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At least 37 records · Page 2

CIV Vacuum Ultraviolet Fabry-Perot Interferometers for Transition-Region Magnetography

The vacuum ultraviolet region allows remote sensing of the upper levels of the solar atmosphere where the magnetic field dominates the physics. Obtaining an imaging interferometer that observes the transition region is the goal of this program. This paper gives a summary of our instrument development program (1998-2005) for a high-spectral-resolution, piezoelectric tunable Vacuum Ultraviolet Fabry-Perot Interferometer (VUV FPI) for obtaining narrow-passband images, magnetograms, and Dopplergrams of the transition region emission line of CN (155nm). A VUV interferometer will allow us to observe the magnetic field, flows, and heating events in the mid-transition region. The MSFC VUV FPI has measured values of FWHM approx. 9pm, FSR approx. 62pm, finesse approx. 5.3 and transmittance approx. 50% at 157nm. For the measurements, the University of Toronto's F2 eximer laser was used as an appropriate proxy for CIV 155nm. This has provided the first tunable interferometer with a FWHM compatible to VUV filter magnetograph.

Gary, G. Allen↗

Table-Top High Photon Energy Sources for Chemical Dynamics Investigations

Time-resolved spectroscopies using high-energy photons in the vacuum ultraviolet (VUV) to the X-ray region of the electromagnetic spectrum, have proven to be powerful probes of chemical dynamics. These high-energy photons can access valence and core orbitals of molecules and materials, providing key information on molecular and electronic structure and their time evolution. This report details the development of table-top sources of extreme ultraviolet (XUV) and VUV pulses at Sandia National Laboratories for use in studies of gas phase chemical dynamics. Femtosecond duration XUV pulses are produced using laser-driven high harmonic generation and their detected range span ~40-140 eV photon energies. These pulses are used in conjunction with ultraviolet pulses in a pump-probe scheme to study excited state dynamics of gas phase molecules. VUV pulses at 7.75 eV are generated using a four-wave-mixing scheme driven by 800 nm and 266 nm pulses in an argon-filled hollow-core fiber.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Laser-based conversion electron Mössbauer spectroscopy of 229 ThO 2

The exceptionally low-energy 229 Th nuclear isomeric state is expected to provide several new and powerful applications, including the construction of a robust and portable solid-state nuclear clock, perhaps contributing to a redefinition of the second, exploration of nuclear superradiance and tests of fundamental physics. Further, analogous to the capabilities of traditional Mössbauer spectroscopy, the sensitivity of the nucleus to its environment can be used to realize laser Mössbauer spectroscopy and, with it, new types of strain and temperature sensors and a new probe of the solid-state environment, all with excellent sensitivity. However, current models for examining the nuclear transition in a solid require the use of a high-bandgap, vacuum ultraviolet (VUV) transmissive host, severely limiting the applicability of these techniques. Here we report the first, to the authors’ knowledge, demonstration of laser-induced conversion electron Mössbauer spectroscopy (CEMS) of the 229 Th isomer in a thin ThO 2 sample whose bandgap (approximately 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). Unlike fluorescence spectroscopy of the 229 Th isomeric transition, this technique is compatible with materials whose bandgap is less than the nuclear transition energy, opening a wider class of systems to study and the potential of a conversion-electron-based nuclear clock.

36 MATERIALS SCIENCE↗

Thermal and Catalytic Decomposition of 2-Hydroxyethylhydrazine and 2-Hydroxyethylhydrazinium Nitrate Ionic Liquid

To develop chemical kinetics models for the combustion of ionic liquid-based monopropellants, identification of the elementary steps in the thermal and catalytic decomposition of components such as 2-hydroxyethylhydrazinium nitrate (HEHN) is needed but is currently not well understood. The first decomposition step in protic ionic liquids such as HEHN is typically the proton transfer from the cation to the anion, resulting in the formation of 2-hydroxyethylhydrazine (HEH) and HNO 3 . In the first part of this investigation, the high-temperature thermal decomposition of HEH is probed with flash pyrolysis (<1400 K) and vacuum ultraviolet (10.45 eV) photoionization time-of-flight mass spectrometry (VUV-PI-TOFMS). Next, the investigation into the thermal and catalytic decomposition of HEHN includes two mass spectrometric techniques: (1) tunable VUV-PI-TOFMS (7.4-15 eV) and (2) ambient ionization mass spectrometry utilizing both plasma and laser ionization techniques whereby HEHN is introduced onto a heated inert or iridium catalytic surface and the products are probed. The products can be identified by their masses, their ionization energies, and their collision-induced fragmentation patterns. Further, formation of product species indicates that catalytic surface recombination is an important reaction process in the decomposition mechanism of HEHN. The products and their possible elementary reaction mechanisms are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultralow Energy Electron Attachment at Sub-Millielectron Volt Resolution

