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NASA NTRS2021

Tropospheric Age-of-Air: Influence of SF6 Emissions on Recent Surface Trends and Model Biases

The mean age since air was last at the Northern Hemisphere (NH) midlatitude surface is a fundamental property of tropospheric transport. Here we approximate the mean age in terms of an "SF6 age" (ΓSF6), derived from surface and aircraft measurements of SF6 that are broader in spatial scope and cover a longer time period (1997-2018) than considered previously. At the surface, ΓSF6 increases from near-zero values north of 30°N to ~1.5 years over the Southern Hemisphere (SH) extratropics, with the largest meridional gradients occurring in the tropics. By comparison, vertical gradients in ΓSF6 are weak throughout, with only slight increases/decreases with height in the NH/SH. The broader spatial coverage of the measurements reveals strong variations in the seasonal cycle of ΓSF6 within the (sub)tropics that are weaker over the Atlantic and Paci c oceans, compared to over the Indian Ocean. Observations from 2000-2018 reveal that the SF6 age at sites in the SH has been decreasing by ~0.12 yr/dec. However, this decrease is not due to changes in transport but, rather, is likely related to changes in emissions, which have increased globally and reportedly shifted from northern midlatitudes into the subtropics. Simulations, which reproduce the SF6 age trends, show no decreases in an age-of-air tracer, reinforcing the fact that ΓSF6 represents only an approximation to the mean age. Finally, the modeled SF6 ages are older than observed, by ~0.3-0.4 years throughout the southern extratropics. We show that this bias is partly related to an overestimation in simulated SF6 near emissions regions,

Mean age↗
NASA NTRS1990

Infrared spectroscopic detection of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere

This paper reports the detection and identification of the unresolved SF6 nu-3 band Q branch at 947.9/cm in high-resolution solar occultation spectra of the lower stratosphere and upper troposphere, which was made from the analysis of data recorded on April 30 to May 1, 1985 by the spaceborne Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer as part of the Spacelab 3 mission. On the basis of SF6 line-by-line parameters obtained from the laboratory studies of Bobin et al. (1987) and Schatz and Hornig (1953), the measured absorption was analyzed to deduce SF6 volume mixing ratios in the altitude range 12-22 km. It was found that, in this altitude range, the SF6 volume mixing ratio is independent of altitude, with an average measured value of 1.42 parts per trillion by volume (pptv) at 31 deg N latitude.

Rinsland, C. P.↗
NASA NTRS1993

ATMOS/ATLAS 1 measurements of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere

Vertical profiles of sulfur hexafluoride (SF6) in the lower stratosphere and upper troposphere have been retrieved from 0.01/cm resolution infrared solar occultation spectra recorded by the Atmospheric Trace Molecule Spectroscopy (ATMOS) Fourier transform spectrometer during the ATLAS (Atmospheric Laboratory for Applications and Science) 1 shuttle mission of March 24 to April 2, 1992. Based on measurements of the unresolved absorption by the SF6 mu(sub 3) band Q branch at 947.9/cm, average SF6 volume mixing ratios and 1-sigma uncertainties of 3.20 +/- 0.54 parts per trillion by volume (pptv; 10(exp -12) ppv) at 200 mbar (approximately 11.8 km) declining to 2.86 +/- 0.29 pptv at 100 mbar (approximately 16.2 km) and 1.95 +/- 0.50 pptv at 30 mbar (approximately 23.9 km) have been retrieved. The profiles show no obvious dependence with latitude over the range of the measurements (eight occultations spanning 28 deg S to 54 deg S). Assuming an exponential growth model and applying a correction for the interhemispheric concentration difference, an average SF6 rate of increase of 8.7 +/- 2.2% per year, 2 sigma, between 12 and 18 km has been derived by fitting the present measurements, ATMOS measurements from the April-May 1985 Spacelab 3 mission, and balloon-borne IR measurements obtained in March 1981 and June 1988.

