Millimeter and Submillimeter Spectroscopy in support of Upper Atmospheric Research: Recent Results of the Spectra and Molecular Properties of simple Halogen Oxides and Oxoacids
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The H + OCS hot atom reaction - CO state distributions and translational energy from time-resolved infrared absorption spectroscopy
Time-resolved infrared diode laser spectroscopy has been used to probe CO internal and translational excitation from the reaction of hot H atoms with OCS. Product distributions should be strongly biased toward the maximum 1.4 eV collision energy obtained from 278 nm pulsed photolysis of HI. Rotations and vibrations are both colder than predicted by statistical density of states theory, as evidenced by large positive surprisal parameters. The bias against rotation is stronger than that against vibration, with measurable population as high as v = 4. The average CO internal excitation is 1920/cm, accounting for only 13 percent of the available energy. Of the energy balance, time-resolved sub-Doppler line shape measurements show that more than 38 percent appears as relative translation of the separating CO and SH fragments. Studies of the relaxation kinetics indicate that some rotational energy transfer occurs on the time scale of our measurements, but the distributions do not relax sufficiently to alter our conclusions. Vibrational distributions are nascent, though vibrational relaxation of excited CO is unusually fast in the OCS bath, with rates approaching 3 percent of gas kinetic for v = 1.
Nickolaisen, Scott L.↗
Far-infrared spectroscopy of the galactic center - Neutral and ionized gas in the central 10 parsecs of the Galaxy
The present mapping of the 3P1-3P2 fine structure line emission from neutral atomic oxygen near the galactic center shows the emission to be extended over more than 12 pc along the galactic plane, centered on the position of Sgr A West. The rotational velocity of the O I gas at R of about 1 corresponds to a mass within the central parsec of about 3 million solar masses. The forbidden O I line probably arises in a predominantly neutral atomic region immediately outside the ionized central parsec of the Galaxy. Gas temperatures are greater than 100 K, and the total integrated luminosity radiated in the line, which is about 100,000 solar luminosities, substantially contributes to the cooling of the gas. The 3P1-3P0 fine structure line of the O III forbidden line has also been detected at 88 microns toward Sgr A West, coming from high density ionized gas.
Genzel, R.↗
Technology Development of Miniaturized Far-Infrared Sources for Biomolecular Spectroscopy
The objective of this project was to develop a purely solid-state based, thus miniaturized, far-infrared (FIR) (also known as terahertz (THz)) wave source using III-V semiconductor nanostructures for biomolecular detection and sensing. Many biomolecules, such as DNA and proteins, have distinct spectroscopic features in the FIR wavelength range as a result of vibration-rotation-tunneling motions and various inter- and intra-molecule collective motions. Spectroscopic characterization of such molecules requires narrow linewidth, sufficiently high power, tunable (in wavelength), and coherent FIR sources. Unfortunately, the FIR frequency is one of the least technologically developed ranges in the electromagnetic spectrum. Currently available FIR sources based on non-solid state technology are bulky, inefficient, and very often incoherent. In this project we investigated antimonide based compound semiconductor (ABCS) nanostructures as the active medium to generate FIR radiation. The final goal of this project was to demonstrate a semiconductor THz source integrated with a pumping diode laser module to achieve a compact system for biomolecular applications.
Kono, Junichiro↗
Interactions of amorphous Ta(x)Cu(1-x) (x = 0.93 and 0.80) alloy films with Au overlayers and GaAs substrates
Amorphous Ta(93)Cu(7) and Ta(80)Cu(20) alloy films are prepared by cosputtering of pure Ta and pure Cu targets with a rotating sample holder table. To investigate the possible application of these materials as diffusion barriers for the Au-GaAs system, vacuum annealings are made in the temperature range from 200 to 800 C. Resistivity change, X-ray diffraction, and Auger electron spectroscopy measurements are performed to find the chemical and metallurgical stabilities of these materials in this system. The reaction temperature for Ta(x)Cu(1-x) in contact with GaAs lies between 500 and 700 C. For Au in contact with Ta(x)Cu(1-x) the reaction occurs at about 600 C. Amorphous Ta(93)Cu(7) shows different interdiffusion characteristics with surrounding elements than does Ta(80)Cu(20).
