A dedicated study of new particle formation and fate in the coastal environment (PARFORCE): overview of objectives and achievements

A dedicated study into the formation of new particles, New Particle Formation and Fate in the Coastal Environment (PARFORCE), was conducted over a period from 1998 to 1999 at the Mace Head Atmospheric Research Station on the western coast of Ireland. Continuous measurements of new particle formation were taken over the 2-year period while two intensive field campaigns were also conducted, one in September 1998 and the other in June 1999. New particle events were observed on ∼90% of days and occurred throughout the year and in all air mass types. These events lasted for, typically, a few hours, with some events lasting more than 8 hours, and occurred during daylight hours coinciding with the occurrence of low tide and exposed shorelines. During these events, peak aerosol concentrations often exceeded 106 cm−3 under clean air conditions, while measured formation rates of detectable particle sizes (i.e., d > 3 nm) were of the order of 104–105 cm−3 s−1. Nucleation rates of new particles were estimated to be, at least, of the order of 105–106 cm−3 s−1 and occurred for sulphuric acid concentrations above 2 × 106 molecules cm−3; however, no correlation existed between peak sulphuric acid concentrations, low tide occurrence, or nucleation events. Ternary nucleation theory of the H2SO4-H2O-NH3 system predicts that nucleation rates far in excess of 106 cm−3 s−1 can readily occur for the given sulphuric acid concentrations; however, aerosol growth modeling studies predict that there is insufficient sulphuric acid to grow new particles (of ∼1 nm in size) into detectable sizes of 3 nm. Hygroscopic growth factor analysis of recently formed 8-nm particles illustrate that these particles must comprise some species significantly less soluble than sulphate aerosol. The nucleation-mode hygroscopic data, combined with the lack of detectable VOC emissions from coastal biota, the strong emission of biogenic halocarbon species, and the fingerprinting of iodine in recently formed (7 nm) particles suggest that the most likely species resulting in the growth of new particles to detectable sizes is an iodine oxide as suggested by previous laboratory experiments. It remains an open question whether nucleation is driven by self nucleation of iodine species, a halocarbon derivative, or whether first, stable clusters are formed through ternary nucleation of sulphuric acid, ammonia, and water vapor, followed by condensation growth into detectable sizes by condensation of iodine species. Airborne measurements confirm that nucleation occurs all along the coastline and that the coastal biogenic aerosol plume can extend many hundreds of kilometers away from the source. During the evolution of the coastal plume, particle growth is observed up to radiatively active sizes of 100 nm. Modeling studies of the yield of cloud-condensation nuclei suggest that the cloud condensation nuclei population can increase by ∼100%. Given that the production of new particles from coastal biogenic sources occurs at least all along the western coast of Europe, and possibly many other coastlines, it is suggested that coastal aerosols contribute significantly to the natural background aerosol population.