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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 NTRS1994

Ozone and aerosol distributions in the summertime troposphere over Canada

Measurements of ozone (O3) and aerosol distributions were made with an airborne lidar system in the lowland and boreal forest regions of eastern Canada during July - August 1990 as part of the NASA Global Tropospheric Experiment/Arctic Boundary Layer Expedition (ABLE) 3B. Aerosol and O3 profiles were measured simultaneously above and below the Electra aircraft from near the surface to above the tropopause on long-range flights over these important ecosystems. A broad range of atmospheric conditions were encountered during repeated flights over intensive study sites in the Hudson Bay lowlands near Moosonee, Ontario, and over the boreal forest near Schefferville, Quebec. The tropospheric composition in this high-latitude region was found to be strongly influenced by stratospheric intrusions. Regions of low aerosol scattering and enhanced O3 mixing ratios were correlated with descending air from the lower stratosphere. Over 33% of the troposphere (0-12 km) along our flight track at latitudes from about 45 deg to 55 deg N had significantly enhanced O3 due to stratospheric intrusions, and in the middle to upper troposphere the extent of the enhanced O3 gnerally exceeded 40%. Ozone mixing ratios of 80 parts per billion by volume (ppbv) near 6 km were common in strong intrusions. In the boundary layer over the lowlands, O3 was in the 20-30 ppbv range with a vertical O3 gradient of 6.7 ppbv/km to about 45 ppbv at 3 km. Above 6 km the background tropospheric O3 profile was nearly constant with an average value of 53 ppbv. Due to forest fires in Canada and Alaska, plumes from biomass-burning sources were observed on many flights. Biomass-burning plumes influenced about 25% of the free troposphere below 4 km, and in some of the plumes, O3 was enhanced by 10-20 ppbv over ambient levels of 30-45 ppbv. Several air masses transported from the tropical Pacific were observed over Canada in the middle to upper troposphere with O3 levels 10-20 ppbv below background values of 50-55 ppbv.

Browell, E. V.↗
NASA NTRS1994

Chemical composition of the atmospheric aerosol in the troposphere over the Hudson Bay lowlands and Quebec-Labrador regions of Canada

Atmospheric aerosols were collected in the boundary layer and free troposphere over continental and coastal subarctic regions of Canada during the July - August 1990 joint U.S.-Canadian Arctic Boundary Layer Expedition (ABLE) 3B/Northern Wetlands Study (NOWES). The samples were analyzed for the following water soluble species: sulfate, nitrate, ammonium, potassium, sodium, chloride, oxalate, methylsulfonate, and total amine nitrogen. Ammonium and sulfate were the major water soluble components of these aerosols. The nearly neutral (overall) chemical composition of summertime aerosol particles contrasts their strongly acidic wintertime composition. Aerosol samples were separated into several air mass categories and characterized in terms of chemical composition, associated mixing ratios of gaseous compounds, and meteorological parameters. The fundamental category represented particles associated with 'background' air masses. The summertime atmospheric aerosols in background air over the North American subarctic and Arctic regions were characterized by relatively small and spatially uniform mixing ratios of the measured species. These aerosol particles were aged to the extent that they had lost their primary source signature. The chemical profile of the background air aerosols was frequently modified by additions from biomass fire plumes, aged tropical marine air, and intrusions of upper tropospheric/lower stratospheric air. Aerosols in boundary layer background air over the boreal forest region of Quebec-Labrador had significantly larger mixing ratios of ammonium and sulfate relative to the Hudson Bay region. This may reflect infiltration of anthropogenic pollution or be due to natural emissions from this region.

