Patterns of CO2 and radiocarbon across high northern latitudes during International Polar Year 2008

High-resolution in situ CO2 measurements were conducted aboard the NASA DC-8 aircraft during the ARCTAS/POLARCAT field campaign, a component of the wider 2007-2008 International Polar Year activities. Data were recorded during large-scale surveys spanning the North American sub-Arctic to the North Pole from 0.04 to 12 km altitude in spring and summer of 2008. Influences on the observed CO2 concentrations were investigated using coincident CO, black carbon, CH3CN, HCN, O3, C2Cl4, and Δ14CO2 data, and the FLEXPART model. In spring, the CO2 spatial distribution from 55̊N to 90̊N was largely determined by the long-range transport of air masses laden with Asian anthropogenic pollution intermingled with Eurasian fire emissions evidenced by the greater variability in the mid-to-upper troposphere. At the receptor site, the enhancement ratios of CO2 to CO in pollution plumes ranged from 27 to 80 ppmv ppmv-1 with the highest anthropogenic content registered in plumes sampled poleward of 80̊N. In summer, the CO2 signal largely reflected emissions from lightning-ignited wildfires within the boreal forests of northern Saskatchewan juxtaposed with uptake by the terrestrial biosphere. Measurements within fresh fire plumes yielded CO2 to CO emission ratios of 4 to 16 ppmv ppmv-1 and a mean CO2 emission factor of 1698 ± 280 g kg-1 dry matter. From the 14C in CO2 content of 48 whole air samples, mean spring (46.6 ± 4.4%) and summer (51.5 ± 5%) D14CO2 values indicate a 5%seasonal difference. Although the northern midlatitudes were identified as the emissions source regions for the majority of the spring samples, depleted Δ14CO2 values were observed in <1% of the data set. Rather, ARCTAS Δ14CO2 observations (54%) revealed predominately a pattern of positive disequilibrium (1-7%) with respect to background regardless of season owing to both heterotrophic respiration and fire-induced combustion of biomass. Anomalously enriched Δ14CO2 values (101-262%) measured in emissions from Lake Athabasca and Eurasian fires speak to biomass burning as an increasingly important contributor to the mass excess in Δ14CO2 observations in a warming Arctic, representing an additional source of uncertainty in the quantification of fossil fuel CO2

Spatial and temporal patterns of visibility in Las Vegas, July 2000--July 2001

The Clark County Department of Air Quality Management and the Nevada Department of Motor Vehicles funded a one-year study of visibility trends in Las Vegas. The Desert Research Institute conducted this study from July 2000 to July 2001. The monitoring sites for this study were chosen to represent three areas in Las Vegas, urban, suburban and background/transport. Strong diurnal patterns were found at the urban and suburban sites. The background site had low levels of air pollution, and most of the haze at this site was due to light scattering by particles. The suburban site followed a well-defined diurnal pattern during the cold season, and showed the influences of local activities (such as road construction) during the study. Overall, the urban site had the highest levels of visibility impairment, but during midday the visibility at this site improved and was comparable to that of the suburban site. This thesis presents the data from this study

Comparison of chemical characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign

This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska, USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Approximately 500 smoke plumes from biomass burning emissions that varied in age from minutes to days were segregated by fire source region and urban emission influences. The normalized excess mixing ratios (NEMR) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen and ozone) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared. A detailed statistical analysis of the different plume categories for different gaseous and aerosol species is presented in this paper. The comparison of NEMR values showed that CH4 concentrations were higher in air-masses that were influenced by urban emissions. Fresh biomass burning plumes mixed with urban emissions showed a higher degree of oxidative processing in comparison with fresh biomass burning only plumes. This was evident in higher concentrations of inorganic aerosol components such as sulfate, nitrate and ammonium, but not reflected in the organic components. Lower NOx NEMRs combined with high sulfate, nitrate and ammonium NEMRs in aerosols of plumes subject to long-range transport, when comparing all plume categories, provided evidence of advanced processing of these plumes

Characterization of soluble bromide measurements and a case study of BrO observations during ARCTAS

A focus of the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission was examination of bromine photochemistry in the spring time high latitude troposphere based on aircraft and satellite measurements of bromine oxide (BrO) and related species. The NASA DC-8 aircraft utilized a chemical ionization mass spectrometer (CIMS) to measure BrO and a mist chamber (MC) to measure soluble bromide. We have determined that the MC detection efficiency to molecular bromine (Br2), hypobromous acid (HOBr), bromine oxide (BrO), and hydrogen bromide (HBr) as soluble bromide (Br−) was 0.9±0.1, 1.06+0.30/−0.35, 0.4±0.1, and 0.95±0.1, respectively. These efficiency factors were used to estimate soluble bromide levels along the DC-8 flight track of 17 April 2008 from photochemical calculations constrained to in situ BrO measured by CIMS. During this flight, the highest levels of soluble bromide and BrO were observed and atmospheric conditions were ideal for the space-borne observation of BrO. The good agreement (R2 = 0.76; slope = 0.95; intercept = −3.4 pmol mol−1) between modeled and observed soluble bromide, when BrO was above detection limit (\u3e2 pmol mol−1) under unpolluted conditions (NOmol−1), indicates that the CIMS BrO measurements were consistent with the MC soluble bromide and that a well characterized MC can be used to derive mixing ratios of some reactive bromine compounds. Tropospheric BrO vertical column densities (BrOVCD) derived from CIMS BrO observations compare well with BrOTROPVCD from OMI on 17 April 2008

Comparison of the chemical evolution and characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign

