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ABSTRACTInstantaneous determinations of photosynthetically active radiation (PAR) over the sea from the Ocean and Land Color Instrument (OLCI) on Sentinel-3 are compared with in-situ measurements at the island of Lampedusa in the central Mediterranean Sea. Radiative transfer calculations show that the PAR measured at the island site is representative for open ocean conditions. Satellite data show a good agreement (5.2% positive bias, R2 = 0.97) with in-situ data, in line with similar analyses for other satellite sensors. Larger satellite-in situ differences are found during summer, and the possible role of aerosols in degrading PAR estimate has been investigated by comparing AOD values measured at Lampedusa and derived by OLCI. The relative difference between OLCI and in-situ PAR appears to be negatively correlated with the relative differences between OLCI and in-situ AOD, suggesting that a more accurate determination of AOD, in particular, for cases with AOD > 0.2, mostly related to Saharan dust, may lead to improved satellite PAR estimates.

Ground-based high resolution observations of downward longwave irradiance (DLI), surface air temperature, water vapor surface partial pressure and column amount, zenith sky infrared (IR) radiance in the atmospheric window, and all-sky camera images are regularly obtained at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5° N, 68.8° W), northwestern Greenland. The datasets for the years 2017 and 2018 have been used to assess the performance of different empirical formulas used to infer clear sky DLI. An algorithm to identify clear sky observations has been developed, based on value, variability, and persistence of zenith sky IR radiance. Seventeen different formulas to estimate DLI have been tested against the THAAO dataset, using the originally determined coefficients. The formulas that combine information on total column water vapor and surface air temperature appear to perform better than others, with a mean bias with respect to the measured DLI smaller than 1 W m−2 and a root mean squared error (RMSE) around 6 W m−2. Unexpectedly, some formulas specifically developed for the Arctic are found to produce poor statistical results. This is attributed partly to limitations in the originally used dataset, which does not cover a whole year or is relative to very specific condition (i.e., the presence of an ice sheet). As expected, the bias displays a significant improvement when the coefficients of the different formulas are calculated using the THAAO dataset. The presence of 2 full years of data allows the determination and the applicability of the coefficients for singular years and the evaluation of results. The smallest values of the bias and RMSE reach 0.1 and 5 W m−2, respectively. Overall, the best results are found for formulas that use both surface parameters and total water vapor column content, and have been developed from global datasets. Conversely, formulas that express the atmospheric emissivity as a linear function of the logarithm of the column integrated water vapor appear to reproduce poorly the observations at THAAO.

The Arctic climate is influenced by the interaction of shortwave (SW) and longwave (LW) radiation with the atmosphere and the surface. The comprehensive evolution of the Surface Radiative Fluxes (SRF) on different time scales is of paramount importance to understanding the complex mechanisms governing the Arctic climate. However, only a few sites located in the Arctic region provide long-term time series of SRF allowing for capturing of the seasonality of atmospheric and surface parameters and for carrying out validation of satellite products and/or reanalyses. This paper presents the daily and monthly SRF record collected at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5∘ N, 68.8∘ W), in North-Western Greenland. The downwelling components of the SW (DSI) and the LW (DLI) irradiances have been measured at THAAO since 2009, whereas the collection of the upwelling SW (USI) and LW (ULI) irradiance was started in 2016, together with additional measurements, such as meteorological parameters and column water vapour. The datasets of DSI (Meloni et al., 2022a; https://doi.org/10.13127/thaao/dsi), USI (Meloni et al., 2022b; https://doi.org/10.13127/thaao/usi), DLI (Meloni et al., 2022c; https://doi.org/10.13127/thaao/dli), ULI (Meloni et al., 2022d; https://doi.org/10.13127/thaao/uli), and near-surface air temperature (Muscari et al., 2018; https://doi.org/10.13127/thaao/met), can be accessed through the THAAO web site (https://www.thuleatmos-it.it/data, last access: 16 January 2024). The DSI is absent (solar zenith angle ≥90∘) from 29 October to 13 February, assuming maxima in June (monthly mean of 277.0 Wm−2), when it is about half of the total incoming irradiance. The USI maximum occurs in May (132.4 Wm−2) owing to the combination of moderately high DSI values and high albedo. The shortwave surface albedo (A) assumes an average of 0.16 during summer, when the surface is free of snow. Differently, during months of snow-covered surface, when solar radiation allows A to be estimated, its values are greater than 0.6. A large interannual variability is observed in May and September, months characterized by rapidly changing surface conditions, having a link with air temperature anomalies. The DLI and ULI maxima occur in July and August, and the minima in February and March. ULI is always larger than DLI and shows a wider annual cycle. ULI is well described by a fourth-order polynomial fit to the air temperature (R2>0.99 for monthly data and R2>0.97 for daily data). The Surface Radiation Budget (SRB) is positive from April to August, when absorption of solar radiation exceeds the infrared net cooling, with a maximum value of 153.2 Wm−2 in June. From November to February, during the polar night, the LW net flux varies between −34.5 and −43.0 Wm−2. In March and September, the negative LW net flux overcomes the positive SW contribution, producing a negative SRB. The THAAO measurements show clear evidence of the influence of several regional weather/climate events, that appear strongly linked with SRF anomalies. These anomalies were found, for example, during summer 2012, when a large ice melting event took place over Greenland, and during winter 2019–2020, which was extraordinarily cold in the Arctic region.

