 to 11.1 microns using laser emission modes that exhibit characteristics suitable for local-oscillator operation. Spectra showing absorption features of HNO3, O3, CO2, and H2O are presented along with comparisons of experimental and synthetic spectra calculated using a line-by-line atmospheric transmission model.

Hoell, J. M., Jr.↗
NASA NTRS1988

Spectroscopy and diode laser-pumped operation of Tm, Ho:YAG

Spectroscopic measurements and analysis of diode laser-pumped operation of Tm, Ho:YAG at 2.1 microns at room temperature have been performed. The peak effective stimulated emission cross section is measured to be 9 x 10-21 sq cm at 2.091 microns and the upper state lifetime is 8.5 ms. Under diode laser pumping, thresholds of 4.4 mW of absorbed power and slope efficiency of 19 percent have been demonstrated. Calculations of threshold power are performed based on the spectroscopic measurements. An energy transfer upconversion process is identified which leads to a sublinear rise in upper-state population with pump power.

Fan, Tso Yee↗
NASA NTRS1996

An Integrated Approach to Laser Crystal Development

Norfolk State University has developed an integrated research program in the area of laser crystal development, including crystal modeling, crystal growth, spectroscopy, and laser modeling. This research program supports a new graduate program in Chemical Physics, designed in part to address the shortage of minority scientists.

Ries, Heidi R.↗
NASA NTRS1994

Spectroscopy of Solid State Laser Materials

We retrieved the vertical distribution of ozone from a series 0.005-0.013/cm resolution infrared solar spectra recorded with the McMath Fourier Transform spectrometer at the Kitt Peak National Solar Observatory. The analysis is based on a multi-layer line-by-line forward model and a semi-empirical version of the optimal estimation inversion method by Rodgers. The 1002.6-1003.2/cm spectral interval has been selected for the analysis on the basis of synthetic spectrum calculations. The characterization and error analysis of the method have been performed. It was shown that for the Kitt Peak spectral resolution and typical signal-to-noise ratio (greater than or equal to 100) the retrieval is stable, with the vertical resolution of approximately 5 km attainable near the surface degrading to approximately 10 km in the stratosphere. Spectra recorded from 1980 through 1993 have been analyzed. The retrieved total ozone and vertical profiles have been compared with total ozone mapping spectrometer (TOMS) satellite total columns for the location and dates of the Kitt Peak Measurements and about 100 ozone ozonesoundings and Brewer total column measurements from Palestine, Texas, from 1979 to 1985. The total ozone measurements agree to +/- 2%. The retrieved profiles reproduce the seasonally averaged variations with altitude, including the ozone spring maximum and fall minimum measured by Palestine sondes, but up to 15% differences in the absolute values are obtained.

Buoncristiani, A. M.↗
NASA NTRS1998

The Identification of Complex Organic Molecules in the Interstellar Medium: Using Lasers and Matrix Isolation Spectroscopy to Simulate the Interstellar Environment

The Astrochemistry Group at NASA Ames Research Center is interested in the identification of large organic molecules in the interstellar medium Many smaller organic species (e.g. hydrocarbons, alcohols, etc.) have been previously identified by their radiofrequency signature due to molecular rotations. However, this becomes increasingly difficult to observe as the size of the molecule increases. Our group in interested in the identification of the carriers of the Diffuse Interstellar Bands (absorption features observed throughout the visible and near-infrared in the spectra of stars, due to species in the interstellar medium). Polycyclic Aromatic Hydrocarbons (PAHs) and related molecules are thought to be good candidates for these carriers. Laboratory experiments am performed at Ames to simulate the interstellar environment, and to compare spectra obtained from molecules in the laboratory to those derived astronomically. We are also interested in PAHs with respect to their possible connection to the UIR (Unidentified infrared) and ERE (Extended Red Emission) bands - emission features found to emanate from particular regions of our galaxy (e.g. Orion nebula, Red Rectangle, etc.). An old, "tried and proven spectroscopic technique, matrix isolation spectroscopy creates molecular conditions ideal for performing laboratory astrophysics.

