Tropospheric sulfate distribution during SUCCESS: Contributions from jet exhaust and surface sources

The distribution of SO4= aerosol over the central US during SUCCESS indicates that surface sources of SO4= and SO2 in the western US caused SO4= enhancements up to 10 km altitude. The mean (median) SO4= mixing ratio in the mid- and upper-troposphere increased from 24 (16) pptv over the Pacific ocean to 58 (29) pptv over the central plains. Above 10 km the SO4=mixing ratio was essentially the same in both regions, and also when the geographic classifications were further partitioned into upper tropospheric and lower stratospheric categories (mean near 40 pptv). No obvious enhancements of SO4= could be detected in jet exhaust plumes, but this may reflect the difficulty of keeping a large airborne sampling platform within a turbulent wake for time periods longer than a few seconds. Expected SO4=enhancements (based on observed CO2 enhancements and emission factors for these two species) were generally much smaller than the variability of ambient SO4= mixing ratios, so our null result does not mean that aircraft do not emit H2SO4

Influence of vertical transport on free tropospheric aerosols over the central USA in springtime

Measurements of the atmospheric aerosol chemical composition during the Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) indicate substantial vertical transport of boundary layer aerosol to the free troposphere over the south-central United States during springtime. Mixing ratios of water-soluble aerosol Ca 2+ at 6 - 12 km altitude exhibited a median mixing ratio of 20 pptv, with 15% of the measurements \u3e 100 pptv and a maximum of ! 235 pptv. In air parcels with enhanced Ca 2+, the ratios K+/Ca 2+, Mg2+/Ca 2+, and Na+/Ca 2+ in the bulk aerosol were distinctly characteristic of those in limestone and/or cement. Significantly enhanced mixing ratios of aerosol SO42-, NO3-, and NH4 + were also concomitant with the elevated Ca 2+, suggesting transport of both crustal and anthropogenic aerosols to the upper troposphere. The mass concentration of water-soluble aerosol material was in the range 0.1 - 6 pg m -3 STP, and estimated crustal dust levels were 7 - 160 pg m \u273 ST

Soluble acidic species in air and snow at Summit, Greenland

Simultaneous measurements of the concentrations of soluble acidic species in the gas, aerosol and snow phases at Summit, Greenland were made during summer 1993. Mean concentrations of gas phase HCOOH, CH3COOH, and HNO3 (49±28, 32±17 and 0.9±0.6 nmol m−3 STP, respectively) exceeded the concentrations of aerosol-associated HCOO−, CH3COO−, and NO3−by 1–3 orders of magnitude. On average, SO2 concentrations (0.9±0.6 nmol m−3 STP) were approximately 1/3 those of aerosol SO4=, but this ratio varied widely due largely to changes in the concentration of aerosol SO4=. Concentrations of aerosol SO4= plus SO2 consistently exceeded the sum of aerosol NO3− plus HNO3, yet NO3− was 3–20 times as abundant as SO4=in surface snow. Gas phase concentrations of HCOOH and CH3COOH at Summit were unexpectedly as large as those previously reported for several high latitude continental sites. However, carboxylate concentrations in snow were lower than those of SO4=. Our observation of post-depositional loss of these carboxylic acids within hours after a snowfall must partially explain the low concentrations found in snow. The relative abundance of soluble acids in summer snow at Summit was opposite of that in the overlying atmosphere. Our results highlight the need for improved understanding of the processes controlling transfer of soluble atmospheric species between air and snow

Simultaneous measurements of particulate and gas-phase water-soluble organic carbon concentrations at remote and urban-influenced locations

