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At least 775 records · Page 43

Interchange for Joint Research Entitled: Miniature Laser Spectrometer for Stable Isotope Measurements

As a first step in successfully measuring carbon isotopes optically we have previously demonstrated the measurement of C-13/C-12 to a precision of 0.1% using a tunable diode laser and CO2 spectral lines in the 2300/cm spectral region. This precision of 0.1% (1 per mil) for carbon isotopes is a value sufficiently precise to provide important isotopic data of interest to astrobiologists. The precision presently attainable in gases is sufficient to permit our instrument to be used in the measurement of isotopic ratios of interest to astrobiologists as well as geologists and planetary scientists. A small stable isotope laser spectrometer with a 10 cm path gas cell was designed and constructed. The cell was integrated with a liquid nitrogen cooled tunable diode laser and indium antimonide detector for evaluation. Using the small gas cell, preliminary measurements of 13C/12C in CO2 were made employing single-beam sequential acquisitions of the required spectral data. The results indicate an accuracy of 0.1% which is sufficiently high to make meaningful measurements of martian samples. In addition, improvements in the spectrometer gas handling system have been made to markedly reduce C-13/C-12 isotopic fractionation during sample gas cell loading which we expect will lead to further improvements in precision and accuracy. An important part of making isotopic ratio measurements in solid samples using diode lasers is the conversion of the elements of interest to molecules that have absorption spectra in the mid-ir spectral range accessible by tunable diode lasers. In this project we have investigated the necessary sample preparation procedures to extract carbon, an element of astrobiological importance, from model soil compounds and to convert it to CO2, a molecule with appropriate optical absorption characteristics for reliable laser spectrometer isotopic ratio measurements of 13C/12C. We have considered calcium carbonate as a model for a component of the martian regolith, and we have formulated a simple heating protocol for extracting carbon in the form of CO2.

Becker, J. F.↗

Local enhancement in transient absorption spectroscopy by gating the resonance in the time domain

The concept of resonant perfect absorption, enabled by the combined action of pulse propagation and an auxiliary gate pulse, was recently proposed and demonstrated in a group of two-level systems [Y. He , ]. Here we exploit this method in a more realistic scenario by solving the coupled time-dependent Schrödinger equation and the Maxwell wave equation in helium. Through emptying the population of the 1 s 2 p excited state after its excitation, we explore the evolution of the spectral profile with time delay and propagation distance and link the observations to the controlled interference between the original field and the gated new field. We find that resonant absorption for higher-lying states can also be strongly enhanced, in spite of the congestion of multiple resonances and the presence of complex laser-induced couplings. Our results show that interferometric control of absorption using intense laser fields can be applied selectively in both the temporal and spatial domains. Published by the American Physical Society 2024

He, Yu (ORCID:0000000152120176)↗

Spectral line absorption measurement using optical cavities.

A simple technique using a conventional gas laser with spherical mirrors having identical radii of curvature in the nonoscillating regime for spectral line absorption measurements is described and applications for laser work are suggested. The theory of the measurement carried out in the geometrical optical approach for Doppler-broadened lines was checked experimentally and conditions are specified for which measurement inaccuracies of the order of 1% for the peak value of the line absorption coefficient can be obtained. Since the device provides a fine adjustment of the cavity losses, formation of the diffraction modes could be observed in the preoscillating regime of the optical cavity.

Blanaru, D. L.↗

Observation and origin of multi-THz quantum beats in superfluorescent emission from argon

We report observation of multi-THz quantum beats in the amplitude of superfluorescence in pure argon gas, using a time delayed 780-nm probe beam that interrogates the relevant population densities. The superfluorescence is induced by three-photon absorption of an ultrashort 260.5-nm laser pulse that creates coherent and coupled populations in multiple closely spaced 3⁢d and 5⁢s Ar levels. Argon pressure and pump laser focusing parameters are seen to modify the frequency of the quantum beats, which is attributed to the absorption of the self-generated, nonresonant third harmonic of the pump from Ar near the zero of the real part of the overlapping linear susceptibilities of the closely spaced 3⁢d and 5⁢s excited states. The self-absorption of the phase-matched THG photons creates a coherent population of atoms which acts like an atomic excited state (3⁢ω-induced state). Furthermore, we have also observed a new two-step superfluorescent cascade that results from the population redistribution enabled by the 780-nm probe pulse between the 3⁢d'[5/2] 3 and the 3⁢ω-induced state and gives rise to a previously unknown transition that emits on 1587 nm.