Gorzelska, K.↗
NASA NTRS1994

Summertime tropospheric ozone distributions over central and eastern Canada

Ozone measurements were obtained between the surface and the 6-km altitude on aircraft flights over central and eastern Canada during the summer 1990 NASA Global Tropospheric Experiment Arctic Boundary Layer Expedition (GTE/ABLE 3B). Tropospheric O3 budgets for these regions were observed to be highly variable and significantly impacted by long-range transport and regional scale air mass modification processes. For example, integrated O3 abundance below 5-km altitude averaged 40% and 30% greater in air masses influenced by anthropogenic sources and biomass burning, respectively, than in background (polar) air. Conversely, aged air transported from subtropical areas of the Pacific at times reduced O3 abundance in this height interval by up to 20%. Though intrusion of anthropogenic air was infrequent during the experiment period, the influence of biomass-burning emissions was particularly notable as two thirds of the flights sampled air influenced by plumes from fires burning in Alaska and western Canada. The impinging pollution, both natural and anthropogenic, not only elevated O3 levels directly but also was a source of reactive nitrogen (and nonmethane hydrocarbons) which generally increases the tropospheric lifetime of O3 via moderation of photochemical destruction rates.

Anderson, B. E.↗
NASA NTRS1994

Stratospheric/tropospheric exchange affecting the northern wetlands regions of Canada during summer 1990

The Arctic Boundary Layer Expedition (ABLE) 3B was conducted over the northern wetlands region of Canada during July and August 1990. Several stratospheric/tropospheric exchange events were noted by zenith-looking airborne lidar and in situ measurements of ozone and other trace gas species. Isentropic trajectories and potential vorticity analyses are utilized to determine the frequency of stratospheric inputs which would have affected the tropospheric column over the Moosonee and Schefferville regions and to describe the favored pathways of transport of stratospheric air arriving at these locations. At the 310 K potential temperature level (middle troposphere), trajectories having 'aged stratospheric' values of potential vorticity at some point in their 5-day history arrived at Moosonee or Schefferville roughly 40% of the time during the ABLE 3B study period, most often via large-scale subsidence enroute from 'stratospheric input regions' over the Arctic Ocean or northern and central Canada. At 325 K (upper troposphere), 'fresh' stratospheric input was evident on about 80% of the trajectories, most often associated with jet streaks within the polar and Arctic jet streams. A case study is presented which illustrates both of these general stratospheric input processes.

Bachmeier, A. Scott↗
NASA NTRS1994

Summertime distribution of PAN and other reactive nitrogen species in the northern high-latitude atmosphere of eastern Canada

Aircraft measurements of key reactive nitrogen species (NO, NO2, HNO3, PAN, PPN, NO3(-), NO(y)), C1 to C6 hydrocarbons, acetone, O3, chemical tracers (C2Cl4, CO), and important meteorological parameters were performed over eastern Canada during July to August 1990 at altitudes between 0 and 6 km as part of an Arctic Boundary Layer Expedition (ABLE3B). In the free troposphere, PAN was found to be the single most abundant reactive nitrogen species constituting a major fraction of NO(y) and was significantly more abundant than NO(x) and HNO3. PAN and O3 were well correlated both in their fine and gross structures. Compared to data previously collected in the Arctic/subarctic atmosphere over Alaska (ABLE3A), the lower troposphere (0-4 km) over eastern Canada was found to contain larger reactive nitrogen and anthropogenic tracer concentrations. At higher altitudes (4-6 km) the atmospheric composition was in many ways similar to what was seen over Alaska and supports the view that a large-scale reservoir of PAN (and NO(y)) is present in the upper troposphere over the entire Arctic/subarctic region. The reactive nitrogen budget based on missions conducted from the North Bay site (missions 2-10) showed a small shortfall, whereas the budget for data collected from the Goose Bay operation (missions 11-19) showed essential balance. It is calculated that 15-20 ppt of the observed NO(x) may find its source from the available PAN reservoir. Meteorological considerations as well as relationships between reactive nitrogen and tracer species suggest that the atmosphere over eastern Canada during summer is greatly influenced by forest fires and transported industrial pollution.

