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Herein we provide a description of the atmospheric infrared sounder (AIRS) version 5 (v5) carbon monoxide (CO) retrieval algorithm and its validation with the DACOM in situ measurements during the INTEX-A and -B campaigns. All standard and support products in the AIRS v5 CO retrieval algorithm are documented. Building on prior publications, we describe the convolution of in situ measurements with the AIRS v5 CO averaging kernel and first-guess CO profile as required for proper validation. Validation is accomplished through comparison of AIRS CO retrievals with convolved in situ CO profiles acquired during the NASA Intercontinental Chemical Transport Experiments (INTEX) in 2004 and 2006. From 143 profiles in the northern mid-latitudes during these two experiments, we find AIRS v5 CO retrievals are biased high by 6% 10% between 900 and 300 hPa with a root-mean-square error of 8% 12%. No significant differences were found between validation using spiral profiles coincident with AIRS overpasses and in-transit profiles under the satellite track but up to 13 h off in time. Similarly, no significant differences in validation results were found for ocean versus land, day versus night, or with respect to retrieved cloud top pressure or cloud fraction.

We have developed an instrument concept that will enable the measurement of CO from the top of the atmosphere to the Earth's surface with very high sensitivity and at the high spatial and temporal resolutions required by the NRC Decadal Survey mission Active Sensing of Carbon Dioxide (CO2) over Nights, Days and Seasons (ASCENDS). We are developing an innovative CO sensor that will enable the ASCENDS mission to differentiate between anthropogenic and natural sources and sinks of global carbon. The NRC Decadal Survey places particular emphasis on retrieving CO information for the planetary boundary layer. Measurement made using both the 2.3 micron and 4.7 micron channels are needed to achieve the sensitivity required in the lower atmosphere where the degree of CO - CO2 correlation is indicative of anthropogenic sources of CO2. Measurements made using only the 4.7 micron channel cannot provide sufficient sensitivity to CO in the very lowest layers of the atmosphere. The fundamental method we use is Gas Filter Correlation Radiometry (GFCR), a highly successful technique used in other airborne and space-based missions for detecting trace species in the Earth's atmosphere. Our version of GFCR overcomes many of the limitations encountered by prior and existing instruments, allowing us to measure weak signals from small targets very quickly and with extremely high specificity by employing a new dual beam radiometer concept using a focal plane array. Our design will provide a means to make the desired CO measurements for the ASCENDS mission. A simple change in gas filter cell contents would allow the same hardware to measure CH4 with high precision under the nominal ASCENDS mission spatial and temporal constraints. All critical components in the sensor design are mature, many subsystems tested, and the system has been extensively modeled, bringing it to a present Technology Readiness Level (TRL) of 3 (though some individual components are at TRLs 6-9). We are presently developing critical components for the new spectrometer and advancing our understanding of the measurement requirements for both CO and CH4. This new GFCR technique/sensor will enable measurements of trace gases with high sensitivity while maintaining the inherent robustness and simplicity of the more traditional radiometer hardware. Initial estimates of cost/risk of a spacebased 2-channel GFCR indicate that our design is extremely cost effective and will fit within existing ASCENDS mission budget constraints as determined by the NRC Decadal Survey and a NASA-sponsored mission study.

