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Sachse, G. W.

Publications and source records attributed to Sachse, G. W..

At least 55 records · Page 3

Factors influencing atmospheric composition over subarctic North America during summer

Elevated concentrations of hydrocarbons, CO, and nitrogen oxides were observed in extensive haze layers over northeastern Canada in the summer of 1990, during ABLE 3B. Halocarbon concentrations remained near background in most layers, indicating a source from biomass wildfires. Elevated concentrations of C2Cl4 provided a sensitive indicator for pollution from urban/industrial sources. Detailed analysis of regional budgets for CO and hydrocarbons indicates that biomass fires accounted for approximately equal to 70% of the input to the subarctic for most hydrocarbons and for acetone and more than 50% for CO. Regional sources for many species (including CO) exceeded chemical sinks during summer, and the boreal region provided a net source to midlatitudes. Interannual variations and long-term trends in atmospheric composition are sensitive to climatic change; a shift to warmer, drier conditions could increase the areas burned and thus the sources of many trace gases.

Wofsy, Steven C.↗

The role of airborne eddy correlation measurements in global change studies

We have obtained measurements of the mean and turbulent quantities of heat, moisture, momentum, O3, CO, and CH4 from an airborne platform. Species flux measurements obtained from these data provide unique regional-scale information which can be used to evaluate 'scaled-up' flux estimates based on smaller scale observations. Airborne flux data also provide a basis for assessing the uncertainties associated with large-scale ground level flux extrapolations. Airborne constituent budget analyses are possible with this suite of measurements. The local change in the mean value of a parameter can be explained in terms of horizontal advection, vertical turbulent transport, and, in the case of chemically reactive species (i.e., O3), in situ production or destruction. This technique is used to indicate a direct relationship between O3 precursors and the measured in situ production rate.

Ritter, J. A.↗

Low Ozone in the Marine Boundary Layer of the Tropical Pacific Ocean

Aircraft measurements of ozone, its key precursors, and a variety of chemical tracers were made in the troposphere of the western and central Pacific in October 1991. These data are presented and analyzed to examine the occurrence of low ozone concentrations in the remote marine boundary layer of the tropical and equatorial Pacific Ocean. The data from these flights out of Guam, covering an area extending from the equator to 20 N and from south of the Philippines to Hawaii, show average O3 concentrations as low as 8-9 ppb (ppb=10(exp-9)v/v) at altitudes of 0.3-0.5 km in the boundary layer. Individual measurements as low as 2-5 ppb were recorded. Low O3 concentrations do not always persist in space and time. High O3, generally associated with the transport of upper tropospheric air, was also encountered in the boundary layer. In practically all cases, O3 increased to values as large as 25-30 ppb within 2 km above the boundary layer top. Steady state model computations are used to suggest that these low O3 concentrations are a result of net photochemical O3 destruction in a low NO environment, sea-surface deposition, and extremely low net entrainment rates (1-2 mm per second) from the free troposphere. Day/night measurements of ethane, propane, gaseous and aerosol Cl suggest that daytime (morning) Cl atom concentrations in the vicinity of 10(exp 5) molecules per cubic centimeter may be present in the marine boundary layer. This Cl atom abundance can be rationalized only if sea salt aerosols can release free chlorine (Cl2) to the gas phase in the presence of sun light (and possibly O3). These Cl atom concentrations, however, are still insufficient and Cl (or Br) chemistry is not likely to be an important cause of the observed low O3.

Singh, Hanwant B.↗

The impact of U.S. continental outflow on ozone and aerosol distributions over the western Atlantic

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.

Anderson, B. E.↗

Factors influencing dry season ozone distributions over the tropical South Atlantic

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.

Anderson, B. E.↗

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.↗

AASE-2 in-situ tracer correlations of methane, nitrous oxide, and ozone as observed aboard the DC-8

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.

Collins, J. E., Jr.↗

Stratospheric NO(y) measurements on the NASA DC-8 during AASE 2

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).

Weinheimer, A. J.↗

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.↗

AASE-2 In-Situ Tracer Correlations of Methane Nitrous Oxide and Ozone as Observed Aboard the DC-8

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 II 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-II 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 a compared to January and February results.

Collins, J. E., Jr.↗

Stratospheric NO(y) Measurements on the NASA DC-8 during AASE 2

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 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.

