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A joint instrumental Super Site, combining observation in urban (“Sapienza” University) and semi-rural (ESA-ESRIN and CNR-ISAC) environment, for atmospheric studies and satellites Cal/Val activities, has been set-up in the Rome area (Italy). Ground based active and passive remote sensing instruments located in both sites are operating in synergy, offering information for a wide range of atmospheric parameters. In this work, a comparison of aerosol and water vapor measurements derived by the Rayleigh-Mie-Raman (RMR) lidars, operating simultaneously in both experimental sites, is presented.

Ceilometer technology is increasingly applied to the monitoring and the characterization of tropospheric aerosols. In this work, a method to estimate some key aerosol parameters (extinction coefficient, surface area concentration and volume concentration) from ceilometer measurements is presented. A numerical model has been set up to derive a mean functional relationships between backscatter and the above mentioned parameters based on a large set of simulated aerosol optical properties. A good agreement was found between the modeled backscatter and extinction coefficients and the ones measured by the EARLINET Raman lidars. The developed methodology has then been applied to the measurements acquired by a prototype Polarization Lidar-Ceilometer (PLC). This PLC instrument was developed within the EC- LIFE+ project “DIAPASON” as an upgrade of the commercial, single-channel Jenoptik CHM15k system. The PLC run continuously (h24) close to Rome (Italy) for a whole year (2013-2014). Retrievals of the aerosol backscatter coefficient at 1064 nm and of the relevant aerosol properties were performed using the proposed methodology. This information, coupled to some key aerosol type identification made possible by the depolarization channel, allowed a year-round characterization of the aerosol field at this site. Examples are given to show how this technology coupled to appropriate data inversion methods is potentially useful in the operational monitoring of parameters of air quality and meteorological interest.

Chemical and dynamical processes lead to the formation of aerosol layers in the upper planetary boundary layer (PBL) and above it. Through vertical mixing and entrainment into the PBL these layers may contribute to the ground-level particulate matter (PM); however, to date a quantitative assessment of such a contribution has not been carried out. This study investigates this aspect by combining chemical and physical aerosol measurements with WRF/Chem (Weather Research and Forecasting with Chemistry) model simulations. The observations were collected in the Milan urban area (northern Italy) during the summer of 2007. The period coincided with the passage of a meteorological perturbation that cleansed the lower atmosphere, followed by a high-pressure period favouring pollutant accumulation. Lidar observations revealed the formation of elevated aerosol layers and evidence of their entrainment into the PBL. We analysed the budget of ground-level PM2.5 (particulate matter with an aerodynamic diameter less than 2.5 μm) with the help of the online meteorology-chemistry WRF/Chem model, focusing in particular on the contribution of upper-level processes. Our findings show that an important player in determining the upper-PBL aerosol layer is particulate nitrate, which may reach higher values in the upper PBL (up to 30% of the aerosol mass) than in the lower PBL. The nitrate formation process is predicted to be largely driven by the relative-humidity vertical profile, which may trigger efficient aqueous nitrate formation when exceeding the ammonium nitrate deliquescence point. Secondary PM2.5 produced in the upper half of the PBL may contribute up to 7-8 μg m-3 (or 25%) to ground-level concentrations on an hourly basis. The residual aerosol layer above the PBL is also found to potentially play a large role, which may occasionally contribute up to 10-12 μg m-3 (or 40%) to hourly ground-level PM2.5 concentrations during the morning hours. Although the results presented here refer to one relatively short period in one location, this study highlights the importance of considering the interplay between chemical and dynamical processes occurring within and above the PBL when interpreting ground-level aerosol observations. [ABSTRACT FROM AUTHOR]

Characterizing chemical and physical aerosol properties is important to understand their sources, effects, and feedback mechanisms in the atmosphere. This study proposes a scheme to classify aerosol populations based on their spectral optical properties (absorption and scattering). The scheme is obtained thanks to the outstanding set of information on particle size and composition these properties contain. The spectral variability of the aerosol single scattering albedo (dSSA), and the extinction, scattering and absorption Angstrom exponents (EAE, SAE and AAE, respectively) were observed on the basis of two-year measurements of aerosol optical properties (scattering and absorption coefficients at blue, green and red wavelengths) performed in the suburbs of Rome (Italy). Optical measurements of various aerosol types were coupled to measurements of particle number size distributions and relevant optical properties simulations (Mie theory). These latter allowed the investigation of the role of the particle size and composition in the bulk aerosol properties observed. The combination of simulations and measurements suggested a general "paradigm" built on dSSA, SAE and AAE to optically classify aerosols. The paradigm proved suitable to identify the presence of key aerosol populations, including soot, biomass burning, organics, dust and marine particles. The work highlights that (i) aerosol populations show distinctive combinations of SAE and dSSA times AAE, these variables being linked by a linear inverse relation varying with varying SSA; (ii) fine particles show EAE>1.5, whilst EAE<2 is found for both coarse particles and ultrafine soot-rich aerosols; (iii) fine and coarse particles both show SSA>0.8, whilst ultrafine urban Aitken mode and soot particles show SSA<0.8. The proposed paradigm agrees with aerosol observations performed during past major field campaigns, this indicating that relations concerning the paradigm have a general validity. [ABSTRACT FROM AUTHOR]