The sources, sinks, and overall importance of watersoluble organic carbon (WSOC) in the atmosphere are not well understood. Although the primary historical focus has been on particulate WSOC (WSOCP), here we also present results obtained using a newly developed technique that additionally measures gas-phase water-soluble organic carbon (WSOCG). These first-of-their-kind measurements show that WSOCG can often be more than ten times larger than WSOCP at both urban and remote locations. The average fraction of WSOC residing in the gas phase (fg = WSOCG/(WSOCG + WSOCP)) at five various field sites ranged from 0.64 to 0.93, implying significant differences in WSOC phase partitioning between locations. At Houston, TX, and Summit, Greenland, a repeatable diurnal pattern was observed, with minimum values for fg occurring at night. These trends likely are due, at least in part, to temperature and/or relative humidity related gas-to-particle partitioning. These coincident measurements of WSOC in both the gas and particle phases indicate that a relatively large reservoir of water-soluble organic mass is not taken into account by measurements focused only on WSOCP. In addition, a significant amount of WSOCG is available to form WSOCP or enter cloud droplets depending on the chemical and physical properties of the droplets and/or aerosols present. Citation: Anderson, C., J. E. Dibb, R. J. Griffin, and M. H. Bergin (2008), Simultaneous measurements of particulate and gas-phase water-soluble organic carbon concentrations at remote and urban-influenced locations, Geophys. Res. Lett., 35, L13706, doi:10.1029/2008GL033966

Sulfate and MSA in the air and snow on the Greenland Ice Sheet

Sulfate and methanesulfonic acid (MSA) concentrations in aerosol, surface snow, and snowpit samples have been measured at two sites on the Greenland Ice Sheet. Seasonal variations of the concentrations observed for these chemical species in the atmosphere are reproduced in the surface snow and preserved in the snowpit sequence. The amplitude of the variations over a year are smaller in the snow than in the air, but the ratios of the concentrations are comparable. The seasonal variations for sulfate are different at the altitude of the Ice Sheet compared to those observed at sea level, with low concentrations in winter and short episodes of elevated concentrations in spring. In contrast, the variations in concentrations of MSA are similar to those measured at sea level, with a first sequence of elevated concentrations in spring and another one during summer, and a winter low resulting from low biogenic production. The ratio MSA/sulfate clearly indicates the influence of high-latitude sources for the summer maximum of MSA, but the large impact of anthropogenic sulfate precludes any conclusion for the spring maximum. The seasonal pattern observed for these species in a snowpit sampled according to stratigraphy indicates a deficit in the accumulation of winter snow at the summit of the Greenland Ice Sheet, in agreement with some direct observations. A deeper snowpit covering the years 1985–1992 indicates the consistency of the seasonal pattern for MSA over the years, which may be linked to transport and deposition processes

A summer time series of particulate carbon in the air and snow at Summit, Greenland

Carbonaceous particulate matter is ubiquitous in the lower atmosphere, produced by natural and anthropogenic sources and transported to distant regions, including the pristine and climate-sensitive Greenland Ice Sheet. During the summer of 2006, ambient particulate carbonaceous compounds were characterized on the Greenland Ice Sheet, including the measurement of particulate organic (OC) and elemental (EC) carbon, particulate water-soluble organic carbon (WSOC), particulate absorption coefficient (σap), and particle size-resolved number concentration (PM0.1–1.0). Additionally, parallel ∼50-day time series of water-soluble organic carbon (WSOC), water-insoluble organic carbon (WIOC), and elemental carbon (EC) were quantified at time increments of 4–24 h in the surface snow. Measurement of atmospheric particulate carbon found WSOC (average of 52 ng m−3) to constitute a major fraction of particulate OC (average of 56 ng m−3), suggesting that atmospheric organic compounds reaching the Greenland Ice Sheet in summer are highly oxidized. Atmospheric EC (average of 7 ng m−3) was well-correlated with σap (r = 0.95) and the calculated mass-absorption cross-section (average of 24 m2 g−1) appears to be similar to that measured using identical techniques in an urban environment in the United States. Comparing surface snow to atmospheric particulate matter concentrations, it appears the snow has a much higher OC (WSOC+WIOC) to EC ratio (205:1) than air (10:1), suggesting that snow is additionally influenced by water-soluble gas-phase compounds. Finally, the higher-frequency (every 4–6 h) sampling of snow-phase WSOC revealed significant loss (40–54%) of related organic compounds in surface snow within 8 h of wet deposition