Weinheimer, A. J.↗

Summertime tropospheric observations related to N(x)O(y) distributions and partitioning over Alaska - Arctic Boundary Layer Expedition 3A

Measurements of NO, NO2, PAN and NO(y) are presented for the summertime middle/lower troposphere over northern high latitudes. Chemical signatures from concurrent measurements of O3, CO, C2H2, C2H6, C3H8, C2Cl4, and H2O are used to characterize factors affecting the budget and distribution of N(x)O(y) in the Arctic and Sub-Arctic tropospheric air masses sampled over Alaska during the NASA Arctic Boundary Layer Expedition (ABLE 3A). The results implicate biomass burning in Siberia as the probable source of about one-third of the NO(y) abundance within the middle lower troposphere over Alaska and the downward transport of air from altitude in the vicinity of the tropopause as a major contributor to the abundance of NO(y) within the lower 6 km column over Alaska.

Sandholm, S. T.↗

Atmospheric measurements of peroxyacetyl nitrate and other organic nitrates at high latitudes - Possible sources and sinks

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.

Singh, H. B.↗

Atmospheric chemistry in the Arctic and subarctic - Influence of natural fires, industrial emissions, and stratospheric inputs

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.

Wofsy, S. C.↗

Airborne tunable diode laser sensor for high-precision concentration and flux measurements of carbon monoxide and methane

An airborne tunable diode laser instrument is described that is capable of operating in two measurement modes. One mode provides high precision (0.1 percent CH4; 1 percent CO) measurements of CH4 and CO with a 5 second response time, and a second mode achieves the very fast response time that is necessary to make airborne eddy correlation flux measurements. Examples of data from atmospheric expeditions of the Global Tropospheric Experiment are presented.

Sachse, G. W.↗

Carbon monoxide over the Amazon Basin during the wet season

Measurements of the distribution of carbon monoxide in the lower atmosphere (150-5000 m) over the Amazon region of Brazil during the wet season, taken in conjunction with the 1987 NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment (ABLE 2B), are analyzed. About 100 hr of airborne, in situ CO measurements were obtained using a tunable diode laser system, providing insights into factors influencing the basin-scale distribution of CO in the Amazonian troposphere during wet season conditions. Distribution of CO over the altitudes 0.15-4.5 km was influenced by such factors as surface emissions from biological sources and long-range transport of pollutants from Northern Hemisphere sources. It is noted that the disruption of mixed layer growth and decay processes has a particularly important influence on CO concentration in the daytime lower troposphere and that the correlation of CO with O3 was positive under conditions influenced by Northern Hemisphere air and negative under all other conditions observed.

Harriss, R. C.↗

Atmospheric peroxyacetyl nitrate measurements over the Brazilian Amazon Basin during the wet season - Relationships with nitrogen oxides and ozone

An analysis is presented on the distribution and variability of PAN as well as its relationship with measured chemical and meteorological parameters. The chemicals of most interest for which measurements were available are PAN, NO(x), O3, CO, and C2Cl4. PAN was measured by the electron capture gas chromatographic technique, and the technique for calibrations and measurements are detailed. Data show that significant concentrations of PAN (5-125 ppt) are present during the wet season and this PAN is 1-5 times more abundant than NO(x). PAN levels at different atmospheric locations are discussed, and it is noted that PAN shows evidence of a possible latitudinal gradient in the free troposphere, with values falling rapidly from the northern midlatitudes toward the equator. High correlations between O3 and PAN levels suggest that nonmethane hydrocarbons may contribute significantly to high O3 in the free troposphere. Evidence indicates that virtually all of the NO(x) above 4 km could result from PAN decomposition.

Singh, H. B.↗

Measurements of NO(x) over the eastern Pacific Ocean and southwestern United States during the spring 1984 NASA GTE aircraft program

Measurements of NO, NO(x) (NO + NO2), O3, and CO are presented from seven aircraft flights made over the eastern Pacific Ocean and the southwestern United States in spring of 1984. The sampling region was characterized by large- and small-scale variability for all of the measurements, likely as a result of vigorous synoptic scale meteorology and the influence of tropopause folds. Median values for NO, NO(x), O3, and CO from the flights made over the ocean in the region of 5.8-7.6 km were 10 parts per trillion by volume (pptv), 32 pptv, 46 parts per billion by volume (ppbv), and 120 ppbv, respectively. Corresponding values from two flights made over the continent at similar altitudes were 16 pptv, 38 pptv, 42 ppbv, and 111 ppbv. There was a strong tendency for NO or NO(x) to be correlated positively with O3 and to be anticorrelated with dew-point/frost-point measurements. No significant overall correlation occurred between NO(x) and CO for the ocean data. The variability of NO(x) was such that regions of net destruction and regions of net production of O(3) were sampled both over the ocean and over the continent. However, in the middle free troposphere over the ocean, net O(3) destruction was predominant.

Ridley, B. A.↗