Spatial Representativeness Error in the Ground-Level Observation Networks for Black Carbon Radiation Absorption.

There is high uncertainty in the direct radiative forcing of black carbon (BC), an aerosol that strongly absorbs solar radiation. The observation-constrained estimate, which is several times larger than the bottom-up estimate, is influenced by the spatial representativeness error due to the mesoscale inhomogeneity of the aerosol fields and the relatively low resolution of global chemistry-transport models. Here we evaluated the spatial representativeness error for two widely used observational networks (AErosol RObotic NETwork and Global Atmosphere Watch) by downscaling the geospatial grid in a global model of BC aerosol absorption optical depth to 0.1° × 0.1°. Comparing the models at a spatial resolution of 2° × 2° with BC aerosol absorption at AErosol RObotic NETwork sites (which are commonly located near emission hot spots) tends to cause a global spatial representativeness error of 30%, as a positive bias for the current top-down estimate of global BC direct radiative forcing. By contrast, the global spatial representativeness error will be 7% for the Global Atmosphere Watch network, because the sites are located in such a way that there are almost an equal number of sites with positive or negative representativeness error.

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.

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.

A global view on the effect of water uptake on aerosol particle light scattering.

A reference dataset of multi-wavelength particle light scattering and hemispheric backscattering coefficients for different relative humidities (RH) between RH = 30 and 95% and wavelengths between λ = 450 nm and 700 nm is described in this work. Tandem-humidified nephelometer measurements from 26 ground-based sites around the globe, covering multiple aerosol types, have been re-analysed and harmonized into a single dataset. The dataset includes multi-annual measurements from long-term monitoring sites as well as short-term field campaign data. The result is a unique collection of RH-dependent aerosol light scattering properties, presented as a function of size cut. This dataset is important for climate and atmospheric model-measurement inter-comparisons, as a means to improve model performance, and may be useful for satellite and remote sensing evaluation using surface-based, in-situ measurements.

Aerosol Absorption: Progress Towards Global and Regional Constraints.

PURPOSE OF REVIEW: Some aerosols absorb solar radiation, altering cloud properties, atmospheric stability and circulation dynamics, and the water cycle. Here we review recent progress towards global and regional constraints on aerosol absorption from observations and modeling, considering physical properties and combined approaches crucial for understanding the total (natural and anthropogenic) influences of aerosols on the climate. RECENT FINDINGS: We emphasize developments in black carbon absorption alteration due to coating and ageing, brown carbon characterization, dust composition, absorbing aerosol above cloud, source modeling and size distributions, and validation of high-resolution modeling against a range of observations. SUMMARY: Both observations and modeling of total aerosol absorption, absorbing aerosol optical depths and single scattering albedo, as well as the vertical distribution of atmospheric absorption, still suffer from uncertainties and unknowns significant for climate applications. We offer a roadmap of developments needed to bring the field substantially forward.