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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
NASA NTRS1991

High-resolution threshold photoionization of N2O

Pulsed field ionization (PFI) has been used in conjunction with a coherent VUV source to obtain high-resolution threshold photoelectron spectra for the (000), (010), (020), and (100) vibrational states of the N2O(+) cation. Simulations for the rotational profiles of each vibronic level were obtained by fitting the Buckingham-Orr-Sichel equations using accurate spectroscopic constants for the ground states of the neutral and the ion. The relative branch intensities are interpreted in terms of the partial waves of the outgoing photoelectron to which the ionic core is coupled and in terms of the angular momentum transferred to the core.

Wiedmann, R. T.↗
NASA NTRS1993

Stratospheric N2O5, CH4, and N2O profiles from IR solar occultation spectra

Stratospheric volume mixing ratio profiles of N2O5, CH4, and N2O have been retrieved from a set of 0.052/cm resolution (FWHM) solar occultation spectra recorded at sunrise during a balloon flight from Aire sur l'Adour, France (44 N latitude) on 12 October 1990. The N2O5 results have been derived from measurements of the integrated absorption by the 1246/cm band. Assuming a total intensity of 4.32 x 10 exp -17 cm/molecule/sq cm independent of temperature, the retrieved N2O5 volume mixing ratios in ppbv, interpolated to 2 km height spacings, are 1.64 +/- 0.49 at 37.5 km, 1.92 +/- 0.56 at 35.5 km, 2.06 +/- 0.47 at 33.5 km, 1.95 +/- 0.42 at 31.5 km, 1.60 +/- 0.33 at 29.5 km, 1.26 +/- 0.28 at 27.5 km, and 0.85 +/- 0.20 at 25.5 km. Error bars indicate the estimated 1-sigma uncertainty including the error in the total band intensity. The retrieved profiles are compared with previous measurements and photochemical model results.

Camy-Peyret, C.↗
NASA NTRS1993

The protonation of N2O reexamined - A case study on the reliability of various electron correlation methods for minima and transition states

The protonation of N2O and the intramolecular proton transfer in N2OH(+) are studied using various basis sets and a variety of methods, including second-order many-body perturbation theory (MP2), singles and doubles coupled cluster (CCSD), the augmented coupled cluster (CCSD/T/), and complete active space self-consistent field (CASSCF) methods. For geometries, MP2 leads to serious errors even for HNNO(+); for the transition state, only CCSD/T/ produces a reliable geometry due to serious nondynamical correlation effects. The proton affinity at 298.15 K is estimated at 137.6 kcal/mol, in close agreement with recent experimental determinations of 137.3 +/- 1 kcal/mol.

Martin, J. M. L.↗
NASA NTRS1993

Absorption of solar radiation by O2 - Implications for O3 and lifetimes of N2O, CFCl3, and CF2Cl2

An accurate line-by-line model is used to evaluate effects of absorption in the Schumann-Runge bands of O2 on transmission of UV radiation. The model is used to evaluate rates of photolysis for N2O, CFCl3, and CF2Cl2, and to infer global loss rates and instantaneous lifetimes appropriate for 1980. A parameterized version of the line-by-line model enabling rapid evaluation of transmission in the Schumann-Runge region is described. Photochemical calculations employing the parameterization and constrained by data from the Atmospheric Trace Molecule Spectroscopy experiment are used to examine the budget of odd oxygen. Consistent with previous studies, it is shown that photochemical loss of odd oxygen exceeds production by photolysis of O2 for altitudes above 40 km. The imbalance between production and loss is shown to be consistent with a source of odd oxygen proportional to the product of the mixing ratio and photolysis rate of ozone, which suggests that processes involving vibrationally excited O2 may play an important role in production of odd oxygen.

Minschwaner, K.↗
NASA NTRS1994

Vertical distribution of CH4 and N2O over the tropical site Hyderabad

Vertical distribution profiles of N2O and CH4 have been measured from Hyderabad, India using a balloon-borne cryogenic air sampler. The samples have been analyzed using gas chromatographic techniques. Results for two balloon flights made in 1987 and 1990 show effects of tropical characteristics like higher tropopause and upwelling motion due to Hadley circulation. These profiles also exhibit perturbations around 25 km height, which are likely to be due to dynamical effects. A comparison with the SAMS data show that the SAMS values for both these gases are higher by a factor of about 1.5 to 2 around 30 km height.

