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We analyze cirrus cloud measurements from two dual-instrument cloud spectrometers, two hygrometers and a backscattersonde with the goal of connecting cirrus optical parameters usually accessible by remote sensing with microphysical size-resolved and bulk properties accessible in situ. Specifically, we compare the particle backscattering coefficient and depolarization ratio to the particle size distribution, effective and mean radius, surface area density, particle aspherical fraction, and ice water content. Data were acquired by instruments on board the M55 Geophysica research aircraft in July and August 2017 during the Asian Monsoon campaign based in Kathmandu, Nepal, in the framework of the StratoClim (Stratospheric and upper tropospheric processes for better climate predictions) project. Cirrus clouds have been observed over the Himalayan region between 10 km and the tropopause, situated at 17–18 km. The observed particle number densities varied between 10 and 10−4 cm−3 in the dimensional range from 1.5 to 468.5 µm in radius. Correspondingly, backscatter ratios from 1.1 up to 50 have been observed. Optical-scattering theory has been used to compare the backscattering coefficients computed from the measured particle size distribution with those directly observed by the backscattersonde. The aspect ratio of the particles, modeled as spheroids for the T-matrix approach, was left as a free parameter to match the calculations to the optical measures. The computed backscattering coefficient can be brought into good agreement with the observed one, but the match between simulated and measured depolarization ratios is insufficient. Relationships between ice particle concentration, mean and effective radius, surface area density, and ice water content with the measured backscattering coefficient are investigated for an estimate of the bulk microphysical parameters of cirrus clouds from remote sensing lidar data. The comparison between particle depolarization and aspherical fraction as measured by one of the cloud spectrometers equipped with a detector for polarization represents a novelty since it was the first time the two instruments were operated simultaneously on an aircraft. The analysis shows the difficulty of establishing an univocal link between depolarization values and the presence and amount of aspherical scatterers. This suggests the need for further investigation that could take into consideration not only the fraction of aspheric particles but also their predominant morphology.

Scattering codes are used to study the optical properties of polar stratospheric clouds (PSCs). Particle backscattering and depolarization coefficients can be computed with available scattering codes once the particle size distribution (PSD) is known and a suitable refractive index is assumed. However, PSCs often appear as external mixtures of supercooled ternary solution (STS) droplets, solid nitric acid trihydrate (NAT) and possibly ice particles, making the assumption of a single refractive index and a single morphology to model the scatterers questionable. Here we consider a set of 15 coincident measurements of PSCs above McMurdo Station, Antarctica, using ground-based lidar, a balloon-borne optical particle counter (OPC) and in situ observations taken by a laser backscattersonde and OPC during four balloon stratospheric flights from Kiruna, Sweden. This unique dataset of microphysical and optical observations allows us to test the performances of optical scattering models when both spherical and aspherical scatterers of different composition and, possibly, shapes are present. We consider particles as STS if their radius is below a certain threshold value Rth and NAT or possibly ice if it is above it. The refractive indices are assumed known from the literature. Mie scattering is used for the STS, assumed spherical. Scattering from NAT particles, considered spheroids of different aspect ratio (AR), is treated with T-matrix results where applicable. The geometric-optics–integral-equation approach is used whenever the particle size parameter is too large to allow for a convergence of the T-matrix method. The parameters Rth and AR of our model have been varied between 0.1 and 2 µm and between 0.3 and 3, respectively, and the calculated backscattering coefficient and depolarization were compared with the observed ones. The best agreement was found for Rth between 0.5 and 0.8 µm and for AR less than 0.55 and greater than 1.5. To further constrain the variability of AR within the identified intervals, we have sought an agreement with the experimental data by varying AR on a case-by-case basis and further optimizing the agreement by a proper choice of AR smaller than 0.55 and greater than 1.5 and Rth within the interval 0.5 and 0.8 µm. The ARs identified in this way cluster around the values 0.5 and 2.5. The comparison of the calculations with the measurements is presented and discussed. The results of this work help to set limits to the variability of the dimensions and asphericity of PSC solid particles, within the limits of applicability of our model based on the T-matrix theory of scattering and on assumptions on a common particle shape in a PSD and a common threshold radius for all the PSDs.

A polarization diversity elastic backscatter lidar was deployed on the equatorial island of Palau in February and March 2016 in the framework of the EU StratoClim project. The system operated unattended in the Palau Atmosferic Observatory from 15 February to 25 March 2016 during the nighttime. Each lidar profile extends from the ground to 30 km height. Here, the dataset is presented and discussed in terms of the temperature structure of the upper troposphere–lower stratosphere (UTLS) obtained from co-located radiosoundings. The cold-point tropopause (CPT) was higher than 17 km. During the campaign, several high-altitude clouds were observed, peaking approximately 3 km below the CPT. Their occurrence was associated with cold anomalies in the upper troposphere (UT). Conversely, when warm UT anomalies occurred, the presence of cirrus was restricted to a 5 km thick layer centred 5 km below the CPT. Thin and subvisible cirrus (SVC) were frequently detected close to the CPT. The particle depolarization ratios of these cirrus were generally lower than the values detected in the UT clouds. CPT cirrus occurrence showed a correlation with cold anomalies likely triggered by stratospheric wave activity penetrating the UT. The back-trajectories study revealed a thermal and convective history compatible with the convective outflow formation for most of the cirrus clouds, suggesting that the majority of air masses related to the clouds had encountered convection in the past and had reached the minimum temperature during its transport in less than 48 h before the observation. A subset of SVC with low depolarization and no sign of significative recent uplifting may have originated in situ.