Stone, Bradley M.↗
NASA NTRS2010

Dual Wavelength Lasers

Dual wavelength lasers are discussed, covering fundamental aspects on the spectroscopy and laser dynamics of these systems. Results on Tm:Ho:Er:YAG dual wavelength laser action (Ho at 2.1 m and Er at 2.9 m) as well as Nd:YAG (1.06 and 1.3 m) are presented as examples of such dual wavelength systems. Dual wavelength lasers are not common, but there are criteria that govern their behavior. Based on experimental studies demonstrating simultaneous dual wavelength lasing, some general conclusions regarding the successful operation of multi-wavelength lasers can be made.

Walsh, Brian M.↗
NASA NTRS2015

Development of a Sodium LIDAR for Spaceborne Missions

We are currently developing laser and electro-optic technologies to remotely measure Sodium (Na) by adapting existing lidar technology with space flight heritage. The developed instrumentation will serve as the core for the planning of a Heliophysics mission targeted to study the composition and dynamics of Earths mesosphere based on a spaceborne lidar that will measure the mesospheric Na layer. There is a pressing need in the Ionosphere Thermosphere - Mesosphere (ITM) community for high-resolution measurements that can characterize small-scale dynamics (i.e. Gravity Waves with wavelengths smaller than a few hundred km) and their effects in the Mesosphere-Lower-Termosphere (MLT) on a global basis. This is compelling because they are believed to be the dominant contributors to momentum transport and deposition in the MLT, which largely drive the global circulation and thermal structure and interactions with the tides and planetary waves in this region. We are developing a spaceborne remote sensing technique that will enable acquisition of global Na density, temperature and wind measurements in the MLT with the spatial and temporal resolution required to resolve issues associated with the structure, chemistry, dynamics, and energetics of this regionA nadir-pointing spaceborne Na Doppler resonance fluorescence LIDAR on board of the ISS will essentially make high-resolution, in time and space, Na density, temperature and vertical wind measurements, from 75-115 km (MLT region). Our instrument concept consisted of a high-energy laser transmitter at 589 nm and highly sensitive photon counting detector that allows for range-resolved atmospheric-sodium-temperature profiles. The atmospheric temperature is deduced from the linewidth of the resonant fluorescence from the atomic sodium vapor D2 line as measured by our tunable laser. We are currently developing a high power energy laser that allows for some day time sodium lidar observations with the help of a narrow bandpass filter based on etalon or atomic sodium Faraday filter with 5 to 10 pm optical bandwidth. The current baseline detector for the lidar instrument is a 16-channel Photomultiplier Tube with receiver electronics that has been space-qualified for the ICESat-2ATLAS mission. Our technique uses the 16-channels as a photon-number-resolving single detector to provide the required full-spectroscopic sodium lineshape waveform for recovering Mesospheric temperature profiles. In this paper, we will describe our instrument concept for a future Heliophysics space mission based on board of the International Space Station (ISS).

lidar↗
NASA NTRSDate not supplied

Examination of Mars2020 Shock-Layer Conditions Via Infrared Emission Spectroscopy of CO2

A new test series was performed in the Electric Arc Shock Tube (EAST) facility, with the aim of reproducing flight conditions encountered during the Mars2020 mission entry into Mars atmosphere. For this test series, the EAST facility was instrumented with two spectrometers for Optical Emission Spectroscopy (OES) measurements and three mid-infrared lasers for Tunable Diode Laser Absorption Spectroscopy (TDLAS). This study focuses on the spectrally and spatially resolved radiance measured with OES. Comparison with CEA/NEQAIR and DPLR/NEQAIR simulations were made. For velocity above 2.7 km/s, measurements are found to lie between the different tested kinetic models, within ± 10%. Below 2.7 km/s, the chemistry appears to be frozen and measured radiance profiles are typically 10% above CEA predictions. This difference is explained by shock deceleration effects. Finally, comparison between OES and TDLAS data are made and show a good agreement on the measured temperature and CO2 number density profiles using the two diagnostics, typically within 10 and 5%, respectively.

