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1. Field measurements of organic and inorganic composition in the Rambouillet Forest during ACROSS campaign

Author: Fanny Bachelier, Chaoyang Xue, Jérôme Houny, Max McGillen, Alexandre Kukui, Benoit Grosselin, Abdelwahid Mellouki, and Véronique Daële
Abstract: Rambouillet Forest is a large forested location, situated about 50km from central Paris. It covers some 200km² and contains mainly a mix of oak and pine trees. Its size and proximity towards Paris makes it an interesting site to study the interaction between polluted air masses and biogenic emissions and the impact on air quality in areas surrounding polluted cities. The ACROSS (Atmospheric ChemistRy Of the Suburban forest) campaign represents a large international collaboration between various French, European and American institutes, which aims to further characterize these interactions. For our contribution, different instruments from ICARE and LPC2E CNRS Orléans performed in-situ measurements in this forest during June and July of 2022, including: VOCs/ BVOCs (GC-MS/FID); oxidants (OH radicals, CIMS); oxidant precursors (NOx, NOy, Ecophysics, CAPS, LOPAP); and highly oxidized products (orbitrap). In general, data coverage for all instrumentation was high throughout the campaign, furthermore this instrumentation was calibrated and characterized under field condition where possible. These observations represent a broad look at the composition of the forested environment, and contain information on organic emissions, their oxidized products, oxidants and oxidant precursors. We therefore anticipate that these measurements will contribute significantly to the understanding of the atmospheric chemistry operating during the ACROSS campaign.
Published: 2023
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2. Report on selected measurements in the canopy of a Rambouillet forest site during the ACROSS field campaign

Author: Alexandre Kukui, Chaoyang Xue, Jérôme Houny, Max Mcgillen, Fanny Bachelier, Benoit Grosselin, Véronique Daële, and Wahid Mellouki
Abstract: In this contribution we report on a subset of ground-based measurements performed by LPC2E and ICARE at a forest site of Rambouillet during June-July of 2022 in the frame of the project ACROSS (Atmospheric ChemistRy Of the Suburban foreSt). In particular, we present the following time-concentration profiles:- OH and sum of peroxy radicals (CIMS , LPC2E);- gaseous H2SO4 (CIMS, LPC2E);- large number of volatile organic compounds (VOCs) and their oxidation products, including N-containing oxygenated organic molecules (OOMs) (Orbitrap High Resolution CIMS, LPC2E);- directly emitted VOCs and their oxidation products measured by GC-MS/FID (ICARE)- HONO (LOPAP, ICARE)- NO and NO2 (ICARE)Based on a first analysis of this reduced data-set some preliminary conclusions are made about an influence of VOCs emissions and NOx variability on the composition of OOMs oxidation products, HONO formation and oxidation capacity in the forest canopy.
Published: 2023
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3. Observations of trace gases above & below a forest canopy during ACROSS

Author: Sébastien Dusanter, Joel de Brito, Ahmad Lahib, Alexandre Tomas, Marina Jamar, Estephanie Alhajj Moussa, Astrid Bauville, Christopher Cantrell, Vincent Michoud, Mathieu Cazaunau, Paola Formenti, Fanny Bachelier, Benoit Grosselin, Max McGillen, Veronique Daele, Wahid Mellouki, Chaoyang Xue, Jérôme Houny, and Alexandre Kukui
Abstract: The ACROSS campaign (Atmospheric chemistry of the suburban forest) is a collaborative effort to better understand how the mixing between urban and biogenic air masses impacts atmospheric composition and reactivity. A main objective is to provide a detailed description of physico-chemical processes involved in atmospheric transformations of biogenic Volatile Organic Compounds (VOCs), and the myriad of intermediate species formed as a consequence, which have yet to be characterized. This multi-platform campaign took place during summer 2022 for a duration of 6 weeks and included a supersite in the Rambouillet forest located on the path of pollution plumes from Paris. An unprecedented suite of analytical instruments was deployed at this site to probe air masses at the ground level and above the forest canopy using a 40-m tower.This presentation will focus on trace gas observations, including VOCs, ROx (OH+HO2+RO2) and selected inorganic species (O3, NOx – NO+NO2), both above and below the forest canopy. A descriptive analysis will be presented to highlight biogenic VOC oxidation regimes taking place under unpolluted (oceanic air masses) and polluted (Paris plumes) conditions, with a focus on primary/secondary species. Chemical compositions observed above and below-canopy will also be contrasted. On the basis of these observations, this presentation will highlight scientific questions related to ROx, VOC and NOx budgets that will be further investigated to fill important gaps in our understanding of biogenic VOC transformations and secondary organic aerosol formation. Acknowledgments. This work is supported by the French national research agency (ANR-20-CE01-0010) & LABEX-CaPPA (ANR-11-LABX-005-01) and the French national program LEFE/CHAT INSU.
Published: 2023
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4. Supplementary material to 'Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions'

