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Detailed knowledge on the formation of new aerosol particles in the atmosphere from precursor gases, and their subsequent growth, commonly known as new particle formation (NPF) events, is one of the largest challenges in atmospheric aerosol science. High pre-existing particle loadings are expected to suppress the formation of new atmospheric aerosol particles due to high coagulation and condensation (CS) sinks. However, NPF events are regularly observed in conditions with high concentrations of pre-existing particles and even during intense desert dust intrusions that imply discrepancies between the observations and theory. In this study, we present a multi-site analysis of the occurrence of NPF events under the presence of desert dust particles in dust-influenced areas. Characterization of NPF events at five different locations highly influenced by desert dust outbreaks was done under dusty and non-dusty conditions using continuous measurements of aerosol size distribution in both fine and coarse size fractions. Contrary to common thought, our results show that the occurrence of NPF events is highly frequent during desert dust outbreaks, showing that NPF event frequencies during dusty conditions are similar to those observed during non-dusty conditions. Furthermore, our results show that NPF events also occur during intense desert dust outbreaks at all the studied sites, even at remote sites where the amounts of precursor vapours are expected to be low. Our results show that the condensation sink associated with coarse particles (CSC) represents up to the 60 % of the total CS during dusty conditions, which highlights the importance of considering coarse-fraction particles for NPF studies in desert-dust-influenced areas. However, we did not find a clear pattern of the effect of desert dust outbreaks on the strength of NPF events, with differences from site to site. The particle growth rate (GR) did not present a clear dependence on the CS during dusty and non-dusty conditions. This result, together with the fact that desert dust has different effects on the growth and formation rates at each site, suggests different formation and growth mechanisms at each site between dusty and non-dusty conditions, probably due to differences in precursor vapours' origins and concentrations as well as changes in the oxidative capacity of pre-existing particles and their effectiveness acting as CS. Further investigation based on multiplatform measurement campaigns and chamber experiments with state-of-the-art gaseous and particulate physical and chemical properties measurements is needed to better understand the role of catalyst components present in desert dust particles in NPF. Finally, our results reveal a significant impact of NPF events on the cloud condensation nuclei (CCN) budget during desert dust outbreaks at the studied sites. Therefore, since desert dust contributes to a major fraction of the global aerosol mass load, and since there is a foreseeable increase in the frequency, duration and intensity of desert dust episodes due to climate change, it is imperative to improve our understanding of the effect of desert dust outbreaks on NPF and the CCN budget for better climate change prediction.

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50 % and 60 % were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75 %) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (∼ 102 cm−3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day–night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (∼ 103–104 cm−3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (∼ 102–103 cm−3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50 nm or >100 nm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of ∼ 10 to 1000 cm−3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol–cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.

The Sierra Nevada Lidar aerOsol Profiling Experiment I and II (SLOPE I and II) campaigns were intended to determine the vertical structure of aerosols by remote sensing instruments and test the various retrieval schemes for obtaining aerosol microphysical and optical properties with in situ measurements. The SLOPE I and II campaigns were developed during the summers of 2016 and 2017, respectively, combining active and passive remote sensing with in situ measurements at stations belonging to the AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere) in the Granada area (Spain). In this work, we use the in situ measurements of these campaigns to evaluate aerosol properties retrieved by the GRASP code (Generalized Retrieval of Atmosphere and Surface Properties) combining lidar and sun–sky photometer measurements. We show an overview of aerosol properties retrieved by GRASP during the SLOPE I and II campaigns. In addition, we evaluate the GRASP retrievals of total aerosol volume concentration (discerning between fine and coarse modes), extinction and scattering coefficients, and for the first time we present an evaluation of the absorption coefficient. The statistical analysis of aerosol optical and microphysical properties, both column-integrated and vertically resolved, from May to July 2016 and 2017 shows a large variability in aerosol load and types. The results show a strong predominance of desert dust particles due to North African intrusions. The vertically resolved analysis denotes a decay of the atmospheric aerosols with an altitude up to 5 km a.s.l. Finally, desert dust and biomass burning events were chosen to show the high potential of GRASP to retrieve vertical profiles of aerosol properties (e.g. absorption coefficient and single scattering albedo) for different aerosol types. The aerosol properties retrieved by GRASP show good agreement with simultaneous in situ measurements (nephelometer, aethalometer, scanning mobility particle sizer, and aerodynamic particle sizer) performed at the Sierra Nevada Station (SNS) in Granada. In general, GRASP overestimates the in situ data at the SNS with a mean difference lower than 6 µm3 cm−3 for volume concentration, and 11 and 2 Mm−1 for the scattering and absorption coefficients. On the other hand, the comparison of GRASP with airborne measurements also shows an overestimation with mean absolute differences of 14 ± 10 and 1.2 ± 1.2 Mm−1 for the scattering and absorption coefficients, showing a better agreement for the absorption (scattering) coefficient with higher (lower) aerosol optical depth. The potential of GRASP shown in this study will contribute to enhancing the representativeness of the aerosol vertical distribution and provide information for satellite and global model evaluation.