The technique of rare-gas photoionization has been extended by use of direct laser ionization to electron energies epsilon in the range 0-100 meV, with a resolution Delta(epsilon) of 0.4-0.5 meV (FWHM). Tunable UV light at (Lambda)276 nm is produced using a pulsed Nd:YAG laser and nonlinear mixing techniques. The beam is frequency tripled in a pulsed jet of xenon. The VUV radiation, tunable at (Lambda)92 nm, is then used to photoionize Xe at its 2P(sub 1/2) threshold (single-photon ionization). The photoelectrons produced interact with admixed target gas to generate negative ions through the s-wave capture process. Recent results in electron attachment to SF(sub 6) will be reported which show resonance structure at the opening of the ground-state vibrational channels. This structure corresponds to the process of vibrational excitation + attachment, which is superimposed on the underlying s-wave (direct) capture process. It should be a general phenomenon, present in a wide variety of zero-energy electron attaching molecules.

Chutjian, A.↗

Tunable VUV photofragment monochromator

A versatile tunable VUV photofragment monochromator is described. The instrument uses a unique flashlamp and a single slit monochromator to produce the photofragments. A tunable dye laser is used to detect these fragments via laser induced fluorescence. The results of preliminary design parameter measurements are presented along with the first photofragment spectra obtained with this instrument. It is shown that the SNR is adequate to assign single quantum state photofragment distributions.

Miller, G. E.↗

Characterization of CO Thermochemistry in Incident Shockwaves

Incident shock waves in pure CO have been characterized in the Electric Arc ShockTube facility at NASA Ames Research Center. Spectrally and spatially resolved emissionspectra characterize radiative signatures from CO in the VUV and mid-infrared and atomiccarbon and C2 in the visible. CO absorption of a single vibrational line is also measuredwith a tunable diode laser. The experimental data analyzed here are at a pressure of 0.25Torr in the driven section and span a shock velocity range from 3.4-9.5 km/s. The emissionand absorption signals are analyzed to extract temperature relaxation behind the shockwhich is used to derive the rate of CO dissociation. The emission spectra are compared toresults using different kinetic parameters for CO dissociation and C2 dissociation andexchange. Different rates from the literature are found to match the data from 3.4-6.6 km/sand 6.6-9.5 km/s. Areas for improvement in CO and C2 radiation modeling are suggested onthe basis of the analysis.

CO↗

Characterization of CO Thermochemistry in Incident Shockwaves

Incident shock waves in pure CO have been characterized in the Electric Arc Shock Tube facility at NASA Ames Research Center. Spectrally and spatially resolved emission spectra characterize radiative signatures from CO in the VUV (Vacuum Ultra-Violet) and mid-infrared and atomic carbon and C2 in the visible. CO absorption of a single vibrational line is also measured with a tunable diode laser. The experimental data analyzed here are at a pressure of 0.25 Torr in the driven section and span a shock velocity range from 3.4-9.5 km/s. The emission and absorption signals are analyzed to extract temperature relaxation behind the shock which is used to derive the rate of CO dissociation. The emission spectra are compared to results using different kinetic parameters for CO dissociation and C2 dissociation and exchange. Different rates from the literature are found to match the data from 3.4-6.6 km/s and 6.6-9.5 km/s. Areas for improvement in CO and C2 radiation modeling are suggested on the basis of the analysis.

Entry↗

Quantum efficiency measurements for several waveshifter coatings in the extreme vacuum ultraviolet

Quantum efficiency measurements are given for coronene and liumogen coatings designed to enhance UV sensitivity for silicon charge coupled device imaging detectors. Coatings on quartz and on UDT PIN 10DP photodiodes were tested. The wavelength range extended from 153.7 to 50.0 nm in the vacuum ultraviolet. Similar measurements were made for coronene, liumogen, and stilbene-3 laser dye films on quartz disks relative to sodium salicylate. Sodium salicylate and coronene are the most efficient waveshifters down to 50 nm so far observed. Coronene's fairly constant quantum efficiency over such a wide wavelength range into the far VUV makes it a useful waveshifter for UV and VUV applications.