OH and HO2 were measured with the Airborne Tropospheric Hydrogen Oxides Sensor (ATHOS) as part of a large measurement suite from the NASA DC-8 aircraft during the Intercontinental Chemical Transport Experiment - A (INTEX-A). This mission, which was conducted mainly over North America and the western Atlantic Ocean in summer 2004, was an excellent test of atmospheric oxidation chemistry. Throughout the troposphere, observed OH was generally 0.60 of the modeled OH; below 8 km, observed HO2 was generally 0.78 of modeled HO2. If the over-prediction of tropospheric OH is not due to an instrument calibration error, then it implied less global tropospheric oxidation capacity and longer lifetimes for gases like methane and methyl chloroform than currently thought. This discrepancy falls well outside uncertainties in both the OH measurement and rate coefficients for known reactions and points to a large unknown OH loss. If the modeled OH is forced to agree with observed values by introducing of an undefined OH loss that removed HOx (HOx=OH+HO2), the observed and modeled HO2 and HO2/OH ratios are largely reconciled within the measurement uncertainty. HO2 behavior above 8 km was markedly different. The observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 ratio increased from approximately 1 at 8 km to more than approximately 2.5 at 11 km with the observed-to-modeled ratio correlating with NO. The observed-to-modeled HO2 and NO were both considerably greater than observations from previous campaigns. In addition, the observed-to-modeled HO2/OH, which is sensitive to cycling reactions between OH and HO2, increased from approximately 1.2 at 8 km to almost 4 above 11 km. In contrast to the lower atmosphere, these discrepancies above 8 km suggest a large unknown HOx source and additional reactants that cycle HOx from OH to HO2. In the continental planetary boundary layer, the OH observed-to-modeled ratio increased from 0.6 when isoprene was less than 0.1 ppbv to over 3 when isoprene was greater than 2 ppbv, suggesting that forests throughout the United States are emitting unknown HOx sources. Progress in resolving these discrepancies requires further examinations of possible unknown OH sinks and HOx sources and a focused research activity devoted to ascertaining the accuracy of the OH and HO2 measurements.

Each of two sensors, positioned to simultaneously detect electromagnetic radiation absorption along a path, is calibrated to define a unique response curve associated therewith that relates a change in voltage output for each sensor to a change in optical density. A ratio-of-responses curve is defined by a ratio of the response curve associated with the first sensor to the response curve associated with the second sensor. A ratio of sensor output changes is generated using outputs from the sensors. An operating point on the ratio-of-responses curve is established using the ratio of sensor output changes. The established operating point is indicative of an optical density. When the operating point is in the non-linear response region of at least one of the sensors, the operating point and optical density corresponding thereto can be used to establish an actual response of at least one of the sensors whereby the actual sensor output can be used in determining changes in the optical density.

Global ozone analyses, based on assimilation of stratospheric profile and ozone column measurements, and NOy predictions from the Real-time Air Quality Modeling System (RAQMS) are used to estimate the ozone and NOy budget over the Continental US during the July-August 2004 Intercontinental Chemical Transport Experiment-North America (INTEX-A). Comparison with aircraft, satellite, surface, and ozonesonde measurements collected during the INTEX-A show that RAQMS captures the main features of the global and Continental US distribution of tropospheric ozone, carbon monoxide, and NOy with reasonable fidelity. Assimilation of stratospheric profile and column ozone measurements is shown to have a positive impact on the RAQMS upper tropospheric/lower stratosphere ozone analyses, particularly during the period when SAGE III limb scattering measurements were available. Eulerian ozone and NOy budgets during INTEX-A show that the majority of the Continental US export occurs in the upper troposphere/lower stratosphere poleward of the tropopause break, a consequence of convergence of tropospheric and stratospheric air in this region. Continental US photochemically produced ozone was found to be a minor component of the total ozone export, which was dominated by stratospheric ozone during INTEX-A. The unusually low photochemical ozone export is attributed to anomalously cold surface temperatures during the latter half of the INTEX-A mission, which resulted in net ozone loss during the first 2 weeks of August. Eulerian NOy budgets are shown to be very consistent with previously published estimates. The NOy export efficiency was estimated to be 24 percent, with NOx+PAN accounting for 54 percent of the total NOy export during INTEX-A.

