ALBERT

Description: Airborne measurements of trace gas and aerosol species were obtained in the lower troposphere (less than 5 km) over the western Atlantic Ocean between 13 deg S and 40 deg N during the August/September 1990 NASA Chemical Instrument Test and Evaluation (CITE 3) experiment. The largest background O3 mixing ratios, averaging 35 and 70 ppbv within the mixed layer (ML) and free troposphere (FT; altitudes greater than 2.4 km), respectively, were found over the tropical South Atlantic. Several competing processes were observed to regulate O3 budgets in this region. Within the ML, rapid photochemical destruction produced a diurnal O3 variation of 8 ppbv and an O3/altitude gradient between the surface and 5 km of almost 10 ppbv (O3)/km. ML O3 concentrations were replenished by atmospheric downwelling which occurred at rates of up to and exceeding 1 cm/s. Ozone values within the subsiding FT air were enriched both by long-range transport of O3 produced photochemically within biomass combustion plumes and the downward propagation of dry, upper tropospheric air masses. Overall, the tropospheric O3 column below 3.3 km averaged 13.5 Dobson units (DU) over the South Atlantic region, which is 8-9 DU higher than observed during CITE 3 ferry flights over the northern tropical Atlantic Ocean or measured by ozonesondes over coastal Brazil during the wet season. An examination of simultaneous dew point and combustion tracer (e.g., CO) measurements suggests that the dry subsiding layers and biomass burning layers make approximately equal contributions to the observed O3 enhancement.

Description: Aircraft measurements of selected trace gas species, aerosols, and meteorological parameters were performed in the lower troposphere off the U.S. east coast during August and September 1989 as part of the NASA Global Tropospheric Experiment (GTE) Chemical Instrumentation Test and Evaluation (CITE 3) expedition. In this paper, we examine these data to assess the impact of continental outflow on western Atlantic O3 and small aerosol budgets. Results show that mixed layer (ML) O3 concentrations and small aerosol number densities (Np) were enhanced by factors of 3 and 6, respectively, within air masses of predominantly continental origin compared with clean maritime background air. These enhancements exhibited a marked altitude dependence, declining rapidly above the ML to the point where only slight to moderate differences in O3 and Np, respectively, were notable above 2.4 km. Within continentally influenced ML's, both O3 and Np were correlated with CO, exhibiting linear regression slopes averaging 0.4 ppbv (O3)/ppbv(CO) for O3 and 7.7 (particles/cc)/ppbv(CO) for Np and indicating a primarily anthropogenic origin for the observed enhancement of these species. Comparisons between profiles in continental and background maritime air masses suggest that photochemical production below 1.4-km altitude adds over 10% to western Atlantic tropospheric column O3 abundance in continental outflow regimes. For aerosols, eastward advection of low-level continental air contributes an average net flux of 2.8 metric tons of submicron (accumulation mode) particles per kilometer of shoreline per day to the western Atlantic troposphere.

Description: We report in situ stratospheric measurements of CH4, N2O, and O3 obtained aboard the NASA DC-8 during the January-March 1992 Airborne Arctic Stratospheric Expedition 2 field campaign. These data demonstrate a strong linear correlation between N2O and CH4 in the lower stratosphere thus indicating that both species are effective tracers of stratospheric air motion. Measurements of both species on constant geometric height surfaces indicate that significant subsidence of the arctic stratospheric air mass occurred at DC-8 altitudes over the course of the AASE-2 expedition. In addition, a widespread reduction in O3 mixing ratios (up to 20%) relative to these conserved tracers was also observed in the lower stratosphere in March as compared to January and February results.

Description: Measurements of PAN and other reactive nitrogen species during the NASA Arctic Boundary Layer Expedition (ABLE 3A) are described, their north-south and east-west gradients in the free troposphere are characterized, and the sources and sinks of PAN and NO(y) are assessed. Large concentrations of PAN and NO(y) are present in the Arctic/sub-Arctic troposphere of the Northern Hemisphere during the summer. Mixing ratios of PAN and a variety of other molecules are more abundant in the free troposphere compared to the boundary layer. Coincident PAN and O3 atmospheric structures suggest that phenomena that define PAN also define the corresponding O3 behavior. Model calculations, correlations between NO(y) and anthropogenic tracers, and the compositions of NO(y) itself suggest that the Arctic/sub-Arctic reactive nitrogen measured during ABLE 3A is predominantly of anthropogenic origin with a minor component from the stratosphere.