Butner, C. L.↗

Ultraviolet /UV/ sensitive phosphors for silicon imaging detectors

The fluorescence properties of UV sensitive organic phosphors and the radiometric properties of phosphor coated silicon detectors in the VUV, UV, and visible wavelengths are described. With evaporated films of coronene and liumogen, effective quantum efficiencies of up to 20% have been achieved on silicon photodiodes in the vacuum UV. With thin films of methylmethacrylate (acrylic), which are doped with organic laser dyes and deposited from solution, detector quantum efficiencies of the order of 15% for wavelengths of 120-165 nm and of 40% for wavelengths above 190 nm have been obtained. The phosphor coatings also act as antireflection coatings and thereby enhance the response of coated devices throughout the visible and near IR.

Viehmann, W.↗

Dynamics of Product Branching from Radical Intermediates in Elementary Combustion Reactions (Final Technical Report)

While the total rate constant for many elementary reactions is well-characterized, understanding the product branching in complex reactions presents a formidable challenge. To gain an incisive probe of such reactions, our experiments investigate the dynamics of the product channels that arise from transient radical intermediates along the bimolecular reaction coordinates. Our recent published work uses the methodology developed in my group in the last fifteen years, using both imaging and scattering apparatuses. The experiments generate a particular isomeric form of an unstable radical intermediate along a bimolecular reaction coordinate and study the branching between the ensuing product channels of the energized radical as a function of its internal rotational and vibrational energy under collision-less conditions. The experiments use a combination of: 1) measurement of product velocity and angular distributions in a crossed laser-molecular beam apparatus, with electron bombardment detection in my lab in Chicago or 2) with tunable vacuum ultraviolet photoionization detection at Taiwan's National Synchrotron Radiation Research Center (NSRRC), and 3) velocity map imaging using state-selective REMPI and single photon VUV ionization of radical intermediates and reaction products. We also employ tunable VUV photoionization detection in our imaging apparatus, using difference frequency four-wave mixing to produce photoionization light tunable from 8 to 10.8 eV. This year of support funded our work to photolytically generate the radical intermediate important in the OH + propene reaction when OH adds to an end carbon. Our other major result this past year was on the photoionization detection of vinoxy radicals. Our experiments at the NSRRC definitively show that vinoxy dissociatively ionizes to both CH 3 + and HCO + , and establishes the absolute partial photoionization cross section of vinoxy to CH 3 + at 10.5 and 11.44 eV. This should allow experimentalists detecting vinoxy radicals produced in bimolecular reactions such as OH + propene to get good branching fractions to that product channel. Finally we initiated studies of the photodissociation of 1-bromo-2-chloroethane and 1,1-bromochloroethane at 193 nm at the NSRRC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High temperature UF6 and plasma research

Research currently under way on technology for uranium plasma core reactors is reviewed. A feeder system to provide a controlled and steady flow of UF6 at rates up to 5 g/sec and temperatures up to 500 K into rf plasma test chambers operating at pressures of up to 20 atm has been developed. Plasma emission and dye laser absorption measurements have been used to estimate the radial distribution of uranium atom number density within the plasma. X-ray absorption equipment and techniques have also been employed to measure the amount of uranium in the plasma, and dc plasma torch experiments have shown variations in plasma VUV emission with temperature. Analysis of residues deposited on various test-chamber components after plasma tests reveals traces of several uranium oxides, including UO2F2, and various exhaust duct configurations with flow augmentation are under investigation as means of preventing uranium deposition. Other areas of research include off- and on-line exhaust gas diagnostics, and a UF6/Ar injection, separation and recirculation system.

Roman, W. C.↗

Efficient lasing in mixtures of helium and fluorine in diffuse discharges formed by runaway electrons

The parameters of stimulated lasing in diffuse discharges formed in mixtures of helium and fluorine in a strongly inhomogeneous electric field are investigated. Lasing is obtained in the visible and VUV spectral regions on the transitions of fluorine atoms and molecules. It is shown that lasing in He – F{sub 2} mixtures at a wavelength of 157 nm continues for several half-periods of the discharge current. Due to the homogeneity of the diffuse discharge, the maximum lasing efficiency of the F{sub 2} laser is 0.15 %, which corresponds to the efficiency of this type of lasers pumped by pre-ionised transverse volume discharges. (paper)

74 ATOMIC AND MOLECULAR PHYSICS↗

Raman-shifting an ArF excimer laser to generate new lines for obtaining optical diagnostic based information in flow fields

