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Rowland, F. S.

Publications and source records attributed to Rowland, F. S..

13 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1994

Meridional distributions of NO(X), NO(Y), and other species in the lower statosphere and upper troposphere during AASE 2

The meridional distribution of NO(x) in the lower stratosphere and upper troposphere is inferred form 10 flights of the NASA DC-8 in the northern winter of 1992 along with like distributions of NO(y), NO(x)/NO(y), CO, and C2Cl4. In the lowest few km of the stratosphere there is little vertical gradient in NO(x) over the range of latitiudes measured (40 deg-90 deg N). There is a substantial latitudinal gradient, with 50 pptv above the pole and 120 pptv near 40 deg N. In the uppermost few km of the troposphere, background values range from 30 pptv over the pole to 90 pptv near 40 deg N. On two occasions higher values, up to 140 pptv in the mean, were seen 2-3 km below the tropopause in association with frontal systems. The meridional distributions of CO and C2Cl4 show the same feature, suggesting that the source of the elevated NO(x) is near the earth's system.

Weinheimer, A. J.↗
NASA NTRS1994

Effects of biomass burning on summertime nonmethane hydrocarbon concentrations in the Canadian wetlands

Approximately 900 whole air samples were collected and assayed for selected C2-C10 hydrocarbons and seven halocarbons during the 5-week Arctic Boundary Layer Expedition (ABLE) 3B conducted in eastern Canadian wetland areas. In more than half of the 46 vertical profiles flown, enhanced nonmethane hydrocarbon (NMHC) concentrations attributable to plumes from Canadian forest fires were observed. Urban plumes, also enhanced in many NMHCs, were separately identified by their high correlation with elevated levels of perchloroethene. Emission factors relative to ethane were determined for 21 hydrocarbons released from Canadian biomass burning. Using these data for ethane, ethyne, propane, n-butane, and carbon monoxide enhancements from the literature, global emissions of these four NMHCs were estimated. Because of its very short atmospheric lifetime and its below detection limit background mixing ratio, 1,3-butadiene is an excellent indicator of recent combustion. No statistically significant emissions of nitrous oxide, isoprene, or CFC 12 were observed in the biomass-burning plumes encountered during ABLE 3B. The presence of the short-lived biogenically emitted isoprene at altitudes as high as 3000 m implies that mixing within the planetary boundary layer (PBL) was rapid. Although background levels of the longer-lived NMHCs in this Canadian region increase during the fire season, isoprene still dominated local hydroxyl radical photochemistry within the PBL except in the immediate vicinity of active fires. The average biomass-burning emission ratios for hydrocarbons from an active fire sampled within minutes of combustion were, relative to ethane, ethene, 2.45; ethyne 0.57; propane, 0.25; propene, 0.73; propyne, 0.06; n-butane, 0.09; i-butane, 0.01; 1-butene, 0.14; cis-2-butene, 0.02; trans-2-butene, 0.03; i-butylene, 0.07; 1,3-butadiene, 0.12; n-pentane, 0.05; i-pentane, 0.03; 1-pentene, 0.06; n-hexane, 0.05; 1-hexene, 0.07; benzene, 0.37; toluene, 0.16.

Blake, D. R.↗
NASA NTRS1993

AASE-2 observations of trace carbon species distributions in the mid to upper troposphere

We report tropospheric (altitudes greater than 5 km) observations of CO2, CO, CH4, and light hydrocarbons (C2-C4) over the latitude range from 90 deg N to 23 deg S recorded onboard the NASA DC-8 aircraft during the winter 1992 Second Airborne Arctic Stratospheric Expedition (AASE-2). Mixing ratios for these species exhibited significant north-south gradients with maximum values in subpolar and arctic regions and minima over the southern tropics. At latitudes greater than 40 deg N, the mixing ratios of most species increased significantly over the course of the 3-month measurement period. Also at high northern latitudes, the variations of all relatively long-lived reactive carbon species were linearly correlated with fluctuations of CO2 with CO, CH4, C2H6, C2H2, C3H8, and n-C4H10 exhibiting average enhancement ratios in terms of ppbv(X)/ppmb(CO2) of 13.8, 8.4, 0.21, 0.075, 0.085, and 0.037, respectively.