Singh, H. B.↗
NASA NTRS1994

Summertime partitioning and budget of NO(y) compounds in the troposphere over Alaska and Canada: ABLE 3B

As part of NASA's Arctic Boundary Layer Expedition 3A and 3B field measurement programs, measurements of NO(x), HNO3, PAN, PPN, and NO(y) were made in the middle to lower troposphere over Alaska and Canada during the summers of 1988 and 1990. These measurements are used to assess the degree of closure within the reactive odd nitrogen (N(x)O(y)) budget through the comparison of the values of NO(y) measured with a catalytic convertor to the sum of individually measured NO(y) (i) compounds (i.e., sigmaNO(y)(i) = NO(x) + HNO3 + PAN + PPN). Significant differences were observed between the various study regions. In the lower 6 km of the troposphere over Alaska and the Hudson Bay lowlands of Canada a significant fraction of the NO(y) budget (30 to 60%) could not be accounted for by the measured sigmaNO(y)i. This deficit in the NO(y) budget is about 100 to 200 parts per trillion by volume (pptv) in the lower troposphere (0.15 to 3 km) and about 200 to 400 pptv in the middle free troposphere (3 to 6.2 km). Conversely, the NO(y) budget in the northern Labrador and Quebec regions of Canada is almost totally accounted for within the combined measurement uncertainties of NO(y) and the various NO(y)(i) compounds. A substantial portion of the NO(y) budget's 'missing compounds' appears to be coupled to the photochemical and/or dynamical parameters influencing the tropospheric oxidative potential over these regions. A combination of factors are suggested as the causes for the variability observed in the NO(y) budget. In addition, the apparent stability of compounds represented by the NO(y) budget deficit in the lower-altitude range questions the ability of these compounds to participate as reversible reservoirs for 'active' odd nitrogen and suggest that some portion of the NO(y) budget may consist of relatively unreactive nitrogen-containing compounds.

Sandholm, S.↗
NASA NTRS1994

Summertime distribution and relations of reactive odd nitrogen species and NO(y) in the troposphere over Canada

We report here large-scale features of the distribution of NO(x), HNO3, PAN, particle NO3, and NO(y) in the troposphere from 0.15 to 6 km altitude over central Canada. These measurements were conducted in July - August 1990 from the NASA Wallops Electra aircraft as part of the joint United States-Canadian Arctic Boundary Layer Expedition (ABLE) 3B-Northern Wetlands Study. Our findings show that this region is generally NO(x) limited, with NO(x) mixing ratios typically 20-30 parts per trillion by volume (pptv). We found little direct evidence for anthropogenic enhancement of mixing ratios of reactive odd nitrogen species and NO(y) above those in 'background' air. Instead, it appears that enhancements in the mixing ratios of these species were primarily due to emissions from several day old or CO-rich-NO(x)-poor smoldering local biomass-burning fires. NO(x) mixing ratios in biomass-burning impacted air masses were usually less than 50 pptv, but those of HNO3 and PAN were typically 100-300 pptv representing a twofold-threefold enhancement over 'background' air. During our study period, inputs of what appeared to be aged tropical air were a major factor influencing the distribution of reactive odd nitrogen in the midtroposphere over northeastern North America. These air masses were quite depleted in NO(y) (generally less than 150 pptv), and a frequent summertime occurrence of such air masses over this region would imply a significant influence on the reactive odd nitrogen budget. Our findings show that the chemical composition of aged air masses over subarctic Canada and those documented in the Arctic during ABLE 3A have strikingly similar chemistries, suggesting large-scale connection between the air masses influencing these regions.

Talbot, R. W.↗
NASA NTRS1994

Reactive nitrogen oxides and ozone above a taiga woodland

Measurements of reactive nitrogen oxides (NO(x) and NO(y)) and ozone (O3) were made in the planetary boundary layer (PBL) above a taiga woodland in northern Quebec, Canada, during June-August, 1990, as part of NASA Artic Boundary Layer Expedition (ABLE) 3B. Levels of nitrogen oxides and O3 were strongly modulated by the synoptic scale meteorology that brought air from various source regions to the site. Industrial pollution from the Great Lakes region of the U.S. and Canada appears to be a major source for periodic elevation of NO(x), and NO(y) and O3. We find that NO/NO2 ratios at this site at midday were approximately 50% those expected from a simple photochemical steady state between NO(x) and O3, in contrast to our earlier results from the ABLE 3A tundra site. The difference between the taiga and tundra sites is likely due to much larger emissions of biogenic hydrocarbons (particularly isoprene) from the taiga vegetation. Hydrocarbon photooxidation leads to relatively rapid production of peroxy radicals, which convert NO to NO2, at the taiga site. Ratios of NO(x) to NO(y) were typically 2-3 times higher in the PBL during ABLE 3B than during ABLE 3A. This is probably the result of high PAN levels and suppressed formation of HNO3 from NO2 due to high levels of biogenic hydrocarbons at the ABLE 3B site.

