The ACE‐2 HILLCLOUD experiment was carried out on the island of Tenerife in June–July 1997 to investigate the interaction of the boundary layer aerosol with a hill cap cloud forming over a ridge to ...the north‐east of the island. The cloud was used as a natural flow through reactor to investigate the dependence of the cloud microphysics and chemistry on the characteristics of the aerosols and trace gases entering cloud, and to simultaneously study the influence of the physical and chemical processes occurring within the cloud on the size distribution, chemical and hygroscopic properties of the aerosol exiting cloud. 5 major ground base sites were used, measuring trace gases and aerosols upwind and downwind of the cloud, and cloud microphysics and chemistry and interstitial aerosol and gases within the cloud on the hill. 8 intensive measurement periods or runs were undertaken during cloud events, (nocturnally for seven of the eight runs) and were carried out in a wide range of airmass conditions from clean maritime to polluted continental. Polluted air was characterised by higher than average concentrations of ozone (>50 ppbv), fine and accumulation mode aerosols (>3000 and >1500 cm−3, respectively) and higher aerosol mass loadings. Cloud droplet number concentrations N, increased from 50 cm−3 in background maritime air to >2500 cm−3 in aged polluted continental air, a concentration much higher than had previously been detected. Surprisingly, N was seen to vary almost linearly with aerosol number across this range. The droplet aerosol analyser (DAA) measured higher droplet numbers than the corrected forward scattering spectrometer probe (FSSP) in the most polluted air, but at other times there was good agreement (FSSP=0.95 DAA with an r2=0.89 for N<1200 cm−3). Background ammonia gas concentrations were around 0.3 ppbv even in air originating over the ocean, another unexpected but important result for the region. NO2 was present in background concentrations of typically 15 pptv to 100 pptv and NO˙3 (the nitrate radical) was observed at night throughout. Calculations suggest NO˙3 losses were mainly by reaction with DMS to produce nitric acid. Low concentrations of SO2(∼30 pptv), HNO3 and HCl were always present. HNO3 concentrations were higher in polluted episodes and calculations implied that these exceeded those which could be accounted for by NO2 oxidation. It is presumed that nitric and hydrochloric acids were present as a result of outgassing from aerosol, the HNO3 from nitrate rich aerosol transported into the region from upwind of Tenerife, and HCl from sea salt aerosol newly formed at the sea surface. The oxidants hydrogen peroxide and ozone were abundant (i.e., were well in excess over SO2 throughout the experiment). Occasions of significant aerosol growth following cloud processing were observed, particularly in cleaner cases. Observations and modelling suggested this was due mainly to the take up of nitric acid, hydrochloric acid and ammonia by the smallest activated aerosol particles. On a few occasions a small contribution was made by the in‐cloud oxidation of S(IV). The implications of these results from HILLCLOUD for the climatologically more important stratocumulus Marine Boundary Layer (MBL) clouds are considered.
Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 ...and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm−3 and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm−3. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm−3, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm−3, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.
An ultrafine tandem differential mobility analyzer has been developed for measurements of the hygroscopicity of ultrafine aerosol particles, between 8 and 50 nm in mobility diameter. In this paper, ...the main operation features of the device are presented along with a detailed evaluation for the limits of its operation. The instrument is suitable for both laboratory‐generated and atmospheric aerosol measurements. Hygroscopic growth data are presented for ammonium sulphate particles in the ultrafine size range, and comparisons are made with both experimental literature data and with theory. The data include determination of hygroscopic growth curves, deliquescence behavior, and hysteresis. These data will find applications in studies of the formation and growth of atmospheric aerosols.
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 × 106 molecules cm−3 and under polluted conditions as high as 1.2 × 108 molecules cm−3.
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