Quantification of an atmospheric nucleation and growth process as a single source of aerosol particles in a city

Abstract

Effects of a new aerosol particle formation (NPF) and particle diameter growth process as a single source of atmospheric particle number concentrations were evaluated and quantified on the basis of experimental data sets obtained from particle number size distribution measurements in the city centre and near-city background of Budapest for 5 years. Nucleation strength factors for a nucleation day (NSFNUC) and for a general day (NSFGEN) were derived separately for seasons and full years. The former characteristic represents the concentration increment of ultrafine (UF) particles specifically on nucleation days with respect to accumulation-mode (regional background) concentrations (particles with equivalent diameters of 100–1000 nm; N100−1000) due solely to the nucleation process. The latter factor expresses the contribution of nucleation to particle numbers on general days; thus, it represents a longer time interval such as season or year. The nucleation source had the largest effect on the concentrations around noon and early afternoon, as expected. During this time interval, it became the major source of particles in the near-city background. Nucleation increased the daily mean concentrations on nucleation days by mean factors of 2.3 and 1.58 in the near-city background and city centre, respectively. Its effect was largest in winter, which was explained by the substantially lower N100−1000 levels on nucleation days than those on non-nucleation days. On an annual timescale, 37 % of the UF particles were generated by nucleation in the near-city background, while NPF produced 13 % of UF particles in the city centre. The differences among the annual mean values, and among the corresponding seasonal mean values, were likely caused by the variability in controlling factors from year to year. The values obtained represent the lower limits of the contributions. The shares determined imply that NPF is a non-negligible or substantial source of particles in near-city background environments and even in city centres, where the vehicular road emissions usually prevail. Atmospheric residence time of nucleation-mode particles was assessed by a decay curve analysis, and a mean of 02:30 was obtained. The present study suggests that the health-related consequences of the atmospheric NPF and growth process in cities should also be considered in addition to its urban climate implications.