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The Cloud-AerosoL InteractionS in the Helmos background TropOsphere (CALISHTO) campaign took place in autumn 2021 at the NCSR Demokritos background high-altitude Helmos Hellenic Atmospheric Aerosol & Climate Change station (HAC)2 to study the interactions between aerosols and clouds. The current study presents the chemical characterization of the Non-Refractory (NR) PM1 aerosol fraction using a Time-of-Flight Aerosol Chemical Speciation Monitor (ToF-ACSM). A comparative offline aerosol filter analysis by a High-Resolution Time-of-Flight Aerosol Mass Spectrometry (HR-ToF-AMS) showed consistent results regarding the species determined. Source apportionment applied on both datasets (ACSM-ToF and offline AMS analysis on filter extracts) yielded the same factors for the organic aerosol (one primary and two secondary factors). Additionally, the Positive Matrix Factorization (PMF) model was applied on the total PM1 fraction by the ToF-ACSM (including both organic and inorganic ions). Five different types were identified, including a primary organic factor, ammonium nitrate, ammonium sulphate, and two secondary organic aerosols; one more and one less oxidized. The prevailing atmospheric conditions at the station, i.e. cloud presence, influence from emissions from the Planetary Boundary Layer (PBL) and air mass origin were also incorporated in the study. The segregation between PBL and Free Troposphere (FT) conditions was made by combining data from remote sensing and in-situ measurement techniques. The types of air masses arriving at the site were grouped as continental, marine, dust and marine-dust based on back trajectories data. Significant temporal variability in the aerosol characteristics was observed throughout the campaign; in September, air masses from within the PBL were sampled most of the time, resulting in much higher mass concentrations compared to October and November when concentrations were reduced by a factor of 5. Both in-cloud and FT measurement periods resulted in much lower concentration levels, while similar composition was observed in PBL and FT conditions. We take advantage of using a recently developed "virtual filtering" technique to separate interstitial from activated aerosol sampled from a PM10 inlet during cloudy periods. This allows the determination of the chemical composition of the interstitial aerosol during in-cloud periods. Ammonium sulphate, the dominant PMF factor in all conditions, contributed more when air masses were arriving at (HAC)2 during Dust events, while higher secondary organic aerosol contribution was observed when air masses arrived from continental Europe. [ABSTRACT FROM AUTHOR]

The purpose of this study is to understand the drivers of cloud droplet formation in orographic clouds. We used a combination of modeling, in-situ and remote sensing measurements at the high-altitude Helmos Hellenic Atmospheric Aerosol and Climate Change station ((HAC)2), which is located at the top of Mt. Helmos (1314 metres above sea level), Greece during the Cloud-AerosoL InteractionS in the Helmos background TropOsphere (CALISTHO) campaign in Fall 2021 (https://calishto.panacea-ri.gr/) to examine the origins of the aerosols (i.e., local aerosol from the Planetary Boundary Layer (PBL), or long-range transported aerosol from the Free Tropospheric Layer (FTL) contributing to the Cloud Condensation Nuclei (CCN), their characteristics (hygroscopicity, size distribution and mixing state), as well as the vertical velocities distributions and resulting supersaturations. We found that the characteristics of the PBL aerosol were considerably different from FTL aerosol and use the aerosol particle number and equivalent mass concentration of the black carbon (eBC) in order to determine when the (HAC)2 was within the FTL or PBL based on timeseries of the height of the PBL. During the (HAC)2 cloud events we sample a mixture of interstitial aerosol and droplet residues, which we characterize using a new approach that utilizes the in-situ droplet measurements to determine time periods where the aerosol sample is purely interstitial. From the dataset we determine the properties (size distribution and hygroscopicity) of the pre-cloud, activated and interstitial aerosol. The hygroscopicity of activated aerosol is found to be higher than that of the interstitial or pre-cloud aerosol. A series of closure studies with the droplet parameterization shows that cloud droplet concentration (N d) and supersaturation can be predicted to within 25 % of observations when the aerosol size distributions correspond to pre-cloud conditions. Analysis of the characteristic supersaturation of each aerosol population indicates that droplet formation in clouds is aerosol-limited when formed in FTL airmasses – hence droplet formation is driven by aerosol variations, while clouds formed in the PBL tend to be velocity limited and droplet variations are driven by fluctuations in vertical velocity. Given that the cloud dynamics do not vary significantly between airmasses, the variation in aerosol concentration and type is mostly responsible for these shifts in cloud microphysical state and sensitivity to aerosol. With these insights, remote sensing of cloud droplets in such clouds can be used to infer either CCN spectra (when in the FTL) or vertical velocity (when in the PBL). In conclusion, we show that a coordinated measurement of aerosol and cloud properties, together with the novel analysis approaches presented here allow for the determination of the drivers of droplet formation in orographic clouds and their sensitivity to aerosol and vertical velocity variations. [ABSTRACT FROM AUTHOR]