74 ATOMIC AND MOLECULAR PHYSICS↗

New acousto-ultrasonic techniques applied to aerospace materials

The use of an NdYAG pulsed laser for generating ultrasonic waves for NDE in resin matrix composites was investigated. A study was conducted of the use of the 1.064 micron wavelength NdYAG pulsed laser with the neat, unreinforced resin as well as graphite fiber/polymer composite specimens. In the case of the neat resins it was found that, at normal incidence, about 25 percent of the laser pulse energy was reflected at the incident surface. An attenuation coefficient for the polyimide resin, PMR-15 was determined to be approximately 5.8 np/cm. It was found in energy balance studies that graphite fiber/polymer specimens attenuate the laser beam more than do neat resins. The increase absorption is in the graphite fibers. The occurrence of laser induced surface damage was also studied. For the polymer neat resin, damage appears as pit formation over a small fraction of the pulse impact area and discoloration over a larger part of the area. A damage threshold was inferred from observed damage as a function of pulse energy. The 600 F cured PMR-15 and PMR-11 exhibit about the same amount of damage for a given laser pulse energy. The damage threshold is between 0.06 and 0.07 J/sq cm.

Kautz, Harold E.↗

Isotope separation using metallic vapor lasers

The isotope U235 is separated from a gasified isotope mixture of U235 and U238 by selectively exciting the former from the ground state utilizing resonant absorption of radiation from precisely tuned lasers. The excited isotope is then selectively ionized by electron bombardment. It then is separated from the remaining isotope mixture by electromagnetic separation.

Russell, G. R.↗

Emission phases of implosion sources for x-ray absorption fine structure spectroscopy

At the Laboratory for Laser Energetics' Omega Laser Facility, thin plastic shells were directly driven with ∼20 kJ resulting in a time-integrated x-ray yield of ∼1012 ph/eV/sr at 7 keV. Using temporally, spatially, and spectrally discriminating diagnostics, three x-ray emission phases were identified: corona emission produced by the laser ablation of the shell, core stagnation, and afterglow emission due to the expanding hot material after stagnation. The newly measured corona and afterglow emission phases account for ∼25% of the total x-ray signal and produce x-ray emission at a different time or larger radius than previously considered. The resulting implications of this additional emission for x-ray absorption fine structure spectroscopy are discussed. Finally, improvements to the laser drive intensity and uniformity produced a factor-of-2 increase in total x-ray emission while decreasing the size of the stagnated core.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Study of x-ray fluorescence spectroscopy from high-energy-density plasmas (Final Report)

The primary objective of this subcontract was to support the development of x-ray fluorescence spectroscopy (XFS) as a diagnostic tool for high-energy-density (HED) plasmas. Several experimental campaigns were completed to develop and benchmark XFS at various plasmas conditions of interest for inertial confinement fusion and HED science. The experimental measurements at the Omega laser facility used x-ray absorption spectroscopy (XAS) to determine the plasma temperature from the shape of the K-edge to benchmark XFS data. During the course of these experiments, it was found that XAS can also constrain ionization from bound-bound absorption features, and it became a primary diagnostic in this study. Several experimental campaigns were conducted at the Omega laser facility to refine XAS and XFS measurements of warm dense copper.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Monitoring Trace Gases in the Atmosphere

Tunable laser spectrometer uses reflections from ordinary objects. Topographic target (ordinary feature of surroundings) returns enough energy to receiver so absorption by trace gases detected. Chopping laser beam allows return to be compared with original signal. Amplifier locks in on chopping frequency or laser modulation frequency. In laboratory simulations, spectrometer detected nitrogen dioxide in concentrations of only few parts per million.

Webster, C. R.↗

INPIStron switched pulsed power for dense plasma pinches

The inverse plasma switch INPIStron was employed for 10kJ/40kV capacitor bank discharge system to produce focused dense plasmas in hypocycloidal-pinch (HCP) devices. A single unit and an array of multiple HCP's were coupled as the load of the pulsed power circuit. The geometry and switching plasma dynamics were found advantageous and convenient for commutating the large current pulse from the low impedance transmission line to the low impedance plasma load. The pulse power system with a single unit HCP, the system A, was used for production of high temperature plasma focus and its diagnostics. The radially running down plasma dynamics, revealed in image converter photographs, could be simulated by a simple snow-plow model with a correction for plasma resistivity. The system B with an array of 8-HCP units which forms a long coaxial discharge chamber was used for pumping a Ti-sapphire laser. The intense UV emission from the plasma was frequency shifted with dye-solution jacket to match the absorption band of the Ti crystal laser near 500 nm. An untuned laser pulse energy of 0.6 J/pulse was obtained for 6.4 kJ/40 kV discharge, or near 103 times of the explosion limit of conventional flash lamps. For both systems the advantages of the INPIStron were well demonstrated: a single unit is sufficient for a large current (greater than 50 kA) without increasing the system impedance, highly reliable and long life operation and implied scalability for the high power ranges above I(sub peak) = 1 MA and V(sub hold) = 100 kV.