Oh, Jae E.↗
The Age-Related Properties of the HD 98800 System
We present optical spectroscopy of the field K star system HD 98800, which has been found to have significant infrared emission from circumstellar material. The lithium abundances of the stars in HD 98800 are well above those of Pleiades of similar color, but activity levels and rotation in these stars are at or below Pleiades level. Thus, it is not yet possible to say whether HD 98800 is or is not a pre-main-sequence system, and it is possible that its components are on or near the zero-age main sequence. However, the two visible objects that make up HD 98800 both have high levels of lithium and activity, strongly suggesting that they are physically related to one another. As shown by Torres and coworkers, having these stars physically tied implies that their relative orbit is highly eccentric and highly inclined to our line of sight, and it also means that we are viewing the HD 98800 system at an unusual time in its orbit.
Soderblom, David R.↗
Spectroscopic Parameters of H2S Polyads Between 3400 and 8000 cm x 10 to -1 exponent
The absorption spectra of hydrogen sulfide from 0.8 to 5 micro- meters were recorded with three spectral resolutions using the Fourier transform spectrometer at Kitt Peak National Observatory. Twenty bands were previously assigned so that accurate band origins and vi- brational parameters could be determined. Described are the analyses of the rotational structure of resonating hydrogen sulfide states.
molecular spectroscopy hydrogen sulfide absorption↗
Application of Tunable Diode Laser Spectrometry for Isotopic Analysis
Lead-salt tunable diode lasers are now commercially available with operating temperatures above 77 K and excellent single-mode characteristics which make them very useful for spectroscopy in the mid-IR spectral range. Using these lasers for absorption measurements in the 4.3 micrometer spectral region we have made accurate measurements of isotopic abundances in CO2. The method involves assembly language controlled data acquisition of spectra of selected adjacent isotopic rotational lines, an etalon spectral frequency calibration technique, the fitting of multiple Voigt profiles to the data, and the ratioing of absorbances from simultaneously acquired sample and reference data scans. The accuracy achieved is better than 0.4% for the C-13/C-12 ratio and 1% for the O-18/O-16 ratio. Higher accuracy is expected from improvements now being implemented.
Sauke, T. B.↗
Laboratory Spectroscopy of CH(+) and Isotopic CH
The A1II - X1(Epsilon) electronic band of the CH(+) ion has been used as a probe of the physical and dynamical conditions of the ISM for 65 years. In spite of being one of the first molecular species observed in the ISM and the very large number of subsequent observations with large derived column densities, the pure rotational spectra of CH+ has remained elusive in both the laboratory and in the ISM as well. We report the first laboratory measurement of the pure rotation of the CH(+) ion and discuss the detection of CH-13(+) in the ISM. Also reported are the somewhat unexpected chemical conditions that resulted in laboratory production.
Pearson, John C.↗
Defect Clustering and Nano-phase Structure Characterization of Multicomponent Rare Earth-Oxide-Doped Zirconia-Yttria Thermal Barrier Coatings
Advanced thermal barrier coatings (TBCs) have been developed by incorporating multicomponent rare earth oxide dopants into zirconia-based thermal barrier coatings to promote the creation of the thermodynamically stable, immobile oxide defect clusters and/or nanophases within the coating systems. In this paper, the defect clusters, induced by Nd, Gd, and Yb rare earth dopants in the zirconia-yttria thermal barrier coatings, were characterized by high-resolution transmission electron microscopy (TEM). The TEM lattice imaging, selected area diffraction (SAD), and electron energy-loss spectroscopy (EELS) analyses demonstrated that the extensive nanoscale rare earth dopant segregation exists in the plasma-sprayed and electron-physical-vapor-deposited (EB PVD) thermal barrier coatings. The nanoscale concentration heterogeneity and the resulting large lattice distortion promoted the formation of parallel and rotational defective lattice clusters in the coating systems. The presence of the 5-to 100-nm-sized defect clusters and nanophases is believed to be responsible for the significant reduction of thermal conductivity, improved sintering resistance, and long-term high temperature stability of the advanced thermal barrier coating systems.
Zhu, Dongming↗
Circular polarimetry of EXO 033319-2554.2 - A new eclipsing AM Herculis star
This Letter presents circular polarimetry that unequivocally identifies EXO 033319-2554.2 as only the third eclipsing AM Her star and brings the total number of AM Her stars now identified to 14. The orbital period is 126.4 minutes, as previously reported, and defines a new short-period edge to the period gap seen in all classes of cataclysmic variable stars. EXO 033319-2554.2 shows 2.5 mag deep eclipses of the predominantly accreting magnetic pole on the white dwarf. Before the eclipse, the pole rotates into the line of sight and shows white-light circular polarization, due to cyclotron radiation, that reaches values as high as 10 percent. There is some evidence that the second pole is emitting cyclotron radiation too. How high time resolution photometry, linear polarimetry, and spectroscopy will be of great value in understanding this system.
