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Abstract. The CANOPEE project aims to better understand the biosphere–atmosphere exchanges of biogenic volatile organic compounds (BVOCs) in the case of Mediterranean ecosystems and the impact of in-canopy processes on the atmospheric chemical composition above the canopy. Based on an intensive field campaign, the objective of our work was to determine the chemical composition of the air inside a canopy as well as the net fluxes of reactive species between the canopy and the boundary layer. Measurements were carried out during spring 2012 at the field site of the Oak Observatory of the Observatoire de Haute Provence (O3HP) located in the southeast of France. The site is a forest ecosystem dominated by downy oak, Quercus pubescens Willd., a typical Mediterranean species which features large isoprene emission rates. Mixing ratios of isoprene, its degradation products methylvinylketone (MVK) and methacrolein (MACR) and several other oxygenated VOC (OxVOC) were measured above the canopy using an online proton transfer reaction mass spectrometer (PTR-MS), and fluxes were calculated by the disjunct eddy covariance approach. The O3HP site was found to be a very significant source of isoprene emissions, with daily maximum ambient concentrations ranging between 2–16 ppbv inside and 2–5 ppbv just above the top of the forest canopy. Significant isoprene fluxes were observed only during daytime, following diurnal cycles with midday net emission fluxes from the canopy ranging between 2.0 and 9.7 mg m−2 h1. Net isoprene normalized flux (at 30 °C, 1000 μmol quanta m−2 s−1) was estimated at 7.4 mg m−2 h−1. Evidence of direct emission of methanol was also found exhibiting maximum daytime fluxes ranging between 0.2 and 0.6 mg m−2 h−1, whereas flux values for monoterpenes and others OxVOC such as acetone and acetaldehyde were below the detection limit. The MVK+MACR-to-isoprene ratio provided useful information on the oxidation of isoprene, and is in agreement with recent findings proposing weak production yields of MVK and MACR, in remote forest regions where the NOx concentrations are low. In-canopy chemical oxidation of isoprene was found to be weak and did not seem to have a significant impact on isoprene concentrations and fluxes above the canopy.

Abstract. The ChArMEx (Chemistry and Aerosols Mediterranean Experiments) SOP2 (special observation period 2) field campaign took place from 15 July to 5 August 2013 in the western Mediterranean Basin at Ersa, a remote site in Cape Corse. During the campaign more than 80 volatile organic compounds (VOCs), including oxygenated species, were measured by different online and offline techniques. At the same time, an exhaustive description of the chemical composition of fine aerosols was performed with an aerosol chemical speciation monitor (ACSM). Low levels of anthropogenic VOCs (typically tens to hundreds of parts per trillion for individual species) and black carbon (0.1-0.9 µg m −3 ) were observed, while significant levels of biogenic species (peaking at the ppb level) were measured. Furthermore, secondary oxygenated VOCs (OVOCs) largely dominated the VOC speciation during the campaign, while organic matter (OM) dominated the aerosol chemical composition, representing 55 % of the total mass of non-refractory PM 1 on average (average of 3.74 ± 1.80 µg m −3 ), followed by sulfate (27 %, 1.83 ± 1.06 µg m −3 ), ammonium (13 %, 0.90 ± 0.55 µg m −3 ) and nitrate (5 %, 0.31 ± 0.18 µg m −3 ).Positive matrix factorization (PMF) and concentration field (CF) analyses were performed on a database containing 42 VOCs (or grouped VOCs), including OVOCs, to idenPublished by Copernicus Publications on behalf of the European Geosciences Union. 8838V. Michoud et al.: Organic carbon at a remote site of the western Mediterranean Basin tify the covariation factors of compounds that are representative of primary emissions or chemical transformation processes. A six-factor solution was found for the PMF analysis, including a primary and secondary biogenic factor correlated with temperature and exhibiting a clear diurnal profile. In addition, three anthropogenic factors characterized by compounds with various lifetimes and/or sources have been identified (long-lived, medium-lived and short-lived anthropogenic factors). The anthropogenic nature of these factors was confirmed by the CF analysis, which identified potential source areas known for intense anthropogenic emissions (north of Italy and southeast of France). Finally, a factor characterized by OVOCs of both biogenic and anthropogenic origin was found. This factor was well correlated with submicron organic aerosol (OA) measured by an aerosol chemical speciation monitor (ACSM), highlighting the close link between OVOCs and organic aerosols; the latter is mainly associated (96 %) with the secondary OA fraction. The source apportionment of OA measured by ACSM led to a three-factor solution identified as hydrogenlike OA (HOA), semi-volatile oxygenated OA (SV-OOA) and low volatility OOA (LV-OOA) for averaged mass concentrations of 0.13, 1.59 and 1.92 µg m −3 , respectively.A combined analysis of gaseous PMF factors with inorganic and organic fractions of aerosols helped distinguish between anthropogenic continental and biogenic influences on the aerosol-and gas-phase compositions.