Author: Valérie Gros, Karine Sellegri, Michel Chartier, Thierry Bourrianne, Hui Chen, Sebastien Dusanter, Alexandre Kukui, Vincent Michoud, Stéphane Sauvage, Jinhe Wang, Jean-Marc Pichon, and Nadine Locoge
Subjects: Mediterranean climate, chemistry.chemical_compound, chemistry, Environmental chemistry, Cape, Biogenic emissions, Environmental science, Sulfuric acid
Published: 2021
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5. Shedding light on tropospheric H2SO4 production from Criegee intermediates + SO2: a comprehensive laboratory chamber study using the highly instrumented HELIOS platform

Author: Max R. McGillen, Abdelwahid Mellouki, Alexandre Kukui, Véronique Daële, Yangang Ren, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National d’Études Spatiales [Paris] (CNES), interaction Clouds Aerosols Radiations - ICARE/AERIS Data and Services Center - UMS 2877 (ICARE), Centre National de la Recherche Scientifique (CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Université de Lille, ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), and Centre National d'Études Spatiales [Toulouse] (CNES)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Troposphere, 13. Climate action, Environmental science, HeliOS, Laboratory chamber, Atmospheric sciences, 7. Clean energy, ComputingMilieux_MISCELLANEOUS
Abstract: Although the dominant source of H2SO4 in the atmosphere is generally considered to be the reaction of SO2 with OH, it is probable that the rapid reactions of Criegee intermediates (CIs) with SO2 can contribute significantly to the tropospheric H2SO4 budget under certain conditions. CIs are produced from alkene ozonolysis, and the vast quantities of unsaturated biogenic and anthropogenic volatile organic compounds emitted could provide a large and diverse flux of CIs to the atmosphere. There remain several key uncertainties regarding the global importance of CIs towards SO2 oxidation, which are principally related to the ambient concentrations of CIs and the competition between CI reaction with SO2 against the many other bimolecular and unimolecular loss processes. This is especially true of the larger, more complex CIs that are produced from terpene ozonolysis.We present experimental studies of the ozonolysis of tetramethylethylene, α-pinene and limonene, using the HELIOS chamber. HELIOS is a highly instrumented large-scale outdoor atmospheric simulation chamber and consists of a hemispheric 90 m3 Teflon-foil reactor, which is interfaced to a variety of on-line measurements including FTIR, PTR-ToF-MS, FIGAERO-ToF-CIMS, OH/H2SO4-CIMS, Aerolaser HCHO, LOPAP and SMPS, together with several GC-MS/FID and LC-MS instruments and a suite of monitors (NO, NO2, O3). Equipped with this range of instrumentation we are able to conduct alkene ozonolysis under near-ambient conditions, whilst we also have a high coverage of key reactive species in the systems of interest.From our results, we are able to provide new information regarding kinetic and mechanistic behaviour of several atmospherically important CIs and their reactive intermediates, providing new constraints on the role of CIs on the tropospheric H2SO4 budget.Keywords: ozonolysis, Criegee Intermediate, sulfur dioxide, sulfuric acid, kinetics
Published: 2021
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6. Measurements and modeling of the spectral properties of sunlight at the irradiated volume and surface of an indoor environment: The impact on the oxidation capacity

Author: Gandolfo, A., Tlili, S., Chen, H., Alexandre Kukui, Durand, A., Temime-Roussel, B., Kleffmann, J., Wortham, H., Gligorovski, S., Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), University of Wuppertal, and KUKUI, Alexandre
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Architectural model, HONO photolysis frequencies, photochemistry, oxidative capacity, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, Irradiated volume, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2020

