Abstract. The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental setup also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote-sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modeling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to producing high levels of atmospheric pollutants or intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign, with the main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 and 0.6 (at 440 nm) over the western and central Mediterranean basins. One important point of this experiment concerns the direct observations of aerosol extinction onboard the ATR-42, using the CAPS system, showing local maxima reaching up to 150 M m −1 within the dust plume. Non-negligible aerosol extinction (about 50 M m −1 ) has also been observed within the marine boundary layer (MBL). By combining the ATR-42 extinction coefficient observations with absorption and scattering measurements, we performed a complete optical closure revealing excellent agreement with estimated optical properties. This additional information on extinction properties has allowed calculation of the dust single scattering albedo (SSA) with a high level of confidence over the western Mediterranean. Our results show a moderate variability from 0....

Desert dust interacts with shortwave (SW) and longwave (LW) radiation, influencing the Earth radiation budget and the atmospheric vertical structure. Uncertainties on the dust role are large in the LW spectral range, where few measurements are available and the dust optical properties are not well constrained. The first airborne measurements of LW irradiance vertical profiles over the Mediterranean were carried out during the Ground-based and Airborne Measurements of Aerosol Radiative Forcing (GAMARF) campaign, which took place in spring 2008 at the island of Lampedusa. The experiment was aimed at estimating the vertical profiles of the SW and LW aerosol direct radiative forcing (ADRF) and heating rates (AHR), taking advantage of vertically resolved measurements of irradiances, meteorological parameters, and aerosol microphysical and optical properties. Two cases, characterized respectively by the presence of a homogeneous dust layer (3 May, with aerosol optical depth, AOD, at 500 nm of 0.59) and by a low aerosol burden (5 May, with AOD of 0.14), are discussed. A radiative transfer model was initialized with the measured vertical profiles and with different aerosol properties, derived from measurements or from the literature. The simulation of the irradiance vertical profiles, in particular, provides the opportunity to constrain model-derived estimates of the AHR. The measured SW and LW irradiances were reproduced when the model was initialized with the measured aerosol size distributions and refractive indices. For the dust case, the instantaneous (solar zenith angle, SZA, of 55.1°) LW-to-SW ADRF ratio was 23% at the surface and 11% at the top of the atmosphere (TOA), with a more significant LW contribution on a daily basis (52% at the surface and 26% at TOA), indicating a relevant reduction of the SW radiative effects. The AHR profiles followed the aerosol extinction profile, with comparable peaks in the SW (0.72 ± 0.11 K d À1) and in the LW (À0.52 ± 0.12 K d À1) for the considered SZA. On a daily basis, the absolute value of the heating rate was larger in the LW than in the SW, producing a net cooling effect at specific levels. These are quite unexpected results, emphasizing the important role of LW radiation.

Abstract. The Mediterranean basin is characterized by large concentrations of aerosols from both natural and anthropogenic sources. These aerosols affect tropospheric photochemistry by modulating the photolytic rates. Three simulations of the atmospheric composition at basin scale have been performed with the CHIMERE chemistry-transport model for the period from 6 June to 15 July 2013 covered by the ADRIMED campaign, a campaign of intense measurements in the western Mediterranean basin. One simulation takes into account the radiative effect of the aerosols on photochemistry, the second one does not, and the third one is designed to quantify the model sensitivity to a bias in the ozone column.These simulations are compared to satellite and groundbased measurements, with a particular focus on the area of Lampedusa. Values of the aerosol optical depth (AOD) are obtained from the MODIS instrument on the AQUA and TERRA satellites as well as from stations in the AERONET network and from the MFRSR sun photometer deployed at Lampedusa. Additional measurements from instruments deployed at Lampedusa either permanently or exceptionally are used for other variables: MFRSR sun photometer for AOD, diode array spectrometer for actinic fluxes, LIDAR for the aerosol backscatter, sequential sampler for speciation of aerosol and Brewer spectrophotometer for the total ozone column. It is shown that CHIMERE has a significant ability to reproduce observed peaks in the AOD, which in Lampedusa are mainly due to dust outbreaks during the ADRIMED period, and that taking into account the radiative effect of the aerosols in CHIMERE considerably improves the ability of the model to reproduce the observed day-to-day variations of the photolysis rate of ozone to S. Mailler et al.: Impact of aerosols on photolysis rates at Lampedusaspheric ozone column are very important in representing correctly the day-to-day variations, the day-to-day variations of J (NO 2 ) are captured almost completely by the model when the optical effects of the aerosols are taken into account.Finally, it is shown that the inclusion of the direct radiative effect of the aerosols in the CHIMERE model leads to reduced J (O 1 D) and J (NO 2 ) values over all the simulation domain, which range from a few percents over continental Europe and the north-east Atlantic Ocean to about 20 % close to and downwind from Saharan dust sources. The effect on the modelled ozone concentration is 2-fold: the effect of aerosols leads to reduced ozone concentrations over the Mediterranean Sea and continental Europe, close to the sources of NO x , but it also leads to increased ozone concentrations over remote areas such as the Sahara and the tropical Atlantic Ocean.