We experimentally quantified the impact of cloud fraction and cloud type on the heating rate (HR) of black and brown carbon (HRBC and HRBrC). In particular, we examined in more detail the cloud effect on the HR detected in a previous study (Ferrero et al., 2018). High-time-resolution measurements of the aerosol absorption coefficient at multiple wavelengths were coupled with spectral measurements of the direct, diffuse and surface reflected irradiance and with lidar–ceilometer data during a field campaign in Milan, Po Valley (Italy). The experimental set-up allowed for a direct determination of the total HR (and its speciation: HRBC and HRBrC) in all-sky conditions (from clear-sky conditions to cloudy). The highest total HR values were found in the middle of winter (1.43 ± 0.05 K d−1), and the lowest were in spring (0.54 ± 0.02 K d−1). Overall, the HRBrC accounted for 13.7 ± 0.2 % of the total HR, with the BrC being characterized by an absorption Ångström exponent (AAE) of 3.49 ± 0.01. To investigate the role of clouds, sky conditions were classified in terms of cloudiness (fraction of the sky covered by clouds: oktas) and cloud type (stratus, St; cumulus, Cu; stratocumulus, Sc; altostratus, As; altocumulus, Ac; cirrus, Ci; and cirrocumulus–cirrostratus, Cc–Cs). During the campaign, clear-sky conditions were present 23 % of the time, with the remaining time (77 %) being characterized by cloudy conditions. The average cloudiness was 3.58 ± 0.04 oktas (highest in February at 4.56 ± 0.07 oktas and lowest in November at 2.91 ± 0.06 oktas). St clouds were mostly responsible for overcast conditions (7–8 oktas, frequency of 87 % and 96 %); Sc clouds dominated the intermediate cloudiness conditions (5–6 oktas, frequency of 47 % and 66 %); and the transition from Cc–Cs to Sc determined moderate cloudiness (3–4 oktas); finally, low cloudiness (1–2 oktas) was mostly dominated by Ci and Cu (frequency of 59 % and 40 %, respectively). HR measurements showed a constant decrease with increasing cloudiness of the atmosphere, enabling us to quantify for the first time the bias (in %) of the aerosol HR introduced by the simplified assumption of clear-sky conditions in radiative-transfer model calculations. Our results showed that the HR of light-absorbing aerosol was ∼ 20 %–30 % lower in low cloudiness (1–2 oktas) and up to 80 % lower in completely overcast conditions (i.e. 7–8 oktas) compared to clear-sky ones. This means that, in the simplified assumption of clear-sky conditions, the HR of light-absorbing aerosol can be largely overestimated (by 50 % in low cloudiness, 1–2 oktas, and up to 500 % in completely overcast conditions, 7–8 oktas). The impact of different cloud types on the HR was also investigated. Cirrus clouds were found to have a modest impact, decreasing the HRBC and HRBrC by −5 % at most. Cumulus clouds decreased the HRBC and HRBrC by −31 ± 12 % and −26 ± 7 %, respectively; cirrocumulus–cirrostratus clouds decreased the HRBC and HRBrC by −60 ± 8 % and −54 ± 4 %, which was comparable to the impact of altocumulus (−60 ± 6 % and −46 ± 4 %). A higher impact on the HRBC and HRBrC suppression was found for stratocumulus (−63 ± 6 % and −58 ± 4 %, respectively) and altostratus (−78 ± 5 % and −73 ± 4 %, respectively). The highest impact was associated with stratus, suppressing the HRBC and HRBrC by −85 ± 5 % and −83 ± 3 %, respectively. The presence of clouds caused a decrease of both the HRBC and HRBrC (normalized to the absorption coefficient of the respective species) of −11.8 ± 1.2 % and −12.6 ± 1.4 % per okta. This study highlights the need to take into account the role of both cloudiness and different cloud types when estimating the HR caused by both BC and BrC and in turn decrease the uncertainties associated with the quantification of their impact on the climate.

Polar stratospheric clouds (PSCs) have been observed from 2014 to 2018 from the lidar observatory at the Antarctic Concordia station (Dome C), included as a primary station in the NDACC (Network for Detection of Atmospheric Climate Change). Many of these measurements have been performed in coincidence with overpasses of the satellite-borne CALIOP (Cloud Aerosol Lidar with Orthogonal Polarization) lidar, in order to perform a comparison in terms of PSC detection and composition classification. Good agreement has been obtained, despite intrinsic differences in observation geometry and data sampling. This study reports, to our knowledge, the most extensive comparison of PSC observations by ground-based and satellite-borne lidars. The PSCs observed by the ground-based lidar and CALIOP form a complementary and congruent dataset and allow us to study the seasonal and interannual variations in PSC occurrences at Dome C. Moreover, a strong correlation with the formation temperature of NAT (nitric acid trihydrate), TNAT, calculated from local temperature, pressure, and H2O and HNO3 concentrations is shown. PSCs appear at Dome C at the beginning of June up to 26 km and start to disappear in the second half of August, when the local temperatures start to rise above TNAT. Rare PSC observations in September coincide with colder air masses below 18 km.