Particulate matter mass concentrations measured in the city of Rome (Italy) in the period 2001-2004 have been cross-analysed with concurrent Saharan dust advection events to infer the impact these natural episodes bear on the standard air quality parameter PM10 observed at two city stations and at one regional background station. Natural events as Saharan dust advections are associated to a definite health risk. At the same time, the Directive 2008/50/EC allows subtraction of PM exceedances caused by natural contributions from statistics used to determine air-quality of EU sites. In this respect, it is important to detect and characterize such advections by means of reliable, operational techniques. To assess the PM10 increase we used both the regional-background method" suggested by EC Guidelines and a "local background" one, demonstrated to be most suited to this central Mediterranean region. The two approaches provided results within 20% from each other. The sequence of Saharan advections over the city has been either detected by Polarization Lidar (laser radar) observations or forecast by the operational numerical regional mineral dust model BSC-DREAM8b of the Barcelona Supercomputing Centre. Lidar observations were also employed to retrieve the average physical properties of the dust clouds as a function of height. Along the four-year period, Lidar measurements 703 evenly distributed days) revealed Saharan plumes transits over Rome on 28.6% of the days, with minimum occurrence in wintertime. Dust was observed to reach the ground on 17.5% of the days totalling 88 episodes. Most (90 %) of these advections lasted up to 5 days, averaging to ~3 days. Median time lag between advections was 7 days. Typical altitude range of the dust plumes was 0-6 km, with centre of mass at ~3 kma.g.l. BSC-DREAM8b model simulations (1461 days) predicted Lidar detectable 532nm extinction coefficient >0.005 km-1) dust advections on 25.9% of the days, with ground contacts on 13% of the days. As in the Lidar case, the average dust centre of mass was forecast at ~3 km. Along the 703-day Lidar dataset, model forecast and Lidar detection of the presence of dust coincided on 80% of the cases, 92% coincidences are found within a ±1-day window. Combination of the BSC-DREAM8b and Lidar records leads to about 21% of the days being affected by presence of Saharan dust at the ground. This combined dataset has been used to compute the increase in PM with respect to dust-unaffected previous days. This analysis has shown Saharan dust events to exert a meaningful impact on the PM10 records, causing average increases of the order of 11.9 µg m-3. Conversely, PM10 increases computed relying only on the Lidar detections (i.e., presence of dust layers actually observed) were of the order of 15.6 µg m-3. Both analyses indicate the annual average contribution of dust advections to the city PM10 mass concentrations to be of the order of 2.35 µg m-3. These results confirm Saharan advections in the central Mediterranean as important modulators of PM10 loads and exceedances. [ABSTRACT FROM AUTHOR]

Characterizing chemical and physical aerosol properties is important to understand their sources, effects, and feedback mechanisms in the atmosphere. This study proposes a scheme to classify aerosol populations based on their spectral optical properties (absorption and scattering). The scheme is obtained thanks to the outstanding set of information on particle size and composition these properties contain. The spectral variability of the aerosol Single Scattering Albedo (dSSA), and the Scattering and Absorption Angstrom Exponents (SAE and AAE, respectively) were observed on the basis of two-year measurements of aerosol optical properties (scattering and absorption coefficients at blue, green and red wavelengths) performed in the suburbs of Rome (Italy). Optical measurements of various aerosol types were coupled to measurements of particle number size distributions and relevant optical properties simulations (Mie theory). These latter allowed to investigate the role of the particle size and composition in the bulk aerosol properties observed. The combination of simulations and measurements suggested a general "paradigm" built on dSSA, SAE and AAE to optically classify aerosols. The paradigm proved suitable to identify the presence of key aerosol populations, including soot, biomass burning, organics, dust and marine particles. The work highlights that: (i) aerosol populations show distinctive combinations of SAE and dSSA times AAE, these variables being linked by a linear inverse relation varying with varying SSA; (ii) fine particles show SAE > 1.5, whilst SAE < 1 is found for both coarse particles and ultrafine soot-rich aerosols; (iii) fine and coarse particles both show SSA > 0.8, whilst ultrafine urban Aitken mode and soot particles show SSA < 0.8. A strict agreement was found when comparing the proposed paradigm to aerosol observations performed during past major field campaigns. [ABSTRACT FROM AUTHOR]