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Abstract. The Chemistry-Aerosol Mediterranean Experiment (ChArMEx; http://charmex.lsce.ipsl.fr) is a collaborative research program federating international activities to investigate Mediterranean regional chemistry-climate interactions. A special observing period (SOP-1a) including intensive airborne measurements was performed in the framework of the Aerosol Direct Radiative Forcing on the Mediterranean Climate (ADRIMED) project during the Mediterranean dry season over the western and central Mediterranean basins, with a focus on aerosol-radiation measurements and their modeling. The SOP-1a took place from 11 June to 5 July 2013. Airborne measurements were made by both the ATR-42 and F-20 French research aircraft operated from Sardinia (Italy) and instrumented for in situ and remote-sensing measurements, respectively, and by sounding and drifting balloons, launched in Minorca. The experimental set-up also involved several ground-based measurement sites on islands including two ground-based reference stations in Corsica and Lampedusa and secondary monitoring sites in Minorca and Sicily. Additional measurements including lidar profiling were also performed on alert during aircraft operations at EARLINET/ACTRIS stations at Granada and Barcelona in Spain, and in southern Italy. Remote sensing aerosol products from satellites (MSG/SEVIRI, MODIS) and from the AERONET/PHOTONS network were also used. Dedicated meso-scale and regional modelling experiments were performed in relation to this observational effort. We provide here an overview of the different surface and aircraft observations deployed during the ChArMEx/ADRIMED period and of associated modeling studies together with an analysis of the synoptic conditions that determined the aerosol emission and transport. Meteorological conditions observed during this campaign (moderate temperatures and southern flows) were not favorable to produce high level of atmospheric pollutants nor intense biomass burning events in the region. However, numerous mineral dust plumes were observed during the campaign with main sources located in Morocco, Algeria and Tunisia, leading to aerosol optical depth (AOD) values ranging between 0.2 to 0.6 (at 440 nm) over the western and central Mediterranean basins. Associated aerosol extinction values measured on-board the ATR-42 within the dust plume show local maxima reaching up to 150 Mm−1. Non negligible aerosol extinction (about 50 Mm−1) was also been observed within the Marine Boundary Layer (MBL). By combining ATR-42 extinction, absorption and scattering measurements, a complete optical closure has been made revealing excellent agreement with estimated optical properties. Associated calculations of the dust single scattering albedo (SSA) have been conducted, which show a moderate variability (from 0.90 to 1.00 at 530 nm). In parallel, active remote-sensing observations from the surface and onboard the F-20 aircraft suggest a complex vertical structure of particles and distinct aerosol layers with sea-salt and pollution located within the MBL, and mineral dust and/or aged north American smoke particles located above (up to 6–7 km in altitude). Aircraft and balloon-borne observations show particle size distributions characterized by large aerosols (> 10 μm in diameter) within dust plumes. In terms of shortwave (SW) direct forcing, in-situ surface and aircraft observations have been merged and used as inputs in 1-D radiative transfer codes for calculating the direct radiative forcing (DRF). Results show significant surface SW instantaneous forcing (up to −90 W m−2 at noon). Associated 3-D modeling studies from regional climate (RCM) and chemistry transport (CTM) models indicate a relatively good agreement for simulated AOD compared with measurements/observations from the AERONET/PHOTONS network and satellite data, especially for long-range dust transport. Calculations of the 3-D SW (clear-sky) surface DRF indicate an average of about −10 to −20 W m−2 (for the whole period) over the Mediterranean Sea together with maxima (−50 W m−2) over northern Africa. The top of the atmosphere (TOA) DRF is shown to be highly variable within the domain, due to moderate absorbing properties of dust and changes in the surface albedo. Indeed, 3-D simulations indicate negative forcing over the Mediterranean Sea and Europe and positive forcing over northern Africa.

