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An improved tropospheric nitrogen dioxide (NO2) retrieval algorithm from the Global Ozone Monitoring Experiment-2 (GOME-2) instrument based on air mass factor (AMF) calculations performed with more realistic model parameters is presented. The viewing angle-dependency of surface albedo is taken into account by improving the GOME-2 Lambertian-equivalent reflectivity (LER) climatology with a directionally dependent LER (DLER) dataset over land and an ocean surface albedo parametrization over water. A priori NO2 profiles with higher spatial and temporal resolutions are obtained from the IFS(CB05BASCOE) chemistry transport model based on recent emission inventories. A more realistic cloud treatment is provided by a Cloud-As-Layers (CAL) approach, which treats the clouds as uniform layers of water droplets, instead of the current Clouds-as-Reflecting-Boundaries (CRB) model, which assumes the clouds as Lambertian reflectors. Improvements in the AMF calculation affect the tropospheric NO2 columns on average within ±15 % in winter and ±5 % in summer over largely polluted regions. In addition, the impact of aerosols on our tropospheric NO2 retrieval is investigated by comparing the concurrent retrievals based on ground-based aerosol measurements (explicit aerosol correction) and aerosol-induced cloud parameters (implicit aerosol correction). Compared to the implicit aerosol correction through the CRB cloud parameters, the use of CAL reduces the AMF errors by more than 10 %. Finally, to evaluate the improved GOME-2 tropospheric NO2 columns, a validation is performed using ground-based Multi-AXis Differential Optical Absorption Spectroscopy (MAXDOAS) measurements at the BIRA-IASB Xianghe station. The improved tropospheric NO2 dataset shows good agreement with coincident ground-based measurements with a correlation coefficient of 0.94 and a relative difference of −9.9 % on average.

A comprehensive analysis of the seasonal variability of the optical properties of Saharan dust aerosols over Athens, Greece, is presented for a 17-year time period (2000-2016), as derived from multi-wavelength Raman lidar measurements (57 dust events with more than 80 hours of measurements). The profiles of the derived aerosol optical properties (aerosol backscatter and extinction coefficients, lidar ratio and aerosol Ångström exponent) at 355 nm are presented. For these dust events we found a mean value of the lidar ratio of ~52±13 sr at 355 nm and of ~58±8 sr (not shown) at 532 nm (2-4 km a.s.l. height). For our statistical analysis, presented here, we used monthly-mean values and time periods under cloud-free conditions. The number of dust events was greatest in late spring, summer, and early autumn periods. In this paper we also present a selected case study (04 April 2016) of desert dust long-range transport from the Saharan desert.

The EOLE multi-wavelength aerosol Ramandepolarization lidar, and the AIAS depolarization lidar, in synergy with a sun photometer (CIMEL), were used, in the period 2007-2016, to provide the vertical profiles of the aerosol optical properties over Athens, Greece. More than 30 biomass burning events (fresh and aged smoke particles) were observed, with smoke layers between 1.5 up to 4-5 km height, while their duration ranged from 1-3 days. Lidar ratio (LR) values ranged from 40-105 sr (at 355 nm) and from 40-100 sr (at 532 nm), while the linear particle depolarization ratio (LPDR) at both 355 and 532 nm, remained a) at 355 nm/532 nm) ranged from 0.3 to 2.1. Additionally, a case of a near-range transport of biomass burning aerosols arriving over Athens up to 4 km height, between 27 and 28 June 2016, was studied. For this case, we found LRs of the order of 70±5 sr (355 nm) and 65±15 sr (532 nm) and AEa(355 nm/532 nm) around 1.

Measurements of cloud condensation nuclei (CCN) concentrations (cm−3 ) at five levels of supersaturation between 0.2–1%, together with remote sensing profiling and aerosol size distributions, were performed at an urban background site of Athens during the Hygroscopic Aerosols to Cloud Droplets (HygrA-CD) campaign. The site is affected by local emissions and long-range transport, as portrayed by the aerosol size, hygroscopicity and mixing state. Application of a state-of-the-art droplet parameterization is used to link the observed size distribution measurements, bulk composition, and modeled boundary layer dynamics with potential supersaturation, droplet number, and sensitivity of these parameters for clouds forming above the site. The sensitivity is then used to understand the source of potential droplet number variability. We find that the importance of aerosol particle concentration levels associated with the background increases as vertical velocities increase. The updraft velocity variability was found to contribute 58–90% (68.6% on average) to the variance of the cloud droplet number, followed by the variance in aerosol number (6–32%, average 23.2%). Therefore, although local sources may strongly modulate CCN concentrations, their impact on droplet number is limited by the atmospheric dynamics expressed by the updraft velocity regime.

