Seasonal distributions of fine aerosol sulfate in the North American Arctic basin during TOPSE

We used the mist chamber/ion chromatography technique to quantify fine aerosol SO4=(\u3c2.7 μm) in the Arctic during the Tropospheric Ozone Production about the Spring Equinox Experiment (TOPSE) with about 2.5 min time resolution. Our effective sample area ranged from 50° to 86°N and 53° to 100°W. The seasonal evolution of fine aerosol sulfate in the Arctic troposphere during TOPSE was consistent with the phenomenon of Arctic haze. Arctic haze has been attributed to pollution from sources in the Arctic and pollution transported meridionally along stable isentropes into the Arctic in geographically broad but vertically narrow bands. These layers became more prevalent at higher altitudes as the season progressed toward summer, and the relevant isentropes are not held so close to the surface. Mean fine particle SO4= mixing ratios during TOPSE in February below 1000 m were elevated (112 pptv) and highly variable (between 28 and 290 pptv) but were significantly lower at higher altitudes (about 40 pptv). As the season progressed, elevated mixing ratios and higher variability were observed at higher altitudes, up to 7 km. In May, mixing ratios at the lowest altitudes declined but still remained higher than in February at all altitudes. The high variability in our measurements likely reflects the vertical heterogeneity of the wintertime Arctic atmosphere as the airborne sampling platform passed in and out of these layers. It is presumed that mixing ratios and variability will continue to decline at all altitudes into the summer as wet deposition processes become important in removing aerosol SO4= from the troposphere

Aerosol chemical composition in Asian continental outflow during the TRACE-P campaign: Comparison with PEM-West B

Aerosol associated soluble ions and the radionuclide tracers 7Be and 210Pb were quantified in 414 filter samples collected in spring 2001 from the DC-8 during the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign. Binning the data into near Asia (flights from Hong Kong and Japan) and remote Pacific (all other flights) revealed large enhancements of NO3−, SO4=, C2O4=, NH4+, K+, Mg2+, and Ca2+ near Asia. The boundary layer and lower troposphere were most strongly influenced by continental outflow, and the largest enhancements were seen in Ca2+ (a dust tracer) and NO3− (reflecting uptake of HNO3 onto the dust). Comparing the TRACE P near Asia bin with earlier results from the same region during PEM-West B (in 1994) shows at least twofold enhancements during TRACE P in most of the ions listed above. Calcium and NO3− were most enhanced in this comparison as well (more than sevenfold higher in the boundary layer and threefold higher in the lower troposphere). Independent estimation of Asian emissions of gaseous precursors of the aerosol-associated ions suggest only small changes between the two missions, and precipitation fields do not suggest any significant difference in the efficiency of the primary sink, precipitation scavenging. It thus appears that with the possible exception of dust, the enhancements of aerosol-associated species during TRACE P cannot be explained by stronger sources or weaker sinks. We argue that the enhancements largely reflect the fact that TRACE P focused on characterizing Asian outflow, and thus the DC-8 was more frequently flown into regions that were influenced by well-organized flow off the continent

Stratospheric influence on the northern North American free troposphere during TOPSE: 7Be as a stratospheric tracer

We use 7Be, with HNO3 and O3, to identify air masses sampled from the NCAR C-130 during TOPSE that retained clear evidence of stratospheric influence. A total of 43 such air masses, spread fairly evenly across the February to May sampling period, and 40°N–86°N latitude range, were encountered. South of 55°N, nearly all clear stratospheric influence was restricted to altitudes above 6 km. At higher latitudes stratospherically influenced air masses were encountered as low as 2 km. Approximately 12% of all TOPSE sampling time at altitudes above 2 km was spent in stratospherically impacted air, above 6 km this increased to more than half of the time. Because it is not certain how much of this stratospherically influenced air irreversibly injected mass (and chemical compounds) into the troposphere, we estimate the stratospheric fraction of O3 in high latitude TOPSE samples based on a linear relationship to7Be and compare it to in situ O3. This analysis indicates that the stratospheric source can account for a dominant fraction (\u3e85%) of in situ O3 throughout TOPSE, but that the stratospheric contribution was nearly constant through the 4 month campaign. In February and March the 7Be based estimates of stratospheric O3 account for 10–15% more O3 than was measured, but by April and May there is up to about 10% more O3 than expected from the stratospheric source. This trend suggests that a seasonal transition from O3 depletion to photochemical production in the high latitude North American troposphere is the major cause of the springtime increase in O3

Chemical and physical properties of bulk aerosols within four sectors observed during TRACE-P

Chemical and physical aerosol data collected on the DC-8 during TRACE-P were grouped into four sectors based on back trajectories. The four sectors represent long-range transport from the west (WSW), regional circulation over the western Pacific and Southeast Asia (SE Asia), polluted transport from northern Asia with substantial sea salt at low altitudes (NNW) and a substantial amount of dust (Channel). WSW has generally low mixing ratios at both middle and high altitudes, with the bulk of the aerosol mass due to non-sea-salt water-soluble inorganic species. Low altitude SE Asia also has low mean mixing ratios in general, with the majority of the aerosol mass comprised of non-sea-salts, however, soot is also relatively important in this region. NNW had the highest mean sea salt mixing ratios, with the aerosol mass at low altitudes (\u3c2 km) evenly divided between sea salts, non-sea-salts, and dust. The highest mean mixing ratios of water-soluble ions and soot were observed at the lowest altitudes (\u3c2 km) in the Channel sector. The bulk of the aerosol mass exported from Asia emanates from Channel at both low and midaltitudes, due to the prevalence of dust compared to other sectors. Number densities show enhanced fine particles for Channel and NNW, while their volume distributions are enhanced due to sea salt and dust. Low-altitude Channel exhibits the highest condensation nuclei (CN) number densities along with enhanced scattering coefficients, compared to the other sectors. At midaltitudes (2–7 km), low mean CN number densities coupled with a high proportion of nonvolatile particles (≥65%) observed in polluted sectors (Channel and NNW) are attributed to wet scavenging which removes hygroscopic CN particles. Low single scatter albedo in SE Asia reflects enhanced soot