Berriman, Graham↗
Width-Increased Dual-Pump Enhanced Coherent Anti-Stokes Raman Spectroscopy (WIDECARS)
WIDECARS is a dual-pump coherent anti-Stokes Raman Spectroscopy technique that is capable of simultaneously measuring temperature and species mole fractions of N2, O2, H2, C2H4, CO, and CO2. WIDECARS is designed for measurements of all the major species (except water) in supersonic combustion flows fueled with hydrogen and hydrogen/ethylene mixtures. The two lowest rotational energy levels of hydrogen detectable by WIDECARS are H2 S(3) and H2 S(4). The detection of these lines gives the system the capability to measure temperature and species concentrations in regions of the flow containing pure hydrogen fuel at room temperature.
Tedder, Sarah A.↗
Width-Increased Dual-Pump Enhanced Coherent Anti-Stokes Raman Spectroscopy (WIDECARS)
WIDECARS is a dual-pump coherent anti-Stokes Raman Spectroscopy technique that is capable of simultaneously measuring temperature and species mole fractions of N2, O2, H2, C2H4, CO, and CO2. WIDECARS is designed for measurements of all the major species (except water) in supersonic combustion flows fueled with hydrogen and hydrogen/ethylene mixtures. The two lowest rotational energy levels of hydrogen detectable by WIDECARS are H2 S(3) and H2 S(4). The detection of these lines gives the system the capability to measure temperature and species concentrations in regions of the flow containing pure hydrogen fuel at room temperature.
Tedder, Sarah A.↗
Spectroscopy of V711 Tauri (= HR 1099) - Fundamental properties and evidence for starspots
New orbital elements have been determined for the bright RS CVn-type system V711 Tau. The spectroscopic period has been refined to 2.83774 d + or - 0.00001 d. The eccentricity is determined to be 0.014 + or - 0.009, and the inclination of the system is 33 deg + or - 2 deg. The masses, radii, and equatorial rotational velocities for each component are stated.Evolutionary models suggest that mass transfer may begin in 70 to 80 million years. High SNR Reticon observations at red wavelengths show substantial differences in rotational velocity and line strength between the two components, as well as asymmetries in all absorption lines of the more massive, active, cooler star. These asymmetries are correlated with photometric variations and move across the line profiles with time. They are the result of starspot regions rotating in and out of view.
Fekel, F. C., Jr.↗
The Presence of Methane in the Atmosphere of an Extrasolar Planet
Molecules present in the atmospheres of extrasolar planets are expected to influence strongly the balance of atmospheric radiation, to trace dynamical and chemical processes, and to indicate the presence of disequilibrium effects. As molecules have the potential to reveal atmospheric conditions and chemistry, searching for them is a high priority. The rotational-vibrational transition bands of water, carbon monoxide and methane are anticipated to be the primary sources of non-continuum opacity in hot-Jupiter planets. As these bands can overlap in wavelength, and the corresponding signatures from them are weak, decisive identification requires precision infrared spectroscopy. Here we report a near-infrared transmission spectrum of the planet HD 189733b that shows the presence of methane. Additionally, a resolved water vapour band at 1.9 (micro)m confirms the recent claim4 of water in this object. On thermochemical grounds, carbon monoxide is expected to be abundant in the upper atmosphere of hot-Jupiter planets, but is not identifiable here; therefore the detection of methane rather than carbon monoxide in such a hot planet could signal the presence of a horizontal chemical gradient away from the permanent dayside, or it may imply an ill-understood photochemical mechanism that leads to an enhancement of methane.
