Differential mobility particle sizer (DMPS) aerosol concentrations (N_13-800) were collected over a one-year-period (2004) at an urban background site in Barcelona, North-Eastern Spain. Quantitative contributions to particle number concentrations of the nucleation (33–39%), Aitken (39–49%) and accumulation mode (18–22%) were estimated. We examined the source and time variability of atmospheric aerosol particles by using both K-means clustering and Positive Matrix Factorization (PMF) analysis. Performing clustering analysis on hourly size distributions, nine K-means DMPS clusters were identified and, by directional association, diurnal variation and relationship to meteorological and pollution variables, four typical aerosol size distribution scenarios were identified: traffic (69% of the time), dilution (15% of the time), summer background conditions (4% of the time) and regional pollution (12% of the time). According to the results of PMF, vehicle exhausts are estimated to contribute at least to 62–66% of the total particle number concentration, with a slightly higher proportion distributed towards the nucleation mode (34%) relative to the Aitken mode (28–32%). Photochemically induced nucleation particles make only a small contribution to the total particle number concentration (2–3% of the total), although only particles larger than 13 nm were considered in this study. Overall the combination of the two statistical methods is successful at separating components and quantifying relative contributions to the particle number population.