Ocean surface radiation measurement best practices have been developed as a first step to support the interoperability of radiation measurements across multiple ocean platforms and between land and ocean networks. This document describes the consensus by a working group of radiation measurement experts from land, ocean, and aircraft communities. The scope was limited to broadband shortwave (solar) and longwave (terrestrial infrared) surface irradiance measurements for quantification of the surface radiation budget. Best practices for spectral measurements for biological purposes like photosynthetically active radiation and ocean color are only mentioned briefly to motivate future interactions between the physical surface flux and biological radiation measurement communities. Topics discussed in these best practices include instrument selection, handling of sensors and installation, data quality monitoring, data processing, and calibration. It is recognized that platform and resource limitations may prohibit incorporating all best practices into all measurements and that spatial coverage is also an important motivator for expanding current networks. Thus, one of the key recommendations is to perform interoperability experiments that can help quantify the uncertainty of different practices and lay the groundwork for a multi-tiered global network with a mix of high-accuracy reference stations and lower-cost platforms and practices that can fill in spatial gaps.

The present work describes the implementation of the state of the art Cloud-J v7.3 photolysis rate calculation code in the EMEP MSC-W chemistry-transport model. Cloud-J calculates photolysis rates and accounts for cloud and aerosol optical properties at model run time, replacing the old system based on tabulated values. The performance of Cloud-J is evaluated against aerial photolysis rate observations made over the Pacific Ocean and against surface observations from three measurement sites in Europe. Numerical experiments are performed to investigate the sensitivity of the calculated photolysis rates to the spatial and temporal model resolution, input meteorology model, simulated ozone column, and cloud effect parameterization. These experiments indicate that the calculated photolysis rates are most sensitive to the choice of input meteorology model and cloud effect parameterization while also showing that surface ozone photolysis rates can vary by up to 20 % due to daily variations in total ozone column. Further analysis investigates the impact of Cloud-J on the oxidizing capacity of the troposphere, aerosol–photolysis interactions, and surface air quality predictions. Results find that the annual mean mass-weighted tropospheric hydroxyl concentration is increased by 26 %, while the photolytic impact of aerosols is mostly limited to large tropical biomass-burning regions. Overall, Cloud-J represents a major improvement over the tabulated system, leading to improved model performance for predicting carbon monoxide and daily maximum ozone surface concentrations.

An international team of researchers finds high potential for improving climate projections by a more comprehensive treatment of largely ignored Arctic vegetation types, underscoring the importance of Arctic energy exchange measuring stations.