Measurements of air pollutants such as black carbon (BC) and particle mass concentration in general, using mobile platforms equipped with high-time-resolution instruments, have gained popularity over the last decade due to their wide range of applicability. Assuring the quality of mobile measurement, data have become more essential, particularly when the personal exposure to pollutants is related to their spatial distribution. In the following, we suggest a methodology to achieve data from mobile measurements of equivalent black carbon (eBC) and PM2.5 mass concentrations with high data quality. Besides frequent routine quality assurance measures of the instruments, the methodology includes the following steps: (a) measures to ensure the quality of mobile instruments through repeated collocated measurements using identical instrumentation, (b) inclusion of a fixed station along the route containing quality-assured reference instruments, and (c) sufficiently long and frequent intercomparisons between the mobile and reference instruments to correct the particle number and mass size distributions obtained from mobile measurements. The application of the methodology can provide the following results. First, collocated mobile measurements with sets of identical instruments allow identification of undetected malfunctions of the instruments. Second, frequent intercomparisons against the reference instruments will ensure the quality of the mobile measurement data of the eBC mass concentration. Third, the intercomparison data between the mobile optical particle size spectrometer (OPSS) and a reference mobility particle size spectrometer (MPSS) allow for the adjustment of the OPSS particle number size distribution using physically meaningful corrections. Matching the OPSS and MPSS volume particle size distributions is crucial for the determination of PM2.5 mass concentration. Using size-resolved complex refractive indices and time-resolved fine-mode volume correction factors of the fine-particle range, the calculated PM2.5 from the OPSS was within 5 % of the reference instruments (MPSS+APSS). However, due to the nonsphericity and an unknown imaginary part of the complex refractive index of supermicrometer particles, a conversion to a volume equivalent diameter yields high uncertainties of the particle mass concentration greater than PM2.5. The proposed methodology addresses issues regarding the quality of mobile measurements, especially for health impact studies, validation of modeled spatial distribution, and development of air pollution mitigation strategies.

Mountainous regions are often considered pristine environments; however they can be affected by pollutants emitted in more populated and industrialised areas, transported by regional winds. Based on experimental evidence, further supported by modelling tools, here we demonstrate and quantify the impact of air masses transported from the Po Valley, a European atmospheric pollution hotspot, to the northwestern Alps. This is achieved through a detailed investigation of the phenomenology of near-range (a few hundred kilometres), trans-regional transport, exploiting synergies of multi-sensor observations mainly focussed on particulate matter. The explored dataset includes vertically resolved data from atmospheric profiling techniques (automated lidar ceilometers, ALCs), vertically integrated aerosol properties from ground (sun photometer) and space, and in situ measurements (PM10 and PM2.5, relevant chemical analyses, and aerosol size distribution). During the frequent advection episodes from the Po basin, all the physical quantities observed by the instrumental setup are found to significantly increase: the scattering ratio from ALC reaches values >30, aerosol optical depth (AOD) triples, surface PM10 reaches concentrations >100 µg m−3 even in rural areas, and contributions to PM10 by secondary inorganic compounds such as nitrate, ammonium, and sulfate increase up to 28 %, 8 %, and 17 %, respectively. Results also indicate that the aerosol advected from the Po Valley is hygroscopic, smaller in size, and less light-absorbing compared to the aerosol type locally emitted in the northwestern Italian Alps. In this work, the phenomenon is exemplified through detailed analysis and discussion of three case studies, selected for their clarity and relevance within the wider dataset, the latter being fully exploited in a companion paper quantifying the impact of this phenomenology over the long-term (Diémoz et al., 2019). For the three case studies investigated, a high-resolution numerical weather prediction model (COSMO) and a Lagrangian tool (LAGRANTO) are employed to understand the meteorological mechanisms favouring transport and to demonstrate the Po Valley origin of the air masses. In addition, a chemical transport model (FARM) is used to further support the observations and to partition the contributions of local and non-local sources. Results show that the simulations are important to the understanding of the phenomenon under investigation. However, in quantitative terms, modelled PM10 concentrations are 4–5 times lower than the ones retrieved from the ALC and maxima are anticipated in time by 6–7 h. Underestimated concentrations are likely mainly due to deficiencies in the emission inventory and to water uptake of the advected particles not fully reproduced by FARM, while timing mismatches are likely an effect of suboptimal simulation of up-valley and down-valley winds by COSMO. The advected aerosol is shown to remarkably degrade the air quality of the Alpine region, with potential negative effects on human health, climate, and ecosystems, as well as on the touristic development of the investigated area. The findings of the present study could also help design mitigation strategies at the trans-regional scale in the Po basin and suggest an observation-based approach to evaluate the outcome of their implementation.