Anderson, B. E.↗
NASA NTRS1993

AASE-2 Observations of Trace Carbon Species Distributions in the Mid to Upper Troposphere

We report tropospheric (altitudes greater than 5 km) observations of CO2, CO, CH4, and light hydrocarbons (C2-C4) over the latitude range from 90 deg N to 23 deg S recorded onboard the NASA DC-8 aircraft during the winter 1992 Second Airborne Arctic Stratospheric Expedition (AASE-II). Mixing ratios for these species exhibited significant north-south gradients with maximum values in subpolar and arctic regions and minima over the southern tropics. At latitudes greater than 40 deg N, the mixing ratios of most species increased significantly over the course of the 3-month measurement period. Also at high northern latitudes, the variations of all relatively long-lived reactive carbon species were linearly correlated with fluctuations of CO2 with CO, CH4, C2H6, C2H2, C3H8, and n-C4H10 exhibiting average enhancement ratios in terms of ppbv(X)/ppmv(CO2) of 13.8, 8.4, 0.21, 0.075, 0.085, and 0.037, respectively.

Anderson, B. E.↗
NASA NTRS1992

Summertime measurements of selected nonmethane hydrocarbons in the Arctic and Subarctic during the 1988 Arctic Boundary Layer Expedition (ABLE 3A)

The concentration distributions of several nonmethane hydrocarbons (NMHIC) in the Arctic and Subarctic regions of Alaska are discussed using data obtained during July and August of 1988 as part of the Arctic Boundary Layer Expedition (ABLE 3A). Plume enhancement of some or all of the measured NMHIC were observed on more than half of the 33 missions flown during the project. The usual summer vertical profile of reactive hydrocarbons at these high latitudes has elevated concentrations at high altitudes, with mixing ratio variations largely controlled by hydroxyl radical reactions. Wildfires were established as a significant source of various NMHIC. Biomass burning emission ratios relative to ethane were established for ethyne (0.38 +/- 0.04) and propane (0.08 +/- 0.03). Activities associated with oil drilling are a probable source of enhanced levels of alkanes observed as much as 300 km northeast of Prudhoe Bay.

Blake, Donald R.↗
NASA NTRS1989

Trends in total column ozone measurements

It is important to ensure the best available data are used in any determination of possible trends in total ozone in order to have the most accurate estimates of any trends and the associated uncertainties. Accordingly, the existing total ozone records were examined in considerable detail. Once the best data set has been produced, the statistical analysis must examine the data for any effects that might indicate changes in the behavior of global total ozone. The changes at any individual measuring station could be local in nature, and herein, particular attention was paid to the seasonal and latitudinal variations of total ozone, because two dimensional photochemical models indicate that any changes in total ozone would be most pronounced at high latitudes during the winter months. The conclusions derived from this detailed examination of available total ozone can be split into two categories, one concerning the quality and the other the statistical analysis of the total ozone record.

Rowland, F. S.↗
NASA NTRS1989

Trends in source gases

Source gases are defined as those gases that, by their breakdown, introduce into the stratosphere halogen, hydrogen, and nitrogen compounds that are important in stratospheric ozone destruction. Given here is an update of the existing concentration time series for chlorocarbons, nitrous oxide, and methane. Also reviewed is information on halogen containing species and the use of these data for establishing trends. Also reviewed is evidence on trends in trace gases that influence tropospheric chemistry and thus the tropospheric lifetimes of source gases, such as carbon dioxide, carbon monoxide, or nitrogen oxides. Much of the information is given in tabular form.