7. Impact of photocatalytic paints on indoor VOCs in a full-scale study: Focus on regulated and reactive compounds

Author: Gandolfo, A., Chen, H., Alexandre Kukui, Durand, A., Temime-Roussel, B., Kleffmann, J., Wortham, H., Gligorovski, S., Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), University of Wuppertal, and KUKUI, Alexandre
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, VOCs, TiO2, formaldehyde, Photocatalysis, ComputingMilieux_MISCELLANEOUS, PTR-ToF-MS
Abstract: International audience
Published: 2020

8. Evidence of atmospheric nanoparticle formation from emissions of marine microorganisms

Author: David Parin, Nicolas Marchand, Karine Sellegri, A.N. Schwier, Sébastien Mas, Jorge Pey, A. Culot, Barbara D'Anna, Bruno Charrière, Clémence Rose, Alexandre Kukui, Brice Temime-Roussel, Richard Sempéré, Alfonso Saiz-Lopez, Anoop S. Mahajan, and H. L. Dewitt
Subjects: 010504 meteorology & atmospheric sciences, Microorganism, Nucleation, Nanoparticle, Climate change, Pelagic zone, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Aerosol, Atmosphere, Geophysics, 13. Climate action, General Earth and Planetary Sciences, Particle, Environmental science, 14. Life underwater, 0105 earth and related environmental sciences
Abstract: Earth, as a whole, can be considered as a living organism emitting gases and particles into its atmosphere, in order to regulate its own temperature. In particular, oceans may respond to climate change by emitting particles that ultimately will inﬂuence cloud coverage. At the global scale, a large fraction of the aerosol number concentration is formed by nucleation of gas-phase species, but this process has never been directly observed above oceans. Here we present, using semicontrolled seawater-air enclosures, evidence that nucleation may occur from marine biological emissions in the atmosphere of the open ocean. We identify iodine-containing species as major precursors for new particle clusters’ formation, while questioning the role of the commonly accepted dimethyl sulﬁde oxidation products, in forming new particle clusters in the region investigated and within a time scale on the order of an hour. We further show that amines would sustain the new particle formation process by growing the new clusters to larger sizes. Our results suggest that iodine-containing species and amines are correlated to different biological tracers. These observations, if generalized, would call for a substantial change of modeling approaches of the sea-to-air interactions.
Published: 2016
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9. Atmospheric chamber measurements of H2SO4: characterization of formation and loss rates during the ozonolysis and aerosol formation studies

Author: Yangang Ren, Alexandre Kukui, Waed Ahmad, Francois Bernard, Joris Leglise, Li Zhou, Min Cai, Clara Coujou, Roland Benoit, Valéry Catoire, Véronique DAËLE, Wahid Mellouki, KUKUI, Alexandre, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere
Abstract: International audience; Sulphuric acid, H2SO4, has been identified to play major role in atmospheric new particle formation and in subsequent particle growth. The oxidation of sulfur dioxide (SO2) to sulfur trioxide (SO3) initiated by the reaction with the hydroxyl radicals (OH) is assumed to be the dominant formation pathway of sulfuric acid (H2SO4) in the troposphere. It has been suggested in the recent years that the reactions of Criegee Intermediates (CIs) with SO2 may also contribute to the H2SO4 formation, although the significance of this pathway compared to the reaction of OH with SO2 is still under discussion. As the ozonolysis of anthropogenic and biogenic terpenes emitted into the atmosphere may represent an important source of OH and CIs a better understanding of the ozonolysis mechanism in relation to the H2SO4 formation is required. In this study, we present the results obtained during the investigation of the ozonolysis of several unsaturated volatile organic compounds, including tetramethylethylene, α-pinene and limonene, using a newly constructed large atmospheric simulation chamber, HELIOS (ICARE-CNRS, Orléans, France). The HELIOS facility consists of a large outdoor simulation chamber (volume of 90 m3) equipped with a wide range of in-situ on-line and off-line analytical instrumentation (FTIR, PTR-TOF-MS, GC-MS, CIMS (OH and H2SO4), SMPS, Figaero-API-TOF-CIMS, HCHO monitor and others). The results of kinetic and mechanistic studies of the reactions of different CIs with SO2 induced by the ozonolysis of the studied VOCs under different conditions will be presented. The H2SO4 loss on the Teflon chamber wall and by the aerosol uptake were characterized using direct H2SO4 and particle measurements. Keywords: ozonolysis, Criegee Intermediate, sulfur dioxide, sulfuric acid, HELIOS
Published: 2019