We analyze aircraft observations obtained during INTEX-A (1 July 14 - August 2004) to examine the summertime influence of Asian pollution in the free troposphere over North America. By applying correlation analysis and Principal Component Analysis (PCA) to the observations between 6-12 km, we find dominant influences from recent convection and lightning (13 percent of observations), Asia (7 percent), the lower stratosphere (7 percent), and boreal forest fires (2 percent), with the remaining 71 percent assigned to background. Asian airmasses are marked by high levels of CO, O3, HCN, PAN, acetylene, benzene, methanol, and SO4(2-). The partitioning of reactive nitrogen species in the Asian plumes is dominated by peroxyacetyl nitrate (PAN) (approximately 600 pptv), with varying NO(x)/HNO3 ratios in individual plumes consistent with different plumes ages ranging from 3 to 9 days. Export of Asian pollution in warm conveyor belts of mid-latitude cyclones, deep convection, and lifting in typhoons all contributed to the five major Asian pollution plumes. Compared to past measurement campaigns of Asian outflow during spring, INTEX-A observations display unique characteristics: lower levels of anthropogenic pollutants (CO, propane, ethane, benzene) due to their shorter summer lifetimes; higher levels of biogenic tracers (methanol and acetone) because of a more active biosphere; as well as higher levels of PAN, NO(x), HNO3, and O3 (more active photochemistry possibly enhanced by injection of lightning NO(x)). The high delta O3/delta CO ratio (0.76 mol mol(exp -1)) of Asian plumes during INTEX-A is due to a combination of strong photochemical production and mixing with stratospheric air along isentropic surfaces. The GEOS-Chem global chemical transport model captures the timing and location of the Asian plumes remarkably well. However, it significantly underestimates the magnitude of the enhancements.

We use observations from two aircraft during the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) campaign over the eastern United States and North Atlantic during summer 2004, interpreted with a global 3-D model of tropospheric chemistry (GEOS-Chem) to test current understanding of the regional sources, chemical evolution, and export of nitrogen oxides. The boundary layer NO(x) data provide top-down verification of a 50% decrease in power plant and industry NO(x) emissions over the eastern United States between 1999 and 2004. Observed 8-12 8 km NO(x) concentrations in ICARTT were 0.55 +/- 36 ppbv, much larger than in previous United States aircraft campaigns (ELCHEM, SUCCESS, SONEX). We show that regional lightning was the dominant source of this NO(x) and increased upper tropospheric ozone by 10 ppbv. Simulating the ICARTT upper tropospheric NO(x) observations with GEOS-Chem require a factor of 4 increase in the model NO(x) yield per flash (to 500 mol/flash). Observed OH concentrations were a factor of 2 lower than can be explained from current photochemical models, and if correct would imply a broader lightning influence in the upper troposphere than presently thought.An NO(y)-CO correlation analysis of the fraction f of North American NO(x) emissions vented to the free troposphere as NO(y) (sum of NO(x) and its oxidation products PAN and HNO3) s shows observed f=16+/-10 percent and modeled f=14 +/- 8 percent, consistent with previous studies. Export to the lower free troposphere is mostly HNO3 but at higher altitudes is mostly PAN. The model successfully simulates NO(y) export efficiency and speciation, supporting previous model estimates of a large U.S. contribution to tropospheric ozone through NO(x) and PAN export.

The Intercontinental Chemical Transport Experiment-North America (INTEX-NA) is an international field campaign envisioned to investigate the transport and transformation of gases and aerosols on transcontinental/intercontinental scales and assess their impact on air quality and climate. Phase B (INTEX-B) of the mission was conducted during a 10- week period from March 1 to May 15, 2006 and focused initially on pollution outflow from the Mexico City Metropolitan Area, later addressing the transport of pollution from Asia to North America during springtime meteorological conditions. During the deployment, fast-response (1-s resolution) CO2 measurements were recorded aboard the NASA DC-8 providing valuable regional-scale information on carbon sources and sinks over sparsely sampled areas of North America and adjacent ocean basins. When coupled with the enormously sophisticated chemistry payload on the DC-8, these measurements collectively afford extremely powerful multi-tracer constraints for carbon source/sink attribution. Preliminary examination of the two data sets from the INTEX-B campaign, acquired one month apart, reveals not only the influence of the CO2 seasonal cycle, but also the preponderance of human population and industrial activity in the northern hemisphere. In this presentation, a synergy of the ensemble of airborne and surface observations, bottomup emission inventories, as well as transport history are invoked in a GIS framework to elucidate the source/sink processes reflected in the observations. The airborne CO2 data, along with simultaneous surface measurements (e.g. NOAA ESRL), are examined to establish the vertical distribution and variability of CO2 as a function of location. The role of localized sources, long-range transport, the biosphere, stratospheric exchange, and dynamical processes on the CO2 spatial variability observed throughout the tropospheric column will be discussed.