Lal, Shyam↗
NASA NTRS1993

In-situ measurements of changes in stratospheric aerosol and the N2O-aerosol relationship inside and outside of the polar vortex

Two optical particle counters on the ER-2, together covering a particle size diameter range from 0.1 microns to 23 microns, were used to measure the aerosol bulk quantities integral number, aerosol surface and volume, as well as detailed size distributions inside and outside of the polar vortex in the lower stratosphere. While AAES I (Arctic Airborne Stratospheric Expedition, (Dec. 88 - Feb. 89) was conducted in a period of relative volcanic quiescence, enhancements in aerosol number, surface and volume of factors around 10, 25 and 100 were observed during AASE 2 (Aug. 91 - Mar. 92) due to the eruption of Mt. Pinatubo. The changes in these bulk quantities as well as in the size distributions measured both outside and inside the polar vortex are presented and compared with those obtained in polar stratospheric cloud events (AASE I). Except for a shift towards larger aerosol mixing ratios the general shape of correlograms between the measured N2O and particle mixing ratios remain similar before and after the eruption. Similar correlograms are used to interpret data from vertical profiles inside and outside of the polar vortex.

Borrmann, S.↗
NASA NTRS1996

Collisional Removal of OH (X (sup 2)Pi, nu=7) by O2, N2, CO2, and N2O

Collisional removal rate constants for the OH (X 2PI, nu = 7) radical are measured for the colliders O2, CO2, and N2O, and an upper limit is established for N2. OH(nu = 4) molecules, generated in a microwave discharge flow cell by the reaction of hydrogen atoms with ozone, are excited to v = 7 by the output of a pulsed infrared laser via direct vibrational overtone excitation. The temporal evolution of the P = 7 population is probed as a function of the collider gas partial pressure by a time-delayed pulsed ultraviolet laser. Fluorescence from the B 21 + state is detected in the visible spectral region.

Knutsen, Karen↗
NASA NTRS1993

In-Situ Measurements of Changes in Stratospheric Aerosol and the N2O - Aerosol Relationship inside and outside of the Polar Vortex

Two optical particle counters on the ER-2, together covering a particle size diameter range from 0.1 micrometers to 23 micrometers, were used to measure the aerosol bulk quantities integral number, aerosol surface and volume, as well as detailed size distributions inside and outside of the polar vortex in the lower stratosphere. While AASE I (Arctic Airborne Stratospheric Expedition, (Dec. 1988 - Feb. 1989) was conducted in a period of relative volcanic quiescence, enhancements in aerosol number, surface and volume of factors around 10, 25 and 100 were observed during AASE II (Aug. 1991 - Mar. 1992) due to the eruption of Mt. Pinatubo. The changes in these bulk quantities as well as in the size distributions measured both outside and inside the the polar vortex are presented and compared with those obtained in polar stratospheric cloud events (AASE I). Except for a shift towards larger aerosol mixing ratios the general shape of correlograms between the measured N2O and particle mixing ratios remain similar before and after the eruption. Similar correlograms are used to interpret data from vertical profiles inside and outside of the polar vortex.

Borrmann, S.↗
NASA NTRS1993

Stratospheric N2O5, CH4, and N2O Profiles from IR Solar Occultation Spectra

Stratospheric volume mixing ratio profiles of N2O5, CH4, and N2O have been retrieved from a set of 0.052/ cm resolution (FWHM) solar occultation spectra recorded at sunrise during a balloon flight from Aire sur I'Adour, France (44 deg N latitude) on 12 October 1990. The N2O5 results have been derived from measurements of the integrated absorption by the 1246/ cm band. Assuming a total intensity of 4.32 x 10(exp 17)cm(exp -1) molecule sq cm(exp -2) independent of temperature, the retrieved N2O5 volume mixing ratios in ppbv (parts per billion by volume, 10(exp -9)), interpolated to 2 km height spacings, are 1.64 +/- 0.49 at 37.5 km, 1.92 +/- 0.56 at 35.5 km, 2.06 +/- 0.47 at 33.5 km, 1.95 +/- 0.42 at 31.5 km, 1.60 +/- 0.33 at 29.5 km, 1.26 +/- 0.28 at 27.5 km, and 0.85 +/- 0.20 at 25.5 km. Error bars indicate the estimated I-sigma uncertainty including the error in the total band intensity (+/- 20% has been assumed). The retrieved profiles are compared with previous measurements and photochemical model results.