This paper presents the results of simultaneous high time-resolution measurements of biogenic aerosol (methane sulfonic acid (MSA), non-sea salt sulfate nssSO42-) with its gaseous precursor dimethylsulfide (DMS), performed at the Italian coastal base Mario Zucchelli Station (MZS) in Terra Nova Bay (MZS) during two summer campaigns (2018–2019 and 2019–2020). Data on atmospheric DMS concentration are scarce, especially in Antarctica. The DMS maximum at MZS occurs in December, one month earlier than at other Antarctic stations. The maximum of DMS concentration is connected with the phytoplanktonic senescent phase following the bloom of Phaeocystis antarctica that occurs in the polynya when sea ice opens up. The second plankton bloom occurs in January and, despite the high dimethylsufoniopropionate (DMSP) concentration in seawater, atmospheric DMS remains low, probably due to its fast biological turnover in seawater in this period. The intensity and timing of the DMS evolution during the two years suggest that only the portion of the polynya close to the sampling site produces a discernible effect on the measured DMS. The closeness to the DMS source area and the occurrence of air masses containing DMS and freshly formed oxidation products allow us to study the kinetic of biogenic aerosol formation and the reliable derivation of the branch ratio between MSA and nssSO42- from DMS oxidation that is estimated to be 0.84±0.06. Conversely, for aged air masses with low DMS content, an enrichment of nssSO42- with respect to MSA, is observed. We estimate that the mean contribution of freshly formed biogenic aerosol to PM10 is 17 % with a maximum of 56 %. The high contribution of biogenic aerosol to the total PM10 mass in summer in this area highlights the dominant role of the polynya on biogenic aerosol formation. Finally, due to the regional and year-to-year variability of DMS and related biogenic aerosol formation, we stress the need for long-term measurements of seawater and atmospheric DMS and biogenic aerosol along the Antarctic coast and in the Southern Ocean.

The impact of the aerosol optical properties on the ultraviolet index (UVI) in the urban area of Rome is investigated in this study. In particular, the influence of aerosol optical depth (AOD) and single scattering albedo (SSA), estimated at the wavelength of 340 nm, and of the Ångström exponent, calculated in the range 340–500 nm, over a period of 11 years (2010–2020) in the months from March to September are analyzed. The UVI is monitored by a Brewer spectrophotometer, whereas measurements of the direct Sun and diffuse sky irradiances are performed by a co-located PREDE-POM sun–sky radiometer of the ESR/SKYNET network; the aerosol optical properties are obtained by the Skyrad MRIv2 retrieval. A novel method, based on physical principles and easily adaptable to other contexts, is developed to extrapolate the aerosol properties to the UV range during periods when only visible to near-infrared measurements are available. The retrievals from the sun–sky radiometer are consistent with the chemical characterization of urban PM10 (particulate matter 10 mm or less in diameter) samples collected during an intensive field campaign held in summer 2011 at the same site (URBan Sustainability Related to Observed and Monitored Aerosol – URBS ROMA). The PM macro components identified during the campaign are grouped in order to evaluate the contribution of the main macro sources (soil, sea, secondary inorganic, organics, and traffic) whose relative role is indeed expected to strongly affect the aerosol absorption capability. The surface forcing efficiency, calculated as the change in the UV index for a unit AOD variation, shows that AOD is the primary parameter affecting the surface irradiance under clear-sky conditions in Rome. SSA and the Ångström exponent are also identified as secondary influencing factors, i.e., the surface forcing efficiency is found to be greater for smaller zenith angles and for larger and more absorbent particles in the UV range (such as, e.g., mineral dust).

The short- and long-term variability of the surface spectral solar ultraviolet (UV) irradiance is investigated across Italy using high-quality ground-based measurements from three locations: Aosta (45.7∘ N, 7.4∘ E, 570 m a.s.l.), Rome (41.9∘ N, 12.5∘ E, 15 75 m a.s.l.), and Lampedusa (35.5∘ N, 12.6∘ E, 50 m a.s.l.). The three sites are characterized by different environmental conditions and represent almost the full latitudinal extent of the Italian territory. Data of two periods were analysed: 2006–2020 (all sites) and 1996–2020 (Rome only). The main objective of this study is to quantify the effect of the geopotential height (GPH) at 250 hPa on total ozone, and spectral irradiance at 307.5 and 324 nm. We first show that monthly anomalies in GPH, total ozone, and spectral irradiances are correlated amongst the three sites, suggesting that Italy is often affected by the same synoptical weather systems. We further find statistically significant anticorrelations between GPH and monthly anomalies in total ozone for all stations and months. Conversely, we identify positive correlations between GPH and monthly anomalies in spectral irradiance at 307.5 nm for most months. The influence of GPH on short-term variability also hold for long-term trends. For example, long-term changes in total ozone over the period 2006–2020 were associated with changes in GPH for all stations. This suggests that observed negative trends in total ozone were mainly driven by changes in lower-stratospheric ozone as upper-stratospheric ozone was increasing over this period. For several months of the year, positive trends in UV irradiance were observed, and we found that these trends were predominantly caused by changes in clouds and/or aerosols instead of total ozone. For the longer period of 1996–2020, a statistically significant annualized decrease in total ozone of ∼ 0.1 % per year was identified for Rome and could subsequently be attributed to decreasing lower-stratospheric ozone. While positive trends in spectral irradiance at 307.5 nm were observed for several months of this extended period, the negative trend in total ozone did not lead to a positive trend in the spectral irradiance at 307.5 nm in the deseasonalized data. Our study provides evidence that dynamical processes taking place in the troposphere lead to significant variability in total ozone and surface solar UV irradiance.

