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We discuss three techniques which allow the use of tunable lasers for high resolution and picosecond time scale spectroscopy of core-excited atomic levels. These are: anti-Stokes absorption spectroscopy, laser induced emission from metastable levels, and laser designation of selected core-excited levels.
Chlorine monoxide (ClO) is thought to play an important role in a photochemical cycle which causes the destruction of ozone in the earth's stratosphere. Since lines of the (1,0) fundamental of ClO lie near C-14O2-16, laser lines, IR heterodyne spectroscopy is potentially an important technique for monitoring the ClO abundance. However, due to the presence of lines from other trace atmospheric gases in this spectral range, the interpretation of such observations is ambiguous unless high resolution laboratory measurements support the identifications. Measured frequencies are reported for spectral lines of seven trace atmospheric gases which absorb near the C-14O2-16 laser transitions relevant to the detection of ClO by IR heterodyne spectroscopy.
Inelastic electron tunneling spectroscopy is a useful technique for the study of vibrational modes of molecules adsorbed on the surface of oxide layers in a metal-insulator-metal tunnel junction. The technique involves studying the effects of adsorbed molecules on the tunneling spectrum of such junctions. The data give useful information about the structure, bonding, and orientation of adsorbed molecules. One of the major advantages of inelastic electron tunneling spectroscopy is its sensitivity. It is capable of detecting on the order of 10 to the 10th molecules (a fraction of a monolayer) on a 1 sq mm junction. It has been successfully used in studies of catalysis, biology, trace impurity detection, and electronic excitations. Because of its high sensitivity, this technique shows great promise in the area of solid-state electronic chemical sensing.
Contemporary gamma-ray spectroscopy instruments and their results are reviewed. Sensitivities of 10 to the -4th to 10 to the -3rd ph/sq cm-sec have been achieved for steady sources and 10 to the -2nd to 1 ph/sq cm-sec for transient sources. This has led to the detection of gamma-ray lines from more than 40 objects representing 6 classes of astrophysical phenomena. The lines carry model-independent information and are of fundamental importance to theoretical modeling and our understanding of the objects. The objectives and anticipated results of future instruments are discussed. Several instruments in development will have a factor of 10 sensitivity improvement to certain phenomena over contemporary instruments. A factor of 100 improvement in sensitivity will allow the full potential of gamma-ray spectroscopy to be realized. Instrument concepts which would achieve this with both present and advanced techniques are discussed.
The use of infrared heterodyne spectroscopy for the study of planetary atmospheres is discussed. Infrared heterodyne spectroscopy provides a convenient and sensitive method for measuring the true intensity profiles of atmospheric spectral lines. Application of radiative transfer theory to measured lineshapes can then permit the study of molecular abundances, temperatures, total pressures, excitation conditions, and dynamics of the regions of line formation. The theory of formation of atmospheric spectral lines and the retrieval of the information contained in these molecular lines is illustrated. Notable successes of such retrievals from infrared heterodyne measurements on Venus, Mars, Jupiter and the earth are given. A discussion of developments in infrared heterodyne technology is also presented. Previously announced in STAR as N83-28551
IR gas correlation spectroscopy is a sensitive technique for the measurement of small Doppler shifts in spectra. This technique also exhibits several important advantages over alternative methods in the remote sensing of stratospheric and mesospheric winds from spacecraft. Attention is presently given to laboratory tests demonstrating gas correlation spectroscopy's quantitative measurement of small Doppler shifts in spectra, whose close agreement with theoretical predictions suggests that measurements of the change in the radiant flux through a gas correlation spectrometer can be used to measure the relative velocity between gas and instrument for a moving parcel of gas.
A new extension to optogalvanic spectroscopy, in which electrons detached from negative ions formed in the discharge are observed as a function of incident laser wavelength, has been developed. The determination of the electron affinities of I(-) and Cl(-) atomic ions is described. The potential of the technique for studying the spectroscopy of molecular negative ions is also discussed.
The planetary atmosphere of Mars was studied during the opposition of May, 1984, by means of a 10-micron heterodyne receiver mounted at the Cassegrain focus of a 3-m telescope. On the basis of a model of the Martian atmosphere, the isotopic ratios derived from the fully resolved absorption spectra obtained were compared with the results of Viking probe in situ measurements and terrestrial values; agreement is obtained within statistical errors. It is shown that highly resolving spectroscopy allows for the determination of isotopic ratios in remote sensing with a precision that is comparable to that of in situ mass spectroscopy.
A discussion is presented of IR spectroscopy, particularly high-resolution spectroscopy in the approximately 1-20 micron band, as it impacts the study of circumstellar envelopes. The molecular bands within this region contain an enormous amount of information, especially when observed with sufficient resolution to obtain kinematic information. In a single spectrum, it is possible to resolve lines from up to 50 different rotational/vibrational levels of a given molecule and to detect several different isotopic variants. When high resolution techniques are combined with mapping techniques and/or time sequence observations of variable stars, the resulting information can paint a very detailed picture of the mass-loss phenomenon. To date, near-IR observations have been made of 20 molecular species. CO is the most widely observed molecule and useful information has been gleaned from the observed rotational excitation, kinematics, time variability and spatial structure of its lines. Examples of different observing techniques are discussed in the following sections.
Infrared spectroscopic studies of the solar system in support of spacecraft investigations were researched. The studies include the physical behavior of comets, the atmospheres of the gaseous planets, and the solid surfaces of satellites and asteroids. Studies of the gaseous and solid emanations of comets using the techniques of CCD spectroscopy and imaging were focused on. An intensive observational effort was mounted, to observe comet Halley with the recently developed state of the art CCD camera system. Comet P/Giacobini-Zinner was observed. The major emphasis was placed on spectroscopy and a synoptic spectrum at least once a month was obtained. A large number of images of Halley for particular emission species and continuum regions were also obtained. The species in vestigated were: C3 (4060 A), CO+ (4505), C2 (5139), NH2 (5980), H2O+ (6185), OI (6300) and CN (9180).
