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Blake, Donald R.

Publications and source records attributed to Blake, Donald R..

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NASA NTRS2003

Large-scale Distribution of CH4 in the Western North Pacific: Sources and Transport from the Asian Continent

Methane (CH4) mixing ratios in the northern Pacific Basin were sampled from two aircraft during the TRACE-P mission (Transport and Chemical Evolution over the Pacific) from late February through early April 2001 using a tunable diode laser system. Described in more detail by Jacob et al., the mission was designed to characterize Asian outflow to the Pacific, determine its chemical evolution, and assess changes to the atmosphere resulting from the rapid industrialization and increased energy usage on the Asian continent. The high-resolution, high-precision data set of roughly 13,800 CH4 measurements ranged between 1602 ppbv in stratospherically influenced air and 2149 ppbv in highly polluted air. Overall, CH4 mixing ratios were highly correlated with a variety of other trace gases characteristic of a mix of anthropogenic industrial and combustion sources and were strikingly correlated with ethane (C2H6) in particular. Averages with latitude in the near-surface (0-2 km) show that CH4 was elevated well above background levels north of 15 deg N close to the Asian continent. In the central and eastern Pacific, levels of CH4 were lower as continental inputs were mixed horizontally and vertically during transport. Overall, the correlation between CH4 and other hydrocarbons such as ethane (C2H6), ethyne (C2H2), and propane (C3H8) as well as the urban/industrial tracer perchloroethene (C2Cl4), suggests that for CH4 colocated sources such as landfills, wastewater treatment, and fossil fuel use associated with urban areas dominate regional inputs at this time. Comparisons between measurements made during TRACE-P and those of PEM-West B, flown during roughly the same time of year and under a similar meteorological setting 7 years earlier, suggest that although the TRACE-P CH4 observations are higher, the changes are not significantly greater than the increases seen in background air over this time interval.

Bartlett, Karen B.↗
NASA NTRS2003

Eastern Asian Emissions of Anthropogenic Halocarbons Deduced from Aircraft Concentration Data

The Montreal Protocol restricts production of ozone-depleting halocarbons worldwide. Enforcement of the protocol has relied mainly on annual government statistics of production and consumption of these compounds (bottom-up approach). We show here that aircraft observations of ha1ocarbon:CO enhancement ratios on regional to continental scales can be used to infer halocarbon emissions, providing independent verification of the bottom-up approach. We apply this topdown approach to aircraft observations of Asian outflow &om the TRACE-P mission over the western Pacific (March-April 2001) and derive emissions from eastern Asia (China, Japan, and Korea). We derive an eastern Asian carbon tetrachloride (CCl4) source of 21.5 Gg yr(sup -1), several-fold larger than previous estimates and amounting to -30% of the global budget for this gas. Our emission estimate for CFC-11 from eastern Asia is 50% higher than inventories derived from manufacturing records. Our emission estimates for methyl chloroform (CH3CC13) and CFC-12 are in agreement with existing inventories. For halon 1211 we find only a strong local source originating from the Shanghai area. Our emission estimates for the above gases result in a approximately equal to 40% increase in the ozone depletion potential (ODP) of Asian emissions relative to previous estimates, corresponding to a approximately equal to 10% global increase in ODP.

Palmer, Paul I.↗
NASA NTRS2003

Distributions of Trace Gases and Aerosols during the Dry Biomass Burning Season in Southern Africa

Vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, are presented for five regions of southern Africa during the dry biomass burning season of 2000. The regions are the semiarid savannas of northeast South Africa and northern Botswana, the savanna-forest mosaic of coastal Mozambique, the humid savanna of southern Zambia, and the desert of western Namibia. The highest average concentrations of carbon dioxide (CO2), CO, methane (CH4), O3, black particulate carbon, and total particulate carbon were in the Botswana and Zambia sectors (388 and 392 ppmv, 369 and 453 ppbv, 1753 and 1758 ppbv, 79 and 88 ppbv, 2.6 and 5.5 micrograms /cubic meter and 13.2 and 14.3 micrograms/cubic meter). This was due to intense biomass burning in Zambia and surrounding regions. The South Africa sector had the highest average concentrations of SO2, sulfate particles, and CN (5.1 ppbv, 8.3 micrograms/cubic meter, and per 6400 cubic meter , respectively), which derived from biomass burning and electric generation plants and mining operations within this sector. Air quality in the Mozambique sector was similar to the neighboring South Africa sector. Over the arid Namibia sector there were polluted layers aloft, in which average SO2, O3, and CO mixing ratios (1.2 ppbv, 76 ppbv, and 3 10 ppbv, respectively) were similar to those measured over the other more polluted sectors. This was due to transport of biomass smoke from regions of widespread savanna burning in southern Angola. Average concentrations over all sectors of CO2 (386 +/- 8 ppmv), CO (261 +/- 81 ppbv), SO2 (2.5 +/- 1.6 ppbv), O3 (64 +/- 13 ppbv), black particulate carbon (2.3 +/- 1.9 microgram/cubic meter), organic particulate carbon (6.2 +/- 5.2 microgram/cubic meter), total particle mass (26.0 +/- 4.7 microgram/cubic meter), and potassium particles (0.4 +- 0.1 microgram/cubic meter) were comparable to those in polluted, urban air. Since the majority of the measurements in this study were obtained in locations well removed from industrial sources of pollution, the high average concentrations of pollutants reflect the effects of widespread biomass burning. On occasions, relatively thin (-0.5 km) layers of remarkably clean air were located at -3 km above mean sea level, sandwiched between heavily polluted air. The data presented here can be used for inputs to and validation of regional and global atmospheric chemical models.

