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NASA NTRS1972

Photochemistry and lifetimes of interstellar molecules.

Quantitative discussion of the photochemistry and lifetime against photodecomposition of five interstellar molecules: H2CO, NH3, H2O, CH4, and CO. For the first four molecules, primary photochemical decomposition processes yielding atomic and molecular hydrogen are considered in addition to photoionization. The quantum yield for decomposition of these molecules is unity. For CO, only decomposition to ground-state carbon and oxygen atoms occur, but the quantum yield is not known and may be considerably less than unity. The radiation field in obscuring clouds is estimated, using an interstellar extinction curve for the Perseus region.

Stief, L. J.↗

NASA NTRS1972

Laboratory measurement of the 2-centimeter, 2/11/-2/12/ transition of normal formaldehyde and its carbon-13 and oxygen-18 species.

Beam-maser spectrometric measurements to an accuracy of about 100 Hz have been conducted of the 2(11)-2(12) transition for the isotopic species of greatest astronomical interest - i.e., H2CO, H2(13)CO, and H2C(18)O. The samples used were not isotopically enriched, monomeric formaldehyde vapors. For these species, all the coupling constants required to calculate the hyperfine structure of any rotational transition have been determined.

Tucker, K. D.↗

NASA NTRS1971

Interstellar molecules and dense clouds.

Current knowledge of the interstellar medium is discussed on the basis of recent published studies. The subjects considered include optical identification of interstellar molecules, radio molecular lines, interstellar clouds, isotopic abundances, formation and disappearance of interstellar molecules, and interstellar probing techniques. Diagrams are plotted for the distribution of galactic sources exhibiting molecular lines, for hydrogen molecule, hydrogen atom and electron abundances due to ionization, for the densities, velocities and temperature of NH3 in the direction of Sagitarius B2, for the lower rotational energy levels of H2CO, and for temporal spectral variations in masing H2O clouds of the radio source W49. Future applications of the maser and of molecular microscopy in this field are visualized.

Rank, D. M.↗

NASA NTRS1972

Interstellar hydrogen sulfide.

Hydrogen sulfide has been detected in seven Galactic sources by observation of a single line corresponding to the rotational transition from the 1(sub 10) to the 1(sub 01) levels at 168.7 GHz. The observations show that hydrogen sulfide is only a moderately common interstellar molecule comparable in abundance to H2CO and CS, but somewhat less abundant than HCN and much less abundant than CO.

Thaddeus, P.↗

NASA NTRS1974

Microwave rotational spectroscopy: A physical technique for specific pollutant monitoring

Evidence is presented that microwave rotational spectroscopy can be developed for use in air pollution monitoring, with the employment of a diode-cavity spectrometer capable of detecting small concentrations of NO2, SO2, H2CO, and HN3 gas with very high specificity. The theory behind the technique is discussed, together with its application and experimental results.

Hrubesh, L. W.↗

NASA NTRS1976

The reactions of O(ID) and OH with CH3OH, oxidation of the HCO radial, and the photochemical oxidation of formaldehyde

An experimental, laboratory study of the various photochemical reactions that can occur in the mesosphere and stratosphere is presented. N2O was photolyzed at 2139 A in the presence of CH3OH and CO. The O(id) produced in the photolysis reacted with CH3OH to produce OH radicals, and thus the reactions of both O(id) and OH were able to be studied. Also considered was the oxidation of the HCO radical. Mixtures of Cl2, O2, H2CO, and sometimes N2 or He were irradiated at 3660 A at several temperatures to photodecompose the Cl2. The photochemical oxidation of formaldehyde was studied as follows: formaldehyde in the presence of N2 and/or O2 (usually dry air) was photolyzed with a medium pressure Hg lamp used in conjunction with various filters which transmit different relative amounts of Hg lines from 2894 A to 3660 A. Results are presented and discussed, along with a description of experimental procedures and apparatus, and chemical reaction kinetics.