atmospheric radiation↗
3D Observation of GEMS by Electron Tomography
Amorphous silicates in chondritic porous interplanetary dust particles (CP-IDPs) coming from comets are dominated by glass with embedded metal and sulfides (GEMS). GEMS grains are submicron-sized rounded objects (typically 100-500) nm in diameter) with anaometer-sized (10-50 nm) Fe-Ni metal and sulfide grains embedded in an amorphous silicate matrix. Several formation processes for GEMS grains have been proposed so far, but these models are still being debated [2-5]. Bradley et al. proposed that GEMS grains are interstellar silicate dust that survived various metamorphism or alteration processes in the protoplanetary disk and that they are amorphiation products of crystalline silicates in the interstellar medium by sputter-deposition of cosmic ray irradiation, similar to space weathering [2,4]. This consideration is based on the observation of nano-sized crystals (approximately 10 nm) called relict grains in GEMS grains and their shapes are pseudomorphs to the host GEMS grains. On the other hand, Keller and Messenger proposed that most GEMS formed in the protoplanetary disk as condensates from high temperature gas [3,5]. This model is based on the fact that most GEMS grains have solar isotopic compositions and have extremely heterogeneous and non-solar elemental compositions. Keller and Messenger (2011) also reported that amorphous silicates in GEMS grains are surrounded by sulfide grains, which formed as sulfidization of metallic iron grains located on the GEMS surface. The previous studies were performed with 2D observation by using transmission electron microscopy (TEM) or scanning TEM (STEM). In order to understand the structure of GEMS grains described above more clearly, we observed 3D structure of GEMS grains by electron tomography using a TEM/STEM (JEM-2100F, JEOL) at Kyoto University. Electron tomography gives not only 3D structures but also gives higher spatial resolution (approximately a few nm) than that in conventional 2D image, which is restricted by sample thickness ) approx. or greater than 50 nm). Three cluster IDPs (L2036AA5 cluster4, L2009L8 cluster 13 and W726A2) were used for the observations. ID W726A2 was collected without silicon oil, which is ordinary used to collect IDPs, so this sample has no possibility of contaminations caused by silicon oil or solvent to rinse it [6]. The samples were embedded in epoxy risin and sliced into ultrathin sections (50-300 nm) using an ultramicotome. The sections were observed by BF-TEM and HAADF-STEM (high angle annular dark field-scanning TEM) modes. Images were obtained by rotating the sample tilt angle over a range of +/- 65 deg in 1 deg steps. The obtained images were reconstructed to slice images. Mineral phases in the slice images were estimated by comparing with a 2D elemental map obtained by an EDS (energy dispersive X-ray spectroscopy) system equipped in the TEM/STEM. Careful examination of the slice images confirmed that iron grains are embedded in the amorphous silicate matrix of the GEMS grains, but sulfide grains were mainly present on the surface of the amorphous silicate. These results are consistent with the model that GEMS grains formed as condensates [3,5], although more data are needed to conclude the origin of GEMS grains. The present study is the first successful example adapting the electron tomography to the IDPs. This type of analysis will be important for planetary material sciences in the future.
Matsuno, Junya↗
Stable isotope laser spectroscopy
Recent advances in semiconductor laser technology have produced a reliable lightweight device ideally suited for a spacecraft high resolution molecular spectrometer. Lead-salt tunable diode lasers (TDL) emit in several spectral modes, each with a very narrow linewidth of -0.0003/cm. This spectral resolution is much narrower than typical Doppler broadened molecular linewidths in the mid-IR range. Thus it is possible to detect individual rotational lines within the vibrational band and measure their intensity, which can be used to determine gas concentration. The narrow spectral lines of any impurity gas tend to lie between the narrow lines of the gas of interest. This represents a major advantage over the accepted gas chromatograph mass spectrometer (GCMS) technique for measuring gas concentrations and isotope ratios. The careful and extensive gas purification procedures required to remove impurities for reliable GCMS measurements will not be required for an IR laser gas analysis. The infrared laser gas analysis technique is being developed to measure stable isotopic ratios of gases such as CO2, CH4, N2O, and NH3. This will eventually lead to development of instruments capable of in situ istopic measurements on planets such as Mars. The carbon (C-12, C-13) isotope ratio is indicative of the type of carbon fixation mechanisms (e.g., photosynthesis, respiration) in operation on a planet, while the nitrogen (N-14, N-15) isotope ratio can probably be used to date nitrogen-bearing Martian samples. The absorbance ratio of two adjacent lines of CO2 in the 2300/cm (4.3 micron) region of the spectrum was measured. The precision of the measurement is presently better than 1 percent and significant improvement is anticipated as rapid sweep-integration techniques and computer controlled data acquistion capabilities are incorporated.
Becker, J. F.↗
Ultraviolet and optical spectroscopy of NGC 5548 and the nature of the broad-line region
The structure of the broad-line region in NGC 5548 is investigated by analysis of the integrated flux and profile variations observed in optical and ultraviolet emission lines. It is shown that the observations do not appear to be consistent with models which identify the variable part of the emission lines with a simple rotating disk structure. The variable continuum, and integrated emission-line fluxes are highly correlated and suggest a small broad-line region (18 light days = 5 x 10 to the 16th cm), although the size of the line-emitting region is not well-determined. At least some of the broad emission arises in a component which at times appears very prominently and distinctly in difference spectra. This emission component appears to arise in a region which is physically distinct from the rest of the broad-line region. Although the integrated fluxes in the various optical and ultraviolet emission lines seem to vary together, there clearly are differences between the profiles of various lines, which suggests that there is at least some ionization stratification within the broad-line region.
Peterson, Bradley M.↗