This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Extensive investigations of boreal fire plume evolution were undertaken during ARCTAS-B, where four distinct fire plumes that were intercepted by the aircraft over a range of down-wind distances (0.1 to 16 hr transport times) were studied in detail. Based on these analyses, there was no evidence for ozone production and a box model simulation of the data confirmed that net ozone production was slow (on average 1 ppbv h−1 in the first 3 h and much lower afterwards) due to limited NOx. Peroxyacetyl nitrate concentrations (PAN) increased with plume age and the box model estimated an average production rate of ~80 pptv h−1 in the first 3 h. Like ozone, there was also no evidence for net secondary inorganic or organic aerosol formation. There was no apparent increase in aerosol mass concentrations in the boreal fire plumes due to secondary organic aerosol (SOA) formation; however, there were indications of chemical processing of the organic aerosols. In addition to the detailed studies of boreal fire plume evolution, about 500 smoke plumes intercepted by the NASA DC-8 aircraft were segregated by fire source region. The normalized excess mixing ratios (i.e. ΔX/ΔCO) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen (NOx), ozone, PAN) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared

Development and implementation of a new biomass burning emissions injection height scheme (BBEIH v1.0) for the GEOS-Chem model (v9-01-01)

Biomass burning is a significant source of trace gases and aerosols to the atmosphere, and the evolution of these species depends acutely on where they are injected into the atmosphere. GEOS-Chem is a chemical transport model driven by assimilated meteorological data that is used to probe a variety of scientific questions related to atmospheric composition, including the role of biomass burning. This paper presents the development and implementation of a new global biomass burning emissions injection scheme in the GEOS-Chem model. The new injection scheme is based on monthly gridded Multi-angle Imaging SpectroRadiometer (MISR) global plume-height stereoscopic observations in 2008. To provide specific examples of the impact of the model updates, we compare the output from simulations with and without the new MISR-based injection height scheme to several sets of observations from regions with active fires. Our comparisons with Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) aircraft observations show that the updated injection height scheme can improve the ability of the model to simulate the vertical distribution of peroxyacetyl nitrate (PAN) and carbon monoxide (CO) over North American boreal regions in summer. We also compare a simulation for October 2010 and 2011 to vertical profiles of CO over the Amazon Basin. When coupled with larger emission factors for CO, a simulation that includes the new injection scheme also better matches selected observations in this region. Finally, the improved injection height improves the simulation of monthly mean surface CO over California during July 2008, a period with large fires

Patterns of CO_2 and radiocarbon across high northern latitudes during International Polar Year 2008

High-resolution in situ CO_2 measurements were conducted aboard the NASA DC-8 aircraft during the ARCTAS/POLARCAT field campaign, a component of the wider 2007–2008 International Polar Year activities. Data were recorded during large-scale surveys spanning the North American sub‐Arctic to the North Pole from 0.04 to 12 km altitude in spring and summer of 2008. Influences on the observed CO_2 concentrations were investigated using coincident CO, black carbon, CH_3CN, HCN, O_3, C_2Cl_4, and Δ^(14)CO_2 data, and the FLEXPART model. In spring, the CO_2 spatial distribution from 55°N to 90°N was largely determined by the long-range transport of air masses laden with Asian anthropogenic pollution intermingled with Eurasian fire emissions evidenced by the greater variability in the mid-to-upper troposphere. At the receptor site, the enhancement ratios of CO_2 to CO in pollution plumes ranged from 27 to 80 ppmv ppmv^(−1) with the highest anthropogenic content registered in plumes sampled poleward of 80°N. In summer, the CO_2 signal largely reflected emissions from lightning-ignited wildfires within the boreal forests of northern Saskatchewan juxtaposed with uptake by the terrestrial biosphere. Measurements within fresh fire plumes yielded CO_2 to CO emission ratios of 4 to 16 ppmv ppmv^(−1) and a mean CO_2 emission factor of 1698 ± 280 g kg^(−1) dry matter. From the ^(14)C in CO_2 content of 48 whole air samples, mean spring (46.6 ± 4.4‰) and summer (51.5 ± 5‰) Δ^(14)CO_2 values indicate a 5‰ seasonal difference. Although the northern midlatitudes were identified as the emissions source regions for the majority of the spring samples, depleted Δ^(14)CO_2 values were observed in <1% of the data set. Rather, ARCTAS Δ^(14)CO_2 observations (54%) revealed predominately a pattern of positive disequilibrium (1–7‰) with respect to background regardless of season owing to both heterotrophic respiration and fire-induced combustion of biomass. Anomalously enriched Δ^(14)CO_2 values (101–262‰) measured in emissions from Lake Athabasca and Eurasian fires speak to biomass burning as an increasingly important contributor to the mass excess in Δ^(14)CO_2 observations in a warming Arctic, representing an additional source of uncertainty in the quantification of fossil fuel CO_2

Investigating water soluble organic aerosols: sources and evolution

An existing method for the measurement of atmospheric gaseous species was modified to collect data on aerosol concentrations. Data from biomass burning events in different regions (Canada, the Arctic and California) were collected during April to July, 2008 and the concentrations and evolution of secondary organic aerosols were discussed. And finally, data on the light absorbing properties of water soluble organic aerosols were collected in Atlanta, GA and compared with filter data for the same properties. The results presented in this thesis showed that a negative ion chemical ionization mass spectrometer (CIMS), can be modified by the addition of a thermally denuded inlet to measure aerosol phase sulfuric acid. This system can also be used to measure other aerosol phase organic acids. In the biomass burning plumes studied in the second part, no clear indication of formation of secondary aerosol or gaseous species was observed, except for peroxyacetyl nitrate (PAN). Filter data collected from FRM sites in the Southeastern U.S. showed that biomass burning is the most dominant source of water soluble light absorbing carbonaceous aerosol in this region. The data from a study in Atlanta, GA showed that the online PILS-LWCC-WSOC system might be used for measurements of light absorbing properties of aerosols and WSOC.Ph.D