The application of tunable excimer lasers in combustion and flow diagnostics is almost routine nowadays. The properties of this laser system that enable density and temperature measurements in supersonic and hypersonic flow fields to be conducted are its high power, high repetition rate, and high spectral brightness. The limitation imposed by this system on these measurements is the paucity of lines in the wavelength region, the vacuum-ultraviolet, where species of interest, such as OH, N2, O2, H2, H2O, CO, NO, etc., are susceptible to electronic excitation to high-lying states. To circumvent this problem one normally resorts to nonlinear optical techniques such as frequency conversion via stimulated Raman scattering (SRS), more commonly known as Raman shifting or Raman mixing, to extend these nonintrusive and nonperturbing techniques to the shorter wavelengths in the VUV region and, for that matter, to longer wavelengths in the infrared region, if the need arises. The theoretical basis of SRS and its application are well documented in the literature. In essence, the Raman shift is a consequence of the inelastic scattering of the incident radiation by the sample. Most of the scattered radiation from the molecules of the sample is unchanged in frequency. However, a small fraction of the incident radiation is changed in frequency. This shift is a result of the fact that some of the incident photons on colliding with the molecules of the sample give up some of their energy and emerge with a lower energy resulting in the lower-frequency Stokes radiation. Other incident photons may increase their energy by colliding with the vibrationally excited molecules of the medium and emerge as higher-frequency antistokes radiation. The generation of the latter is the main objective of this project. The process, however, depends on several factors, including the beam quality of the pump laser, the cross-section of the gaseous medium, the gas pressure, and the ambient temperature of the gas near the focal region. Furthermore, since the Raman shifting process is polarization sensitive, it is necessary to have all of the laser energy in a single polarization. These factors were taken into consideration in the execution of the project. The implementation of the Raman shift was accomplished by focusing the 193 nm output of an ArF excimer laser (Lamda-Physik LPX 150) into a 1-meter long high pressure recirculating Raman cell filled with H2 gas. The laser system was modified in order to improve the mode quality of the pump beam to enhance the Raman shifting. To accomplish this feat, a prism beam expander and grating on the oscillator discharge provided wavelength tuning over the excimer gain profile. Furthermore, a triple-pass configuration, as opposed to unstable resonator optics, was employed in the operation of the amplifier cavity so that when the oscillator output radiation, focused by a 51-cm focal length fused silica lens through a 50 micron pinhole (serving as a spatial filter) and recollimated with a 25-cm focal length lens, was fed into the amplifier, it was injection locked, thereby providing tunable radiation with relatively low divergence. The forward scattered radiation emanating from the impingement of the modified pump beam on the Raman cell was detected using an energy meter after the latter had been separated from it using a dispersing prism.

Koker, Edmond B.↗

Dependence of the impurity transport on the dominant turbulent regime in ELM-y H-mode discharges on the DIII-D tokamak

Laser blow-off injections of aluminum and tungsten have been performed on the DIII-D tokamak to investigate the variation of impurity transport in a set of dedicated ion and electron heating scans with a fixed value of the external torque. The particle transport is quantified via the Bayesian inference method, which, constrained by a combination of a charge exchange recombination spectroscopy, soft X-ray measurements, and VUV spectroscopy provides a detailed uncertainty quantification of transport coefficients. Contrasting discharge phases with a dominant electron and ion heating reveal 3-fold drop in the impurity confinement time and order of magnitude increase in midradius impurity diffusion, when additional electron heating is applied. Further, the calculated stationary aluminum density profiles reverse from peaked in electron heated to hollow in the ion heated case, following a similar trend as electron and carbon density. Comparable values of a core diffusion have been observed for W and Al ions, while differences in the propagation dynamics of these impurities are attributed to pedestal and edge transport. Modeling of the core transport with non-linear gyrokinetics code CGYRO, significantly underpredicts the magnitude of the variation in Al transport. Diffusion increases 3-times steeper with additional electron heat flux and 10-times lower diffusion is observed in ion heated case than predicted by the modeling. Here, the CGYRO model quantitatively matches the increase of the Al diffusion when approaching the linear threshold for the transition from the ion temperature gradient (ITG) to trapped electron mode (TEM).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Laboratory Studies of Thermal Energy Charge Transfer of Multiply Charged Ions in Astrophysical Plasmas