Osif, T. L.↗

NASA NTRS1975

A survey of carbon monoxide emission in dark clouds

Results are reported of a CO and (C-13)O survey of 68 dark clouds from the Lynds catalog. CO was detected in 63 of the 64 sources in which it was searched for, and the (C-13)O line was seen in 52 of 55 clouds. There is a rather narrow distribution of CO peak line radiation temperatures about a mean of 6 K; this may reflect the presence of a roughly uniform kinetic temperature of 9.5 K in the sources. Despite the probably subthermal excitation temperature of the (C-13)O transition observed, derived (C-13)O column densities are most likely good to within a factor of 2. Typical CO column densities for the clouds surveyed are 5 x 10 to the 17-th power per sq cm, assuming a terrestrial carbon isotope ratio. All 68 clouds have previously been studied by Dieter in 6-cm H2CO absorption; a comparison of line widths shows the (C-13)O lines to generally be wider than their formaldehyde counterparts. Possible explanations of this fact in terms of internal cloud motions are discussed.

Dickman, R. L.↗

NASA NTRS1976

MCSCF potential energy surface for photodissociation of formaldehyde

The ground state potential energy surface for the dissociation of formaldehyde (H2CO to H2 and CO) is calculated with the ab initio MCSCF method with an extended (4-31G) basis set. The location, barrier height, and force constants of the transition state are determined, and the normal coordinate analysis is carried out. The calculated barrier height is 4.5 eV. Based on the calculated quantities, the detailed mechanism of the photochemical dissociation is discussed.

Jaffe, R. L.↗

NASA NTRS1976

Interstellar molecules

Progress in the discovery and study of interstellar molecules is summarized. The 36 molecular species thus far identified in interstellar space are listed in several groups which include simple hydrides, oxides, and sulfides, various derivatives of ammonia, molecules involving linear carbon chains, cyanides, and molecules related in structure to formaldehyde, alcohols, or ethers. Several free radicals are described, the discovery of molecules in external galaxies is discussed, and possible mechanisms for molecular formation are noted. Methods for examining relative isotopic abundances by measuring molecules in interstellar clouds are outlined, mechanisms for the excitation of interstellar molecules are reviewed, and values are presented for the C-12/C-13 abundance ratio in a number of interstellar clouds. The detection of interstellar masers is discussed along with pumping mechanisms and masing transitions in H2CO, CH, OH, and SiO. The nature of dense interstellar clouds is examined in terms of several simple and complex cloud models, with emphasis on multiple condensation models.

Townes, C. H.↗

NASA NTRS1976

Ion cyclotron resonance studies of some reactions of C/+/ ions

Product distributions and rate constants for the reaction of ground state C(+) ions with O2, NO, HCl, CO2, H2S, H2O, HCN, NH3, CH4, H2CO, CH3OH, and CH3NH2 have been measured. Rate constants were obtained using ion cyclotron resonance trapped ion methods, and product distributions were obtained using a tandem mass spectrometer. Rapid carbon isotope exchange has also been observed in C(+)-CO collisions.

Anicich, V. G.↗

NASA NTRS1977

The structure of W49 A as deduced from molecular and recombination line observations

The molecular cloud complex W49 A has been observed in the 2.6-mm CO line, the 2-cm H2CO line, and the H76-alpha recombination line. These observations are most consistent with a picture of the complex in which a large H II region lies between two massive molecular clouds. Using a simple hydrodynamic model coupled with calculations of radiative transfer in the recombination lines, it is found that many of the spectral-line and continuum observations obtained on this region can be naturally explained, including: (1) the multiple structure observed in the molecular lines and the single structure in the recombination lines; (2) the local standard of rest (LSR) velocities of both the molecular and recombination lines; (3) the velocity gradients observed in the lines; (4) the continuum emission from the H II region; and (5) the line widths and line-to-continuum ratios of the recombination lines.

Mufson, S. L.↗

NASA NTRS1977

Observations of formaldehyde absorption in the region of NGC 2264 and other Bok globules

The paper reports observations of 6-cm H2CO absorption over an extended region surrounding the globule in NGC 2264 and toward the globules B68, B72, B133, B134, B227, B238, and B335. The lines observed from the globules are similar to those seen in more extended dark clouds. It is inferred that physical conditions are similar in the two types of region. Negative results for several other globules are reported.

