Joyce M. Harris

Transport of Asian air pollution to North America

Using observations from the Cheeka Peak Observatory in northwestern Washington State during March-April, 1997, we show that Asian anthropogenic emissions significantly impact the concentrations of a large number of atmospheric species in the air arriving to North America during spring. Isentropic back-trajectories can be used to identify possible times when this impact will be felt, however trajectories alone are not sufficient to indicate the presence of Asian pollutants. Detailed chemical and meteorological data from one of these periods (March 29th, 1997) indicates that the surface emissions were lifted into the free troposphere over Asia and then transported to North America in ∼6 days.

The aerosol at Barrow, Alaska: long-term trends and source locations

Abstract Aerosol data consisting of condensation nuclei (CN) counts, black carbon (BC) mass, aerosol light scattering (SC), and aerosol optical depth (AOD) measured at Barrow, Alaska from 1977 to 1994 have been analyzed by three-way positive matrix factorization (PMF3) by pooling all of the different data into one large three-way array. The PMF3 analysis identified four factors that indicate four different combinations of aerosol sources active throughout the year in Alaska. Two of the factors (F1, F2) represent Arctic haze. The first Arctic haze have factor F1 is dominant in January–February while the second factor F2 is dominant in March–April. They appear to be material that is generally ascribed to long-range transported anthropogenic particles. A lower ratio of condensation nuclei to scattering coefficient loadings is obtained for F2 indicating larger particles. Factor F3 is related to condensation nuclei. It has an annual cycle with two maxima, March and July–August indicating some involvement of marine biogenic sources. The fourth factor F4 represents the contribution to the stratospheric aerosol from the eruptions of El Chichon and Mt. Pinatubo. No significant long-term trend for F1 was detected while F2 shows a negative trend over the period from 1982 to 1994 but not over the whole measurement period. A positive trend of F3 over the whole period has been observed. This trend may be related to increased biogenic sulfur production caused by reductions in the sea-ice cover in the Arctic and/or an air temperature increase in the vicinity of Barrow. Potential source contribution function (PSCF) analysis showed that in winter and spring during 1989 to 1993 regions in Eurasia and North America are the sources of particles measured at barrow. In contrast to this, large areas in the North Pacific Ocean and the Arctic Ocean was contributed to observed high concentrations of CN in the summer season. Three-way positive matrix factorization was an effective method to extract time-series information contained in the measured quantities. PSCF was useful for the identification possible source areas and the potential pathways for the Barrow aerosol. The effects of long-distance transport, photochemical aerosol production, emissions from biogenic activities in the ocean, volcanic eruptions on the aerosol measurements made at Barrow were extracted using this combined methodology.

Trends of ozone in the troposphere

Using a set of selected surface ozone (nine stations) and ozone vertical profile measurements (from six stations), we have documented changes in tropospheric ozone at a number of locations. From two stations at high northern hemisphere (NH) latitudes there has been a significant decline in ozone amounts throughout the troposphere since the early 1980s. At midlatitudes of the NH where data are the most abundant, on the other hand, important regional differences prevail. The two stations in the eastern United States show that changes in ozone concentrations since the early 1970s have been relatively small. At the two sites in Europe, however, ozone amounts increased rapidly into the mid-1980s, but have increased less rapidly (or in some places not at all) since then. Increases at the Japanese ozonesonde station have been largest in the lower troposphere, but have slowed in the recent decade. The tropics are sparsely sampled but do not show significant changes. Small increases are suggested at southern hemisphere (SH) midlatitudes by the two surface data records. In Antarctica large declines in the ozone concentration are noted in the South Pole data, and like those at high latitudes of the NH, seem to parallel the large decreases in the stratosphere.