Han, Kwang S.↗

Soot Surface Oxidation in Laminar Hydrocarbon/Air Diffusion Flames at Atmospheric Pressure

Soot surface oxidation was studied experimentally in laminar hydrocarbon/air diffusion flames at atmospheric pressure. Measurements were carried out along the axes of round fuel jets burning in coflowing dry air considering acetylene-nitrogen, ethylene, propyiene-nitrogen, propane and acetylene-benzene-nitrogen in the fuel stream. Measurements were limited to the initial stages of soot oxidation (carbon consumption less than 70%) where soot oxidation occurs at the surface of primary soot particles. The following properties were measured as a function of distance above the burner exit: soot concentrations by deconvoluted laser extinction, soot temperatures by deconvoluted multiline emission, soot structure by thermophoretic sampling and analysis using Transmission Electron Microscopy (TEM), concentrations of major stable gas species (N2, H2O, H2, O2, CO, CO2, CH4, C2H2, C2H6, C3H6, C3H8, and C6H6) by sampling and gas chromatography, concentrations of some radical species (H, OH, O) by deconvoluted Li/LiOH atomic absorption and flow velocities by laser velocimetry. For present test conditions, it was found that soot surface oxidation rates were not affected by fuel type, that direct rates of soot surface oxidation by O2 estimated from Nagle and Strickland-Constable (1962) were small compared to observed soot surface oxidation rates because soot surface oxidation was completed near the flame sheet where O2 concentrations were less than 3% by volume, and that soot surface oxidation rates were described by the OH soot surface oxidation mechanism with a collision efficiency of 0.14 and an uncertainty (95% confidence) of +/- 0.04 when allowing for direct soot surface oxidation by O2, which is in reasonably good agreement with earlier observations of soot surface oxidation rates in both premixed and diffusion flames at atmospheric pressure.

Xu, F.↗

Simultaneous transmission/absorption photometry of particle-laden filters from wildland fires during the Biomass Burning Observation Project (BBOP) field campaign

Transmissivity and absorptivity measurements were carried out simultaneously in the visible (wavelength of 532 nm) at laboratory conditions using particle-laden filters obtained from a three-wavelength particle/soot absorption photometer (PSAP). Here, the particles were collected on filters from wildland fires over the Pacific Northwest during the Department of Energy Biomass Burning Observation Project (BBOP) field campaign in 2013. The objective of this investigation was to apply this measurement approach, referred to as simultaneous transmission/absorption photometry (STAP), to estimate the aerosol extinction coefficient from actual field-campaign filter aerosol, and compare results with the PSAP. The STAP approach offers several advantages over the PSAP, including estimation of the extinction coefficient from temperature measurements (avoiding the complexities associated with filter reflectivity/scattering measurements), as well as determination of the filter optical properties and filter effects on particle absorption (resulting in particle absorption enhancement). The experimental arrangement included a laser probe beam impinging normal to the particle-coated surface of a vertically mounted filter, and a thermocouple placed flush in the middle of (and in thermal contact with) the filter uncoated back surface. With this simple arrangement, the transmissivity and absorptivity were determined simultaneously at a given laser beam wavelength. The measurement repeatability was better than 0.3 K (95% confidence level) for temperature and 0.4 mW for laser power. The limit of detection for the extinction coefficient was estimated to be (8–12) Mm -1 (95% confidence level) at about 1.9 mW laser power. The extinction coefficient was determined through measurement of both PSAP blank and exposed filters. Filters were obtained from nine different aircraft flights conducted during the BBOP campaign, representing different flight patterns, days, stages of burning, landscapes, and wildland fires. The STAP extinction coefficient matched the darkness of the filter coating, however the PSAP-filter results did not follow the same order. Although there were differences in transmissivity between the two techniques, the estimated values for absorption coefficient were in good agreement.

54 ENVIRONMENTAL SCIENCES↗

AlGaAs-GaAs quantum-well lasers for direct solar photopumping

The paper theoretically examines the solar power requirements for low-threshold AlGaAs-GaAs quantum-well lasers directly photopumped by focused sunlight. A model of separate-confinement quantum-well-heterostructure (SCQWH) lasers was developed, which explicitly treats absorption and transport phenomena relevant to solar pumping. The model was used to identify separate-confinement single-quantum-well laser structures which should operate at photoexcitation intensities of less than 10,000 suns.