Rickard, L. J.↗

NASA NTRS1977

Graphite grain surface reactions in interstellar and protostellar environments

Surface reactions on warm (at least 60 K) graphite grains between lattice C atoms and impinging H and O atoms within or in the vicinity of H II regions can provide a prolific source of H2CO and other interstellar molecules. It is proposed that similar reactions in the primitive solar nebula led to the formation of the organic molecules found in carbonaceous chondrites. From this and related evidence, it is argued that most of the solid material in the solar system may have originated as interstellar grains.

Barlow, M. J.↗

NASA NTRS1977

Photoabsorption in formaldehyde

Theoretical studies of the vertical electronic dipole excitation and ionization spectra in molecular formaldehyde are reported. The investigations relied on configuration-interaction calculations and moment-theory techniques. A double-zeta basis of contracted Gaussian-lobe functions supplemented with appropriate polarization and bond functions was used to construct Fock spectra in C(2 nu) symmetry for certain states near the ground state equilibrium geometry. The ionization energies, discrete vertical transition frequencies, and oscillator strengths for occupied and vertical Fock orbitals are in general accord with experimental determinations and other theoretical calculations. Stieltjes and Chebyshev vertical electronic photoionization profiles were calculated and found to be in good agreement with appropriately averaged photoionization-mass spectrometric measurements of the cross section for parent H2CO(+) ion production.

Langhoff, P. W.↗

NASA NTRS1978

Rate constant for the fraction of atomic chlorine with formaldehyde from 200 to 500K

A flash photolysis - resonance fluorescence technique was used to measure rate constant. The results were independent of substantial variations in H2CO, total pressure (Ar), and flash intensity (i.e., initial Cl). The rate constant was shown to be invariant with temperature, the best representation for this temperature range being K = (7.48 + or - 0.50) x 10 to the minus 11 power cu cm molecule-1 s-1 where the error is one standard deviation. The rate constant is theoretically discussed and the potential importance of the reaction in stratospheric chemistry is considered.

Michael, J. V.↗

NASA NTRS1978

Nonequilibrium chemistry in shocked molecular clouds

The gas-phase chemistry is studied behind a 10-km/s shock propagating into a dense molecular cloud. The principal conclusions are that: the concentrations of certain molecules (CO, NH3, HCN, N2) are unperturbed by the shock; other molecules (H2CO, CN, HCO(+)) are greatly decreased in abundance; and substantial amounts of H2O, HCO, and CH4 are produced. Approximately 1 million yr (independent of the density) must elapse after shock passage before chemical equilibrium is attained.

Iglesias, E. R.↗

NASA NTRS1979

Rotational excitation of symmetric top molecules by collisions with atoms. II - Infinite order sudden approximation

The infinite order sudden (IOS) approximation is extended to rotational excitation of symmetric tops by collisions with atoms. After development of a formalism for 'primitive' or 'one-ended' tops, proper parity-adapted linear combinations describing real rotors are considered and modifications needed for asymmetric rigid rotors are noted. The generalized spectroscopic relaxation cross sections are discussed. IOS calculations for NH3-He and H2CO-He are performed and compared with more accurate calculations, and the IOS approximation is found to provide a reasonably accurate description.

Green, S.↗

NASA NTRS1979

Rate constant for the reaction of atomic chlorine with formaldehyde from 200 to 500 K

The absolute rate constant for the reaction of atomic chlorine with formaldehyde has been measured from 200 to 500 K using the flash photolysis-resonance fluorescence technique. The results were independent of substantial variations in (H2CO), total pressure (Ar), and flash intensity (i.e., initial (Cl)). The rate constant was shown to be invariant with temperature, the best representation for this temperature range being k-sub-1 = (7.48 + or - 0.50) times 10 to the -11 cu cm/molecule sec, where the error is one standard deviation. This result is compared with the only previous determination of k-sub-1, which was a relative value obtained at 298 K. The rate constant is theoretically discussed, and the potential importance of the reaction in stratospheric chemistry is considered.

Michael, J. V.↗