Aerosol dynamics in the Copenhagen urban plume during regional transport

Abstract

Abstract. Aerosol particles in the submicrometer size range (PM1) have serious impacts on human health and climate. This work aims at studying the processes relevant for physical particle properties in and downwind Copenhagen and evaluating the capability of a detailed aerosol dynamics and chemistry model (ADCHEM) to describe the submicrometer aerosol dynamics in a complex urbanized region, subjected to a variety of important anthropogenic sources. The study area is the Oresund Region with Copenhagen (about 1.8 million people) as the major city, including the strait separating Denmark and Sweden with intense ship traffic. Modeled aerosol particle number size distributions and NOx concentrations are evaluated against ground-based measurements from two stations in the Copenhagen area in Denmark and one station in southern Sweden. The measured and modeled increments in NOx concentrations from rural background to the urban area showed satisfactory agreement, indicating that the estimated NOx emissions and modeled atmospheric dispersion are reasonable. For three out of five case studies, the modeled particle number concentrations and size distributions are in satisfactory agreement with the measurements at all stations along the trajectories. For the remaining cases the model significantly underestimates the particle number concentration over Copenhagen, but reaches acceptable agreement with the measurements at the downwind background station in Sweden. The major causes for this were identified as being the lack of spatial resolution in the meteorological data in describing boundary layer mixing heights and the uncertainty in the exact air mass trajectory path over Copenhagen. In addition, particle emission factors may also have been too low. It was shown that aerosol dynamics play a minor role from upwind to urban background, but are important 1–2 h downwind the city. Real-world size-resolved traffic number emission factors which take into account the initial ageing in the street canyon can be used to model traffic emissions in urban plume studies.