Abstract. Detailed measurements of radiation, atmospheric and aerosol properties were carried out in summer 2013 during the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) campaign in the framework of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) experiment. This study focusses on the characterization of infrared (IR) optical properties and direct radiative effects of mineral dust, based on three vertical profiles of atmospheric and aerosol properties and IR broadband and narrowband radiation from airborne measurements, made in conjunction with radiosonde and ground-based observations at Lampedusa, in the central Mediterranean. Satellite IR spectra from the Infrared Atmospheric Sounder Interferometer (IASI) are also included in the analysis. The atmospheric and aerosol properties are used as input to a radiative transfer model, and various IR radiation parameters (upward and downward irradiance, nadir and zenith brightness temperature at different altitudes) are calculated and compared with observations. The model calculations are made for different sets of dust particle size distribution (PSD) and refractive index (RI), derived from observations and from the literature. The main results of the analysis are that the IR dust radiative forcing is non-negligible and strongly depends on PSD and RI. When calculations are made using the in situ measured size distribution, it is possible to identify the refractive index that produces the best match with observed IR irradiances and brightness temperatures (BTs). The most appropriate refractive indices correspond to those determined from independent measurements of mineral dust aerosols from the source regions (Tunisia, Algeria, Morocco) of dust transported over Lampedusa, suggesting that differences in the source properties should be taken into account. With the in situ size distribution and the most appropriate refractive index the estimated dust IR radiative forcing efficiency is +23.7 W m−2 at the surface, −7.9 W m−2 within the atmosphere, and +15.8 W m−2 at the top of the atmosphere. The use of column-integrated dust PSD from AERONET may also produce a good agreement with measured irradiances and BTs, but with significantly different values of the RI. This implies large differences, up to a factor of 2.5 at surface, in the estimated dust radiative forcing, and in the IR heating rate. This study shows that spectrally resolved measurements of BTs are important to better constrain the dust IR optical properties, and to obtain a reliable estimate of its radiative effects. Efforts should be directed at obtaining an improved description of the dust size distribution and its vertical distribution, as well as at including regionally resolved optical properties.

29An unprecedented extreme Saharan dust event was registered in winter time from 20 to 30 23 February 2017 over the Iberian Peninsula (IP). We report on aerosol optical Atmos. Chem. Phys. Discuss., https://doi

Abstract.A Microtops II "ozone monitor" with UV channels centered at 305.5, 312.5, and 320 nm has been used routinely in six experimental campaigns carried out in several geographic locations and seasons, covering latitudes from 35 to 68 • N during the last ten years (2001)(2002)(2003)(2004)(2005)(2006)(2007)(2008)(2009)(2010)(2011). The total ozone content is retrieved by Microtops II by using different combinations (Channel I, 305.5/312.5 nm; Channel II, 312.5/320 nm; and Channel III, 305.5/312.5/320 nm) of the signals at the three ultraviolet wavelengths. The long-term performance of the total ozone content determination has been studied taking into account the sensitivities to the calibration, airmass, temperature and aerosols. When a calibration was used and the airmass limit was fixed to 3, the root mean square deviations of the relative differences produced by Microtops II with respect to several Brewers are 0.9, 2, and 2 % respectively for the Channel I, Channel II, and Channel III retrieval. The performance of the Microtops retrieval has been stable during the last ten years. Channel I represents the best option to determine the instantaneous total ozone content. Channels II and III values appear weakly sensitive to temperature, ozone content, and aerosols. Channel II is more stable than Channel I for airmasses larger than 2.6. The conclusions do not show any dependence on latitude and season.