10. Supplementary material to 'Field measurements of methylglyoxal using Proton Transfer Reaction-Time of Flight Mass Spectrometry and comparison to the DNPH/HPLC-UV method'

Author: Vincent Michoud, Stéphane Sauvage, Thierry Léonardis, Isabelle Fronval, Alexandre Kukui, Nadine Locoge, and Sébastien Dusanter
Published: 2018
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11. Field measurements of methylglyoxal using Proton Transfer Reaction-Time of Flight Mass Spectrometry and comparison to the DNPH/HPLC-UV method

Author: Vincent Michoud, Stéphane Sauvage, Thierry Léonardis, Isabelle Fronval, Alexandre Kukui, Nadine Locoge, and Sébastien Dusanter
Abstract: Methylglyoxal (MGLY) is an important atmospheric α-dicarbonyl species whose photolysis acts as a significant source of peroxy radicals, contributing to the oxidizing capacity of the atmosphere and, as such, the formation of secondary pollutants such as organic aerosols and ozone. However, despite its importance, only a few techniques exhibit time resolutions and detection limits that are suitable for atmospheric measurements. This study present, to the best of our knowledge, the first measurements of ambient MGLY using Proton Transfer Reaction-Time of Flight Mass Spectrometry (PTR-ToFMS). These measurements were performed during the ChArMEx SOP2 field campaign. This campaign took place at a Mediterranean site characterized by intense biogenic emissions and low levels of anthropogenic trace gases. Concomitant measurements of MGLY were performed using the 2,4-dinitrophenylhydrazine (DNPH) derivatization technique and High Performance Liquide Chromatography (HPLC) with UV detection. PTR-ToFMS and DNPH-HPLC measurements were compared to determine whether these techniques can perform reliable measurements of MGLY. Ambient time series revealed levels of MGLY ranging from 28–365 pptv, with a clear diurnal cycle due to elevated concentrations of primary biogenic species during daytime, whose oxidation led to large production rates of MGLY. A scatter plot of the PTR-ToFMS and DNPH-HPLC measurements indicates a reasonable correlation (R2 = 0.48) but a slope significantly lower than unity (0.58 ± 0.05) and a significant intercept of 88.3 ± 8.0 pptv. A careful investigation of the differences between the two techniques suggests that this disagreement is not due to spectrometric interferences from H3O+(H2O)3, MEK (or butanal) detected at m/z 73.050 and m/z 73.065, respectively, which are close to the MGLY m/z of 73.029. The differences are more likely due to uncorrected sampling artefacts such as overestimated collection efficiency or loss of MGLY into the sampling line for the DNPH-HPLC technique or unknown isobaric interfering compounds such as acrylic acid and propanediol for the PTR-ToFMS. Calculations of MGLY loss rates with respect to OH-oxidation and direct photolysis indicate similar contributions for these two loss pathways.
Published: 2018
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12. Atmospheric nitrogen oxides (NO and NO2) at Dome C, East Antarctica, during the OPALE campaign

