Relationships between surface and column aerosol radiative properties and air mass transport at a rural New England site

Chemical, physical, and radiative properties of surface and vertical column aerosols were measured at a rural site in southern New Hampshire from July 2000 to September 2001. The primary objective was to determine how intensive and extensive aerosol properties vary in air masses originating in different upwind regions. The data set also allows for an investigation of some of the relationships between surface and column aerosol properties at the site, and provides an estimate of direct radiative forcing by aerosols during the study period. Extensive properties (e.g., optical depth and chemical concentration) were at maximum values during times of south-southwest (S-SW) transport, while minimum values were seen during north-northeast (N-NE) transport. Certain intensive properties such as fine particle mass scattering efficiency did not vary significantly between times of transport from different source regions. Mean optical depth (wavelength = 500 nm) was 0.24 during S-SW transport, compared to 0.10 during N-NE transport. The study period average scattering efficiency for (NH4)2SO4 was 6.54 ± 0.26 m2 g−1 (± standard error) and 3.36 ± 0.49 m2 g−1 for organic carbon, while the absorption efficiency of elemental carbon was 12.85 ± 0.80 m2 g−1. Top of the atmosphere aerosol direct radiative forcing was −0.35 ± 0.83 Wm−2 (±1 standard deviation) in winter 2000–2001 and −9.06 ± 3.77 Wm−2 in summer 2001, differences that can be primarily attributed to seasonal changes in surface reflectance (high in winter, low in summer) and the relatively low values of single scatter albedo observed in winter. The annual average direct radiative forcing was −5.14 ± 4.32 Wm−2. We generally observed a moderate correlation between surface and column aerosol light extinction, suggesting that vertical column aerosol radiative properties measured by surface-based radiometers should be supplemented by boundary layer measurements of aerosol chemical, physical, and radiative properties to help understand the mechanisms contributing to global aerosol variability

Air-snow exchange investigations at Summit, Greenland: An overview

The Greenland Ice Sheet Project 2 (GISP2) and Greenland Ice Core Project (GRIP) deep drilling programs at Summit, Greenland included support (both logistical and scientific) of extensive investigation of atmospheric transport and air-snow exchange processes of gases and particles relevant to the interpretation of the ice-core records. Much of the sampling for the air-snow exchange investigations was conducted at a unique solar-powered camp 30 km southwest of the GISP2 drill camp (even further from the GRIP camp) and was characterized by a high degree of international collaboration and cooperation. The wide range of expertise and analytical capabilities of the 20-plus investigators participating in these studies has provided important insight into the meteorological, physical, and chemical processes which interact to determine the composition of snow and firn at Summit. Evolving understanding of this system will allow improved reconstruction of the composition of the atmosphere over Greenland in the past from the detailed Summit ice-core records. This paper provides an overview of air-snow exchange investigations at Summit, including their development through the course of the drilling programs (1989–1993), significant findings related to both air-snow exchange issues and the present state of the Arctic free troposphere, as well as the major outstanding questions which are being addressed in ongoing experiments at Summit

Airborne sampling of aerosol particles: Comparison between surface sampling at Christmas Island and P-3 sampling during PEM-Tropics B

Bulk aerosol sampling of soluble ionic compounds from the NASA Wallops Island P-3 aircraft and a tower on Christmas Island during PEM-Tropics B provides an opportunity to assess the magnitude of particle losses in the University of New Hampshire airborne bulk aerosol sampling system. We find that most aerosol-associated ions decrease strongly with height above the sea surface, making direct comparisons between mixing ratios at 30 m on the tower and the lowest flight level of the P-3 (150 m) open to interpretation. Theoretical considerations suggest that vertical gradients of sea-salt aerosol particles should show exponential decreases with height. Observed gradients of Na+ and Mg2+, combining the tower observations with P-3 samples collected below 1 km, are well described by exponential decreases (r values of 0.88 and 0.87, respectively), though the curve fit underestimates average mixing ratios at the surface by 25%. Cascade impactor samples collected on the tower show that \u3e99% of the Na+ and Mg2+mass is on supermicron particles, 65% is in the 1–6 micron range, and just 20% resides on particles with diameters larger than 9 microns. These results indicate that our airborne aerosol sampling probes must be passing particles up to at least 6 microns with high efficiency. We also observed that nss SO42− and NH4+, which are dominantly on accumulation mode particles, tended to decrease between 150 and 1000 m, but they were often considerably higher at the lowest P-3 sampling altitudes than at the tower. This finding is presently not well understood