Rinsland, C. P.↗
NASA NTRS1990

Long-Term Trends in the Concentrations of SF6, CHClF2, and COF2 in the Lower Stratosphere from Analysis of High-Resolution Infrared Solar Occultation Spectra

Long-term trends in the concentrations of SF6, CHClF2 (CFC-22), and COF2 in the lower stratosphere have been derived from analysis of ca. 1980 and more recent infrared solar occultation spectra recorded near 32 deg N latitude at approx. 0.02/ cm resolution. Consistent sets of line parameters and spectral calibration methods have been used in the retrievals to minimize systematic error effects. Quoted error limits are 1 sigma estimated precisions. The SF6 and CHClF2 results are based on spectra recorded by balloon-borne interferometers in March 1981 and June 1988 and a comparison of these results with the Atmospheric Trace Molecule Spectroscopy (ATMOS) Experiment/Spacelab 3 measurements obtained in May 1985 near 30 deg N latitude. In the 13-18 km altitude range the mean measured SF6 mixing ratio in parts per trillion by volume (pptv) increased from 1.17 +/- 0.21 in March 1981 to 2.02 +/- 0.20 pptv in June 1988, and the CHClF2 mixing ratio below 15 km altitude increased from 51 +/- 8 pptv in March 1981 to 102 +/- 10 pptv in June 1988. The CHClF2 retrievals used new empirical CHClF2 line parameters derived from 0.03/cm resolution laboratory spectra recorded at six temperatures between 203 and 293 K; the derived mixing ratios are approx. 30% higher than obtained with earlier sets of line parameters, thereby removing a large discrepancy noted previously between IR and in situ measurements of CHClF2. Assuming an exponential growth model for fitting the trends, SF6 and CHClF2 mean increase rates of 7.4% +/- 1.9% and 9.4% +/- 1.3% /year, are obtained, respectively, which correspond to cumulative increases by factors of approx. 1.7 and -2.0 in the concentrations of these gases over the 7.2-year measurement period. Analysis of spectra recorded in October 1979 and April 1989 yields COF2 volume mixing ratios that are respectively 0.44 +/- 0.17 and 1.21 +/- 0.24 times the ATMOS/Spacelab 3 values, from which an average COF2 increase rate of 10.3 +/- 1.8%/ year over this time period has been estimated. The present results are compared with previously reported observations and trends and with one-dimensional model calculations. The model calculated trends are in reasonably good agreement with the observations.

Rinsland, C. P.↗
NASA NTRS1980

Energy-transfer mechanisms in the CH3F-SF6 optically pumped laser

The power of an optically pumped CH3F laser operating on the 496-micron line has been doubled with the addition of SF6 without any corresponding increase in pump absorption. It is suggested that a near-resonant energy transfer between CH3F and SF6 followed by SF6 deactivation is the mechanism responsible for the enhancement.

Lawandy, N. M.↗
NASA NTRS1986

Comparison of calculated and experimental thermal attachment rate constants for SF6 in the temperature range 200-600 K

Electron-attachment cross sections are calcualted for the process e(-) + SF6 yields SF6(-) in the energy range 1-200 meV. An electron scattering approximation is used in which diatomiclike potential energy curves near the equilibrium SF6 ground state are constructed from recent spectroscopic data. Excellent agreement is found over the entire energy range with experimental attachment cross sections at a temperature of 300 K for s-wave (l = 0) scattering. The same calculation, with appropriate adjustment of the thermal populations, is used to calculate attachment rate constants in the range 50-600 K for both s- and p-wave scattering.

Orient, O. J.↗
NASA NTRS2002

Mass Conservation in a Chemical Transport Model and its Effect on CO2 and SF6 Simulations

Chemical transport models (CTMs) must conserve mass to be useful for applications involving assessment of the effect of various pollutants on the troposphere and stratosphere. Furthermore, calculations of the evolution of constituents such as SF6 are used to evaluate overall model transport, and interpretation of such simulations is clouded if mass conservation is not assured. For realistic simulations or predictions, it is crucial that constituents are not produced or lost by transport or other processes in the CTMs. Analysis of CO2 and SF6 experiments using a CTM shows that problems with mass conservation can seriously degrade the simulations. Failure to conserve mass results from inconsistency of the surface pressure tendency and the divergence of horizontal mass flux when the model is forced by assimilated meteorological data. We have developed an effective method to eliminate the inconsistency by modifying the divergent part of the wind field. The changes in the wind fields are quite small but the impact on mass conservation is large. Parameterizations of physical processes such as convection or turbulent transport can also affect mass conservation. The lack of conservation is small but accumulates when integrations are lengthy such as required for SF6. This lack of conservation is found using winds from either a GCM or from an assimilation system. A simple adjustment removes much of the inaccuracy in the convective parameterization. A CO2 simulation using assimilated winds from the most recent version of the Goddard Earth Observing System Data Assimilation System will be used to illustrate the impact of these transport improvements.