Author: Joel Savarino, Martin D. King, S. Preunkert, Markus M. Frey, Michel Legrand, Howard K. Roscoe, and Alexandre Kukui
Subjects: Atmospheric Science, Ozone, Reactive nitrogen, Planetary boundary layer, Firn, Snow, Atmospheric sciences, Troposphere, chemistry.chemical_compound, chemistry, 13. Climate action, Atmospheric chemistry, Environmental science, NOx
Abstract: Mixing ratios of the atmospheric nitrogen oxides NO and NO2 were measured as part of the OPALE (Oxidant Production in Antarctic Lands & Export) campaign at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), during December 2011 to January 2012. Profiles of NOx mixing ratios of the lower 100 m of the atmosphere confirm that, in contrast to the South Pole, air chemistry at Dome C is strongly influenced by large diurnal cycles in solar irradiance and a sudden collapse of the atmospheric boundary layer in the early evening. Depth profiles of mixing ratios in firn air suggest that the upper snowpack at Dome C holds a significant reservoir of photolytically produced NO2 and is a sink of gas-phase ozone (O3). First-time observations of bromine oxide (BrO) at Dome C show that mixing ratios of BrO near the ground are low, certainly less than 5 pptv, with higher levels in the free troposphere. Assuming steady state, observed mixing ratios of BrO and RO2 radicals are too low to explain the large NO2 : NO ratios found in ambient air, possibly indicating the existence of an unknown process contributing to the atmospheric chemistry of reactive nitrogen above the Antarctic Plateau. During 2011–2012, NOx mixing ratios and flux were larger than in 2009–2010, consistent with also larger surface O3 mixing ratios resulting from increased net O3 production. Large NOx mixing ratios at Dome C arise from a combination of continuous sunlight, shallow mixing height and significant NOx emissions by surface snow (FNOx). During 23 December 2011–12 January 2012, median FNOx was twice that during the same period in 2009–2010 due to significantly larger atmospheric turbulence and a slightly stronger snowpack source. A tripling of FNOx in December 2011 was largely due to changes in snowpack source strength caused primarily by changes in NO3− concentrations in the snow skin layer, and only to a secondary order by decrease of total column O3 and associated increase in NO3− photolysis rates. A source of uncertainty in model estimates of FNOx is the quantum yield of NO3− photolysis in natural snow, which may change over time as the snow ages.
Published: 2015
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13. The fate of OH and RO2 radicals in presence of TiO2 nanoparticles embedded in paints

Author: Gandolfo, A., Chen, H., Alexandre Kukui, Durand, A., Temime-Roussel, B., Wortham, H., Gligorovski, S., KUKUI, Alexandre, Laboratoire Chimie de l'environnement (LCE), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, and Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 2018

14. Pressure Dependence of Butyl Nitrate Formation in the Reaction of Butylperoxy Radicals with Nitrogen Oxide

Author: Marie-Thérèse Rayez, Alexandre Kukui, G. Le Bras, N. I. Butkovskaya, Jean-Claude Rayez, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Institut des Sciences Moléculaires (ISM), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure de Chimie et de Physique de Bordeaux (ENSCPB)-Université Sciences et Technologies - Bordeaux 1-Université Montesquieu - Bordeaux 4-Institut de Chimie du CNRS (INC), ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), and ANR-12-BS06-0017,ONCEM,Chimie des nitrates organiques : sources, puits et impact sur le transport longue distance de l'azote réactif(2012)
Subjects: [PHYS]Physics [physics], chemistry.chemical_classification, Chemical ionization, 010304 chemical physics, Radical, Butyl nitrate, Inorganic chemistry, Analytical chemistry, 010402 general chemistry, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, chemistry, 13. Climate action, Torr, Yield (chemistry), 0103 physical sciences, Potential energy surface, [CHIM]Chemical Sciences, Physical and Theoretical Chemistry, Quadrupole mass analyzer, Alkyl
Abstract: International audience; The yield of 1- and 2-butyl nitrates in the gas-phase reactions of NO with n-C4H9O2 and sec-C4H9O2, obtained from the reaction of F atoms with n-butane in the presence of O2, was determined over the pressure range of 100–600 Torr at 298 K using a high-pressure turbulent flow reactor coupled with a chemical ionization quadrupole mass spectrometer. The yield of butyl nitrates was found to increase linearly with pressure from about 3% at 100 Torr to about 8% at 600 Torr. The results obtained are compared with the available data concerning nitrate formation from NO reaction with other small alkylperoxy radicals. These results are also discussed through the topology of the lowest potential energy surface mainly obtained from DFT(B3LYP/aug-cc-pVDZ) calculations of the RO2 + NO reaction paths. The formation of alkyl nitrates, due essentially to collision processes, is analyzed through a model that points out the pertinent physical parameters of this system.
Published: 2014
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15. Study of the unknown HONO daytime source at a European suburban site during the MEGAPOLI summer and winter field campaigns