Bakwin, Peter S.↗
NASA NTRS1994

The Mbale meteorite shower

On 1992 August 14 at 12:40 UTC, an ordinary chondrite of type L5/6 entered the atmosphere over Mbale, Uganda, broke up, and caused a strewn field of size 3 x 7 km. Shortly after the fall, an expedition gathered eye witness accounts and located the position of 48 impacts of masses between 0.19 and 27.4 kg. Short-lived radionuclide data were measured for two specimens, one of which was only 12 days after the fall. Subsequent recoveries of fragements has resulted in a total of 863 mass estimates by 1993 October. The surfaces of all fragments contain fusion crust. The meteorite shower caused some minor inconveniences. Most remarkably, a young boy was hit on the head by a small specimen. The data interpreted as to indicate that the meteorite had an initial mass between 400-1000 kg (most likely approximately 1000 kg) and approached Mbale from AZ = 185 +/- 15, H = 55 +/- 15, and V(sub infinity) = 13.5 +/- 1.5/s. Orbital elements are given. Fragmentation of the initial mass started probably above 25 km altitude, but the final catastrophic breakup occurred at an altitude of 10-14 km. An estimated 190 +/- 40 kg reached the Earth's surface minutes after the final breakup of which 150 kg of material has been recovered.

Jenniskens, Peter↗
NASA NTRS1994

Evolution of the 1991-1992 Arctic vortex and comparison with the Geophysical Fluid Dynamics Laboratory SKYHI general circulation model

Nitrous oxide (N2O) measured on board the ER-2 aircraft during the Airborne Arctic Stratospheric Expedition 2 (AASE 2) has been used to monitor descent of air inside the Arctic vortex between October 1991 and March 1992. Monthly mean N2O fields are calculated from the flight data and then compared with mean fields calculated from the high-resolution Geophysical Fluid Dynamics Laboratory general circulation model SKYHI in order to evaluate the model's simulation of the polar vortex. From late fall through winter the model vortex evolves in much the same way as the 1991-1992 vortex, with N2O gradients at the edge becoming progressively steeper. The October to March trends in N2O profiles inside the vortex are used to verify daily net heating rates in the vortex that were computed from clear sky radiative heating rates and National Meteorological Center temperature observations. The computed heating rates successfully estimate the descent of vortex air from December through February but suggest that before December, air at high latitudes may not be isolated from the midlatitudes. SKYHI heating rates are in good agreement with the computed rates but tend to be slightly higher (i.e., less cooling) due to meteorological differences between SKYHI and the 1991-1992 winter. Three ER-2 flights measured N2O just north of the subtropical jet. These low-midlatitude profiles show only slight differences from the high-midlatitude profiles (45 deg - 60 deg N), indicating strong meridional mixing in the midlatitude 'surf zone.' Mean midwinter N2O profiles inside and outside the vortex calculated from AASE 2 data are shown to be nearly identical to 1989 AASE profiles, pointing to the N2O/potential temperature relationship as an excellent marker for vortex air.

Strahan, S. E.↗
NASA NTRS1995

A preliminary comparison of two perennially ice-covered lakes in Antarctica: Analogs of past martian lacustrine environments

Perennially ice-covered lakes in the Antarctic have been suggested as analogs to lakes which may have existed on the surface of Mars 3.5 billion years ago. During the 1991-1992 austral summer, a joint Russian/American research effort was directed at studies of ice-covered lakes in the Bunger Hills Oasis, Antarctica (66 deg S, 100 deg E). The primary objective of the expedition was to investigate this ice-free area for features analogous to ancient martian environments that may have been capable of supporting life and to compare the ice-covered lakes of the Bunger Hills with those in the McMurdo Dry Valleys of southern Victoria Land (77 deg S, 166 deg E) as part of the continuing studies of Antarctic-Mars analogs.