Zhu, Z.↗
NASA NTRS1985

s-wave threshold in electron attachment - Observations and cross sections in CCl4 and SF6 at ultralow electron energies

The threshold photoionization method was used to study low-energy electron attachment phenomena in and cross sections of CCl4 and SF6 compounds, which have applications in the design of gaseous dielectrics and diffuse discharge opening switches. Measurements were made at electron energies from below threshold to 140 meV at resolutions of 6 and 8 meV. A narrow resolution-limited structure was observed in electron attachment to CCl4 and SF6 at electron energies below 10 meV, which is attributed to the divergence of the attachment cross section in the limit epsilon, l approaches zero. The results are compared with experimental collisional-ionization results, electron-swarm unfolded cross sections, and earlier threshold photoionization data.

Chutjian, A.↗
NASA NTRS1985

Measurements of CCl3F, CCl2F2, CCl4, N2O and SF6 in the Northern Hemisphere stratosphere

An overview of the Department of Energy's High Altitude Sampling Program and some recent trace gas measurement results are presented. Analysis of whole air samples, collected in pressurized bottles, provides information on stratospheric inventories and distributions for CCl3F, CCl2F2, CCl4, N2O and SF6 in the Northern Hemisphere. Based on a linear regression analysis of the data the estimated mean Northern Hemisphere stratospheric concentration of each gas increased as follows: CCl3F changed from 54 to 142 p1/1 (4/74-11/83); CCl2F2 changed from 133 to 268 p1/1 (4/76-11/83); SF6 changed from 160 to 480 f1/1 (4/74-11/83); CC1, changed from 58 to 91 p1/1 (4/75-11/83); N2O changed from 246 to 261 n1/1 (4/76-11/83). The calculated mean Northern Hemisphere stratospheric concentrations of N2O, CCl3F, CCl2F2, and CCl4 after 1980 show larger than expected fluctuations with time. Recent volcanic activity may be a partial cause for these fluctuations through induced changes in stratospheric dynamical processes.

Leifer, R.↗
NASA NTRS1990

Long-term trends in the concentrations of SF6, CHClF2, and COF2 in the lower stratosphere from analysis of high-resolution infrared solar occultation spectra

Long-term trends in the concentrations of SF6, CHClF2 in the lower stratosphere are derived using results from analyses of the 1980 and of several more recently obtained IR solar occultation spectra. Results show that the increase rates of SF6 and CHClF2 were about 7.4/yr and 9.4/yr, respectively, which correspond to cumulative increases by factors of about 1.7 and 2.0 in the concentrations of these gases over the 7.2 yr measurement period. The average increase rate for COF2 was 10.3/yr over the same time period. The present results are compared with previously reported observations and trends and with one-dimensional model calculations.

Rinsland, C. P.↗
NASA NTRS1996

Trends of OCS, HCN, SF6, CHClF2 (HCFC-22) in the Lower Stratosphere from 1985 and 1994 Atmospheric Trace Molecule Spectroscopy Experiment Measurements Near 30 deg. North Latitude

Volume mixing ratio (VMR) profiles of OCS, HCN, SF6, and CHClF2 (HCFC-22) have been measured near 30 deg N latitude by the Atmospheric Trace Molecule Spectroscopy Fourier transform spectrometer during shuttle flights on 29 April - 6 May 1985 and 3-2 November 1994. The change in the concentration of each molecule in the lower stratosphere has been derived for this 9 1/2-year period by comparing measurements between potential temperatures of 395 to 800 K (approximately 17 to 30 km altitude) relative to simultaneously measured values of the long-lived tracer N2O. Exponential rates of increase inferred for 1985-to 1994 from these comparisons are (0.1 plus or minus 0.4)% yr(exp-1) for OCS, (1.0 plus or minus 1.0)% yr(exp-1) for HCN, (8.0 +/- 0.7)% yr(exp-1) for SF6, and (8.0 +/- 1.0)% yr(exp-1) for CHClF2 (HCFC-22), 1 sigma. The lack of an appreciable trend for OCS suggests the background (i.e. nonvolcanic) source of stratospheric aerosol was the same during the two periods. These results are compared with trends reported in the literature.

Rinsland, C. P.↗
NASA NTRS1976

Absolute elastic differential electron scattering cross sections in the intermediate energy region. III - SF6 and UF6

A recently developed technique has been used to measure the ratios of elastic differential electron scattering cross sections (DCS) for SF6 and UF6 to those of He at electron impact energies of 5, 10, 15, 20, 30, 40, 50, 60, and 75 eV and at scattering angles of 20 to 135 deg. In order to obtain the absolute values of DCS from these ratios, He DCS of McConkey and Preston have been employed in the 20 to 90 deg range. At angles in the 90 to 135 deg range the recently determined cross sections of Srivastava and Trajmar have been utilized. From these DCS, elastic integral and momentum transfer cross sections have been obtained.