Author: Sébastien Perrier, Charbel Afif, Matthias Beekmann, K. Miet, Markus Furger, Aurélie Colomb, Jean-Charles Dupont, Guillaume Siour, Martial Haeffelin, Alexandre Kukui, P. Zapf, Bernard Aumont, Jean-François Doussin, Vincent Michoud, Marie Camredon, Agnès Borbon, W. Ait-Helal, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Analytiques (ISA), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), Université Lille Nord (France), Centre d’Analyses et de Recherche, Centre d’Analyses et de Recherche - Lebanon, TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Paul Scherrer Institute (PSI), Institut Pierre-Simon-Laplace (IPSL), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), ANR-09-BLAN-0356,MEGAPOLI-PARIS,MEGAPOLI - PARIS : Pollution des AéRosols: Impact sur la qualité de l'air et quantification des Sources(2009), ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), European Project: 212520,EC:FP7:ENV,FP7-ENV-2007-1,MEGAPOLI(2008), European Project: 228335,EC:FP7:INFRA,FP7-INFRASTRUCTURES-2008-1,EUROCHAMP-2(2009), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Centre National de la Recherche Scientifique (CNRS)-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École normale supérieure - Lyon (ENS Lyon), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), École normale supérieure - Paris (ENS Paris)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National d'Études Spatiales [Toulouse] (CNES)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), ANR-10-LABX-100-01/10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), and École normale supérieure - Paris (ENS Paris)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, Daytime, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Wind direction, Noon, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, Wind speed, Aerosol, lcsh:Chemistry, lcsh:QD1-999, [SDU]Sciences of the Universe [physics], 13. Climate action, Photostationary state, [SDE]Environmental Sciences, Environmental science, Relative humidity, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Water content, lcsh:Physics, 0105 earth and related environmental sciences
Abstract: Nitrous acid measurements were carried out during the MEGAPOLI summer and winter field campaigns at SIRTA observatory in Paris surroundings. Highly variable HONO levels were observed during the campaigns, ranging from 10 ppt to 500 ppt in summer and from 10 ppt to 1.7 ppb in winter. Significant HONO mixing ratios have also been measured during daytime hours, comprised between some tenth of ppt and 200 ppt for the summer campaign and between few ppt and 1 ppb for the winter campaign. Ancillary measurements, such as NOx, O3, photolysis frequencies, meteorological parameters (pressure, temperature, relative humidity, wind speed and wind direction), black carbon concentration, total aerosol surface area, boundary layer height and soil moisture, were conducted during both campaigns. In addition, for the summer period, OH radical measurements were made with a CIMS (Chemical Ionisation Mass Spectrometer). This large dataset has been used to investigate the HONO budget in a suburban environment. To do so, calculations of HONO concentrations using PhotoStationary State (PSS) approach have been performed, for daytime hours. The comparison of these calculations with measured HONO concentrations revealed an underestimation of the calculations making evident a missing source term for both campaigns. This unknown HONO source exhibits a bell-shaped like average diurnal profile with a maximum around noon of approximately 0.7 ppb h−1 and 0.25 ppb h−1, during summer and winter respectively. This source is the main HONO source during daytime hours for both campaigns. In both cases, this source shows a slight positive correlation with J(NO2) and the product between J(NO2) and soil moisture. This original approach had, thus, indicated that this missing source is photolytic and might be heterogeneous occurring at ground surface and involving water content available on the ground., Atmospheric Chemistry and Physics, 14 (6), ISSN:1680-7375, ISSN:1680-7367
Published: 2014
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16. First investigations of IO, BrO, and NO2summer atmospheric levels at a coastal East Antarctic site using mode-locked cavity enhanced absorption spectroscopy