Vertical profiling of aerosol particles was performed during the PANhellenic infrastructure for Atmospheric Composition and climatE chAnge (PANACEA) winter campaign (10 January 2020–7 February 2020) over the city of Ioannina, Greece (39.65° N, 20.85° E, 500 m a.s.l.). The middle-sized city of Ioannina suffers from wintertime air pollution episodes due to biomass burning (BB) domestic heating activities. The lidar technique was applied during the PANACEA winter campaign on Ioannina city, to fill the gap of knowledge of the spatio-temporal evolution of the vertical mixing of the particles occurring during these winter-time air pollution episodes. During this campaign the mobile single-wavelength (532 nm) depolarization Aerosol lIdAr System (AIAS) was used to measure the spatio-temporal evolution of the aerosols' vertical profiles within the Planetary Boundary Layer (PBL) and the lower free troposphere (LFT; up to 4 km height a.s.l.). AIAS performed almost continuous lidar measurements from morning to late evening hours (typically from 07:00 to 19:00 UTC), under cloud-free conditions, to provide the vertical profiles of the aerosol backscatter coefficient (baer) and the particle linear depolarization ratio (PLDR), both at 532 nm. In this study we emphasized on the vertical profiling of very fresh (~hours) biomass burning (BB) particles originating from local domestic heating activities in the area. In total, 33 out of 34 aerosol layers in the lower free troposphere were characterized as fresh biomass burning ones of local origin, showing a mean particle linear depolarization value of 0.04 ± 0.02 with a range of 0.01 to 0.09 (532 nm) in a height region 1.21–2.23 km a.s.l. To corroborate our findings, we used in situ data, particulate matter (PM) concentrations (PM2.5) from a particulate sensor located close to our station, and the total black carbon (BC) concentrations along with the respective contribution of the fossil fuel (BCff) and biomass/wood burning (BCwb) from the Aethalometer. The PM2.5 mass concentrations ranged from 5.6 to 175.7 μg/m3, while the wood burning emissions from residential heating were increasing during the evening hours, with decreasing temperatures. The BCwb concentrations ranged from 0.5 to 17.5 μg/m3, with an extremely high mean contribution of BCwb equal to 85.4%, which in some cases during night-time reached up to 100% during the studied period. [ABSTRACT FROM AUTHOR]

In this study we present the role of the Planetary Boundary Layer Height (PBLH) on the air pollutant concentrations measured at an urban background station at the megacity of Athens, Greece, an area characterized by complex topography. For this purpose, we utilized in situ measurements of aerosol number concentrations at different size bins (10–200 nm) N 10-200nm , (200–550 nm) N 200-550nm , equivalent Black Carbon (eBC), and wind speed data, for the period of May – July 2020. According to our analysis, both horizontal transport and vertical mixing and dispersion of air pollutants play a critical role in air quality. More precisely, PBLH is negatively correlated with aerosol concentration. The increase in the height of the Planetary Boundary Layer (PBL) favors a reduction in aerosol concentration, which, to some extent, compensates for the increase in aerosol load due to emission sources and horizontal transport from the city center. The horizontal advection process is related to the PBLH, since a deep PBL drives the advection, while a shallow PBL is characterized by weak horizontal wind velocities. On the other hand, under stagnant air mass conditions, when the PBL shrinks, the concentrations of air pollutants increase. On average, a 25% increase in the PBLH results in a 15% reduction in aerosol concentration, whereas a 15% reduction in the PBLH may result in a 10% increase in aerosol concentrations. Overall, N 10-200nm particle concentrations increases, when air masses arrive from the S-NW sector (city center) due to traffic and vehicle emissions, while transport of continental pollution mixed with local and regional emissions along the Balkans-Aegean Sea axis, is originating from the NE axis under high wind speeds. The latter is more clearly recognized from aged aerosol components such as sulphate. Whereas, the N 200-550nm and eBC showed increased concentration load under stagnant air mass conditions, independently of the wind direction. [Display omitted] • Horizontal transport, vertical mixing and dispersion of air pollutants play a critical role in air quality. • PBLH is negatively correlated with aerosol concentration. • The increase in the height of the PBL favors a reduction in aerosol concentration, • Under stagnant air mass conditions, when the PBL shrinks, the concentrations of air pollutants increase. [ABSTRACT FROM AUTHOR]

Air quality forecast systems need reliable and accurate representations of the planetary boundary layer (PBL) to perform well. An important question is how accurately numerical weather prediction models can reproduce conditions in diverse synoptic flow types. Here, observations from the summer 2014 HygrA-CD (Hygroscopic Aerosols to Cloud Droplets) experimental campaign are used to validate simulations from the Weather Research and Forecasting (WRF) model over the complex, urban terrain of the Greater Athens Area. Three typical atmospheric flow types were identified during the 39-day campaign based on 2-day backward trajectories: Continental, Etesians, and Saharan. It is shown that the numerical model simulations differ dramatically depending on the PBL scheme, atmospheric dynamics, and meteorological parameter (e.g., 2-m air temperature). Eight PBL schemes from WRF version 3.4 are tested with daily simulations on an inner domain at 1-km grid spacing. Near-surface observations of 2-m air temperature and relative humidity and 10-m wind speed are collected from multiple meteorological stations. Estimates of the PBL height come from measurements using a multiwavelength Raman lidar, with an adaptive extended Kalman filter technique. Vertical profiles of atmospheric variables are obtained from radiosonde launches, along with PBL heights calculated using bulk Richardson number. Daytime maximum PBL heights ranged from 2.57 km during Etesian flows, to as low as 0.37 km during Saharan flows. The largest differences between model and observations are found with simulated PBL height during Saharan synoptic flows. During the daytime, campaign-averaged near-surface variables show WRF tended to have a cool, moist bias with higher simulated wind speeds than the observations, especially near the coast. It is determined that non-local PBL schemes give the most agreeable solutions when compared with observations. [ABSTRACT FROM AUTHOR]