Ehhalt, D. H.↗
NASA NTRS1988

Thermochemical stabilities and vibrational spectra of isomers of the chlorine oxide dimer

Molecular orbital calculations were performed to determine the relative thermochemical stabilities and IR vibrational spectra of isomers of the ClO dimer. Two straight-chain isomers (ClOOCl and ClOClO) and one branched species (ClClO2) were identified as energy minima on the Cl2O2 potential surface. It is shown that ClOOCl and ClClO2 are comparable in terms of stability, while ClOClO is about 11 kcal/mol higher in energy. The IR spectra obtained by Molina and Molina (1987) as a result of the reaction of chlorine atoms with ClO precursors are consistent with the production of the two most stable forms of Cl2O2.

Mcgrath, M. P.↗
NASA NTRS1988

Wintertime losses of ozone in high northern latitudes

Total column ozone data over the past 22 to 30 years from ground-based Dobson and filter ozonometer stations between 30 N and 80 N are analyzed for residual trends remaining after allowance for the known geophysical variations corresponding to: (1) the change of seasons; (2) the quasi-biennial oscillation; and (3) the 11-year solar sunspot cycle. Examination of the data from several ground stations between 45 and 55 N indicated a seasonal difference in the long-term ozone series, with statistically significant losses in several winter months. Accordingly, the data from individual stations were analyzed with multiple regression analysis, seeking trends on a monthly basis after allowance for the known geophysical cycles. Previous statistical analyses were conducted as tests of 1-D model calculations which do not show any differences with the seasons, and any trend toward change in ozone concentrations is expressed in a yearly trend without seasonal variation. Such a model is inappropriate for calculations with a data set which exhibits a pronounced tendency toward seasonal differences in the trends. Comparisons with model calculations then require 2-D models into which seasonal and latitudinal differences can easily be programmed.

Harris, Neil↗
NASA NTRS1986

Global atmospheric concentrations and source strength of ethane

A study of the variation in ethane (C2H6) concentration between northern and southern latitudes over three years is presented together with a new estimate of its source strength. Ethane concentrations vary from 0.07 to 2 p.p.b.v. (parts per billion by volume) in air samples collected in remote surface locations in the Pacific (latitude 71 N-47 S) in all four seasons between September 1984 and June 1985. The variations are consistent with southerly transport from sources located chiefly in the Northern Hemisphere, further modified by seasonal variations in the strength of the reaction of C2H6 with OH radicals. These global data can be combined with concurrent data for CH4 and the laboratory reaction rates of each with OH to provide an estimate of three months as the average atmospheric lifetime for C2H6 and 13 + or - 3 Mtons for its annual atmospheric release.

Blake, D. R.↗
NASA NTRS1986

World-wide increase in tropospheric methane, 1978-1983

Techniques used to assess methane concentration in the troposphere are described, and data obtained during the period from 1978 to 1983 are presented in detail. Tropospheric methane concentrations in remote locations averaged a yearly world-wide increase of 0.018 + or - 0.002 parts per million by volume (ppmv). Average world-wide tropospheric concentration of methane in dry air was 1.625 ppmv at the end of 1983 measured against an NBS standard certified as 0.97 ppmv. Contributing to this steady increase in methane concentration are increases in the source strengths from cattle and rice fields, which in turn result from CO, CH4 and HO coupling. Among the physical and chemical effects is an increase in greenhouse warming of about 0.04 C per decade.

Blake, D. R.↗
NASA NTRS1984

Methane concentrations and source strengths in urban locations

The results of a six year measurement of trace gases in 18 different urban and remote areas throughout the Northern and Southern Hemispheres are reported. It is found that the measurements are consistent with a yearly atmospheric release of 30 to 60 megatons of CH4 in urban environments. Concentrations of CCl3F, CCl2F2, and CH3CCl3 were also found to be higher in the same urban samples than in corresponding samples from remote areas. The 'urban excess' (urban concentration minus remote concentration) was generally 1000 to 2000 times larger on a molar basis for CH4 than for CCl3F. The fraction of world-wide methane release occurring in the urban environment is estimated from the concentration ratios for CH4 vs CCl3F. It is shown that about 8 to 15 percent of atmospheric methane release occurs in urban areas.

Blake, D. R.↗