Srivastava, S. K.↗
NASA NTRS1977

Electron impact excitation of SF6

A study of the electron impact energy-loss spectrum of SF6 under both optical (low scattering angle, high impact energy) and non-optical conditions (high scattering angle, low impact energy) has revealed a number of electronic excitation processes. With the help of theoretical calculations, several of these transitions have been assigned and approximate cross sections associated with four features have been determined. In addition, a strong resonance at 12 eV has been observed in both elastic and vibrationally inelastic (delta E = 0.092 eV) channels.

Trajmar, S.↗
NASA NTRS1977

Collisionless dissociation of SF6 using two resonant frequency CO2 laser fields

The collisionless dissociation of SF6 has been studied using simultaneous irradiation by two frequencies from a CO2 laser which are both nearly resonant with the SF6nu3 absorption band. It was found that the dissociation was enhanced, and occurred over a wider frequency range, than for single frequency dissociation. No threshold effect was observed for a weak resonant and a much higher energy field pumping slightly off-resonance. For such two frequency irradiation, the peak in the dissociation curve was found to be shifted to lower frequencies with respect to that for single frequency dissociation.

Gower, M. C.↗
NASA NTRS1981

Experimental SF6/-//SF6 and Cl/-//CFC13 electron-attachment cross sections in the energy range 0-200 meV

Experimental cross sections for the electron-attachment processes for SF6(-)/SF6 and Cl(-)/CFl3 are reported in the energy range 0-200 meV by normalizing each attachment line shape to measurement of a thermal rate coefficient. When the same ion states are detected, good agreement is found between present values, for which a monoenergetic electron source is used, and swarm-unfolded results. The present data constitute a new limit for cross sections reported at high resolution at the lowest electron energy.

Chutjian, A.↗
NASA NTRS1982

Calculation of SF6-/SF6 and Cl-/CFCl3 electron attachment cross sections in the energy range 0-100 meV

Electron attachment cross sections for the processes SF6-/SF6 and Cl-/CFCl3 are calculated in a local theory using a model in which diatomic-like potential energy curves for the normal modes are constructed from available spectroscopic data. Thermally populated vibrational and rotational levels are included. Good agreement is found with experimental cross sections in the energy range 5-100 meV for a particular choice of potential energy curve parameters.

Chutjian, A.↗
NASA NTRS1987

Effects on H(-) production in a multicusp ion source by mixture of H2 with H2O, NH3, CH4, N2H4, and SF6

Effects of H(-) production in a multicusp ion source are measured by separately mixing with hydrogen small amounts (0.33-10 percent) of water, ammonia, methane, and hydrazine these are molecules which produce large amounts of H(-) via dissociative attachment (DA) resonances at higher electron energies. The mixing was done in a separate reservoir, with careful measurement of individual pressures. Experimental enhancements of 1.4 and less were observed, whereas calculated enhancements, using accurate DA cross sections for ground-state H2, should have produced factors of 1.5, 3.0, 1.3, and 2.4 enhancements for water, ammonia methane, and hydrazine, respectively, at a mean electron energy of 1.0 eV in the extraction region. The difference is accounted for by including, in the enhancement calculation, vibrationally and rotationally excited H2 molecules, with v-double prime = 5-11, and J-double prime = 0-5, and the large DA cross sections for the excited H2 (v-double prime, J-double prime). The relative populations of H2 (v-double prime, J-double prime) thus obtained are found to be substantially smaller than those predicted by theoretical calculations. The effect on H(-) current was also studied by mixing small amounts of SF6 with H2. A 1.5 percent mixture was found to reduce the H(-) output by one half.

Orient, O. J.↗
NASA NTRS1991

Infrared spectroscopic measurements of the vertical column abundance of sulfur hexafluoride, SF6, from the ground

The solar observations involved in the present monitoring evaluation were made at two facilities, using Fourier-transform spectrometers achieving spectral resolutions of 0.005/cm and signal-to-rms noise ratios for individual scans from near 500 to near 1000. The monthly mean total vertical-column abundances of SF6 above both facilities are reported for time intervals from June 1986 to June 1990 and from March 1981 to June 1990. It is found that the vertical-column abundances increased at mean rates of 6.9 +/- 2.8 pct above one station and 6.6 +/- 7.2 pct above the other. Since all the results were retrieved using the same spectroscopic parameters and similar nonlinear least-squares curve-fitting algorithms validated through intercomparison exercises, the large error reported for the second station is attributed to a larger measurement uncertainty due to stronger H2O and C2O interferences, and a greater variability during each month.

Zander, R.↗