Christoph Kleefeld

Transport of boreal forest fire emissions from Canada to Europe

In August 1998, severe forest fires occurred in many parts of Canada, especially in the Northwest Territories. In the week from August 5 to 11, more than 1000 different fires burned >1 × 106 ha of boreal forest, the highest 1-week sum ever reported throughout the 1990s. In this study we can unambigously show for the first time that these fires caused pronounced large-scale haze layers above Europe and that they influenced concentrations of carbon monoxide and other trace gases at the surface station Mace Head in Ireland over a period of weeks. Transport took place across several thousands of kilometers. An example of such an event, in which a pronounced aerosol layer was observed at an altitude of 3–6 km over Germany during August 1998, is investigated in detail. Backward trajectories ending at the measured aerosol layer are calculated and shown to have their origin in the forest fire region. Simulations with a particle dispersion model reveal how a substantial amount of forest fire emissions was transported across the Atlantic. The resulting aerosol lamina over Europe is captured well by the model. In addition, the model demonstrates that the forest fire emissions polluted large regions over Europe during the second half of August 1998. Surface measurements at Mace Head are compared to the model results for an anthropogenic and a forest fire carbon monoxide tracer, respectively. While wet deposition removed considerable amounts of aerosol during its transport, forest fire carbon monoxide reached Europe in copious amounts. It is estimated that during August 1998, 32%, 10%, and 58% of the carbon monoxide enhancement over the background level at Mace Head were caused by European and North American anthropogenic emissions and forest fire emissions, respectively.

Coastal new particle formation: Environmental conditions and aerosol physicochemical characteristics during nucleation bursts

Nucleation mode aerosol was characterized during coastal nucleation events at Mace Head during intensive New Particle Formation and Fate in the Coastal Environment (PARFORCE) field campaigns in September 1998 and June 1999. Nucleation events were observed almost on a daily basis during the occurrence of low tide and solar irradiation. In September 1998, average nucleation mode particle concentrations were 8600 cm-3 during clean air events and 2200 cm-3 during polluted events. By comparison, during June 1999, mean nucleation mode concentrations were 27,000 cm-3 during clean events and 3350 cm-3 during polluted conditions. Peak concentrations often reached 500,000-1,000,000 cm-3 during the most intense events and the duration of the events ranged from 2 to 8 hours with a mean of 4.5 hours. Source rates for detectable particle sizes (d > 3 nm) were estimated to be between 104 and 106 cm-3 s-1 and initial growth rates of new particles were as high as 0.1-0.35 nm s-1 at the tidal source region. Recently formed 8 nm particles were subjected to hygroscopic growth and were found to have a growth factor of 1.0-1.1 for humidification at 90% relative humidity. The low growth factors implicate a condensable gas with very low solubility leading to detectable particle formation. It is not clear if this condensable gas also leads to homogeneous nucleation; however, measured sulphuric acid and ammonia concentration suggest that ternary nucleation of thermodynamically stable sulphate clusters is still likely to occur. In clear air, significant particle production (>105 cm-3) was observed with sulphuric acid gas-phase concentration as low as 2 × 10 6 molecules cm-3 and under polluted conditions as high as 1.2 × 108 molecules cm-3. Copyright 2002 by the American Geophysical Union.

Relative contribution of submicron and supermicron particles to aerosol light scattering in the marine boundary layer

Measurements of the aerosol light scattering coefficient (σsp) at a wavelength of λ - 550 nm were conducted at a coastal atmospheric research station in the east Atlantic Ocean during June 1999. Size distribution measurements between diameters of 3 nm and 40 um (at ambient humidity) were used to derive scattering coefficients from Mie theory. The calculated scattering coefficients were about a factor of 7.4 higher than the measured scattering coefficients. The discrepancy was explained by a reduced cutoff of the sampling system at particle diameters between 6 and 8 μm, dependent on wind speed. The calculated aerosol scattering was about 1 order of magnitude higher than previously reported measurements in the MBL and is attributed to supermicrometer particles at sizes d > 10 μm dominating aerosol scattering. Copyright 2002 by the American Geophysical Union.

Relationships between condensation nuclei number concentration, tides, and standard meteorological variables at Mace Head, Ireland

The set of hourly averaged condensation nuclei (CN) data collected at Mace Head during 1991–1994 was examined for relationships that might exist between CN number concentrations and the more commonly measured meteorological variables, including tides. CN number concentrations at Mace Head can be characterized by typically low “background” levels (less than about 700 particles cm−3) when the wind is from the west, somewhat higher “background” levels (1000–4000 particles cm−3) when the wind is from the east, with sporadic bursts of short-lived discrete “events” of more than 10,000 cm −3 for several hours. These events occur typically during early afternoon and are normally associated with slack winds and anomalously warm, dry air. They appear to be independent of pressure, wind direction and precipitation. They can occur any time during the year, although the strongest events tend to occur during spring and autumn. Large-amplitude low tides also occur predominantly in the early afternoon during this observing period. We present evidence that large CN concentration events occur preferentially after exceptionally low tides during daylight. A neural network was employed to train the standard meteorological variables to predict CN concentrations. Baseline forecasts of CN counts for the final 180 days of the observing period were made using lagged values of all other variables. Further forecasts were made with some variables removed from the predictor set. The best correlation between the predicted values and the verifying data over the 180 days was 0.67, which was obtained from a 1-hour forecast using knowledge of all variables except temperature. Other variables whose removal improved the forecast (or whose presence degraded it) were pressure and wind speed. The best predictors of CN values were wind direction, relative humidity, and time of day. An elementary “nearest neighbor,” or “historical analogue” approach to predicting the same set of CN values generated lower correlations with the verifying data but generated a much more accurate probability distribution function.

Aerosol concentrations and scattering coefficient at Mace Head, Ireland

In June 1999 an intensive measurement campaign, Particle Formation and Fate in the Coastal Environment (PARFORCE), was conducted at the coastal Global Atmospheric Watch (GAW) research station at Mace Head, Ireland. Reported are the results of the aerosol scattering measurements. Aerosol scattering is dominated by the local sea-salt source and this is supported by closure study results.