Combined multi-wavelength aerosol Raman lidar and sun photometry measurements were performed during the HYGRA-CD campaign over Athens, Greece during May-June 2014. The retrieved aerosol optical properties (3 aerosol backscatter at 355-532-1064 nm and 2 aerosol extinction profiles at 355-532 nm) were used as input to an inversion code to retrieve the aerosol microphysical properties (effective radius reff and number concentration N ) using regularization techniques. Additionally, the volume concentration profile was derived for fine particles using the LIRIC code. In this paper we selected a complex case study of long-range transport of mixed aerosols (biomass burning particles mixed with dust) arriving over Athens between 10-12 June 2014 in the 1.5-4 km height. Between 2-3 km height we measured mean lidar ratios (LR) ranging from 45 to 58 sr (at 355 and 532 nm), while the Angstrom exponent (AE) aerosol extinction-related values (355nm/532nm) ranged between 0.8-1.3. The retrieved values of reff and N ranged from 0.19±0.07 to 0.22±0.07 μm and 460±230 to 2200±2800 cm-3 , respectively. The aerosol linear depolarization ratio (δ) at 532 nm was lower than 5-7% (except for the Saharan dust cases, where δ~10-15%).

Measurements of cloud condensation nuclei (CCN) concentrations between 0.2-1.0% supersaturation and aerosol size distribution were performed at an urban background site of Athens during HygrA-CD. The site is affected by local and long-range transported emissions as portrayed by the external mixing of the particles, as the larger ones appear to be more hygroscopic and more CCN-active than smaller ones. Activation fractions at all supersaturations exhibit a diurnal variability with minimum values around noon, which are considerably lower than unity. This reinforces the conclusion that the aerosol is mostly externally mixed between “fresher”, less hygroscopic components with more aged, CCN active constituents.

Multi-wavelength aerosol Raman lidar measurements with elastic depolarization at 532 nm were combined with sun photometry during the HYGRA-CD campaign over Athens, Greece, on May-June 2014. We retrieved the aerosol optical [3 aerosol backscatter profiles (baer ) at 355-532-1064 nm, 2 aerosol extinction (aaer ) profiles at 355-532 nm and the aerosol linear depolarization ratio (δ ) at 532 nm] and microphysical properties [effective radius (reff ), complex refractive index (m ), single scattering albedo (ω )]. We present a case study of a long distance transport (~3.500-4.000 km) of biomass burning particles mixed with dust from the Russian Federation-Kazakhstan regions arriving over Athens on 21-23 May 2014 (1.7-3.5 km height). On 23 May, between 2-2.75 km we measured mean lidar ratios (LR) of 35 sr (355 nm) and 42 sr (532 nm), while the mean Angstrom exponent (AE) aerosol backscatter-related values (355nm/532nm and 532nm/1064nm) were 2.05 and 1.22, respectively; the mean value of δ at 532 nm was measured to be 9%. For that day the retrieved mean aerosol microphysical properties at 2-2.75 km height were: reff =0.26 μm (fine mode), reff =2.15 μm (coarse mode), m =1.36+0.00024i, ω =0.999 (355 nm, fine mode), ω =0.992(355 nm, coarse mode), ω =0.997 (532 nm, fine mode), and ω =0.980 (532 nm, coarse mode).

The international experimental campaign Hygroscopic Aerosols to Cloud Droplets (HygrA-CD), organized in the Greater Athens Area (GAA), Greece from 15 May to 22 June 2014, aimed to study the physico-chemical properties of aerosols and their impact on the formation of clouds in the convective Planetary Boundary Layer (PBL). We found that under continental (W-NW-N) and Etesian (NE) synoptic wind flow and with a deep moist PBL (~ 2–2.5 km height), mixed hygroscopic (anthropogenic, biomass burning and marine) particles arrive over the GAA, and contribute to the formation of convective non-precipitating PBL clouds (with droplets of ~ 16–20 μm mean diameter) with vertical extent up to 500 m. Under these conditions, high updraft velocities (1–2 m s− 1) and cloud condensation nuclei (CCN) concentrations (~ 2000 cm− 3 at 1% supersaturation), generated clouds with an estimated cloud droplet number of ~ 600 cm− 3. Under Saharan wind flow conditions (S-SW) a shallow PBL (< 1–1.2 km height) develops, leading to much higher CCN concentrations (~ 3500–5000 cm− 3 at 1% supersaturation) near the ground; updraft velocities, however, were significantly lower, with an estimated maximum cloud droplet number of ~ 200 cm− 3 and without observed significant PBL cloud formation. The largest contribution to cloud droplet number variance is attributed to the updraft velocity variability, followed by variances in aerosol number concentration.