Observed correlations between atmospheric concentrations of CO2 and CO represent potentially powerful information for improving CO2 surface flux estimates through coupled CO2-CO inverse analyses. We explore the value of these correlations in improving estimates of regional CO2 fluxes in east Asia by using aircraft observations of CO2 and CO from the TRACE-P campaign over the NW Pacific in March 2001. Our inverse model uses regional CO2 and CO surface fluxes as the state vector, separating biospheric and combustion contributions to CO2. CO2-CO error correlation coefficients are included in the inversion as off-diagonal entries in the a priori and observation error covariance matrices. We derive error correlations in a priori combustion source estimates of CO2 and CO by propagating error estimates of fuel consumption rates and emission factors. However, we find that these correlations are weak because CO source uncertainties are mostly determined by emission factors. Observed correlations between atmospheric CO2 and CO concentrations imply corresponding error correlations in the chemical transport model used as the forward model for the inversion. These error correlations in excess of 0.7, as derived from the TRACE-P data, enable a coupled CO2-CO inversion to achieve significant improvement over a CO2-only inversion for quantifying regional fluxes of CO2.

An optical path switch divides sample path radiation into a time series of alternating first polarized components and second polarized components. The first polarized components are transmitted along a first optical path and the second polarized components along a second optical path. A first gasless optical filter train filters the first polarized components to isolate at least a first wavelength band thereby generating first filtered radiation. A second gasless optical filter train filters the second polarized components to isolate at least a second wavelength band thereby generating second filtered radiation. A beam combiner combines the first and second filtered radiation to form a combined beam of radiation. A detector is disposed to monitor magnitude of at least a portion of the combined beam alternately at the first wavelength band and the second wavelength band as an indication of the concentration of the substance in the sample path.

An optical path switch divides sample path radiation into a time series of alternating first polarized components and second polarized components. The first polarized components are transmitted along a first optical path and the second polarized components along a second optical path. A first gasless optical filter train filters the first polarized components to isolate at least a first wavelength band thereby generating first filtered radiation. A second gasless optical filter train filters the second polarized components to isolate at least a second wavelength band thereby generating second filtered radiation. A beam combiner combines the first and second filtered radiation to form a combined beam of radiation. A detector is disposed to monitor magnitude of at least a portion of the combined beam alternately at the first wavelength band and the second wavelength band as an indication of the concentration of the substance in the sample path.

The NASA Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission was conducted in February-April 2001 over the NW Pacific (1) to characterize the Asian chemical outflow and relate it quantitatively to its sources and (2) to determine its chemical evolution. It used two aircraft, a DC-8 and a P-3B, operating out of Hong Kong and Yokota Air Force Base (near Tokyo), with secondary sites in Hawaii, Wake Island, Guam, Okinawa, and Midway. The aircraft carried instrumentation for measurements of long-lived greenhouse gases, ozone and its precursors, aerosols and their precursors, related species, and chemical tracers. Five chemical transport models (CTMs) were used for chemical forecasting. Customized bottom-up emission inventories for East Asia were generated prior to the mission to support chemical forecasting and to serve as a priori for evaluation with the aircraft data. Validation flights were conducted for the Measurements Of Pollution In The Troposphere (MOPITT) satellite instrument and revealed little bias (6 plus or minus 2%) in the MOPITT measurements of CO columns. A major event of transpacific Asian pollution was characterized through combined analysis of TRACE-P and MOPITT data. The TRACE-P observations showed that cold fronts sweeping across East Asia and the associated warm conveyor belts (WCBs) are the dominant pathway for Asian outflow to the Pacific in spring. The WCBs lift both anthropogenic and biomass burning (SE Asia) effluents to the free troposphere, resulting in complex chemical signatures. The TRACE-P data are in general consistent with a priori emission inventories, lending confidence in our ability to quantify Asian emissions from socioeconomic data and emission factors. However, the residential combustion source in rural China was found to be much larger than the a priori, and there were also unexplained chemical enhancements (HCN, CH3Cl, OCS, alkylnitrates) in Chinese urban plumes. The Asian source of CCl4 was found to be much higher than government estimates. Measurements of HCN and CH3CN indicated a dominant biomass burning source and ocean sink for both gases. Large fractions of sulfate and nitrate were found to be present in dust aerosols. Photochemical activity in the Asian outflow was strongly reduced by aerosol attenuation of UV radiation, with major implications for the concentrations of HOx, radicals. New particle formation, apparently from ternary nucleation involving NH3, was observed in Chinese urban plumes.