Asian dust storm events of spring 2001 and associated pollutants observed in New England by the Atmospheric Investigation, Regional Modeling, Analysis and Prediction (AIRMAP) monitoring network

Between 18 April and 13 May 2001, three statistically extreme dust aerosol events were observed across the entire northeastern United States. High levels of bulk aerosol water-soluble Ca2+ (range = 42–482 pptv) and PM2.5 elemental Ca (range = 19–156 pptv) were observed simultaneously at Atmospheric Investigation, Regional Modeling, Analysis and Prediction (AIRMAP) and Interagency Monitoring of Protected Visual Environments (IMPROVE) stations. On the basis of Ca2+ concentrations, the average bulk dust concentration for all events across all four AIRMAP stations was estimated to be 7.4 μg/m3. There was no evidence of dust outbreaks in North America large enough to explain these events. However, in April 2001, massive dust storms occurred in the Tarim Pendi basin and in the Gobi deserts of southern Mongolia and China. Comparison of elemental ratios of AIRMAP samples to previously reported Asian dust aerosol samples showed that all AIRMAP samples had a chemical composition similar to Asian dust transported over long distances. Within the dust plumes, strong correlations were observed between absorption, scattering, and CO, indicative of an anthropogenic contribution including elemental carbon and SO42− aerosols. Aerosol NO3− was also highly elevated during event days, most likely due to uptake of HNO3 by the dust during transport. A comparison of dust plumes sampled by AIRMAP to those sampled off the Asian coast during the TRACE-P airborne mission and on the U.S. west coast, strongly suggested entrainment of additional pollutants (e.g., CO, aerosol NO3−, and SO42−) as the dust plumes were transported over North America

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

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

Bromide and other ions in the snow, firn air, and atmospheric boundary layer at Summit during GSHOX

Measurements of gas phase soluble bromide in the boundary layer and in firn air, and Br− in aerosol and snow, were made at Summit, Greenland (72.5° N, 38.4° W, 3200 m a.s.l.) as part of a larger investigation into the influence of Br chemistry on HOx cycling. The soluble bromide measurements confirm that photochemical activation of Br− in the snow causes release of active Br to the overlying air despite trace concentrations of Br− in the snow (means 15 and 8 nmol Br− kg−1 of snow in 2007 and 2008, respectively). Mixing ratios of soluble bromide above the snow were also found to be very small (mean \u3c1 ppt both years, with maxima of 3 and 4 ppt in 2007 and 2008, respectively), but these levels clearly oxidize and deposit long-lived gaseous elemental mercury and may perturb HOx partitioning. Concentrations of Br− in surface snow tended to increase/decrease in parallel with the specific activities of the aerosol-associated radionuclides 7Be and 210Pb. Earlier work has shown that ventilation of the boundary layer causes simultaneous increases in 7Be and 210Pb at Summit, suggesting there is a pool of Br in the free troposphere above Summit in summer time. Speciation and the source of this free tropospheric Br− are not well constrained, but we suggest it may be linked to extensive regions of active Br chemistry in the Arctic basin which are known to cause ozone and mercury depletion events shortly after polar sunrise. If this hypothesis is correct, it implies persistence of the free troposphere Br− for several months after peak Br activation in March/April. Alternatively, there may be a ubiquitous pool of Br− in the free troposphere, sustained by currently unknown sources and processes

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

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