A substantial fraction of the atmospheric aerosols originates from secondary new particle formation (NPF), where atmospheric vapours are transformed into particles that subsequently grow to larger sizes, affecting human health and the climate. In this study, we investigate aerosol size distributions at two stations located close to each other (∼ 20 km) but at different altitudes: urban (UGR; 680 m a.s.l., metres above sea level) and high-altitude remote (SNS; 2500 m a.s.l.) sites, both in the area of Granada, Spain, and part of AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere). The analysis shows a significant contribution of nucleation mode aerosol particles to the total aerosol number concentration at both sites, with a contribution of 47 % and 48 % at SNS and UGR, respectively. Due to the important contribution of NPF events to the total aerosol number concentrations and their high occurrence frequency (> 70 %) during the study period, a detailed analysis of NPF events is done in order to get insight into the possible mechanisms and processes involved in NPF events at these contrastive sites. At SNS, NPF is found to be associated with the transport of gaseous precursors from lower altitudes by orographic buoyant upward flows. NPF events at the SNS site are always observed from the smallest measured sizes of the aerosol size distribution (4 nm), implying that NPF takes place in or in the vicinity of the high-altitude SNS station rather than being transported from lower altitudes. Although NPF events at the mountain site seem to be connected with those occurring at the urban site, growth rates (GRs) at SNS are higher than those at the UGR site (GR7−25 of 6.9 and 4.5 nm h−1 and GR4−7 of 4.1 and 3.6 nm h−1 at SNS and UGR, respectively). This fact could have special importance for the production of cloud condensation nuclei (CCN) and therefore for cloud formations which may affect regional/global climate, since larger GRs at mountain sites could translate to a larger survival probability of NPF particles reaching CCN sizes, due to the shorter time period needed for the growth. The analysis of sulfuric acid (H2SO4) shows that the contribution of H2SO4 is able to explain a minimal fraction contribution to the observed GRs at both sites (< 1 % and < 10 % for the 7–25 and 4–7 nm size ranges, respectively), indicating that other condensing vapours are responsible for the majority of particle growth, as well as the differing growth rates between the two sites. Results also show that the condensation sink (CS) does not play a relevant role in NPF processes at both sites and points to the availability of volatile organic compounds (VOCs) as one of the main factors controlling the NPF events at both sites. Finally, a closer analysis of the NPF events that were observed at the SNS site during a Saharan dust episode that occurred during the field campaign was carried out, evidencing the role of TiO2 and F2O3 together with VOCs in promoting new particle formation during this dust intrusion event. Although further investigation is needed to improve our understanding in this topic, this result suggests that climate effects of mineral dust and NPF are not disconnected from each other as it was commonly thought. Therefore, since mineral dust contributes to a major fraction of the global aerosol mass load, dust–NPF interaction should be taken into account in global aerosol-climate modelling for better climate change prediction.