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Abstract:The objective of this work was to assess the yearly contribution of fossil fuel combustion (BC ff ) and wood burning (BC wb ) to equivalent black carbon (eBC) concentrations, in Athens, Greece. Measurements were conducted at a suburban site from March 2013 to February 2014 and included absorption coefficients at seven wavelengths and PM 2.5 chemical composition data for key biomass burning markers, i.e., levoglucosan, potassium (K) and elemental and organic carbon (EC, OC). A well-documented methodology of corrections for aethalometer attenuation coefficients was applied with a resulting annual dataset of derived absorption coefficients for the suburban Athens' atmospheric aerosol. The Aethalometer model was applied for the source apportionment of eBC. An optimum Ångström exponent for fossil fuel (α ff ) was found, based on the combined use of the model with levoglucosan data. The measured eBC concentrations were equal to 2.4 ± 1.0 µg m −3 and 1.6 ± 0.6 µg m −3 , during the cold and the warm period respectively. The contribution from wood burning was significantly higher during the cold period (21 ± 11%, versus 6 ± 7% in the warm period). BC ff displayed a clear diurnal pattern with a morning peak between 8 and 10 a.m. (during morning rush hour) and a second peak during the evening and night hours, due to the shallowing of the mixing layer. Regression analysis between BC wb concentrations and biomass burning markers (levoglucosan, K and OC/EC ratio) supported the validity of the results.

Abstract. Total OH reactivity, defined as the total loss frequency of the hydroxyl radical in the atmosphere, has proved to be an excellent tool to identify the total loading of reactive species in ambient air. High levels of unknown reactivity were found in several forests worldwide and were often higher than at urban sites.Our study presents atmospheric mixing ratios of biogenic compounds and total OH reactivity measured during late spring 2014 at the forest of downy oak trees of the Observatoire de Haute Provence (OHP), France. Air masses were sampled at two heights: 2 m, i.e., inside the canopy, and 10 m, i.e., above the canopy, where the mean canopy height is 5 m.We found that the OH reactivity at the site mainly depended on the main primary biogenic species emitted by the forest, which was isoprene and to a lesser extent by its degradation products and long-lived atmospheric compounds (up to 26 % during daytime). During daytime, no significant missing OH reactivity was reported at the site, either inside or above the canopy. However, during two nights we determined a missing fraction of OH reactivity up to 50 %, possibly due to unmeasured oxidation products. We confirmed that no significant oxidation of the primary species occurred within the canopy; primary compounds emitted by the forest were fast transported to the atmosphere. Finally, the OH reactivity at this site was maximum 69 s−1, which is a high value for a forest characterized by a temperate climate. Observations in various and diverse forests in the Mediterranean region are therefore needed to better constrain the impact of reactive gases over this area.

Understanding the role of short-lived climate forcers such as black carbon (BC) at high northern latitudes in climate change is hampered by the scarcity of surface observations in the Russian Arctic. In this study, highly time-resolved Equivalent BC (EBC) measurements during a ship campaign in the White, Barents, and Kara Seas in October 2015 are presented. The measured EBC concentrations are compared with BC concentrations simulated with a Lagrangian particle dispersion model coupled with a recently completed global emission inventory to quantify the origin of the Arctic BC. EBC showed increased values (100-400 ng m) in the Kara Strait, Kara Sea, and Kola Peninsula and an extremely high concentration (1000 ng m) in the White Sea. Assessment of BC origin throughout the expedition showed that gas-flaring emissions from the Yamal-Khanty-Mansiysk and Nenets-Komi regions contributed the most when the ship was close to the Kara Strait, north of 70° N. Near Arkhangelsk (White Sea), biomass burning in mid-latitudes, surface transportation, and residential and commercial combustion from Central and Eastern Europe were found to be important BC sources. The model reproduced observed EBC concentrations efficiently, building credibility in the emission inventory for BC emissions at high northern latitudes.

Abstract. The scope of this study was to estimate the contribution of fossil fuel and wood burning combustion to black carbon (BC) and carbon monoxide (CO) during wintertime, in Athens. For that purpose, in situ measurements of equivalent black carbon (eBC) and CO were simultaneously conducted in a suburban and an urban background monitoring site in Athens during the 3 months of winter 2014-2015. For the deconvolution of eBC into eBC emitted from fossil fuel (BC ff ) and wood burning (BC wb ), a method based on the spectral dependency of the absorption of pure black carbon and brown carbon was used. Thereafter, BC wb and BC ff estimated fractions were used along with measured CO concentrations in a multiple regression analysis, in order to quantify the contribution of each one of the combustion sources to the ambient CO levels. For a comparative analysis of the results, we additionally estimated the wood burning and fossil fuel contribution to CO, calculated on the basis of their CO / NO x emission ratios. The results indicate that during wintertime BC and CO are mainly emitted by local sources within the Athens Metropolitan Area (AMA). Fossil fuel combustion, mainly from road traffic, is found to be the major contributor to both eBC in PM 2.5 and CO ambient concentrations in AMA. However, wintertime wood burning makes a significant contribution to the observed eBC (of about 30 %) and CO concentrations (on average, 11 and 16 % of total CO in the suburban and urban background sites respectively). Both BC and CO from biomass burning (BC wb and CO wb , respectively) present a clear diurnal pattern, with the highest concentrations during night-time, supporting the theory of local domestic heating being their main source.