Wildland fires represent the major source of fine aerosols, i.e., atmospheric particles with diameters <1 µm. The largest numbers of these fires occur in Africa, Asia and South America, but a not negligible fraction also occurs in Eastern Europe and former USSR countries, particularly in the Russian Federation, Ukraine and Kazakhstan. Besides the impact of large forest fires, recent studies also highlighted the crucial role played by routine agricultural fires in Eastern Europe and Russia on the Arctic atmosphere. An evaluation of the impact of these fires over Europe is currently not available. The assessment of the relative contribution of fires to the European aerosol burden is hampered by the complex mixing of natural and anthropogenic particle types across the continent. In this study we use long term (2002-2007) satellite-based fires and aerosol data coupled to atmospheric trajectory modelling in the attempt to estimate the wildfires contribution to the European aerosol optical thickness (AOT). Based on this dataset, we provide evidence that fires-related aerosols play a major role in shaping the AOT yearly cycle at the continental scale. In general, the regions most impacted by wildfires emissions and/or transport are Eastern and Central Europe as well as Scandinavia. Conversely, a minor impact is found in Western Europe and in the Western Mediterranean. We estimate that in spring 5 to 35% of the European fine fraction AOT (FFAOT) is attributable to wildland fires. The estimated impact maximizes in April (20-35 %) in Eastern and Central Europe as well as in Scandinavia and in the Central Mediterranean. An important contribution of wildfires to the FFAOT is also found in summer over most of the continent, particularly in August over Eastern Europe (28 %) and the Mediterranean regions, from Turkey (34 %) to the Western Mediterranean (25 %). Although preliminary, our results suggest that this fires-related, continent-wide haze plays a not negligible role on the European radiation budget, and possibly, on the European air quality, therefore representing a clear target for mitigation. [ABSTRACT FROM AUTHOR]

In spite of being located at the heart of the highest mountain range in the world, the Himalayan Nepal Climate Observatory (5079m a.s.l.) at the Ev-K2-CNR Pyramid is shown to be affected by the advection of pollution aerosols from the populated regions of southern Nepal and the Indo-Gangetic plains. Such an impact is observed along most of the period April 2006-March 2007 addressed here, with a minimum in the monsoon season. Backtrajectory-analysis indicates long-range transport episodes occurring in this period to originate mainly in the West Asian deserts. At this high altitude site, the measured aerosol optical depth is observed to be: 1) about one order of magnitude lower than the one measured at Gandhi College (60m a.s.l.), in the Indo-Gangetic basin, and 2) maximum during the monsoon period, due to the presence of elevated (cirrus-like) particle layers. Assessment of the aerosol radiative forcing results to be hampered by the persistent presence of these high altitude particle layers, which impede a continuous measurement of both the aerosol optical depth and its radiative properties from sky radiance inversions. Even though the retrieved absorption coefficients of pollution aerosols was rather large (single scattering albedo of the order of 0.6-0.9 were observed in the month of April 2006), the corresponding low optical depths (∼0.03 at 500 nm) are expected to limit the relevant radiative forcings. Still, the high specific forcing of this aerosol and its capability of altering snow surface albedo provide good reason for continuous monitoring. [ABSTRACT FROM AUTHOR]

In September 2002, the first INSPECTRO campaign to study the influence of clouds on the spectral actinic flux in the lower troposphere was carried out in East Anglia, England. Measurements of the actinic flux, the irradiance and aerosol and cloud properties were made from four ground stations and by aircraft. The radiation measurements were modelled using the uvspec model and ancillary data. For cloudless conditions, the measurements of the actinic flux were reproduced by 1-D radiative transfer modelling within the measurement and model uncertainties of about ±10%. For overcast days, the ground-based and aircraft radiation measurements and the cloud microphysical property measurements are consistent within the framework of 1-D radiative transfer and within experimental uncertainties. Furthermore, the actinic flux is increased by between 60-100% above the cloud when compared to a cloudless sky, with the largest increase for the optically thickest cloud. Correspondingly, the below cloud actinic flux is decreased by about 55-65%. Just below the cloud top, the downwelling actinic flux has a maximum that is seen in both the measurements and the model results. For broken clouds the traditional cloud fraction approximation is not able to simultaneously reproduce the measured above-cloud enhancement and below-cloud reduction in the actinic flux. [ABSTRACT FROM AUTHOR]

Results are presented from the Actinic Flux Determination from Measurements of Irradiance (ADMIRA) campaign to measure spectral global UV irradiance and actinic flux at the ground, beneath an atmosphere well defined by supporting measurements. Actinic flux is required to calculate photolysis rates for atmospheric chemistry, yet most spectral UV measurements are of irradiance. This work represents the first part of a project to provide algorithms for converting irradiances to actinic fluxes with specified uncertainties. The campaign took place in northern Greece in August 2000 and provided an intercomparison of UV spectroradiometers measuring different radiation parameters, as well as a comprehensive radiation and atmospheric dataset. The independently calibrated spectroradiometers measuring irradiance and actinic flux agreed to within 5%, while measurements of spectral direct irradiance differed by 9%. Relative agreement for all parameters proved to be very stable during the campaign. A polarization problem in the Brewer spectrophotometer was identified as a problem in making radiance distribution measurements with this instrument. At UV wavelengths actinic fluxes F were always greater than the corresponding irradiance E by a factor between 1.4 and 2.6. The value of the ratio F : E depended on wavelength, solar zenith angle, and the optical properties of the atmosphere. Both the wavelength and solar zenith angle dependency of the ratio decreased when the scattering in the atmosphere increased and the direct beam proportion of global irradiance decreased, as expected. Two contrasting days, one clear and one with higher aerosol and some cloud, are compared to illustrate behavior of the F : E ratio. [ABSTRACT FROM AUTHOR]