Augustin C Tibere-Inglesse↗
NASA NTRSDate not supplied

Examination of Mars2020 Shock-Layer Conditions Via Infrared Emission Spectroscopy of CO2

A new test series was performed in the Electric Arc Shock Tube (EAST) facility, with the aim of reproducing flight conditions encountered during the Mars2020 mission entry into Mars atmosphere. For this test series, the EAST facility was instrumented with two spectrometers for Optical Emission Spectroscopy (OES) measurements and three mid-infrared lasers for Tunable Diode Laser Absorption Spectroscopy (TDLAS). This study focuses on the spectrally and spatially resolved radiance measured with OES. Comparison with CEA/NEQAIR and DPLR/NEQAIR simulations were made. For velocity above 2.7 km/s, measurements are found to lie between the different tested kinetic models, within ± 10%. Below 2.7 km/s, the chemistry appears to be frozen and measured radiance profiles are typically 10% above CEA predictions. This difference is explained by shock deceleration effects. Finally, comparison between OES and TDLAS data are made and show a good agreement on the measured temperature and CO2 number density profiles using the two diagnostics, typically within 10 and 5%, respectively.

Augustin Tibère-Inglesse↗
NASA NTRS1995

Scramjet Performance Assessment Using Water Absorption Diagnostics (U)

Simultaneous multiple path measurements of temperature and H2O concentration will be presented for the AIMHYE test entries in the NASA Ames 16-Inch Shock Tunnel. Monitoring the progress of high temperature chemical reactions that define scramjet combustor efficiencies is a task uniquely suited to nonintrusive optical diagnostics. One application strategy to overcome the many challenges and limitations of nonintrusive measurements is to use laser absorption spectroscopy coupled with optical fibers. Absorption spectroscopic techniques with rapidly tunable lasers are capable of making simultaneous measurements of mole fraction, temperature, pressure, and velocity. The scramjet water absorption diagnostic was used to measure combustor efficiency and was compared to thrust measurements using a nozzle force balance and integrated nozzle pressures to develop a direct technique for evaluating integrated scramjet performance. Tests were initially performed with a diode laser tuning over a water absorption feature at 1391.7 nm. A second diode laser later became available at a wavelength near 1343.3 nm covering an additional water absorption feature and was incorporated in the system for a two-wavelength technique. Both temperature and mole fraction can be inferred from the lineshape analysis using this approach. Additional high temperature spectroscopy research was conducted to reduce uncertainties in the scramjet application. The lasers are optical fiber coupled to ports at the combustor exit and in the nozzle region. The output from the two diode lasers were combined in a single fiber, and the resultant two-wavelength beam was subsequently split into four legs. Each leg was directed through 60 meters of optical fiber to four combustor exit locations for measurement of beam intensity after absorption by the water within the flow. Absorption results will be compared to 1D combustor analysis using RJPA and nozzle CFD computations as well as to data from a nozzle metric balance measuring thrust and integrated pressure measurements along the length of the nozzle. Assessment of its value as a combustor performance evaluation tool will be conducted.

Cavolowsky, John A.↗
DOE OSTI2025

In Situ Spectroscopic Monitoring of MSR Molten Salt and Off-Gas Systems

A significant challenge that must be overcome before commercialization of molten salt reactors is tracking special nuclear material (SNM) through the reactor and subsystems such as fuel chemical processing and off-gas systems. In recent years, several approaches have been explored to track SNM, fission products, and corrosion products in these different subsystems. One such approach is to employ laser and optical spectroscopy to measure the atomic and molecular signals of MSR salts. The advantages of these approaches are that they typically are non-intrusive and offer the capability of process monitoring while still providing low uncertainties. At the Idaho National Laboratory, spectroscopy approaches such as laser-induced breakdown spectroscopy (LIBS) and ultraviolet-visible (UV-Vis) spectroscopy have been utilized to investigate molten salts in an aerosol (LiCl, KCl, RbCl2, NdCl3, and PrCl3) and vapor phases (MgCl5, NdCl5, and ZrCl4) with success. Testing to date has yielded qualitative information on all the above species and quantitative data and analytical figures of merit for species in the vapor phases. These findings, including results from ongoing testing, as well as the experimental conditions and potential applications will be presented.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗
DOE OSTI2023

LIBS Applications to Liquids and Solids in Liquids

In this chapter, LIBS instrumentation and data collection system used for the analysis of liquids and solids in liquids are discussed. LIBS measurements of bulk liquid samples and solids submerged in aqueous media, measurements made by focusing laser pulses on liquid surfaces, and measurements of liquids after various sample treatments are presented. In addition, the working mechanism of NETL‐developed field‐deployable LIBS sensor and its preliminary performance in field measurements are also reported.

atomic emission spectroscopy↗