Trends in atmospheric new-particle formation: 16 years of observations in a boreal-forest environment

Abstract

New-particle formation (NPF) is globally an important source of climatically-relevant atmospheric aerosols. Here we explore the inter-annual variability and trends in sources and sinks of atmospheric nanoparticles in a boreal forest environment. We look into the precursor vapors leading to the aerosol formation, NPF frequency, as well as the formation and growth rates of the freshly-formed particles. The analysis is based on 16 years of data acquired from the Station for Measuring Ecosystem–Atmosphere Relations (SMEAR II) in Hyytiälä, Finland. The results indicate that the probability of NPF is connected to both air mass origin, explaining a large part of the year-to-year variability in the number of NPF events, and concentrations of low-volatile vapours. The probability of NPF increases with increasing gaseous sulphuric acid concentrations, but even better association is found between the NPF probability and product of sulphuric acid and low-volatile organic vapour (proxy) concentrations. While the concentrations of both sulphuric acid (evaluated by proxy) and sulphuric-acid precursor sulphur dioxide decreased over the 16-year measurement period, the new-particle formation and growth rates slightly increased. On the other hand, the proxy concentrations of oxidized organics increased in all seasons except in winter. The contribution of sulphuric acid to the particle growth was minor, and the growth rate had a clear connection with the ambient temperature due to higher emissions of biogenic volatile organic compounds at higher temperatures. For a given sulphuric acid concentration evaluated by proxy, particle formation rates tended to be higher at higher temperatures.