Description: During all eight flights conducted over the equatorial and tropical South Atlantic in the course of the Chemical Instrumentation Test and Evaluation (CITE 3) experiment, we observed haze layers with elevated concentrations of aerosols, O3, CO, and other trace gases related to biomass burning emissions. They occurred at altitudes between 1000 and 5200 m and were usually only some 100-300 m thick. These layers extended horizontally over several 100 km and were marked by the presence of visible brownish haze. Air mass trajectories indicate that these layers originate in the biomass burning regions of Africa and South America and typically have aged at least 10 days since the time of emission. In the haze layers, O3 and CO concentrations up to 90 and 210 ppb were observed, respectively. The two species were highly correlated. The ratio concentrations in plume minus background concentrations of O3/CO is typically in the range 0.2-0.7, much higher than the ratios in the less aged plumes investigated previously in Amazonia. In most cases, aerosol (0.12-3 micrometer diameter) number concentrations were also elevated by up to 400/cu cm in the layers; aerosol enrichments were also strongly correlated with elevated CO levels. Clear correlations between CO and NO(x) enrichments were not apparent due to the age of the plumes, in which most NO(x) would have already reacted away within 1-2 days. Only in some of the plumes could clear correlations between NO(y) and CO be identified; the absence of a general correlation between NO(y) and CO may be due to instrumental limitations and to variable sinks for NO(y). The average enrichment of the ratio concentrations in plume minus background concentrations of NO(y)/CO was quite high, consistent with the efficient production of ozone observed in the plumes. The chemical characteristics of the haze layers, together with remote sensing information and trajectory calculations, suggest that fire emissions (in Africa and/or South America) are the primary source of the haze layer components.

Description: The characteristics of the Southeastern Virginia urban plume were defined with emphasis on the photon-oxidant species. The measurement area was a rectangle, approximately 150 km by 100 km centered around Cape Charles, Virginia. Included in this area are the cities of Norfolk, Virginia Beach, Chesapeake, Newport News, and Hampton. The area is bounded on the north by Wallops Island, Virginia, and on the south by the Hampton Roads area of Tidewater Virginia. The major axis of the rectangle is oriented in the southwest-northeast direction. The data set includes aircraft measurements for carbon monoxide, methane, nonmethane hydrocarbons, and ozone. The experiment shows that CO can be successfully measured as a tracer gas and used as an index for determining localized and urban plumes. The 1978 data base provided sufficient data to assess an automated chromatograph with flame ionization detection used for measuring methane and nonmethane hydrocarbons in flight.

Description: 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.

Description: We survey measurements of stratospheric NO(y) on the NASA DC-8 during AASE 2 in early 1992. Emphasis is on correlations with other long-lived species: O3, N2O, and CH4. No cases of extremely high NO(y)/O3 ratios were seen in 1992. This suggests that denitrification at higher altitudes was less pervasive than in 1989. Values of NO(y)/O3 in 1992 are comparable to, though perhaps lower than, those measured in 1989. The correlation of NO(y) with N2O changes over the course of the mission. Relative to the correlation for the whole season, low values of NO(y) occur in February, most notably on the 22nd. The reason for the low NO(y) is unknown. It is generally too warm at DC-8 altitudes for the presence of Polar Stratospheric Cloud (PSC) particles, but denitrification at higher altitudes, followed by descent, might account for the low values seen on 22 February. However, this may be unlikely since the NASA ER-2, flying during the same period, saw no evidence of denitrification at higher altitudes (Loewenstein et al., 1993).

Description: Layers with enhanced concentrations of trace gases intercepted by the NASA Electra aircraft over Alaska during the Arctic Boundary Layer Expedition (ABLE 3A) in July-August 1988 are discussed. Haze layers apparently associated with boreal fires were enriched in hydrocarbons and NO(y), with emission factors corresponding closely to laboratory data for smoldering combustion. It is argued that atmospheric composition was strongly modified by wildfires during several periods of the ABLE 3A mission. The associated enhancement of NO(y) was smaller than observed for most other combustion processes but was nonetheless significant in the context of very low background concentrations. Ozone production in fire plumes was negligible. Ambient O3 was supplied by the stratosphere, with little direct input from midlatitude source during summer. It is argued that NO(y) was supplied about equally by the stratosphere and by wildfires. Hydrocarbons and CO appear to derive from biomass fires and from human activities.