The meteorological pathways contributing to Asian pollution outflow over the Pacific are examined with a global three-dimensional model analysis of CO observations from the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission (February-April 2001). The model is used also to place the TRACE-P observations in an interannual (1994-2001) and seasonal context. The major process driving Asian pollution outflow in spring is frontal lifting ahead of southeastward-moving cold fronts (the leading edge of cold surges) and transport in the boundary layer behind the cold fronts. Orographic lifting over central and eastern China combines with the cold fronts to promote the transport of Chinese pollution to the free troposphere. Outflow of seasonal biomass burning in Southeast Asia during spring takes place mostly by deep convection but also by northeastward transport and frontal lifting, mixing with the anthropogenic outflow. Boundary layer outflow over the western Pacific is largely devoid of biomass burning influence. European and African (biomass burning) plumes in Asian outflow during TRACE-P were weak (less than 60 ppbv and 20 ppbv CO, respectively) and were not detectable in the observations because of superposition of the much larger Asian pollution signal. Spring 2001 (La Nina) was characterized by unusually frequent cold surge events in the Asian Pacific rim and strong convection in Southeast Asia, leading to unusually strong boundary layer outflow of anthropogenic emissions and convective outflow of biomass burning emissions in the upper troposphere. The Asian outflow flux of CO to the Pacific is found to vary seasonally by a factor of 3-4 (maximum in March and minimum in summer). The March maximum results from frequent cold surge events and seasonal biomass burning emissions.

This paper describes the procedures and algorithms for the laboratory calibration and the field data retrieval of the NASA Langley / Ames Diode Laser Hygrometer as implemented during the NASA Trace-P mission during February to April 2000. The calibration is based on a NIST traceable dewpoint hygrometer using relatively high humidity and short pathlength. Two water lines of widely different strengths are used to increase the dynamic range of the instrument in the course of a flight. The laboratory results are incorporated into a numerical model of the second harmonic spectrum for each of the two spectral window regions using spectroscopic parameters from the HITRAN database and other sources, allowing water vapor retrieval at upper tropospheric and lower stratospheric temperatures and humidity levels. The data retrieval algorithm is simple, numerically stable, and accurate. A comparison with other water vapor instruments on board the NASA DC-8 and ER-2 aircraft is presented.

A system and method are provided for detecting one or more substances. An optical path switch divides sample path radiation into a time series of alternating first polarized components and second polarized components. The first polarized components are transmitted along a first optical path and the second polarized components along a second optical path. A first gasless optical filter train filters the first polarized components to isolate at least a first wavelength band thereby generating first filtered radiation. A second gasless optical filter train filters the second polarized components to isolate at least a second wavelength band thereby generating second filtered radiation. The first wavelength band and second wavelength band are unique. Further, spectral absorption of a substance of interest is different at the first wavelength band as compared to the second wavelength band. A beam combiner combines the first and second filtered radiation to form a combined beam of radiation. A detector is disposed to monitor magnitude of at least a portion of the combined beam alternately at the first wavelength band and the second wavelength band as an indication of the concentration of the substance in the sample path.