A comparison of polar stratospheric cloud (PSC) occurrence from 2006 to 2010 is presented, as observed from the ground-based lidar station at McMurdo (Antarctica) and by the satellite-borne CALIOP lidar (Cloud-Aerosol Lidar with Orthogonal Polarization) measuring over McMurdo. McMurdo (Antarctica) is one of the primary lidar stations for aerosol measurements of the NDACC (Network for Detection of Atmospheric Climate Change). The ground-based observations have been classified with an algorithm derived from the recent v2 detection and classification scheme, used to classify PSCs observed by CALIOP. A statistical approach has been used to compare ground-based and satellite-based observations, since point-to-point comparison is often troublesome due to the intrinsic differences in the observation geometries and the imperfect overlap of the observed areas. A comparison of space-borne lidar observations and a selection of simulations obtained from chemistry–climate models (CCMs) has been made by using a series of quantitative diagnostics based on the statistical occurrence of different PSC types. The distribution of PSCs over Antarctica, calculated by several CCMVal-2 and CCMI chemistry–climate models has been compared with the PSC coverage observed by the satellite-borne CALIOP lidar. The use of several diagnostic tools, including the temperature dependence of the PSC occurrences, evidences the merits and flaws of the different models. The diagnostic methods have been defined to overcome (at least partially) the possible differences due to the resolution of the models and to identify differences due to microphysics (e.g., the dependence of PSC occurrence on T−TNAT). A significant temperature bias of most models has been observed, as well as a limited ability to reproduce the longitudinal variations in PSC occurrences observed by CALIOP. In particular, a strong temperature bias has been observed in CCMVal-2 models with a strong impact on PSC formation. The WACCM-CCMI (Whole Atmosphere Community Climate Model – Chemistry-Climate Model Initiative) model compares rather well with the CALIOP observations, although a temperature bias is still present.

The use of automated lidar ceilometer (ALC) systems for the aerosol vertically resolved characterization has increased in recent years thanks to their low construction and operation costs and their capability of providing continuous unattended measurements. At the same time there is a need to convert the ALC signals into usable geophysical quantities. In fact, the quantitative assessment of the aerosol properties from ALC measurements and the relevant assimilation in meteorological forecast models is amongst the main objectives of the EU COST Action TOPROF (Towards operational ground-based profiling with ALCs, Doppler lidars and microwave radiometers for improving weather forecasts). Concurrently, the E-PROFILE program of the European Meteorological Services Network (EUMETNET) focuses on the harmonization of ALC measurements and data provision across Europe. Within these frameworks, we implemented a model-assisted methodology to retrieve key aerosol properties (extinction coefficient, surface area, and volume) from elastic lidar and/or ALC measurements. The method is based on results from a large set of aerosol scattering simulations (Mie theory) performed at UV, visible, and near-IR wavelengths using a Monte Carlo approach to select the input aerosol microphysical properties. An average continental aerosol type (i.e., clean to moderately polluted continental aerosol conditions) is addressed in this study. Based on the simulation results, we derive mean functional relationships linking the aerosol backscatter coefficients to the abovementioned variables. Applied in the data inversion of single-wavelength lidars and/or ALCs, these relationships allow quantitative determination of the vertically resolved aerosol backscatter, extinction, volume, and surface area and, in turn, of the extinction-to-backscatter ratios (i.e., the lidar ratios, LRs) and extinction-to-volume conversion factor (cv) at 355, 532, and 1064 nm. These variables provide valuable information for visibility, radiative transfer, and air quality applications. This study also includes (1) validation of the model simulations with real measurements and (2) test applications of the proposed model-based ALC inversion methodology. In particular, our model simulations were compared to backscatter and extinction coefficients independently retrieved by Raman lidar systems operating at different continental sites within the European Aerosol Research Lidar Network (EARLINET). This comparison shows good model–measurement agreement, with LR discrepancies below 20 %. The model-assisted quantitative retrieval of both aerosol extinction and volume was then tested using raw data from three different ALCs systems (CHM 15k Nimbus), operating within the Italian Automated LIdar-CEilometer network (ALICEnet). For this purpose, a 1-year record of the ALC-derived aerosol optical thickness (AOT) at each site was compared to direct AOT measurements performed by colocated sun–sky photometers. This comparison shows an overall AOT agreement within 30 % at all sites. At one site, the model-assisted ALC estimation of the aerosol volume and mass (i.e., PM10) in the lowermost levels was compared to values measured at the surface level by colocated in situ instrumentation. Within this exercise, the ALC-derived daily-mean mass concentration was found to reproduce the corresponding (EU regulated) PM10 values measured by the local air quality agency well in terms of both temporal variability and absolute values. Although limited in space and time, the good performances of the proposed approach suggest it could possibly represent a valid option to extend the capabilities of ALCs to provide quantitative information for operational air quality and meteorological monitoring.