This study evaluates the potential of the GRASP algorithm (Generalized Retrieval of Aerosol and Surface Properties) to retrieve continuous day-to-night aerosol properties, both column-integrated and vertically resolved. The study is focused on the evaluation of GRASP retrievals during an intense Saharan dust event that occurred during the Sierra Nevada Lidar aerOsol Profiling Experiment I (SLOPE I) field campaign. For daytime aerosol retrievals, we combined the measurements of the ground-based lidar from EARLINET (European Aerosol Research Lidar Network) station and sun–sky photometer from AERONET (Aerosol Robotic Network), both instruments co-located in Granada (Spain). However, for night-time retrievals three different combinations of active and passive remote-sensing measurements are proposed. The first scheme (N0) uses lidar night-time measurements in combination with the interpolation of sun–sky daytime measurements. The other two schemes combine lidar night-time measurements with night-time aerosol optical depth obtained by lunar photometry either using intensive properties of the aerosol retrieved during sun–sky daytime measurements (N1) or using the Moon aureole radiance obtained by sky camera images (N2). Evaluations of the columnar aerosol properties retrieved by GRASP are done versus standard AERONET retrievals. The coherence of day-to-night evolutions of the different aerosol properties retrieved by GRASP is also studied. The extinction coefficient vertical profiles retrieved by GRASP are compared with the profiles calculated by the Raman technique at night-time with differences below 30 % for all schemes at 355, 532 and 1064 nm. Finally, the volume concentration and scattering coefficient retrieved by GRASP at 2500 m a.s.l. are evaluated by in situ measurements at this height at Sierra Nevada Station. The differences between GRASP and in situ measurements are similar for the different schemes, with differences below 30 % for both volume concentration and scattering coefficient. In general, for the scattering coefficient, the GRASP N0 and N1 show better results than the GRASP N2 schemes, while for volume concentration, GRASP N2 shows the lowest differences against in situ measurements (around 10 %) for high aerosol optical depth values.

An experimental setup to study aerosol hygroscopicity is proposed based on the temporal evolution of attenuated backscatter coefficients from a ceilometer colocated with an instrumented tower equipped with meteorological sensors at different heights. This setup is used to analyze a 4.5-year database at the ACTRIS SIRTA observatory in Palaiseau (Paris, France, 2.208∘ E, 48.713∘ N; 160 m above sea level). A strict criterion-based procedure has been established to identify hygroscopic growth cases using ancillary information, such as online chemical composition, resulting in 8 hygroscopic growth cases from a total of 107 potential cases. For these eight cases, hygroscopic growth-related properties, such as the attenuated backscatter enhancement factor fβ (RH) and the hygroscopic growth coefficient γ, are evaluated. This study shows that the hygroscopicity parameter γ is negatively correlated with the aerosol organic mass fraction but shows a positive correlation with the aerosol inorganic mass fraction. Among inorganic species, nitrate exhibited the highest correlation. This is the first time that hygroscopic enhancement factors are directly retrieved under ambient aerosols using remote-sensing techniques, which are combined with online chemical composition in situ measurements to evaluate the role of the different aerosol species in aerosol hygroscopicity.