Stable isotope composition of waters in southeastern California 1. Modern precipitation

Over a 7-year period from April 1982 to April 1989, integrated samples of rain and snow were collected at 32 sites by oil-sealed storage gage stations in (and adjoining) the southeast California desert; station elevations ranged from −65 m to 2280 m, and the collection network covered an area measuring about 400 km in each dimension. Deuterium (δD) analysis of 406 samples shows that the average δD of summer precipitation was −56 per mil (‰) whereas winter values averaged −78‰, averaged annual values were close to −69‰ because most of the area is in a winter-dominated precipitation regime. We found no correlation between wetness or dryness of a season and the δD of its precipitation. The δ18O versus δD plots show that rain samples define a line of slope 6.5, less than the 8 of the Meteoric Water Line, whereas snow samples define a line of slope 9.2. These differences in slope are the result of isotopic fractionation which occurred during evaporation of raindrops but not during sublimation of snow. Trajectory plots of 68 of the major storm events show that all of the winter storms originated in the Pacific, and passed over high mountains before reaching our collection stations. However, 21 of the 30 summer storms had trajectories that originated either over the Gulf of Mexico or the subtropical Pacific and traveled either west or north to reach our stations, without traversing high mountains. The difference in δD between winter and summer precipitation is due to different air flow patterns during those seasons.

Air mass trajectories to Summit, Greenland: A 44-year climatology and some episodic events

The seasonal variation in atmospheric transport patterns to Summit, Greenland, is examined using a 44-year record of daily, 10-day, isobaric back trajectories at the 500-hPa level. Over 24,000 modeled trajectories are aggregated into distinct patterns using cluster analysis. Ten-day trajectories reaching Summit are longest during winter, with 67% extending upwind (westward) as far back as Asia or Europe. Trajectories are shortest during summer, with 46% having 10-day origins over North America. During all seasons a small percentage (3–7%) of trajectories originate in west Asia/Europe and follow a meridional path over the Arctic Ocean before approaching Summit from the northwest. Trajectories at the 700-hPa level tend to be shorter than at 500 hPa, with many of the 700-hPa trajectories from North America tracking over the North Atlantic and approaching Summit from the south. The long-range transport climatology for Summit is similar to a year-round climatology prepared for Dye 3, located 900 km to the south [Davidson et al., 1993b]. An analysis of several aerosol species measured at Summit during summer 1994 reveals examples of the usefulness and also the limitations of using long-range air trajectories to interpret chemical data.

Aerosol backscatter fraction and single scattering albedo: Measured values and uncertainties at a coastal station in the Pacific Northwest

Light scattering, hemispheric backscattering, and absorption properties of submicrometer and supermicrometer aerosol particles at low relative humidity and 550 nm wavelength are investigated as a function of air mass category during a 2-month campaign at a midlatitude Pacific coastal station at Cheeka Peak, Washington. The main source of uncertainty in single scattering albedo (ω) measurements, namely, the measurement of light absorption, is addressed by the deployment of three identical absorption photometers and by relying on a recent calibration of this device using direct optical measurements. The absorption photometer measurement is corrected for response to light scattering, and measurements of sea-salt aerosol in this campaign provide a partial validation of this correction. Scattering measurements by nephelometry are also corrected for known instrumental nonidealities. Uncertainties stemming from instrumental noise, drift, calibration, and correction factors are propagated to allow comparisons among air mass categories and with other data sets and, ultimately, to constrain the values of ω and other optical properties used in climate models. Marine aerosol over the midlatitude eastern Pacific is found to be weakly absorbing for the sub-μm component and virtually nonabsorbing for the super-μm component (separated at 1 μm, low-relative humidity, aerodynamic diameter). A distinct increase in sub-μm light extinction (especially absorption) observed during 2 days of sustained marine flow appears to be Asian pollution transported across the Pacific. Low levels of gaseous NO x during this period rule out nearby combustion sources, and low levels of particulate Fe, Al, and Si rule out a significant contribution from mineral dust. Excluding this episode, both scattering and absorption properties for marine sampling conditions are similar to those observed in the clean midlatitude Southern Hemisphere (Cape Grim, Tasmania). In general, continental influence, as indicated by trends over the air mass categories, tends to raise the backscatter ratio and lower ω. Light absorption values compared to previous marine and coastal measurements confirm the range of values found by others and the highly variable nature of this quantity.