Studying the vertical distribution of aerosol particle physical and chemical properties in the troposphere is essential to understand the relative importance of local emission processes vs. long-range transport for column-integrated aerosol properties (e.g. the aerosol optical depth, AOD, affecting regional climate) as well as for the aerosol burden and its impacts on air quality at the ground. The main objective of this paper is to investigate the transport of desert dust in the middle troposphere and its intrusion into the planetary boundary layer (PBL) over the Po Valley (Italy), a region considered one of the greatest European pollution hotspots for the frequency that particulate matter (PM) limit values are exceeded. Events of mineral aerosol uplift from local (soil) sources and phenomena of hygroscopic growth at the ground are also investigated, possibly affecting the PM concentration in the region as well. During the PEGASOS 2012 field campaign, an integrated observing–modelling system was set up based on near-surface measurements (particle concentration and chemistry), vertical profiling (backscatter coefficient profiles from lidar and radiosoundings) and Lagrangian air mass transport simulations by FLEXPART model. Measurements were taken at the San Pietro Capofiume supersite (44°39′ N, 11°37′ E; 11 m a.s.l.), located in a rural area relatively close to some major urban and industrial emissive areas in the Po Valley. Mt. Cimone (44°12′ N, 10°42′ E; 2165 m a.s.l.) WMO/GAW station observations are also included in the study to characterize regional-scale variability. Results show that, in the Po Valley, aerosol is detected mainly below 2000 m a.s.l. with a prevalent occurrence of non-depolarizing particles ( > 50 % throughout the campaign) and a vertical distribution modulated by the PBL daily evolution. Two intense events of mineral dust transport from northern Africa (19–21 and 29 June to 2 July) are observed, with layers advected mainly above 2000 m, but subsequently sinking and mixing in the PBL. As a consequence, a non-negligible occurrence of mineral dust is observed close to the ground ( ∼ 7 % of occurrence during a 1-month campaign). The observations unambiguously show Saharan dust layers intruding the Po Valley mixing layer and directly affecting the aerosol concentrations near the surface. Finally, lidar observations also indicate strong variability in aerosol on shorter timescales (hourly). Firstly, these highlight events of hygroscopic growth of anthropogenic aerosol, visible as shallow layers of low depolarization near the ground. Such events are identified during early morning hours at high relative humidity (RH) conditions (RH > 80 %). The process is observed concurrently with high PM1 nitrate concentration (up to 15 µg cm−3) and hence mainly explicable by deliquescence of fine anthropogenic particles, and during mineral dust intrusion episodes, when water condensation on dust particles could instead represent the dominant contribution. Secondly, lidar images show frequent events (mean daily occurrence of ∼ 22 % during the whole campaign) of rapid uplift of mineral depolarizing particles in afternoon–evening hours up to 2000 m a.s.l. height. The origin of such particles cannot be directly related to long-range transport events, being instead likely linked to processes of soil particle resuspension from agricultural lands.

In this study, the Weather Research and Forecasting model with online coupled chemistry (WRF-Chem) is applied to simulate an intense Saharan dust outbreak event that took place over the Mediterranean in May 2014. Comparison of a simulation using a physics-based desert dust emission scheme with a numerical experiment using a simplified (minimal) emission scheme is included to highlight the advantages of the former. The model was found to reproduce well the synoptic meteorological conditions driving the dust outbreak: an omega-like pressure configuration associated with a cyclogenesis in the Atlantic coasts of Spain. The model performances in reproducing the atmospheric desert dust load were evaluated using a multi-platform observational dataset of aerosol and desert dust properties, including optical properties from satellite and ground-based sun photometers and lidars, plus in situ particulate matter mass concentration (PM) data. This comparison allowed us to investigate the model ability in reproducing both the horizontal and the vertical displacement of the dust plume, as well as its evolution in time. The comparison with satellite (MODIS-Terra) and sun photometers (AERONET) showed that the model is able to reproduce well the horizontal field of the aerosol optical depth (AOD) and its evolution in time (temporal correlation coefficient with AERONET of 0.85). On the vertical scale, the comparison with lidar data at a single site (Rome, Italy) confirms that the desert dust advection occurs in several, superimposed "pulses" as simulated by the model. Cross-analysis of the modeled AOD and desert dust emission fluxes further allowed for the source regions of the observed plumes to be inferred. The vertical displacement of the modeled dust plume was in rather good agreement with the lidar soundings, with correlation coefficients among aerosol extinction profiles up to 1 and mean discrepancy of about 50 %. The model–measurement comparison for PM10 and PM2.5 showed a good temporal matching, although it revealed a marked overestimation of PM10 and PM2.5 (of the order of 70 % during the dust peak). For PM10, it was also possible to investigate the accordance between the model- and the measurement-based dust PM10, this confirming the model PM10 overestimation to be related to over-predicted dust mass up to a factor of 140 %. In all the model–measurement comparisons performed, the enhanced capabilities of the physics-based emission scheme with respect to its simplified, minimal version were evident and are documented.

We investigate optical–microphysical–chemical properties of brown carbon (BrC) in the urban ambient atmosphere of the Po Valley. In situ ground measurements of aerosol spectral optical properties, PM1 chemical composition (HR-ToF-AMS), and particle size distributions were carried out in Bologna. BrC was identified through its wavelength dependence of light absorption at visible wavelengths, as indicated by the absorption Ångström exponent (AAE). We found that BrC occurs in particles with a narrow monomodal size distribution peaking in the droplet mode, enriched in ammonium nitrate and poor in black carbon (BC), with a strong dependance on OA-to-BC ratios, and SSA530 of 0.98 ± 0.01. We demonstrate that specific complex refractive index values (k530 = 0.017 ± 0.001) are necessary in addition to a proper particle size range to match the large AAEs measured for this BrC (AAE467 − 660 = 3.2 ± 0.9 with values up to 5.3). In terms of consistency of these findings with literature, this study i. provides experimental evidence of the size distribution of BrC associated with the formation of secondary aerosol;ii. shows that in the lower troposphere AAE increases with increasing OA-to-BC ratios rather than with increasing OA – contributing to sky radiometer retrieval techniques (e.g., AERONET);iii. extends the dependence of AAE on BC-to-OA ratios previously observed in chamber experiments to ambient aerosol dominated by wood-burning emissions. These findings are expected to bear important implications for atmospheric modeling studies and remote sensing observations as regards the parametrization and identification of BrC in the atmosphere.