Sinha, Parikhit↗
NASA NTRS2003

Evolution of Gases and Particles from a Savanna Fire in South Africa

Airborne measurements of particles and gases fiom a 1000-ha savanna fire in South Africa are presented. These measurements represent the most extensive data set reported on the aging of biomass smoke. The measurements include total concentrations of particles (CN), particle sizes, particulate organic carbon and black carbon, light-scattering coefficients, downwelling UV fluxes, and mixing ratios for 42 trace gases and 7 particulate species. The ratios of excess nitrate, ozone, and gaseous acetic acid to excess CO increased significantly as the smoke aged over approximately 40-45 min, indicating that these species were formed by photochemistry in the plume. For 17 other species, the excess mixing ratio normalized by the excess mixing ratio of CO decreased significantly with ' smoke age. The relative rates of decrease for a number of chemical species imply that the average OH concentration in the plume was approximately 1.7 x l0(exp 7) molecules /cubic centimeter. Excess CN, normalized by excess CO, decreased rapidly during the first approximately 5 min of aging, probably due to coagulation, and then increased, probably due to gas-to-particle conversion. The CO-normalized concentrations of particles < 1.5 microns in diameter decreased, and particles >1.5 micron diameter increased, with smoke age. The spectral depletion of solar radiation by the smoke is depicted. The downwelling UV flux near the vertical center of the plume was about two-thirds of that near the top of the plume.

Hobbs, Peter V.↗
NASA NTRS2003

Emissions of Trace Gases and Particles from Savanna Fires in Southern Africa

Airborne measurements made on initial smoke from 10 savanna fires in southern Africa provide quantitative data on emissions of 50 gaseous and particulate species, including carbon dioxide, carbon monoxide, sulfur dioxide, nitrogen oxides, methane, ammonia, dimethyl sulfide, nonmethane organic compounds, halocarbons, gaseous organic acids, aerosol ionic components, carbonaceous aerosols, and condensation nuclei (CN). Measurements of several of the gaseous species by gas chromatography and Fourier transform infrared spectroscopy are compared. Emission ratios and emission factors are given for eight species that have not been reported previously for biomass burning of savanna in southern Africa (namely, dimethyl sulfide, methyl nitrate, five hydrocarbons, and particles with diameters from 0.1 to 3 microns). The emission factor that we measured for ammonia is lower by a factor of 4, and the emission factors for formaldehyde, hydrogen cyanide, and CN are greater by factors of about 3, 20, and 3 - 15, respectively, than previously reported values. The new emission factors are used to estimate annual emissions of these species from savanna fires in Africa and worldwide.

Sinha, Parikhit↗
NASA NTRS2001

Whole Air Sampling During NASA's March-April 1999 Pacific Exploratory Expedition (PEM-Tropics B)

University of California, Irvine (UCI) collected more than 4500 samples whole air samples collected over the remote Pacific Ocean during NASA's Global Tropospheric Experiment (GTE) Pacific Exploratory Mission-Tropics B (PEM-Tropics B) in March and early April 1999. Approximately 140 samples during a typical 8-hour DC-8 flight, and 120 canisters for each 8-hour flight aboard the P-3B. These samples were obtained roughly every 3-7 min during horizontal flight legs and 1-3 min during vertical legs. The filled canisters were analyzed in the laboratory at UCI within ten days of collection. The mixing ratios of 58 trace gases comprising hydrocarbons, halocarbons, alkyl nitrates and DMS were reported (and archived) for each sample. Two identical analytical systems sharing the same standards were operated simultaneously around the clock to improve canister turn-around time and to keep our measurement precision optimal. This report presents a summary of the results for sample collected.