Long‐range transport of anthropogenic aerosols to the National Oceanic and Atmospheric Administration baseline station at Mauna Loa Observatory, Hawaii

Size-segregated measurements of aerosol mass and composition are used to determine the composition and seasonal variations of natural and anthropogenic aerosols at Mauna Loa Observatory (MLO) from 1993 through 1996. Although the springtime transport of Asian dust to MLO is a well-documented phenomenon, this study shows that fine anthropogenic aerosols, including sulfur, black carbon, and enriched trace metals such as As, Cu, Pb, and Zn, are also routinely transported to MLO each spring. It is estimated that at least one third of the sulfate measured at MLO during the spring is anthropogenic. In addition, indirect measurements indicate that the organic aerosol concentrations are often comparable to the sulfate concentrations. This study also combines size- and time-resolved aerosol composition measurements with isentropic, backward air-mass trajectories and gas measurements of 222Rn, CH4, CO, and CO2 to identify some potential source regions of the anthropogenic aerosols. Three types of long-range transport episodes are identified: (1) anthropogenic aerosols mixed with Asian dust, (2) Asian pollution with relatively small amounts of soil dust, and (3) biomass burning emissions from North America. This study shows that anthropogenic aerosols and gases can be efficiently transported to MLO from both Asia and North America during the spring.

Analysis of 10-day isentropic flow patterns for Barrow, Alaska : 1985-1992

Atmospheric transport patterns to Barrow, Alaska, during 1985–1992 were investigated using a newly developed isentropic air trajectory model. The new model features a layer-averaged mode that is activated whenever an air parcel traveling isentropically approaches the Earths surface. A dynamic preprocessing program ensures that trajectories always arrive at a constant, predetermined altitude. Ten-day back trajectories arriving twice daily at 500, 1500, and 3000 m above sea level revealed no long-term trends in flow patterns during the 8-year period. Frequency of transport type was fairly stable from year to year, except in the anomalously warm year of 1989 when increased numbers of trajectories from the Aleutian region were observed. During the Arctic haze season, trajectories suggest that transport of pollution from north central Russia occurs near the surface (about 20% frequency), whereas that from northern Europe occurs at higher elevations (about 10% frequency).

ozone loss in the lower stratosphere over the United States in 1992–1993: Evidence for heterogeneous chemistry on the Pinatubo aerosol

Ozone profiles obtained at Boulder, Colorado and Wallops Island, Virginia indicate that ozone was about 25% below normal during the winter and spring of 1992–93 in the 12–22 km region. This large ozone reduction in the lower stratosphere, though sometimes partially compensated by higher than normal ozone above 24 km, was responsible for the low total column ozone values observed across the United States during this period. Normal temperatures throughout the low ozone region suggest that transport-related effects are probably not the most important cause of the ozone deficits. The region of low ozone at Boulder corresponds closely with the location of the enhanced H2SO4/H2O aerosol from the Pinatubo eruption of 1991 as measured near Boulder and at Laramie, Wyoming. Trajectory analyses suggest that except at low altitudes in spring, air parcels on the days of the ozone measurements generally arrived at Boulder from higher latitude, although seldom higher than 60°N, and hence may have been subjected to heterogeneous chemical processing on the surface of Pinatubo aerosol droplets resulting in chlorine-catalyzed ozone destruction, a process which is believed to be more effective under the lower winter temperatures and sunlight levels of higher latitudes.

Ambient air levels and atmospheric long-range transport of persistent organochlorines to Signy Island, Antarctica

Levels of persistent organic pollutants (POPs), such as polychlorinated biphenyls and pesticides have been determined in ambient air at Signy Island, Antarctica, over a period of 17 weeks. Mean concentrations for single polychlorinated biphenyls (0.02–17 pg/m3), for chlordanes (0.04–0.9 pg/m3), DDT compounds (0.07–0.40 pg/m3) and γ-hexachlorocyclohexane (HCH, 22 pg/m3) were comparable to those in Arctic air. However, α-HCH levels were approximately one order of magnitude lower. Compared to the Arctic, differences were also observed in the concentration ratios of α-/γ-HCH and chlordane compounds. Two possible atmospheric long-range transport episodes from South America were found by comparing 10-day back trajectories with observed concentration changes. The lower limits of determination (LOD) were mainly governed by the field blanks. They were satisfactory for the most volatile PCBs. However, many concentrations for DDT and chlordane compounds were below the LODs (range 0.1–1 pg/m3) or even the instrumental detection limit (0.01–0.03 pg/m3).