This study focuses on the analysis of aerosol hygroscopic growth during the Sierra Nevada Lidar AerOsol Profiling Experiment (SLOPE I) campaign by using the synergy of active and passive remote sensors at the ACTRIS Granada station and in situ instrumentation at a mountain station (Sierra Nevada, SNS). To this end, a methodology based on simultaneous measurements of aerosol profiles from an EARLINET multi-wavelength Raman lidar (RL) and relative humidity (RH) profiles obtained from a multi-instrumental approach is used. This approach is based on the combination of calibrated water vapor mixing ratio (r) profiles from RL and continuous temperature profiles from a microwave radiometer (MWR) for obtaining RH profiles with a reasonable vertical and temporal resolution. This methodology is validated against the traditional one that uses RH from co-located radiosounding (RS) measurements, obtaining differences in the hygroscopic growth parameter (γ) lower than 5 % between the methodology based on RS and the one presented here. Additionally, during the SLOPE I campaign the remote sensing methodology used for aerosol hygroscopic growth studies has been checked against Mie calculations of aerosol hygroscopic growth using in situ measurements of particle number size distribution and submicron chemical composition measured at SNS. The hygroscopic case observed during SLOPE I showed an increase in the particle backscatter coefficient at 355 and 532 nm with relative humidity (RH ranged between 78 and 98 %), but also a decrease in the backscatter-related Ångström exponent (AE) and particle linear depolarization ratio (PLDR), indicating that the particles became larger and more spherical due to hygroscopic processes. Vertical and horizontal wind analysis is performed by means of a co-located Doppler lidar system, in order to evaluate the horizontal and vertical dynamics of the air masses. Finally, the Hänel parameterization is applied to experimental data for both stations, and we found good agreement on γ measured with remote sensing (γ532 = 0.48 ± 0.01 and γ355 = 0.40 ± 0.01) with respect to the values calculated using Mie theory (γ532 = 0.53 ± 0.02 and γ355 = 0.45 ± 0.02), with relative differences between measurements and simulations lower than 9 % at 532 nm and 11 % at 355 nm.

The interest in the use of ceilometers for optical aerosol characterization has increased in the last few years. They operate continuously almost unattended and are also much less expensive than lidars; hence, they can be distributed in dense networks over large areas. However, due to the low signal-to-noise ratio it is not always possible to obtain particle backscatter coefficient profiles, and the vast number of data generated require an automated and unsupervised method that ensures the quality of the profiles inversions. In this work we describe a method that uses aerosol optical depth (AOD) measurements from the AERONET network that it is applied for the calibration and automated quality assurance of inversion of ceilometer profiles. The method is compared with independent inversions obtained by co-located multiwavelength lidar measurements. A difference smaller than 15 % in backscatter is found between both instruments. This method is continuously and automatically applied to the Iberian Ceilometer Network (ICENET) and a case example during an unusually intense dust outbreak affecting the Iberian Peninsula between 20 and 24 February 2016 is shown. Results reveal that it is possible to obtain quantitative optical aerosol properties (particle backscatter coefficient) and discriminate the quality of these retrievals with ceilometers over large areas. This information has a great potential for alert systems and model assimilation and evaluation.

Radiation fog occurs over many locations around the world in stable atmospheric conditions. Air traffic at busy airports can be significantly disrupted because low visibility at the ground makes it unsafe to take off, land and taxi on the ground. Current numerical weather prediction forecasts are able to predict general conditions favorable for fog formation, but not the exact time or location of fog occurrence. A selected set of observations available in near-real time at strategic locations could also be useful to track the evolution of key processes and key parameters that drive fog formation. Such observations could complement the information predicted by numerical weather prediction (NWP) models that is made available to airport forecasters in support of their fog forecast. This paper presents an experimental setup based on collocated automatic lidar and ceilometer measurements, relative humidity measurements and horizontal visibility measurements to study hygroscopic growth of fog condensation nuclei. This process can take several minutes to hours, and can be tracked using lidar- or ceilometer-attenuated backscatter profiles. Based on hygroscopic growth laws we derive a set of parameters that can be used to provide alerts minutes to hours prior to formation of radiation fog. We present an algorithm that uses the temporal evolution of attenuated backscatter measurements to derive pre-fog formation alerts. The performance of the algorithm is tested on 45 independent pre-fog situations at two locations (near Paris, France, and Brussels, Belgium). We find that an alert for pre-fog conditions predominantly occurs 10–50 min prior to fog formation at an altitude ranging 0 to 100 m above ground. In a few cases, alerts can occur up to 100 min prior to fog formation. Alert durations are found to be sensitive to the relative humidity conditions found a few hours prior to the fog.