The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing.

Taking advantage of only the measured aerosol particles spectral evolution as a function of time, a new analytical tool is developed to derive formation and growth properties of nucleation mode aerosols. This method, when used with hygroscopic growth-factors, can also estimate basic composition properties of these recently-formed particles. From size spectra the diameter growth-rate can be obtained, and aerosol condensation and coagulation sinks can be calculated. Using this growth-rate and condensation sink, the concentration of condensable vapours and their source rate can be estimated. Then, combining the coagulation sink together with measured number concentrations and apparent source rates of 3 nm particles, 1 nm particle nucleation rates and concentration can be estimated. To estimate nucleation rates and vapour concentration source rates producing new particle bursts over the Boreal forest regions, three cases from the BIOFOR project were examined using this analytical tool. In this environment, the nucleation mode growth-rate was observed to be 2-3 nm hour−1, which required a condensable vapour concentration of 2.5-4×107 cm−3 and a source rate of approximately 7.5-11×104 cm−3 s−1 to be sustained. The formation rate of 3 nm particles was #1 particle cm−3 s−1 in all three cases. The estimated formation rate of 1 nm particles was 10-100 particles cm−3 s−1, while their concentration was estimated to be between 10,000 and 100,000 particles cm−3. Using hygroscopicity data and mass flux expressions, the mass flux of insoluble vapour is estimated to be of the same order of magnitude as that of soluble vapour, with a soluble to insoluble vapour flux ratio ranging from 0.7 to 1.4 during these nucleation events.

A simple method for correcting for the loading effects of aethalometer data is presented. The formula BC CORRECTED ϭ (1 ϩ k ⅐ ATN) ⅐ BC NONCORRECTED , where ATN is the attenuation and BC is black carbon, was used for correcting aethalometer data obtained from measurements at three different sites: a subway station in Helsinki, an urban background measurement station in Helsinki, and a rural station in Hyytiälä in central Finland. The BC data were compared with simultaneously measured aerosol volume concentrations (V). After the correction algorithm, the BC-to-V ratio remained relatively stable between consequent filter spots, which can be regarded as indirect evidence that the correction algorithm works. The k value calculated from the outdoor sites had a clear seasonal cycle that could be explained by darker aerosol in winter than in summer. When the contribution of BC to the total aerosol volume was high, the k factor was high and vice versa. In winter, the k values at all wavelengths were very close to that obtained from the subway station data. In summer, the k value was wavelength dependent and often negative. When the k value is negative, the noncorrected BC concentrations overestimated the true concentrations.

A B S T R A C TThe hygroscopic properties play a vital role for the direct and indirect effects of aerosols on climate, as well as the health effects of particulate matter (PM) by modifying the deposition pattern of inhaled particles in the humid human respiratory tract. Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) instruments have been used in field campaigns in various environments globally over the last 25 yr to determine the water uptake on submicrometre particles at subsaturated conditions. These investigations have yielded valuable and comprehensive information regarding the particle hygroscopic properties of the atmospheric aerosol, including state of mixing. These properties determine the equilibrium particle size at ambient relative humidities and have successfully been used to calculate the activation of particles at water vapour supersaturation. This paper summarizes the existing published H-TDMA results on the sizeresolved submicrometre aerosol particle hygroscopic properties obtained from ground-based measurements at multiple marine, rural, urban and free tropospheric measurement sites. The data is classified into groups of hygroscopic growth indicating the external mixture, and providing clues to the sources and processes controlling the aerosol. An evaluation is given on how different chemical and physical properties affect the hygroscopic growth.

Taking advantage of only the measured aerosol particles spectral evolution as a function of time, a new analytical tool is developed to derive formation and growth properties of nucleation mode aerosols. This method, when used with hygroscopic growth‐factors, can also estimate basic composition properties of these recently‐formed particles. From size spectra the diameter growth‐rate can be obtained, and aerosol condensation and coagulation sinks can be calculated. Using this growth‐rate and condensation sink, the concentration of condensable vapours and their source rate can be estimated. Then, combining the coagulation sink together with measured number concentrations and apparent source rates of 3 nm particles, 1 nm particle nucleation rates and concentration can be estimated. To estimate nucleation rates and vapour concentration source rates producing new particle bursts over the Boreal forest regions, three cases from the BIOFOR project were examined using this analytical tool. In this environment, the nucleation mode growth‐rate was observed to be 2–3 nm hour−1, which required a condensable vapour concentration of 2.5–4×107 cm−3 and a source rate of approximately 7.5–11×104 cm−3 s−1 to be sustained. The formation rate of 3 nm particles was ≈1 particle cm−3 s−1 in all three cases. The estimated formation rate of 1 nm particles was 10–100 particles cm−3 s−1, while their concentration was estimated to be between 10,000 and 100,000 particles cm−3. Using hygroscopicity data and mass flux expressions, the mass flux of insoluble vapour is estimated to be of the same order of magnitude as that of soluble vapour, with a soluble to insoluble vapour flux ratio ranging from 0.7 to 1.4 during these nucleation events.

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Abstract. 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.

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