Vertical profiles of aerosol particle optical properties were explored in a case study near the San Pietro Capofiume (SPC) ground station during the PEGASOS Po Valley campaign in the summer of 2012. A Zeppelin NT airship was employed to investigate the effect of the dynamics of the planetary boundary layer at altitudes between ∼ 50 and 800 m above ground. Determined properties included the aerosol particle size distribution, the hygroscopic growth factor, the effective index of refraction and the light absorption coefficient. The first three parameters were used to retrieve the light scattering coefficient. Simultaneously, direct measurements of both the scattering and absorption coefficient were carried out at the SPC ground station. Additionally, a single wavelength polarization diversity elastic lidar system provided estimates of aerosol extinction coefficients using the Klett method to accomplish the inversion of the signal, for a vertically resolved comparison between in situ and remote-sensing results. Note, however, that the comparison was for the most part done in the altitude range where the overlap function is incomplete and accordingly uncertainties are larger. First, the airborne results at low altitudes were validated with the ground measurements. Agreement within approximately ±25 and ±20 % was found for the dry scattering and absorption coefficient, respectively. The single scattering albedo, ranged between 0.83 and 0.95, indicating the importance of the absorbing particles in the Po Valley region. A clear layering of the atmosphere was observed during the beginning of the flight (until ∼ 10:00 LT – local time) before the mixing layer (ML) was fully developed. Highest extinction coefficients were found at low altitudes, in the new ML, while values in the residual layer, which could be probed at the beginning of the flight at elevated altitudes, were lower. At the end of the flight (after ∼ 12:00 LT) the ML was fully developed, resulting in constant extinction coefficients at all altitudes measured on the Zeppelin NT. Lidar estimates captured these dynamic features well and good agreement was found for the extinction coefficients compared to the in situ results, using fixed lidar ratios (LR) between 30 and 70 sr for the altitudes probed with the Zeppelin. These LR are consistent with values for continental aerosol particles that can be expected in this region.

We investigated chemical and microphysical processes in the late winter in the Antarctic lower stratosphere, after the first chlorine activation and initial ozone depletion. We focused on a time interval when both further chlorine activation and ozone loss, but also chlorine deactivation, occur. We performed a comprehensive Lagrangian analysis to simulate the evolution of an air mass along a 10-day trajectory, coupling a detailed microphysical box model to a chemistry model. Model results have been compared with in situ and remote sensing measurements of particles and ozone at the start and end points of the trajectory, and satellite measurements of key chemical species and clouds along it. Different model runs have been performed to understand the relative role of solid and liquid polar stratospheric cloud (PSC) particles for the heterogeneous chemistry, and for the denitrification caused by particle sedimentation. According to model results, under the conditions investigated, ozone depletion is not affected significantly by the presence of nitric acid trihydrate (NAT) particles, as the observed depletion rate can equally well be reproduced by heterogeneous chemistry on cold liquid aerosol, with a surface area density close to background values. Under the conditions investigated, the impact of denitrification is important for the abundances of chlorine reservoirs after PSC evaporation, thus stressing the need to use appropriate microphysical models in the simulation of chlorine deactivation. We found that the effect of particle sedimentation and denitrification on the amount of ozone depletion is rather small in the case investigated. In the first part of the analyzed period, when a PSC was present in the air mass, sedimentation led to a smaller available particle surface area and less chlorine activation, and thus less ozone depletion. After the PSC evaporation, in the last 3 days of the simulation, denitrification increases ozone loss by hampering chlorine deactivation.

This work quantifies the spatial distribution of different aerosol types, their seasonal variability and sources.The analysis of four years of CALIOP (Cloud–Aerosol LIdar with Orthogonal Polarization) vertically resolved aerosol data allows the identification of spatial patterns of desert dust and carbonaceous particles in different atmospheric layers. Clusters of Lagrangian back trajectories highlight the transport pathways from source regions during the dusty spring season. The analysis shows a prevalence of dust; at low heights it occurs frequently (up to 70% of available observations) and is distributed north of the Tibetan Plateau with a main contribution from the Gobi and Taklamakan deserts, and west of the Tibetan Plateau, originating from the deserts of southwest Asia and advected by the Westerlies. Above the Himalayas the dust amount is minor but still not negligible (occurrence around 20%) and mainly affected by the transport from more distant deserts sources (Sahara and Arabian Peninsula). Carbonaceous aerosol, produced mainly in northern India and eastern China, is subject to shorter-range transport and is indeed observed closer to the sources, while there is a limited amount reaching the top of the plateau. Data analysis reveals a clear seasonal variability in the frequencies of occurrence for the main aerosol types; dust is regulated principally by the monsoon dynamics, with maximal occurrence in spring. We also highlight relevant interannual differences, showing a larger presence of aerosol in the region during 2007 and 2008. The characterization of the aerosol spatial and temporal distribution in terms of observational frequency is a key piece of information that can be directly used for the evaluation of global aerosol models.