Andersen, D. T.↗
NASA NTRS1994

Three-dimensional model interpretation of NO(x) measurements from the lower stratosphere

A three-dimensional off-line chemistry transport model, driven by European Center for Medium-Range Forecasts winds and temperatures, is used to interpret measurements of NO and NO2 taken from the DC-8 during the second Airborne Arctic Stratospheric Expedition. The model was run in three configurations: gas phase chemistry alone, inclusion of the N2O5 aerosol reaction, and inclusion of both N2O5 and ClONO2 aerosol reactions. The run including the N2O5 aerosol reaction alone usually agreed best with measured NO(x)/NO(y) ratios in midlatitude air masses. The NO(x)/NO(y) ratios of the run with both aerosol reactions were always too low, while the gas phase ratios were usually too high, especially during March. All three simulations generated extremely low NO2/NO(y) ratios in air parcels that had spent several days or more in the polar night. Measured NO2/NO(y) ratios in these types of air masses were sometimes equally low but could also be considerably higher. Observed NO/NO2 ratios differed strongly from known theory.

Folkins, Ian↗
NASA NTRS1993

Interpretation of NO(x)/NO(y) observations from AASE-2 using a model of chemistry along trajectories

In situ measurements of NO and NO(y) are used to derive the ratio NO(x)/NO(y) along the flight track of the NASA ER-2 aircraft. Data are presented for two flights at midlatitudes in October 1991 during the Airborne Arctic Stratospheric Expedition-2 (AASE-2). Aerosol particle surface area was concurrently measured. The observations are compared with a photochemical model integrated along back trajectories from the aircraft flight track. Comparison of observations with the model run along trajectories and at a fixed position clearly and quantitatively demonstrates the importance of an air parcel's dynamic history in interpretation of local chemical observations. Comparison of the data with model runs under different assumptions regarding heterogeneous chemistry further reinforces the case for occurrence of the reaction of N2O5 + H2O on sulfate aerosol surfaces in the atmosphere. Finally, comparisons for which relative changes in the model and the data are not consistent caution that our ability to resolve all the observations is not yet complete.

Kawa, S. R.↗
NASA NTRS1993

New observations of the NOy/N2O correlation in the lower stratosphere

During the Airborne Arctic Stratospheric Expedition 2 (AASE 2), September 1991 through March 1992, in situ measurements of reactive nitrogen (NO(y) and N20 were made in the Northern Hemisphere lower stratosphere. We present an analysis of this new data and compare it with results from similar data taken during AASE in the winter of 1989. In the Northern Hemisphere there is consistent linear correlation of N2O and NO(y) which shows no interannual variation. Cases of departure from a linear correlation are examined and classified as being due to denitrification (NO(y) loss) or sampling air from a region where the photochemical lifetime of NO(y) is decreased. The latter case was observed for the first time in the winter of 1992.

Loewenstein, M.↗
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

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 NTRS1994

Origin of tropospheric NO(x) over subarctic eastern Canada in summer

The original of NO(X) in the summertime troposphere over subarctic eastern Canada is investigated by photochemical modeling of aircraft and ground-based measurements from the Arctic Boundary Layer Expedition (ABLE 3B). It is found that decomposition of peroxyacetyl nitrate (PAN) can account for most of the NO(X) observed between the surface and 6.2 km altitude (aircraft ceiling). Forest fires represent the principal source of PAN in the region, implying the same origin for NO(X). There is, however, evidence for an unidentified source of NO(X) in occasional air masses subsiding from the upper troposphere. Isoprene emissions from boreal forests maintain high NO(X) concentrations in the continental boundary layer over eastern Canada by scavenging OH and NO3, thus slowing down conversion of NO(X) to HNO3, both in the daytime and at night. This effect is partly compensated by the production of CH3CO3 radicals during isoprene oxidation, which slows down the decomposition of PAN subsiding from the free troposphere. The peroxy radical concentrations estimated from concurrent measurements of NO and NO2 concentrations during ABLE 3B are consistent with values computed from our photochemical model below 4 km, but model values are low at higher altitudes. The discrepancy may reflect either a missing radical source in the model or interferences in the NO2 measurement.

Fan, S.-M↗