Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σ_sp) and hemispheric backscattering (σ_bsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σ_sp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σ_sp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intra-annual variability. At mountain sites, higher σ_sp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σ_sp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σ_sp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σ_sp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σ_sp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σ_sp are consistent with those reported for PM_2.5 and PM₁₀ mass concentrations over similar periods across Europe.

The objective of this work was to assess the yearly contribution of fossil fuel combustion (BC_ff) and wood burning (BC_wb) to equivalent black carbon (eBC) concentrations, in Athens, Greece. Measurements were conducted at a suburban site from March 2013 to February 2014 and included absorption coefficients at seven wavelengths and PM_2.5 chemical composition data for key biomass burning markers, i.e., levoglucosan, potassium (K) and elemental and organic carbon (EC, OC). A well-documented methodology of corrections for aethalometer attenuation coefficients was applied with a resulting annual dataset of derived absorption coefficients for the suburban Athens’ atmospheric aerosol. The Aethalometer model was applied for the source apportionment of eBC. An optimum Ångström exponent for fossil fuel (α_ff) was found, based on the combined use of the model with levoglucosan data. The measured eBC concentrations were equal to 2.4 ± 1.0 μg m⁻³ and 1.6 ± 0.6 μg m⁻³, during the cold and the warm period respectively. The contribution from wood burning was significantly higher during the cold period (21 ± 11%, versus 6 ± 7% in the warm period). BC_ff displayed a clear diurnal pattern with a morning peak between 8 and 10 a.m. (during morning rush hour) and a second peak during the evening and night hours, due to the shallowing of the mixing layer. Regression analysis between BC_wb concentrations and biomass burning markers (levoglucosan, K and OC/EC ratio) supported the validity of the results.

The CAPS PMssa monitor is a recently commercialized instrument designed to measure aerosol single-scattering albedo (SSA) with high accuracy (Onasch et al., 2015). The underlying extinction and scattering coefficient measurements made by the instrument also allow calculation of aerosol absorption coefficients via the extinction-minus-scattering (EMS) method. Care must be taken with EMS measurements due to the occurrence of large subtractive error amplification, especially for the predominantly scattering aerosols that are typically found in the ambient atmosphere. Practically this means that although the CAPS PMssa can measure scattering and extinction coefficients with high accuracy (errors on the order of 1 %–10 %), the corresponding errors in EMS-derived absorption range from ∼10 % to greater than 100 %. Therefore, we examine the individual error sources in detail with the goal of constraining these as tightly as possible. Our main focus is on the correction of the scattered light truncation effect (i.e., accounting for the near-forward and near-backward scattered light that is undetectable by the instrument), which we show to be the main source of underlying error in atmospheric applications. We introduce a new, modular framework for performing the truncation correction calculation that enables the consideration of additional physical processes such as reflection from the instrument's glass sampling tube, which was neglected in an earlier truncation model. We validate the truncation calculations against comprehensive laboratory measurements. It is demonstrated that the process of glass tube reflection must be considered in the truncation calculation, but that uncertainty still remains regarding the effective length of the optical cavity. Another important source of uncertainty is the cross-calibration constant that quantitatively links the scattering coefficient measured by the instrument to its extinction coefficient. We present measurements of this constant over a period of ∼5 months that demonstrate that the uncertainty in this parameter is very well constrained for some instrument units (2 %–3 %) but higher for others. We then use two example field datasets to demonstrate and summarize the potential and the limitations of using the CAPS PMssa for measuring absorption. The first example uses mobile measurements on a highway road to highlight the excellent responsiveness and sensitivity of the instrument, which enables much higher time resolution measurements of relative absorption than is possible with filter-based instruments. The second example from a stationary field site (Cabauw, the Netherlands) demonstrates how truncation-related uncertainties can lead to large biases in EMS-derived absolute absorption coefficients. Nevertheless, we use a subset of fine-mode-dominated aerosols from the dataset to show that under certain conditions and despite the remaining truncation uncertainties, the CAPS PMssa can still provide consistent EMS-derived absorption measurements, even for atmospheric aerosols with high SSA. Finally, we present a detailed list of recommendations for future studies that use the CAPS PMssa to measure absorption with the EMS method. These recommendations could also be followed to obtain accurate measurements (i.e., errors less than 5 %–10 %) of SSA and scattering and extinction coefficients with the instrument.

Aerosol–cloud interactions in mixed-phase clouds (MPCs) are one of the most uncertain drivers of the hydrological cycle and climate change. A synergy of in situ, remote-sensing and modelling experiments were used to determine the source of ice-nucleating particles (INPs) for MPCs at Mount Helmos in the eastern Mediterranean. The influences of boundary layer turbulence, vertical aerosol distributions and meteorological conditions were also examined. When the observation site is in the free troposphere (FT), approximately 1 in ×10⁶ aerosol particles serve as INPs around −25 °C. The INP abundance spans 3 orders of magnitude and increases in the following order: marine aerosols; continental aerosols; and, finally, dust plumes. Biological particles are important INPs observed in continental and marine aerosols, whereas they play a secondary, although important, role during Saharan dust events. Air masses in the planetary boundary layer (PBL) show both enriched INP concentrations and a higher proportion of INPs to total aerosol particles, compared with cases in the FT. The presence of precipitation/clouds enriches INPs in the FT but decreases INPs in the PBL. Additionally, new INP parameterizations are developed that incorporate the ratio of fluorescent-to-nonfluorescent or coarse-to-fine particles and predict >90 % of the observed INPs within an uncertainty range of a factor of 10; these new parameterizations exhibit better performance than current widely used parameterizations and allow ice formation in models to respond to variations in dust and biological particles. The improved parameterizations can help MPC formation simulations in regions with various INP sources or different regions with prevailing INP sources.