Impact of urban aerosols on the cloud condensation activity using a clustering model.

The indirect effect of aerosols on climate through aerosol-cloud-interactions is still highly uncertain and limits our ability to assess anthropogenic climate change. The foundation of this uncertainty is in the number of cloud condensation nuclei (CCN), which itself mainly stems from uncertainty in aerosol sources and how particles evolve to become effective CCN. We analyze particle number size distribution (PNSD) and CCN measurements from an urban site in a two-step method: (1) we use an unsupervised clustering model to classify the main aerosol categories and processes occurring in the urban atmosphere and (2) we explore the influence of the identified aerosol populations on the CCN properties. According to the physical properties of each cluster, its diurnal timing, and additional air quality parameters, the clusters are grouped into five main aerosol categories: nucleation, growth, traffic, aged traffic, and urban background. The results show that, despite aged traffic and urban background categories are those with lower total particle number concentrations (Ntot) these categories are the most efficient sources in terms of contribution to the overall CCN budget with activation fractions (AF) around 0.5 at 0.75 % supersaturation (SS). By contrast, road traffic is an important aerosol source with the highest frequency of occurrence (32 %) and relatively high Ntot, however, its impact in the CCN activity is very limited likely due to lower particle mean diameter and hydrophobic chemical composition. Similarly, nucleation and growth categories, associated to new particle formation (NPF) events, present large Ntot with large frequency of occurrence (22 % and 28 %, respectively) but the CCN concentration for these categories is about half of the CCN concentration observed for the aged traffic category, which is associated with their small size. Overall, our results show that direct influence of traffic emissions on the CCN budget is limited, however, when these particles undergo ageing processes, they have a significant influence on the CCN concentrations and may be an important CCN source. Thus, aged traffic particles could be transported to other environments where clouds form, triggering a plausible indirect effect of traffic emissions on aerosol-cloud interactions and consequently contributing to climate change.

Diurnal source apportionment of organic and inorganic atmospheric particulate matter at a high-altitude mountain site under summer conditions (Sierra Nevada; Spain).

High-altitude mountain areas are sentinel ecosystems for global environmental changes such as anthropogenic pollution. In this study, we report a source apportionment of particulate material with an aerodynamic diameter smaller than 10 µm (PM10) in a high-altitude site in southern Europe (Sierra Nevada Station; SNS (2500 m a.s.l.)) during summer 2021. The emission sources and atmospheric secondary processes that determine the composition of aerosol particles in Sierra Nevada National Park (Spain) are identified from the concentrations of organic carbon (OC), elemental carbon (EC), 12 major inorganic compounds, 18 trace elements and 44 organic molecular tracer compounds in PM10 filter samples collected during day- and nighttime. The multivariate analysis of the joint dataset resolved five main PM10 sources: 1) Saharan dust, 2) advection from the urbanized valley, 3) local combustion, 4) smoke from a fire-event, and 5) aerosol from regional recirculation with high contribution of particles from secondary inorganic and organic aerosol formation processes. PM sources were clearly associated with synoptic meteorological conditions, and day- and nighttime circulation patterns typical of mountainous areas. Although a local pollution source was identified, the contribution of this source to PM10, OC and EC was small. Our results evidence the strong influence of middle- and long-range transport of aerosols, mainly from anthropogenic origin, on the aerosol chemical composition at this remote site.

Activation properties of aerosol particles as cloud condensation nuclei at urban and high-altitude remote sites in southern Europe.

Understanding the activation properties of aerosol particles as cloud condensation nuclei (CCN) is important for the climate and hydrological cycle, but their properties are not fully understood. In this study, the CCN activation properties of aerosols are investigated at two different sites in southern Spain: an urban background station in Granada and a high altitude mountain station in the Sierra Nevada National Park, with a horizontal separation of 21 km and vertical separation of 1820 m. CCN activity at the urban environment is driven by primary sources, mainly road traffic. Maximum CCN concentrations occurred during traffic rush hours, although this is also when the activation fraction is lowest. This is due to the characteristics of the rush hour aerosol consisting of ultrafine and less hygroscopic particles. In contrast, the mountain site exhibited larger and more hygroscopic particles, with CCN activity driven by the joint effect of new particle formation (NPF) and vertical transport of anthropogenic particles from Granada urban area by orographic buoyant upward flow. This led to the maximum concentrations of CCN and aerosol particles occurring at midday at the mountain site. Clear differences in the diurnal evolution of CCN between NPF events and non-event days were observed at the Sierra Nevada station, demonstrating the large contribution of NPF to CCN concentrations, especially at high supersaturations. The isolated contribution of NPF to CCN concentration has been estimated to be 175% higher at SS = 0.5% relative to what it would be without NPF. We conclude that NPF could be the major source of CCN at this mountain site. Finally, two empirical models were used to parameterize CCN concentration in terms of aerosol optical or physical parameters. The models can explain measurements satisfactorily at the urban station. At the mountain site both models cannot reproduce satisfactorily the observations at low SS.