Blake, Donald R.↗
NASA NTRS1997

Distribution and Seasonality of Selected Hydrocarbons and Halocarbons over the Western Pacific Basin During PEM-West A and PEM-West B

Nonmethane hydrocarbons (NMHCs) and halocarbons were measured in the troposphere over the northwestern Pacific as part of the airborne component of NASA's Pacific Exploratory Mission-West Phase B (PEM-West B). This study took place in late winter of 1994, a period characterized by maximum outflow from the Asian continent. The results are compared to those from Pacific Exploratory Mission-West Phase A (PEM-West A), which was flown in the same region during late summer of 1991, when flow from the subtropical western Pacific dominated the lower troposphere. Mixing ratios of NMHCs, tetrachloroethene (C2Cl4), and methyl bromide (CH3Br) were significantly higher during PEM-West B than during PEM-West A, particularly at latitudes north of 25 deg N and altitudes lower than 6 km. The primary reasons for these higher ambient concentrations were the seasonal increase in the atmospheric lifetimes of trace gases controlled by HO radical reactions, and the more frequent input of continental air masses. During PEM-West B, air masses of continental origin observed north of 25 deg N latitude were augmented with urban signature gases such as C2Cl4. By contrast, more southerly continental outflow had characteristics associated with combustion sources such as biomass burning, including wood fuel burning. During the summer PEM-West A period, the spatial distribution of methyl iodide (CH3I) was consistent with effective oceanic sources at all latitudes, being especially strong in tropical and subtropical regions. At low latitudes, PEM-West B CH3I mixing ratios in the lower troposphere were similar to PEM-West A, but at latitudes greater than about 25 deg N PEM-West B concentrations were significantly reduced. Equatorial regions exhibited enhanced CH3I mixing ratios extending into the upper tropical troposphere, consistent with fast vertical transport of air from the tropical marine boundary layer.

Blake, Nicola J.↗
NASA NTRS1997

End of Project Report

Nonmethane hydrocarbons (NMHCs) and halocarbons were measured in the troposphere over the northwestern Pacific as part of the airborne component of NASA's Pacific Exploratory Mission-West Phase B (PEM-West B). This study took place in late winter of 1994, a period characterized by maximum outflow from the Asian continent. The results are compared to those from Pacific Exploratory Mission-West Phase A (PEM-West A), which was flown in the same region during late summer of 1991, when flow from the subtropical western Pacific dominated the lower troposphere. Mixing ratios of NMHCS, tetrachloroethene (C2Cl4), and methyl bromide (CH3Br) were significantly higher during PEM-West B than during PEM-West A, particularly at latitudes north of 25 N and altitudes lower than 6 km. The primary reasons for these higher ambient concentrations were the seasonal increase in the atmospheric lifetimes of trace gases controlled by HO radical reactions, and the more frequent input of continental air masses. During PEM-West B, air masses of continental origin observed north of 25 N latitude were augmented with urban signature gases such as C2Cl4. By contrast, more southerly continental outflow had characteristics associated with combustion sources such as biomass burning, including wood fuel burning. During the summer PEM-West A period, the spatial distribution of methyl iodide (CH3I) was consistent with effective oceanic sources at all latitudes, being especially strong in tropical and subtropical regions. At low latitudes, PEM-West B CH3I mixing ratios in the lower troposphere were similar to PEM-West A, but at latitudes greater than about 25 N PEM-West B concentrations were significantly reduced. Equatorial regions exhibited enhanced CH3I mixing ratios extending into the upper tropical troposphere, consistent with fast vertical transport of air from the tropical marine boundary layer.

Blake, Donald R.↗
NASA NTRS1995

Seasonal variations in the atmospheric distribution of a reactive chlorine compound, tetrachloroethene (CCl2 = CCl2)

Tropospheric mixing ratios of CCl2 = CCl2 were measured at remote surface locations in the Pacific between 71 deg N and 47 deg S during September and December of 1989, and March and June of 1990. The observed gradient of decreasing concentrations from the northern to the southern hemisphere, and very low concentrations in the southern hemisphere throughout the year, indicates a predominant input from the northern hemisphere. Seasonal measurements in the northern hemisphere showed maximum CCl2 = CCl2 concentrations occurring in the late summer. This distinct seasonal variation is strongly coupled to the atmompheric abundance of hydroxyl radical, the only important species responsible for CCl2 = CCl2 removal. With the estimated global CCl2 =CCl2 emissions, the lifetime is calculated to be about 5.4 months which is in good agreement with the 4.0 month estimate obtained from the inverse ratio of its measured hydroxyl reaction rate constant compared with that of methyl-chloroform CH3CCl3.