Enhanced secondary organic aerosol formation due to water uptake by fine particles

This study characterizes the partitioning behavior of a significant fraction of the ambient organic aerosol through simultaneous measurements of gas and particle watersoluble organic carbon (WSOC). During the summer in Atlanta, WSOC gas/particle partitioning showed a strong RH dependence that was attributed to particulate liquid water. At elevated RH levels (\u3e70%) a significant increase in WSOC partitioning to the particle phase was observed and followed the predicted water uptake by fine particles. The enhancement in particle-phase partitioning translated to increased median particle WSOC concentrations ranging from 0.3 –0.9 mgCm3 . The results provide a detailed overview of the WSOC partitioning behavior in the summertime in an urban region dominated by biogenic emissions, and indicate that secondary organic aerosol formation involving partitioning to liquid water may be a significant aerosol formation route that is generally not considered. Citation: Hennigan, C. J., M. H. Bergin, J. E. Dibb, and R. J. Weber (2008), Enhanced secondary organic aerosol formation due to water uptake by fine particles, Geophys. Res. Lett., 35, L18801, doi:10.1029/2008GL035046

Temporal and spatial variability of snow accumulation in central Greenland

Snow accumulation records from central Greenland are explored to improve the understanding of the accumulation signal in Greenland ice core records. Results from a “forest” of 100 bamboo poles and automated accumulation monitors in the vicinity of Summit as well as shallow cores collected in the Summit and Crete areas are presented. Based on these accumulation data, a regression has been calculated to quantify the signal-to-noise variance ratio of ice core accumulation signals on a variety of temporal (1 week to 2 years) and spatial (20 m to 200 km) scales. Results are consistent with data obtained from year-round automated accumulation measurements deployed at Summit which suggest that it is impossible to obtain regional snow accumulation data with seasonal resolution using four accumulation monitors positioned over a length scale of ∼30 km. Given this understanding of the temporal and spatial dependence of noise in the ice core accumulation signal, the accumulation records from 17 shallow cores are revisited. Each core spans the time period from 1964 to 1983. By combining the accumulation records, the regional snow accumulation record has been obtained for this period. The results show that 9 of the 20 years can be identified as having an accumulation different from the 20 year mean with 99% confidence. The signal-to-noise variance ratio for the average accumulation signal sampled at annual intervals is 5.8±0.5. The averaged accumulation time series may be useful to climate modelers attempting to validate their models with accurate regional hydrologic data sets

Exploring positive adjustment in people with spinal cord injury.

This study explored adjustment in people with spinal cord injury; data from four focus groups are presented. Thematic analysis revealed four themes, managing goals and expectations, comparison with others, feeling useful and acceptance, showing participants positively engaged in life, positively interpreted social comparison information and set realistic goals and expectations. These positive strategies show support for adjustment theories, such as the Cognitive Adaptation Theory, the Control Process Theory and Response Shift Theory. These results also provide insight into the adjustment process of a person with spinal cord injury and may be useful in tailoring support during rehabilitation

Relationship between continuous aerosol measurements and firn core chemistry over a 10-year period at the South Pole

Before ice core chemistry can be used to estimate past atmospheric chemistry it is necessary to establish an unambiguous link between concentrations of chemical species in the air and snow. For the first time a continuous long-term record of aerosol properties (aerosol light scattering coefficient, σsp, and Ångström exponent, å) at the South Pole are compared with the chemical record from a high resolution firn core (∼10 samples per year) covering the period from 1981 to 1991. Seasonal signals in å, associated with winter minima due to coarse mode seasalt and summer maxima due to accumulation mode sulfate aerosol, are reflected in the firn core SO42−/Na+ concentration ratio. Summertime ratios of σsp and aerosol optical depth, τ to corresponding firn core sulfur concentrations are determined and the ‘calibrations’ are applied to sulfur concentrations in snowpits from a previous study. Results show that σsp estimates from snowpit sulfur concentrations are in agreement with atmospheric measurements while τ estimates are significantly different, which is likely due to the lack of understanding of the processes that mix surface air with air aloft