Atmospheric fluxes of dissolved organic matter (DOM) were studied for the first time on the island of Lampedusa, a remote site in the central Mediterranean Sea (Med Sea), between 19 March 2015 and 1 April 2017. The main goals of this study were to quantify total atmospheric deposition of DOM in this area and to evaluate the impact of Saharan dust deposition on DOM dynamics in the surface waters of the Mediterranean Sea. Our data show high variability in DOM deposition rates without a clear seasonality and a dissolved organic carbon (DOC) input from the atmosphere of 120.7 mmol DOC m−2 yr−1. Over the entire time series, the average dissolved organic phosphorus (DOP) and dissolved organic nitrogen (DON) contributions to the total dissolved pools were 40 % and 26 %, respectively. The data on atmospheric elemental ratios also show that each deposition event is characterized by a specific elemental ratio, suggesting a high variability in DOM composition and the presence of multiple sources. This study indicates that the organic substances transported by Saharan dust on Lampedusa mainly come from a natural sea spray and that Saharan dust can be an important carrier of organic substances even though the load of DOC associated with dust is highly variable. Our estimates suggest that atmospheric input has a larger impact on the Med Sea than on the global ocean. Further, DOC fluxes from the atmosphere to the Med Sea can be up to 6 times larger than total river input. Longer time series combined with modeling would greatly improve our understanding of the response of DOM dynamics in the Med Sea to the change in aerosol deposition pattern due to the effect of climate change.

Since May 2022, the Mediterranean Sea has been experiencing an exceptionally long marine heatwave event. Warm anomalies, mainly occurring in the Western basin, have persisted until boreal spring 2023, making this event the longest Mediterranean marine heat wave of the last four decades. In this work, the 2022/2023 anomaly is characterized, using in-situ and satellite measurements, together with state of the art reanalysis products. The role of atmospheric forcing is also investigated; the onset and growth of sea surface temperature anomalies is found to be related to the prevalence of anticyclonic conditions in the atmosphere, which have also caused severe droughts in the Mediterranean region over the same period. Analysis of in-situ observations from the Lampedusa station and of ocean reanalyzes reveals that wind-driven vertical mixing led to the penetration of the warm anomalies below the sea surface, where they have persisted for several months, particularly in the central part of the basin. The evolution of the 2022/23 event is compared with the severe 2003 event, to put recent conditions in the context of climate change.