With aircraft-mounted in-situ and remote sensing instruments for dynamical, thermal. and chemical measurements, we studied two cases of tropopause folding. In both folds we found Kelvin-Helmholtz billows with horizontal wavelength of about 900 m and thickness of about 120 m. In one case the instability was effectively mixing the bottomside of the fold, leading to the transfer of stratospheric air into the troposphere. Also we discovered in both cases small-scale secondary ozone maxima shortly after the aircraft ascended past the topside of the fold that corresponded to regions of convective instability. We interpreted this phenomenon as convectively breaking gravity waves. Therefore, we posit that convectively breaking gravity waves acting on tropopause folds must be added to the list of important irreversible mixing mechanisms leading to stratosphere-troposphere exchange.

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.

The Pacific Exploratory Mission-West B (PEM-West B) explored atmospheric layer structure using measurements of O3, H2O, CO, and CH4 from the NASA DC-8 fast-response instruments. The mission took place in February-March 1994 over the western Pacific, mainly in the northern hemisphere. Results were compared with similar measurements made during the Pacific Exploratory Mission-West A (PEM-West A) in September-October 1991. PEM-West B sampled 94 vertical profiles, with an average atmospheric depth per profile of 6.4 km, and this sampling yielded 254 discrete layers. PEM-West A sampled 105 profiles, also with a 6.4 km average depth, yielding 538 layers. Both missions revealed that layers containing high ozone and low water vapor were the most abundant, and low ozone and high water vapor layers were the next most abundant. Lidar images and potential vorticity cross sections showed the former associated with subsidence from the stratosphere in middle latitudes, spreading into the tropics. The latter was associated with convection from the boundary layer. The partition among different types of layers only changed slightly in the two missions, although PEM-West B had half as many layers. Compared to PEM-West A, PEM-West B showed only one-third the number of layers associated with polluted continental air. However, PEM-West B revealed significantly more layers showing characteristics of descended clean marine air. In some cases these layers originated from the southern hemisphere. For ozone- and water-vapor-rich layers, the ozone deviation amplitude was higher in low latitudes and lower in high latitudes in PEM-West B. The mean thickness of layers increased from about 450 m in PEM-West A to 680 in in PEM-West B. Layers also existed in the Intertropical Convergence Zone. CO2 measurements had sufficient vertical resolution to show layer structure as well.

The Geostationary Tropospheric Pollution Satellite (GEO TROPSAT) mission is a new approach to measuring the critical constituents of tropospheric ozone chemistry: ozone, carbon monoxide, nitrogen dioxide, and aerosols. The GEO TROPSAT mission comprises a constellation of three instruments flying as secondary payloads on geostationary communications satellites around the world. This proposed approach can significantly reduce the cost of getting a science payload to geostationary orbit and also generates revenue for the satellite owners. The geostationary vantage point enables simultaneous high temporal and spatial resolution measurement of tropospheric trace gases, leading to greatly improved atmospheric ozone chemistry knowledge. The science data processing, conducted as a research (not operational) activity, will provide atmospheric trace gas data many times per day over the same region at better than 25 km ground footprint. The high temporal resolution identifies short time scale processes, diurnal variations, seasonal trends, and interannual variation.