Wang, Charles J.-L.↗
NASA NTRS1994

Analysis of tropospheric aerosol number density for aerosols of 0.2- to 3-micrometers diameter: Central and northeastern Canada

NASA's Atmospheric Boundary Layer Experiment conducted during the summer of 1990 focused on the distribution of trace species in central and northeastern Canada (altitudes less than 6 km) and the importance of surface sources/sinks, local emissions, distant transport, tropospheric/stratospheric exchange. Aircraft flights were based from North Bay, Ontario, and Goose Bay, Labrador, Canada. As part of the aircraft measurements, aerosol number density (0.2- to 3-micrometers diameter) was measured using an optical laser technique. Results show that summertime aerosol budgets of central and northeastern Canada can be significantly impacted by the transport of pollutants from distant source regions. Biomass burning in Alaska and western and central Canada exerts major influences on regional aerosol budgets. Urban emissions transported from the U.S./Canadian border regions are also important. Aerosol enhancements (mixed layer and free troposphere) were most prevalent in air with carbon monoxide mixing ratios greater than 110 parts per billion by volume (ppbv). When data were grouped as to the source of the air (5-day back trajectories) either north or south of the polar jet, aerosol number density in the mixed layer showed a tendency to be enhanced for air south of the jet relative to north of the jet. However, this difference was not observed for measurements at the higher altitudes (4 to 6 km). For some flights, mixed layer aerosol number densities were greater than 100 higher than free-tropospheric values (3- to 6-km altitude). The majority of the observed mixed layer enhancement was associated with transport of effluent-rich air into the Canadian regions. Aerosol emissions from natural Canadian ecosystems were relatively small when compared to transport.

Gregory, Gerald L.↗
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 NTRS1988

Stratospheric feedback from continued increases in tropospheric methane

Tropospheric concentrations of methane have increased steadily over the past ten years at an average rate of 16.5 ppbv per year, to a value in January 1988 of 1.69 ppmv. Measurements of CH sub 4 concentrations in air bubbles trapped in ice cores have shown concentrations of about 0.7 ppmv 200 years ago, with little further change for thousands of years before that. Interpolation earlier into this century suggests a concentration of about 1.1 to 1.2 ppmv in the 1940's. The only important pathway believed to be important for transfer of air from the troposphere to the stratosphere in through the tropical tropopause which is cold enough to reduce the mixing ratio of H sub 2 O in that air to about 3 ppmv. The only other major pathway for the delivery of H to the stratosphere is through the simultaneous injection of gaseous CH sub 4 in the same rising air. The formation of clouds in the stratosphere is dependent upon very low temperatures, and generally upon the amount of water vapor available. The possibility of a positive feedback exists, especially in well-oxidized methane air, that clouds are easier to form than earlier. This could mean enhancement of PSCs in both Antarctic and Arctic locations. Additional H sub 2 O in the stratosphere can also add to some of the greenhouse calculations.

Rowland, F. Sherwood↗
NASA NTRS1988

Continuing worldwide increase in tropospheric methane, 1978 to 1987

The average worldwide tropospheric mixing ratio of methane has increased by 11 percent from 1.52 parts per million by volume (ppmv) in January 1978 to 1.684 ppmv in September 1987, for an increment of 0.016 + or - 0.001 ppmv per year. Within the limits of the present measurements, the global tropospheric mixing ratio for methane over the past decade is consistent either with a linear growth rate of 0.016 + or - 0.001 ppmv per year or with a slight lessening of the rate of growth over the past 5 years. No indications were found of an effect of the El Nino-Southern Oscillation-El Chichon events of 1982-83 on total global methane, although severe reductions were reported in the Pacific Northwest during that time period.The growth in tropospheric methane may have increased the water concentration in the stratosphere by as much as 28 percent since the 1940s and 45 percent over the past two centuries and thus could have increased the mass of precipitable water available for the formation of polar stratospheric clouds.

Blake, Donald R.↗
NASA NTRS1987

C-13/C-12 ratio in methane from the flooded Amazon forest

The C1-C4 hydrocarbon concentrations and the C-13/C-12 ratio in CH4 detected in air samples collected in the Amazon region (3.5 deg S latitude and 5.9 deg W longitude) are analyzed. It is observed that the CH4 concentrations of each sample are enhanced over the background concentration for remote locations, and the C-13/C-12 ratio in this biogenic methane is depleted in C-13 relative to atmospheric CH4. It is concluded, from the C2-C4 hydrocarbon data, that minor yields of C2-C4 hyrocarbons are released coincident with CH4; however, the minor yields do not contribute to the regionally enhanced concentrations of hydrocarbons found in Amazonia and the global atmosphere release of C2-C4 compounds.

Tyler, Stanley C.↗