Investigations into free tropospheric new particle formation in the central Canadian arctic during the winter/spring transition as part of TOPSE

In this paper, we investigate the role of in situ new particle production in the central Canadian sub-Arctic and Arctic as part of the TOPSE experiment. Airborne measurements conducted primarily in the free troposphere were made from 50° to 90°W longitude and 60° to 85°N latitude during the period from February to May 2000. Data pertinent to this paper include 3–4 nm diameter (Dp) particles, ultrafine condensation nuclei (Dp \u3e 3 nm), fine particles (0.2 \u3c Dp \u3c 3 μm), and the possible nucleation precursor, sulfuric acid, and its precursor, sulfur dioxide. For data averaged over this period, most species showed little evidence for a latitudinal trend. Fine aerosol number concentrations, however, showed a slight increase with latitude. The evolution of various species concentrations over the period of the study show that fine particles also had a consistent temporal trend, increasing at all altitudes from February to May, whereas sulfur dioxide at the surface tended to peak in late March. Ultrafine condensation nuclei and 3–4 nm particles showed no temporal trends. Little evidence for in situ new particle production was observed during the study, except for one atypical event where SO2concentrations were 3.5 ppbv, 2 orders of magnitude higher than typical levels. This paper cannot address the question of whether the observed condensation nuclei were produced in situ by a low particle production rate or transported from lower latitudes

Reactive nitrogen in Asian continental outflow over the western Pacific: Results from the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) airborne mission

We present here results for reactive nitrogen species measured aboard the NASA DC-8 aircraft during the Transport and Chemical Evolution over the Pacific (TRACE-P) mission. The large-scale distributions total reactive nitrogen (NOy,sum = NO + NO2 + HNO3 + PAN + C1–C5alkyl nitrates) and O3 and CO were better defined in the boundary layer with significant degradation of the relationships as altitude increased. Typically, NOy,sum was enhanced over background levels of ∼260 pptv by 20-to-30-fold. The ratio C2H2/CO had values of 1–4 at altitudes up to 10 km and as far eastward as 150°E, implying significant vertical mixing of air parcels followed by rapid advection across the Pacific. Analysis air parcels originating from five principal Asian source regions showed that HNO3 and PAN dominated NOy,sum. Correlations of NOy,sum with C2Cl4 (urban tracer) were not well defined in any of the source regions, and they were only slightly better with CH3Cl (biomass tracer). Air parcels over the western Pacific contained a complex mixture of emission sources that are not easily resolvable as shown by analysis of the Shanghai mega-city plume. It contained an intricate mixture of pollution emissions and exhibited the highest mixing ratios of NOy,sum species observed during TRACE-P. Comparison of tropospheric chemistry between the earlier PEM-West B mission and the recent TRACE-P data showed that in the boundary layer significant increases in the mixing ratios of NOy,sum species have occurred, but the middle and upper troposphere seems to have been affected minimally by increasing emissions on the Asian continent over the last 7 years

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

Steady state free radical budgets and ozone photochemistry during TOPSE

A steady state model, constrained by a number of measured quantities, was used to derive peroxy radical levels for the conditions of the Tropospheric Ozone Production about the Spring Equinox (TOPSE) campaign. The analysis is made using data collected aboard the NCAR/NSF C-130 aircraft from February through May 2000 at latitudes from 40° to 85°N, and at altitudes from the surface to 7.6 km. HO2 + RO2 radical concentrations were measured during the experiment, which are compared with model results over the domain of the study showing good agreement on the average. Average measurement/model ratios are 1.04 (σ = 0.73) and 0.96 (σ = 0.52) for the MLB and HLB, respectively. Budgets of total peroxy radical levels as well as of individual free radical members were constructed, which reveal interesting differences compared to studies at lower latitudes. The midlatitude part of the study region is a significant net source of ozone, while the high latitudes constitute a small net sink leading to the hypothesis that transport from the middle latitudes can explain the observed increase in ozone in the high latitudes. Radical reservoir species concentrations are modeled and compared with the observations. For most conditions, the model does a good job of reproducing the formaldehyde observations, but the peroxide observations are significantly less than steady state for this study. Photostationary state (PSS) derived total peroxy radical levels and NO/NO2ratios are compared with the measurements and the model; PSS-derived results are higher than observations or the steady state model at low NO concentrations

Managing on-farm biosecurity risk through pre-emptive breeding: the case of rust on field pea and lentil

Trabajo presentado en la Australasian Plant Pathology Conference, celebrada en Fremantle (Australia) del 14 al 16 de septiembre de 2015.N