The climate in the Arctic is changing faster than anywhere else on earth. Poorly understood feedback processes relating to Arctic clouds and aerosol–cloud interactions contribute to a poor understanding of the present changes in the Arctic climate system, and also to a large spread in projections of future climate in the Arctic. The problem is exacerbated by the paucity of research-quality observations in the central Arctic. Improved formulations in climate models require such observations, which can only come from measurements in situ in this difficult-to-reach region with logistically demanding environmental conditions. The Arctic Summer Cloud Ocean Study (ASCOS) was the most extensive central Arctic Ocean expedition with an atmospheric focus during the International Polar Year (IPY) 2007–2008. ASCOS focused on the study of the formation and life cycle of low-level Arctic clouds. ASCOS departed from Longyearbyen on Svalbard on 2 August and returned on 9 September 2008. In transit into and out of the pack ice, four short research stations were undertaken in the Fram Strait: two in open water and two in the marginal ice zone. After traversing the pack ice northward, an ice camp was set up on 12 August at 87°21' N, 01°29' W and remained in operation through 1 September, drifting with the ice. During this time, extensive measurements were taken of atmospheric gas and particle chemistry and physics, mesoscale and boundary-layer meteorology, marine biology and chemistry, and upper ocean physics. ASCOS provides a unique interdisciplinary data set for development and testing of new hypotheses on cloud processes, their interactions with the sea ice and ocean and associated physical, chemical, and biological processes and interactions. For example, the first-ever quantitative observation of bubbles in Arctic leads, combined with the unique discovery of marine organic material, polymer gels with an origin in the ocean, inside cloud droplets suggests the possibility of primary marine organically derived cloud condensation nuclei in Arctic stratocumulus clouds. Direct observations of surface fluxes of aerosols could, however, not explain observed variability in aerosol concentrations, and the balance between local and remote aerosols sources remains open. Lack of cloud condensation nuclei (CCN) was at times a controlling factor in low-level cloud formation, and hence for the impact of clouds on the surface energy budget. ASCOS provided detailed measurements of the surface energy balance from late summer melt into the initial autumn freeze-up, and documented the effects of clouds and storms on the surface energy balance during this transition. In addition to such process-level studies, the unique, independent ASCOS data set can and is being used for validation of satellite retrievals, operational models, and reanalysis data sets.

We describe an airborne lidar for the characterization of atmospheric aerosol. The system has been set up in response to the need to monitor extended regions where the air traffic may be posed at risk by the presence of potentially harmful volcanic ash, and to study the characteristics of volcanic emissions both near the source region and when transported over large distances. The lidar provides backscatter and linear depolarization profiles at 532 nm, from which aerosol and cloud properties can be derived. The paper presents the characteristics and capabilities of the lidar system and gives examples of its airborne deployment. Observations from three flights, aimed at assessing the system capabilities in unperturbed atmospheric conditions, and at characterizing the emissions near a volcanic ash source (Mt. Etna) and transported far away from the source, are presented and discussed.

A new automated small size lidar system (microlidar or MULID) has been developed and employed to perform aerosol measurements since March 2010 at Ny Ålesund (78.9°N, 11.9°E), Svalbard. The lidar observations have been used to estimate the PBL height by using the gradient method based on abrupt changes in the vertical aerosol profile and monitor its temporal evolution. The scope of the present study is to compare several approaches to estimate the PBL height, by using lidar observations, meteorological measurements by radio soundings, and a zero-order one-dimensional model based on a parameterization of the turbulent kinetic energy budget within the mixing layer, under the assumptions of horizontal homogeneity, and neglecting radiation and latent heat effects. A case study is presented here for a convective PBL, observed in June 2010 in order to verify whether the Gradient Method can be applied to lidar measurements in the Arctic region to obtain the PBL height. The results obtained are in good agreement with the PBL height estimated by the analysis of thermodynamic measurements obtained from radio sounding and with the model.

Associations between indoor air pollution from fine particulate matter (PM with aerodynamic diameter d p  < 2.5 μm) and human health are poorly understood. Here, we analyse the concentration-response curves for fine and ultrafine PM, the gene expression, and the methylation patterns in human bronchial epithelial cells (BEAS-2B) exposed at the air-liquid interface (ALI) within a classroom in downtown Rome. Our results document the upregulation of aryl hydrocarbon receptor (AhR) and genes associated with xenobiotic metabolism (CYP1A1 and CYP1B1) in response to single exposure of cells to fresh urban aerosols at low fine PM mass concentrations within the classroom. This is evidenced by concentrations of ultrafine particles (UFPs, dp < 0.1 μm), polycyclic aromatic hydrocarbons (PAH), and ratios of black carbon (BC) to organic aerosol (OA). Additionally, an interleukin 18 (IL-18) down-regulation was found during periods of high human occupancy. Despite the observed gene expression dysregulation, no changes were detected in the methylation levels of the promoter regions of these genes, indicating that the altered gene expression is not linked to changes in DNA methylation and suggesting the involvement of another epigenetic mechanism in the gene regulation. Gene expression changes at low exposure doses have been previously reported. Here, we add the possibility that lung epithelial cells, when singly exposed to real environmental concentrations of fine PM that translate into ultra-low doses of treatment, may undergo epigenetic alteration in the expression of genes related to xenobiotic metabolism. Our findings provide a perspective for future indoor air quality regulations. We underscore the potential role of indoor UFPs as carriers of toxic molecules with low-pressure weather conditions, when rainfall and strong winds may favour low levels of fine PM., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 National reserch Council of Italy - CNR. Published by Elsevier Ltd.. All rights reserved.)