The laser ablation/ion storage facility at the UNLV Physics Department has been dedicated to the study of atomic and molecular processes in low temperature plasmas. Our program focuses on the charge transfer (electron capture) of multiply charged ions and neutrals important in astrophysics. The electron transfer reactions with atoms and molecules is crucial to the ionization condition of neutral rich photoionized plasmas. With the successful deployment of the Far Ultraviolet Spectroscopic Explorer (FUSE) and the Chandra X-ray Observatory by NASA high resolution VUV and X-ray emission spectra fiom various astrophysical objects have been collected. These spectra will be analyzed to determine the source of the emission and the chemical and physical environment of the source. The proper interpretation of these spectra will require complete knowledge of all the atomic processes in these plasmas. In a neutral rich environment, charge transfer can be the dominant process. The rate coefficients need to be known accurately. We have also extended our charge transfer measurements to KeV region with a pulsed ion beam. The inclusion of this facility into our current program provides flexibility in extending the measurement to higher energies (KeV) if needed. This flexibility enables us to address issues of immediate interest to the astrophysical community as new observations are made by high resolution space based observatories.

Kwong, Victor H. S.↗

Laboratory studies of photodissociation processes relevant to the formation of cometary radicals

The strength of the C2(d 3 Pi g yields a 3 Pi u) Swan band emission in the spectra of cometary comae identifies this species as a prominent constituent of the coma gas. It was previously suggested that the formation of cometary C2 proceeds via the secondary photolysis of the C2H radical. The detection of C2H in the interstellar medium and the recent analysis of the radial variation in C2(delta V=O) surface brightness of Comet Halley support the postulate that C2 is a third-generation molecule. Measurement of the C2 and C2H translational energy distributions produced from the multiphoton dissociation (MPD) of acetylene at 193 nm are identified . Time-resolved FTIR emission studies of the nascent C2H radical formed in the C2H2 yields C2H + H reaction verify that this species is produced both vibrationally and electronically excited. A survey of the internal energy distributions of the C2 fragments produced from the MPD of acetylene using a high intensity ArF laser is currently in progress in the laboratory. Recent experiments have focused on the measurement of rotational energy distribution for the C2(A 1 Pi u, a 3 Pi u) fragments. The C2(a 3 Pi u) detection capability is currently being improved by performing this experiment in a molecular beam, thus allowing for discrimination between initial emission and laser-induced fluorescence (LIF). Although the experiments performed to date provide considerable evidence in support of C2H yields C2 + H reaction, there is an important distinction to be made when comparing the laboratory conditions to those typically found in comets. The C2H radicals generated in the laboratory experiments are formed vibrationally and/or electronically excited. Any rotationally/vibrationally excited C2H present in cometary comae will quickly undergo radiative relaxation in the infrared to their lowest rotational and vibrational state. Experiments are currently under way to confirm the cometary formation of C2 via the VUV dissociation of cold C2H.

Urdahl, R. S.↗

Optical Characterization of Molecular Contaminant Films

A semi-empirical method of optical characterization of thin contaminant films on surfaces of optical components has been conceived. The method was originally intended for application to films that become photochemically deposited on such optical components as science windows, lenses, prisms, thinfilm radiators, and glass solar-cell covers aboard spacecraft and satellites in orbit. The method should also be applicable, with suitable modifications, to thin optical films (whether deposited deliberately or formed as contaminants) on optical components used on Earth in the computer microchip laser communications and thin-film industries. The method is expected to satisfy the need for a means of understanding and predicting the reductions in spectral transmittance caused by contaminant films and the consequent deterioration of performances of sensitive optical systems. After further development, this method could become part of the basis of a method of designing optical systems to minimize or compensate for the deleterious effects of contaminant films. In the original outer-space application, these deleterious effects are especially pronounced because after photochemical deposition, the films become darkened by further exposure to solar vacuum ultraviolet (VUV) radiation. In this method, thin contaminant films are theoretically modeled as thin optical films, characterized by known or assumed values of thickness, index of refraction, and absorption coefficient, that form on the outer surfaces of the original antireflection coating on affected optical components. The assumed values are adjusted as needed to make actual spectral transmittance values approximate observed ones as closely as possible and to correlate these values with amounts of VUV radiation to which the optical components have been exposed. In an initial study, the method was applied in correlating measured changes in transmittance of high-purity fused silica photochemically coated with silicone films of various measured thicknesses and exposed to various measured amounts of VUV radiation. In each case, it was found to be possible to select an index of refraction and absorption coefficient that made the ultraviolet, visible, and infrared transmittance changes predicted by the model match the corresponding measured transmittance changes almost exactly.

Visentine, James T.↗