Author: Daniele Romanini, G. Méjean, Alexandre Kukui, Suzanne Preunkert, Michel Legrand, and Roberto Grilli
Subjects: Detection limit, Marine boundary layer, 010504 meteorology & atmospheric sciences, Absorption spectroscopy, Planetary boundary layer, East antarctica, Atmospheric sciences, 01 natural sciences, 010309 optics, Geophysics, 13. Climate action, 0103 physical sciences, General Earth and Planetary Sciences, Oxidative capacity, 14. Life underwater, Spectroscopy, Enhanced absorption, 0105 earth and related environmental sciences
Abstract: [1] IO, BrO, and NO2 were measured for the first time at Dumont d'Urville (East Antarctic coast) during summer 2011/2012 by using a near-UV-Visible laser spectrometer based on mode-locked cavity-enhanced absorption spectroscopy. IO mixing ratios ranged from the 2σ detection limit (0.04 pptv) up to 0.15 pptv. BrO remained close or below the detection limit (2 pptv) of the instrument. Daily averaged NO2 values ranged between the detection limit (10 pptv) and 60 pptv being far higher than levels of a few pptv commonly observed in the remote marine boundary layer. Data are discussed and compared with those available for another coastal Antarctic station (Halley, West Antarctica). It is shown that the oxidative capacity of the atmospheric boundary layer at coastal Antarctic sites is quite different in nature from West to East Antarctica, with the halogen chemistry being promoted at West and the OH chemistry at East.
Published: 2013
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17. Radical budget analysis in a suburban European site during the MEGAPOLI summer field campaign

Author: K. Miet, Markus Furger, Sébastien Perrier, Valérie Gros, Aurélie Colomb, Alexandre Kukui, Agnès Borbon, P. Zapf, Warda Ait-Helal, Nadine Locoge, Gérard Ancellet, Stéphane Sauvage, Matthias Beekmann, Jean-François Doussin, Marie Camredon, Guillaume Siour, Bernard Aumont, Charbel Afif, Vincent Michoud, R. Durand-Jolibois, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Analytiques (ISA), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Université Lille Nord (France), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), Centre for Materials and Processes (CERI MP - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Chimie Atmosphérique Expérimentale (CAE), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), Paul Scherrer Institute (PSI), ANR-09-BLAN-0356,MEGAPOLI-PARIS,MEGAPOLI - PARIS : Pollution des AéRosols: Impact sur la qualité de l'air et quantification des Sources(2009), European Project: 212520,EC:FP7:ENV,FP7-ENV-2007-1,MEGAPOLI(2008), European Project: 228335,EC:FP7:INFRA,FP7-INFRASTRUCTURES-2008-1,EUROCHAMP-2(2009), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Centre for Materials and Processes (CERI MP), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Centre National de la Recherche Scientifique (CNRS)-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École normale supérieure - Lyon (ENS Lyon), Génie Civil et Environnemental (GCE), and Université Paris-Saclay-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, Daytime, 010504 meteorology & atmospheric sciences, Meteorology, Chemistry, [SDE.MCG]Environmental Sciences/Global Changes, Radical, Diurnal temperature variation, Photodissociation, Analytical chemistry, 010501 environmental sciences, 01 natural sciences, lcsh:QC1-999, Dilution, lcsh:Chemistry, lcsh:QD1-999, 13. Climate action, Ionization, Mixing ratio, lcsh:Physics, NOx, 0105 earth and related environmental sciences
Abstract: Chemical Ionisation Mass Spectrometer measurements of hydroxyl radical (OH) and the sum of hydroperoxy and organic peroxy (HO2+RO2) radicals were conducted during the MEGAPOLI summer field campaign at the SIRTA observatory near Paris, France, in July 2009. OH and (HO2+RO2) showed a typical diurnal variation with averaged daytime maxima values around 5×106 and 1.2×108 molecule cm−3, respectively. Simultaneously, a large number of ancillary measurements, such as NOx, O3, HONO, HCHO and other VOCs were also conducted. These data provide an opportunity to assess our understanding of the radical chemistry in a suburban environment by comparing the radical observations to calculations. First, OH mixing ratios were estimated by a simple Photo Stationary State (PSS) calculation. PSS calculations overestimate the OH mixing ratio by 50%, especially at NOx mixing ratios lower than 10 ppb, suggesting that some loss processes were missing in the calculation at low NOx. Then, a photochemical box model simulation based on the Master Chemical Mechanism (MCM) and constrained by ancillary measurements was run to calculate radical concentrations. Three different modelling procedures were tested, varying the way the unconstrained secondary species were estimated, to cope with the unavoidable lack of their measurements. They led to significant differences in simulated radical concentrations. OH and (HO2+RO2) concentrations estimated by two selected model version were compared with measurements. These versions of the model were chosen because they lead, respectively, to the higher and lower simulated radical concentrations and are thus the two extremes versions. The box model showed better results than PSS calculations, with a slight overestimation of 12% and 5%, for OH and (HO2+RO2) respectively, in average for the reference model, and an overestimation of approximately 20% for OH and an underestimation for (HO2+RO2) for the other selected model version. Thus, we can conclude from our study that OH and (HO2+RO2) radical levels agree on average with observations within the uncertainty range. Finally, an analysis of the radical budget, on a daily basis (06:00–18:00 UTC), indicates that HONO photolysis (~35%), O3 photolysis (~23%), and aldehydes and ketones photolysis (~16% for formaldehyde and 18% for others) are the main radical initiation pathways. According to the MCM modelling, the reactions of RO2 with NO2 (~19%), leading mainly to PAN formation, is a significant termination pathway in addition to the main net loss via reaction of OH with NO2 (~50%).
Published: 2012
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18. Pressure and Temperature Dependence of Ethyl Nitrate Formation in the C2H5O2 + NO Reaction