Measurements of aerosol composition and size distributions were taken during the summer of 2013 at the remote island of Lampedusa in the southern central Mediterranean Sea. These measurements were part of the ChArMEx/ADRIMED (Chemistry and Aerosol Mediterranean Experiment/Aerosol Direct Radiative Forcing on the Mediterranean Climate) framework and took place during Special Observation Period 1a (SOP-1a) from 11 June to 5 July 2013. From compact time-of-flight aerosol mass spectrometer (cToF-AMS) measurements in the size range below 1 µm in aerodynamic diameter (PM1), particles were predominately comprised of ammonium and sulfate. On average, ammonium sulfate contributed 63 % to the non-refractory PM1 mass, followed by organics (33 %). The organic aerosol was generally very highly oxidized (f44 values were typically between 0.25 and 0.26). The contribution of ammonium sulfate was generally higher than organic aerosol in comparison to measurements taken in the western Mediterranean but is consistent with studies undertaken in the eastern basin. Source apportionment of organics using a statistical (positive matrix factorization) model revealed four factors: a hydrocarbon-like organic aerosol (HOA), a methanesulfonic-acid-related oxygenated organic aerosol (MSA-OOA), a more oxidized oxygenated organic aerosol (MO-OOA) and a less oxidized oxygenated organic aerosol (LO-OOA). The MO-OOA was the dominant factor for most of the campaign (53 % of the PM1 OA mass). It was well correlated with SO42-, highly oxidized and generally more dominant during easterly air masses originating from the eastern Mediterranean and central Europe. The LO-OOA factor had a very similar composition to the MO-OOA factor but was more prevalent during westerly winds, with air masses originating from the Atlantic Ocean, the western Mediterranean and at high altitudes over France and Spain from mistral winds. The MSA-OOA factor contributed an average 12 % to the PM1 OA and was more dominant during the mistral winds. The HOA, representing observed primary organic aerosol, only contributed 8 % of the average PM1 OA during the campaign. Even though Lampedusa is one of the most remote sites in the Mediterranean, PM1 concentrations (10 ± 5 µg m−3) were comparable to those observed in coastal cities and sites closer to continental Europe. Cleaner conditions corresponded to higher wind speeds. Nucleation and growth of new aerosol particles was observed during periods of north-westerly winds. From a climatology analysis from 1999 to 2012, these periods were much more prevalent during the measurement campaign than during the preceding 13 years. These results support previous findings that highlight the importance of different large-scale synoptic conditions in determining the regional and local aerosol composition and oxidation and also suggest that a non-polluted surface atmosphere over the Mediterranean is rare.

Measurements of global and diffuse photosynthetically active radiation (PAR) have been carried out on the island of Lampedusa, in the central Mediterranean Sea, since 2002. PAR is derived from observations made with multi-filter rotating shadowband radiometers (MFRSRs) by comparison with a freshly calibrated PAR sensor and by relying on the on-site Langley plots. In this way, a long-term calibrated record covering the period 2002–2016 is obtained and is presented in this work. The monthly mean global PAR peaks in June, with about 160 W m−2, while the diffuse PAR reaches 60 W m−2 in spring or summer. The global PAR displays a clear annual cycle with a semi amplitude of about 52 W m−2. The diffuse PAR annual cycle has a semi amplitude of about 12 W m−2. A simple method to retrieve the cloud-free PAR global and diffuse irradiances in days characterized by partly cloudy conditions has been implemented and applied to the dataset. This method allows retrieval of the cloud-free evolution of PAR and calculation of the cloud radiative effect, CRE, for downwelling PAR. The cloud-free monthly mean global PAR reaches 175 W m−2 in summer, while the diffuse PAR peaks at about 40 W m−2. The cloud radiative effect, CRE, on global and diffuse PAR is calculated as the difference between all-sky and cloud-free measurements. The annual average CRE is about −14.7 W m−2 for the global PAR and +8.1 W m−2 for the diffuse PAR. The smallest CRE is observed in July, due to the high cloud-free condition frequency. Maxima (negative for the global, and positive for the diffuse component) occur in March–April and in October, due to the combination of elevated PAR irradiances and high occurrence of cloudy conditions. Summer clouds appear to be characterized by a low frequency of occurrence, low altitude, and low optical thickness, possibly linked to the peculiar marine boundary layer structure. These properties also contribute to produce small radiative effects on PAR in summer. The cloud radiative effect has been deseasonalized to remove the influence of annual irradiance variations. The monthly mean normalized CRE for global PAR can be well represented by a multi-linear regression with respect to monthly cloud fraction, cloud top pressure, and cloud optical thickness, as determined from satellite MODIS observations. The behaviour of the normalized CRE for diffuse PAR can not be satisfactorily described by a simple multi-linear model with respect to the cloud properties, due to its non-linear dependency, in particular on the cloud optical depth. The analysis suggests that about 77 % of the global PAR interannual variability may be ascribed to cloud variability in winter.

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.