Unnikrishnan, Sreenath↗

Insight into the chemistry of TNT during shock compression through ultrafast absorption spectroscopies

Thin films of trinitrotoluene (TNT) were shock compressed using the ultrafast laser shock apparatus at Los Alamos National Laboratory. Visible (VIS) and mid-infrared (MIR) transient absorption spectroscopies were simultaneously performed to probe for electronic and vibrational changes during shock compression of TNT. Additionally, three shock pressures (16 GPa, 33 GPa, and 45 GPa) were selected to observe no reaction, incipient reaction, and strongly developed reactions for TNT within the experimental time scale of <250 ps. Negligible absorption changes in MIR or VIS absorptions were observed at 16 GPa. At 33 GPa, MIR absorptions in the 3000 cm -1 –4000 cm -1 range were observed to increase during the shock and continue to increase during the rarefaction, in contrast to the VIS absorption measurements, which increased during the shock and almost fully recovered during rarefaction. At 45 GPa, both VIS and MIR absorptions were strong and irreversible. The intense and spectrally broad MIR absorptions were attributed to short lived intermediates with strong, spectrally broad absorptions that dominate the spectral response. The MIR and VIS absorption changes observed at 33 GPa and 45 GPa were credited to shock induced chemistry, most likely including the formation of a very broad hydrogenic stretch feature. The results from these experiments are consistent with the chemical mechanisms that include O–H or N–H formation such as CH 3 oxidation or C–N homolysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

CO2 lasers and applications II; Proceedings of the Third European Congress on Optics, The Hague, Netherlands, Mar. 12-14, 1990

Recent advances in CO2 laser technology and its applications are examined. Topics discussed include the excitation of CO2 lasers by microwave discharge, a compact RF-excited 12-kW CO2 laser, a robotic laser for three-dimensional cutting and welding, three-dimensional CO2-laser material processing with gantry machine systems, and a comparison of hollow metallic waveguides and optical fibers for transmitting CO2-laser radiation. Consideration is given to an aerodynamic window with a pump cavity and a supersonic jet, cutting and welding Al using a high-repetition-rate pulsed CO2 laser, speckle reduction in CO2 heterodyne laser radar systems, high-power-laser float-zone crystal growth, melt dynamics in surface processing with laser radiation, laser hardfacing, surface melting of AlSi10Mg with CO2 laser radiation, material processing with Cu-vapor lasers, light-induced flow at a metal surface, and absorption measurements in high-power CW CO2-laser processing of materials.

Opower, Hans↗

Laser Infrared Desorption Spectroscopy to Detect Complex Organic Molecules on Icy Planetary Surfaces

Laser Desorption-Infrared Spectroscopy (LD-IR) uses an IR laser pulse to desorb surface materials while a spectrometer measures the emission spectrum of the desorbed materials (Figure 1). In this example, laser desorption operates by having the incident laser energy absorbed by near surface material (~10 microns in depth). This desorption produces a plume that exists in an excited state at elevated temperatures. A natural analog for this phenomenon can be observed when comets approach the sun and become active and individual molecular emission spectra can be observed in the IR [1,2,3,4,5]. When this occurs in comets, the same species that initially emit radiation down to the ground state are free to absorb it, reducing the amount of detectable emission features. The nature of our technique results in absorption not occurring, because the laser pulse could easily be moved away form the initial desorption plume, and still have better spatial resolution then reflectance spectroscopy. In reflectance spectroscopy, trace components have a relatively weak signal when compared to the entire active nature of the surface. With LDIR, the emission spectrum is used to identify and analyze surface materials.

Laser Desorption-Infrared Spectroscopy↗

Spectroscopy on the A 1 Π←X 1 Σ + Transition of Buffer-Gas Cooled AlCl

Aluminum monochloride (AlCl) has been proposed as an excellent candidate for laser cooling. Here we present absorption spectroscopy measurements on the A 1 Π←X 1 Σ + transition in AlCl inside a cryogenic helium buffer-gas beam cell. The high resolution absorption data enables a rigorous, quantitative comparison with our high-level ab initio calculations of the electronic and rovibronic energies, providing a comprehensive picture of the AlCl quantum structure. Further, the combination of high resolution spectral data and theory permits the evaluation of spectroscopic constants and associated properties, like equilibrium bond length, with an order of magnitude higher precision. Based on the measured molecular equilibrium constants of the A 1 Π state, we estimate a Franck-Condon factor of the A 1 Π←X 1 Σ + of 99.88%, which confirms that AlCl is amenable to laser cooling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Absorptivity of water vapor for 10.6 micron radiation

Attention is called to recent measurements of the absorptivity of water vapor to 10.6-micron laser radiation made using shock-heated H2O/H2 and H2O/Ar mixtures and a probe CO2 laser. It is noted that these measurements give values about a factor of 2 lower than Ludwig's (1971) low resolution values. It is also argued that Fowler's (1981) high values are not likely to be caused by excited water molecules. It is shown that very intense laser radiation would be required to obtain any appreciable vibrational nonequilibrium. Within the narrow spectral range of 944-948/cm, no significant variation in absorption coefficient (suitably normalized) is observed as a function of laser line, water vapor concentration, total pressure, or diluent gas.

Pugh, E. R.↗