Peyeret, C. Camy↗
NASA NTRS2000

BOREAS TF-1 SSA-OA Weekly Tower CH4 and N2O Flux

The BOREAS TF-1 team collected various trace gas and energy flux data in its efforts to characterize the temporal energy and gas exchanges that occurred over the SSA-OA site. This data set contains methane (CH4) and nitrous oxide (N2O) fluxes that were measured at the BOREAS SSA-OA site. These fluxes were measured from 16-Apr to 16-Sep-1994. The data were averaged to weekly values and are available in tabular ASCII files.

Thurtell, George↗
NASA NTRS2001

Defining the Polar Vortex Edge Using an N2O: Potential Temperature Correlation Versus the Nash Criterion: A Comparison

A prerequisite to study phenomena in the winter stratospheric polar vortex is the separation of measurements inside and outside the dynamical barrier of the vortex edge. We describe a technique to accurately determine the inner edge of the vortex boundary region from measurements of potential temperature and a trace gas, such as N2O, and apply it to in situ aircraft and balloon measurements from the SOLVE/THESE02000 Arctic campaign. The method may be used to refine the Nash algorithm, which, due to the inherently coarser resolution of potential vorticity on which it is dependent, may misidentify the inner edge by up to 466 km, and omit the identification of small, extra-vortex filaments within the vortex.

Greenblatt, Jeffery B.↗
NASA NTRS2002

Argus: a new instrument for the measurement of the stratospheric dynamical tracers, N2O and CH4

We describe here a new instrument for the simultaneous, in situ measurement of the stratospheric tracer molecules, nitrous oxide (N2O) and methane (CH4). Argus is unique in its small size making it well suited for limited payload atmospheric research platforms. Argus employs second harmonic spectroscopy using tunable lead-salt diode lasers emitting in the mid-infrared. We first explain the Argus design philosophy followed by detailed descriptions of the instrument's optical, mechanical, and thermal sub-systems. Argus employs an in-flight calibration system providing real time calibrations and tightly constrained uncertainty estimates of the returned data. Data analysis is carried out using non-linear least-squares model fits to the acquired second harmonic spectra. A sampling of Argus data acquired on a recent stratospheric research campaign in the Arctic winter is presented.

Methane/analysis↗
NASA NTRS2004

Modeling of Isotope Fractionation in Stratospheric CO2, N2O, CH4, and O3: Investigations of Stratospheric Chemistry and Transport, Stratosphere-Troposphere Exchange, and Their Influence on Global Isotope Budgets

We investigated the isotopic fractionation of CH4 and hydrogen (H2) in the stratosphere by incorporating isotope-specific rate coefficients into the Lawrence Livermore National Laboratory (LLNL) 2D model and comparing the model results with new observations from the NASA ER-2 aircraft (funded through a separate task under the Upper Atmosphere Research Program). The model results reveal that fractionation which occurs in the stratosphere has a significant influence on isotope compositions in the free troposphere, an important point which had previously been ignored, unrecognized or unquantified for many long-lived trace gases, including CH4 and H2 which we have focused our efforts on to date. Our analyses of the model results and new isotope observations have also been used to test how well the kinetic isotope effects are known, at least to within the uncertainties in model chemistry and transport. Overall, these results represent an important step forward in our understanding of isotope fractionation in the atmosphere and demonstrate that stratospheric isotope fractionation cannot be ignored in modeling studies which use isotope observations in the troposphere to infer the global budgets of CH4 (an important greenhouse gas) and of H2 (a gas whose atmospheric budget must be better quantified, particularly before a large human perturbation from fuel cell use is realized). Our analyses of model results and observations from the NASA ER-2 aircraft are briefly summarized separately below for CH4, H2, and H2O and for the contribution of these modeling studies to date to our understanding of isotope fractionation for N2O, CO2, and O3 as well.

Boering, Kristie A.↗