Particulate matter with aerodynamic diameters lower than 10 µm, (PM10) aerosol samples were collected during summer 2013 within the framework of the Chemistry and Aerosol Mediterranean Experiment (ChArMEx) at two sites located north (Capo Granitola) and south (Lampedusa Island), respectively, of the main Mediterranean shipping route in the Straight of Sicily. The PM10 samples were collected with 12 h time resolutions at both sites. Selected metals, main anions, cations and elemental and organic carbon were determined. The evolution of soluble V and Ni concentrations (typical markers of heavy fuel oil combustion) was related to meteorology and ship traffic intensity in the Straight of Sicily, using a high-resolution regional model for calculation of back trajectories. Elevated concentration of V and Ni at Capo Granitola and Lampedusa are found to correspond with air masses from the Straight of Sicily and coincidences between trajectories and positions of large ships; the vertical structure of the planetary boundary layer also appears to play a role, with high V values associated with strong inversions and a stable boundary layer. The V concentration was generally lower at Lampedusa than at Capo Granitola V, where it reached a peak value of 40 ng m−3. Concentrations of rare earth elements (REEs), La and Ce in particular, were used to identify possible contributions from refineries, whose emissions are also characterized by elevated V and Ni amounts; refinery emissions are expected to display high La ∕ Ce and La ∕ V ratios due to the use of La in the fluid catalytic converter systems. In general, low La ∕ Ce and La ∕ V ratios were observed in the PM samples. The combination of the analyses based on chemical markers, air mass trajectories and ship routes allows us to unambiguously identify the large role of the ship source in the Straight of Sicily. Based on the sampled aerosols, ratios of the main aerosol species arising from ship emission with respect to V were estimated with the aim of deriving a lower limit for the total ship contribution to PM10. The estimated minimum ship emission contributions to PM10 were 2.0 µg m−3 at Lampedusa and 3.0 µg m−3 at Capo Granitola, corresponding with 11 and 8.6 % of PM10, respectively.

We describe and implement a data selection algorithm aimed at identifying background atmospheric CO2 observations from in situ continuous measurements. Several selection criteria for detecting the background data have been developed and are currently used: the main objective of this work was to define a common methodology to extract the atmospheric background signal minimizing heterogeneities due to the use of different selection algorithms. The algorithm used in this study, (BaDS, Background Data Selection) was tested and optimized using data (from 2014 to 2018) from four Italian stations characterized by markedly different environmental conditions (i.e., mountain, coastal and marine): Plateau Rosa (PRS), Mt. Cimone (CMN), Capo Granitola (CGR) and Lampedusa (LMP). Their locations extend from the Alps to the central Mediterranean. The adopted algorithm proved to be effective in separating the local/regional from the background signal in the CO2 time series. About 6% of the data at LMP, 11% at PRS, 20–38% at CMN and 65% at CGR were identified as non-background. LMP and PRS can be used as reference sites for the central Mediterranean, while CMN and CGR were more impacted by regional sources and sinks. Finally, we discuss a possible application of BaDS screened data.

The present work describes the implementation of the state of the art Cloud- J v7.3 photolysis rate calculation code in the EMEP MSC-W chemistry-transport model. Cloud- J calculates photolysis rates and accounts for cloud and aerosol optical properties at model run time, replacing the old system based on tabulated values. The performance of Cloud- J is evaluated against aerial photolysis rate observations made over the Pacific Ocean and against surface observations from three measurement sites in Europe. Numerical experiments are performed to investigate the sensitivity of the calculated photolysis rates to the spatial and temporal model resolution, input meteorology model, simulated ozone column, and cloud effect parameterization. These experiments indicate that the calculated photolysis rates are most sensitive to the choice of input meteorology model and cloud effect parameterization while also showing that surface ozone photolysis rates can vary by up to 20 % due to daily variations in total ozone column. Further analysis investigates the impact of Cloud- J on the oxidizing capacity of the troposphere, aerosol–photolysis interactions, and surface air quality predictions. Results find that the annual mean mass-weighted tropospheric hydroxyl concentration is increased by 26 %, while the photolytic impact of aerosols is mostly limited to large tropical biomass-burning regions. Overall, Cloud- J represents a major improvement over the tabulated system, leading to improved model performance for predicting carbon monoxide and daily maximum ozone surface concentrations. [ABSTRACT FROM AUTHOR]