Airborne heat, moisture, O3, CO, and CH4 flux measurements were obtained over the Hudson Bay lowlands (HBL) and northern boreal forest regions of Canada during July - August 1990. The airborne flux measurements were an integral part of the NASA/Arctic Boundary Layer Expedition (ABLE) 3B field experiment executed in collaboration with the Canadian Northern Wetlands Study (NOWES). Airborne CH4 flux measurements were taken over a large portion of the HBL. The surface level flux of CH4 was obtained from downward extrapolations of multiple-level CH4 flux measurements. Methane source strengths ranged from -1 to 31 mg m(exp -2)/d, with the higher values occurring in relatively small, isolated areas. Similar measurements of the CH4 source strength in the boreal forest region of Schefferville, Quebec, ranged from 6 to 27 mg m(exp -2)/d and exhibited a diurnal dependence. The CH4 source strengths found during the ABLE 3B expedition were much lower than the seasonally averaged source strength of 51 mg m(exp -2)/d found for the Yukon-Kuskokwim delta region of Alaska during the previous ABLE 3A study. Large positive CO fluxes (0.31 to 0.53 parts per billion by volume (ppbv) m/s) were observed over the inland, forested regions of the HBL study area, although the mechanism for the generation of these fluxes was not identified. Repetitive measurements along the same ground track at various times of day near the Schefferville site also suggested a diurnal dependence for CO emissions. Measurements of surface resistance to the uptake of O3 (1.91 to 0.80 s/cm) for the HBL areas investigated were comparable to those observed near the Schefferville site (3.40 to 1.10 s/cm). Surface resistance values for the ABLE 3B study area were somewhat less than those observed over the Yukon-Kuskokwim delta during the previous ABLE 3A study. The budgets for heat, moisture, O3, CO, and CH4 were evaluated. The residuals from these budget studies indicated, for the cases selected, a moderate net photochemical production of O3 present in the boundary layer over the HBL that coincided with an in situ destruction of CO, although the mechanism responsible for the destruction of CO was not identified. Results from the O3 budget analysis indicate the importance of in situ photochemical production and its possible dominance over surface deposition to the local O3 budget at the Schefferville site. Measurements of the in situ production of O3 indicated a direct relationship between the presence of biomass burning or large-scale pollution effects. Residuals from budget calculations for conserved quantities (heat, moisture, and CH4) were compared with their respective surface fluxes to provide a measure of the internal self-consistency of the flux measurements.

Although several methods exist for the determination of the flux of an atmospheric species, the airborne eddy correlation method has the advantage of providing direct flux measurements that are representative of regional spatial domains. The design criteria pertinent to the construction of chemical instrumentation suitable for use in airborne eddy correlation flux measurements are discussed. A brief overview of the advantages and limitations of the current instrumentation used to obtain flux measurements for CO, CH4, O3, CO2, and water vapor are given. The intended height of the measurement within the convective boundary layer is also shown to be an important design criteria. The sensitivity, or resolution, which is required in the measurement of a scalar species to obtain an adequate species flux measurement is discussed. The relationship between the species flux resolution and the more commonly stated instrumental resolution is developed and it is shown that the standard error of the flux estimate is a complicated function of the atmospheric variability and the averaging time that is used. The use of the recently proposed intermittent sampling method to determine the species flux is examined. The application of this technique may provide an opportunity to expand the suite of trace gases for which direct flux measurements are possible.

Enhanced concentrations of CH4 in the unpolluted atmospheric mixed layer over both Arctic and subarctic tundra landscapes are documented here using data from the NASA Arctic Boundary Layer Expedition (ABLE 3A). The CH4 concentration gradients were determined mainly by interactions of biogenic emission from wet tundra and turbulent mixing proceses. The gradient were most frequently associated with intrusion of upper tropospheric or stratospheric air into the midtroposphere, emissions from forest and tundra fires, and long-range transport of enhanced concentration of these gases from unidentified sources. Summertime haze layers exhibited midtropospheric enhancements of CH4 similar to those measured in winter Arctic events. The observations confirm the importance of Arctic and Subarctic wetland environments as a regional source of global atmospheric CH4.

In situ airborne flux values for O3, CO, an CH4 over selected wetlands of Alaska are reported, and airborne CH4 flux measurements are presented for the first time. The source/sink distribution over the Yukon-Kuskokwim Delta (YKD) is qualitatively correlated with surface vegetation type. The CH4 source strength over the YKD ranged from 25 to 85 mg/sq m/d. A spatially averaged, seasonally adjusted source strength of 51 mg/sq m/d was established for the YKD. Indirect CH4 flux estimates obtained over the Alaskan North Slope indicate a much lower source strength. The global CH4 emission from tundra are estimated to be 44 Tg/a at an upper limit. Airborne CO flux measurements over the YKD indicate low negative flux values over the coastal areas, while some positive fluxes were observed in the inland sparsely forested regions. An inspection of the cospectrum of CO with vertical velocity for sample runs in coastal areas indicate the possibility of in situ photochemical destruction/production of CO.