Exposures to fine particulate matter (PM[Formula: see text]) have been associated with health impacts, but the understanding of the PM[Formula: see text] concentration-response (PM[Formula: see text]-CR) relationships, especially at low PM[Formula: see text], remains incomplete. Here, we present novel data using a methodology to mimic lung exposure to ambient air (2[Formula: see text] 60 [Formula: see text]g m[Formula: see text]), with minimized sampling artifacts for nanoparticles. A reference model (Air Liquid Interface cultures of human bronchial epithelial cells, BEAS-2B) was used for aerosol exposure. Non-linearities observed in PM[Formula: see text]-CR curves are interpreted as a result of the interplay between the aerosol total oxidative potential (OP[Formula: see text]) and its distribution across particle size (d[Formula: see text]). A d[Formula: see text]-dependent condensation sink (CS) is assessed together with the distribution with d[Formula: see text] of reactive species . Urban ambient aerosol high in OP[Formula: see text], as indicated by the DTT assay, with (possibly copper-containing) nanoparticles, shows higher pro-inflammatory and oxidative responses, this occurring at lower PM[Formula: see text] concentrations (< 5 [Formula: see text]g m[Formula: see text]). Among the implications of this work, there are recommendations for global efforts to go toward the refinement of actual air quality standards with metrics considering the distribution of OP[Formula: see text] with d[Formula: see text] also at relatively low PM[Formula: see text]., (© 2023. The Author(s).)

Wherever a loose bed of sand is subject to sufficiently strong winds, aeolian dunes form at predictable wavelengths and growth rates. As dunes mature and coarsen, however, their growth trajectories become more idiosyncratic; nonlinear effects, sediment supply, wind variability and geologic constraints become increasingly relevant, resulting in complex and history-dependent dune amalgamations. Here we examine a fundamental question: do aeolian dunes stop growing and, if so, what determines their ultimate size? Earth's major sand seas are populated by giant sand dunes, evolved over tens of thousands of years. We perform a global analysis of the topography of these giant dunes, and their associated atmospheric forcings and geologic constraints, and we perform numerical experiments to gain insight on temporal evolution of dune growth. We find no evidence of a previously proposed limit to dune size by atmospheric boundary layer height. Rather, our findings indicate that dunes may grow indefinitely in principle; but growth depends on morphology, slows with increasing size, and may ultimately be limited by sand supply., (© 2022. The Author(s).)

Current shipping activities employ about 3% of the world-delivered energy. Most of this energy is conveyed by diesel engines. In Europe, release of NO x and particulate matter (PM) from shipping is expected to equal the road-transport one by the year 2020. This paper addresses a typical central Mediterranean city-port condition to evaluate the relative contribution of shipping activities to the local air quality. A 3-year long air quality dataset collected at the boundary between the port of Civitavecchia (the major port in central Italy) and the city itself was analyzed to evaluate the long-term, relative contribution of the port and of the city at determining the loads of EU-regulated pollutants (NO 2 , PM 10 and SO 2 ). In addition, black carbon and ultrafine-to-coarse particles data collected along a short-term, intensive campaign were used to assess the port's role at emitting these unregulated pollutants. Cross-analysis of the measurements, allowed to assess which shipping-related activities and port's sectors represent the principal emitters. At the city-port boundary, the annual share of regulated pollutants originating in the port area by shipping and ground movements is of 33% for PM 10 , 43% for NO 2 , and 60% for SO 2 . Analysis of non-regulated pollutants shows the in-port, high polluting potential of some ship categories, in particular those employing low-sulfur but poorly refined oils. These conditions appear to be more often associated with Ro-Ro passenger ships. Piers closest to the Civitavecchia urban settlements are also observed to host the largest emissions. Meteorology and location of the piers with respect to residential areas are confirmed to govern the port's share at impacting the city air quality. Even though air quality thresholds for regulated pollutants are not exceeded in Civitavecchia, constant consideration of an enlarged set of environmental variables should drive actions implemented to mitigate the port's impact onto the nearby city's air quality., (Copyright © 2019 The Author(s). Published by Elsevier B.V. All rights reserved.)

Air pollution and particulate matter are recognised cause of increased disease incidence in exposed population. The toxicological processes underlying air pollution associated effects have been investigated by in vivo and/or in vitro experimentation. The latter is usually performed by exposing cells cultured under submerged condition to particulate matter concentration quite far from environmental exposure expected in humans. Here we report for the first time the feasibility of a direct exposure of air liquid interface cultured cells to environmental concentration of particulate matter. Inflammatory proteins release was analysed in cell medium while differential expression of selected genes was analysed in cells. Significant association of anti-oxidant genes was observed with secondary and aged aerosol, while cytochrome activation with primary and PAHs enriched ultrafine particles. The results obtained clearly show the opportunity to move from the lab bench to the field for properly understanding the toxicological effects also of ultrafine particles on selected in vitro models., (Copyright © 2018 Elsevier Ltd. All rights reserved.)