The ability of the Thermal Infrared Multispectral Scanner (TIMS) data to identify rock composition using thermal-infrared spectroscopy was assessed. A region was selected with a wide range of rock and soil types in an arid environment, and the spectra acquired by TIMS was compared to laboratory spectra of collected samples. A TIMS image was acquired of the Kelso-Baker region in the Mojave desert of California at a surface resolution of approximately 7 m. This image was then used to map the areal extent of each geologic component. The TIMS data provided an excellent means for discriminating and mapping rocks of very similar mineralogy. These findings suggest that thermal-infrared spectroscopy can provide a powerful tool for identifying and mapping rock composition on the Earth and other terrestrial planets.
In collaboration with NASA/Langley Research Center, a truly nonintrusive and nonseeding method for measuring supersonic molecular flow parameters was proposed and developed at Colorado State University. The feasibility of this Raman Doppler Velocimetry (RDV), currently operated in a scanning mode, was demonstrated not only in a laboratory environment at Colorado State University, but also in a major wind tunnel at NASA/Langley Research Center. The research progress of the RDV development is summarized. In addition, methods of coherent Rayleigh-Brillouin spectroscopy and single-pulse coherent Raman spectroscopy are investigated, respectively, for measurements of high-pressure and turbulent flows.
The applicability of CCD detectors to astronomical extreme ultraviolet (EUV) spectroscopy (100-1250 A) is discussed. The advantages of CCDs in this spectral region include internal electron yield, the potential for very high quantum efficiency (about 50-90 percent), and broad wavelength response. Visible light suppression is achieved by a combination of low grating scattering, greater than unity electron yield in the EUV, and various filter techniques. For the current generation of CCDs, detection of only a few EUV photons will rapidly overwhelm the read noise; thus, for all practical S/N ratios used in astronomical spectroscopy, read noise will be negligible compared to the poisson statistics of the detected photons. A model based on experimental data for the quantum efficiency and electron yield of CCDs in the EUV is discussed.
A unique scanning tunneling microscope (STM) system has been developed for spectroscopy of the superconducting energy gap. High-resolution control of tunnel current and voltage allows for measurement of superconducting properties at tunnel resistance levels 100-1000 greater than that achieved in prior work. The previously used STM methods for superconductor spectroscopy are compared to those developed for the work reported here. Superconducting energy-gap spectra are reported for three superconductors, Pb, PbBi, and NbN, over a range of tunnel resistance. The measured spectra are compared directly to theory.
An assembly language program using the Intel 80386 CPU and 80387 math co-processor chips was written to increase the speed of data gathering and processing, and provide control of a scanning CW ring dye laser system. This laser system is used in high resolution (better than 0.001 cm-1) water vapor spectroscopy experiments. Laser beam power is sensed at the input and output of white cells and the output of a Fabry-Perot. The assembly language subroutine is called from Basic, acquires the data and performs various calculations at rates greater than 150 faster than could be performed by the higher level language. The width of output control pulses generated in assembly language are 3 to 4 microsecs as compared to 2 to 3.7 millisecs for those generated in Basic (about 500 to 1000 times faster). Included are a block diagram and brief description of the spectroscopy experiment, a flow diagram of the Basic and assembly language programs, listing of the programs, scope photographs of the computer generated 5-volt pulses used for control and timing analysis, and representative water spectrum curves obtained using these programs.
A generalized theory for optical heterodyne spectroscopy with phase modulated laser radiation is used which allows the calculation of signal line shapes for frequency modulation spectroscopy of Lorentzian gas absorption lines. In particular, synthetic spectral line shapes for both single-tone and two-tone modulation of lead-salt diode lasers are presented in which the contributions from both amplitude and frequency modulations are included.
Recent advances in imaging spectroscopy for remote sensing applications are discussed, reviewing the results of recent investigations. The advantages offered by the higher spectral resolution of imaging spectroscopy relative to scanners such as Landsat MSS and TM are explained; the design and performance of the Airborne Imaging Spectrometer (Vane et al., 1984) are described and illustrated with drawings, photographs, and sample images; data processing and analysis techniques are outlined; and applications to geological and botanical research are considered.
High resolution infrared spectoscopy provides unique insights into the chemistry and dynamics of the atmospheres of Jupiter and Saturn. The 5 micrometer spectral region, which is transparent to deep levels, is particularly useful for the identification of molecules that are present at very low (parts per billion) concentrations. These are tracers of convective and strongly non-equilibrium processes in the atmosphere. High resolution ground-based spectroscopy complements Voyager and Galileo measurements. Spectroscopy is sensitive to lower mixing levels for selected molecules, while the on-board mass spectrometers probe molecules that are spectroscopically inaccessible. Analysis and modeling of the 4.7 micrometer carbon monoxide in Jupiter was completed. CO is present at a mole fraction of 1.6 plus or minus 0.3 x 10 to the 9th power and concentrated in the troposphere. At this abundance, it must be convected upward from much deeper levels in Jupiter where the temperature is near 1100 K. Thus CO is a tracer of the deep atmosphere which is otherwise unobservable. The oxygen abundance in Jupiter (as measured by the CO abundance) is near solar. Chemical or physical process must deplete the major oxygen carrier, water. Germane, GeH4, was discovered on Saturn at amole fraction of 4 plus or minus 2 x 10 to the 10th power.