Author: Georges Le Bras, N. I. Butkovskaya, Alexandre Kukui, Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS - CNRS), and Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Chemical ionization, 010504 meteorology & atmospheric sciences, [CHIM.ORGA]Chemical Sciences/Organic chemistry, Branching fraction, Analytical chemistry, 010402 general chemistry, Ethyl nitrate, Mass spectrometry, 01 natural sciences, 0104 chemical sciences, chemistry.chemical_compound, chemistry, 13. Climate action, Torr, Yield (chemistry), Physical and Theoretical Chemistry, 0105 earth and related environmental sciences
Abstract: International audience; The branching ratio β = k1b/k1a for the formation of ethyl nitrate, C2H5ONO2, in the gas-phase C2H5O2 + NO reaction, C2H5O2 + NO → C2H5O + NO2 (1a), C2H5O2 + NO → C2H5ONO2 (1b), was determined over the pressure and temperature ranges 100−600 Torr and 223−298 K, respectively, using a turbulent flow reactor coupled with a chemical ionization mass spectrometer. At 298 K the C2H5ONO2 yield was found to increase linearly with pressure from about 0.7% at 100 Torr to about 3% at 600 Torr. At each pressure, the branching ratio of C2H5ONO2 formation increases with the decrease of temperature. The following parametrization equation has been derived in the pressure and temperature ranges of the study: β(P,T) (%) = (3.88 × 10−3*P (Torr) + 0.365)*(1 + 1500(1/T − 1/298)). The atmospheric implication of the results obtained is briefly discussed, in particular the impact of β on the evolution of ethyl nitrate in urban plumes.
Published: 2009
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19. Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign

Author: Jaime Gil Roca, Alexandre Kukui, Joel Savarino, Nicolas Caillon, S. Preunkert, William Vicars, Bruno Jourdain, Michel Legrand, Markus M. Frey, Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Colorado Department of Public Health and Environment, University of Colorado [Denver], Institute of Arctic and Alpine Research (INSTAAR), University of Colorado [Boulder], British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), European Community's Seventh Framework Programme (FP7/2007-2013), INSU (LEFE Programme), Agence Nationale de la Recherche (ANR), IPEV (programme SUNITEDC n° 1011), ANR-05-PGCU-0004,OPALE,Risque d'inondation en ville et évaluation de scénarios(2005), ANR-10-LABX-0056,OSUG@2020,Innovative strategies for observing and modelling natural systems(2010), European Project: 237890,EC:FP7:PEOPLE,FP7-PEOPLE-ITN-2008,INTRAMIF(2009), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), CNRS-INSU : LEFE programThe Institute Polaire Paul-Emile Victor (IPEV)the program SUNITEDC No. 1011, Université Grenoble Alpes (UGA), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), ANR: OPALE,NT09-451281, ANR-10-LABX-0056/10-LABX-0056,OSUG@2020,Innovative strategies for observing and modelling natural systems(2010), ANR10 LABX56,ANR10 LABX56, and Institute of Arctic Alpine Research [University of Colorado Boulder] (INSTAAR)
Subjects: Hydrology, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, Ozone, 010504 meteorology & atmospheric sciences, δ18O, 010401 analytical chemistry, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Isotopes of oxygen, lcsh:QC1-999, 0104 chemical sciences, lcsh:Chemistry, chemistry.chemical_compound, Isotopic signature, chemistry, Nitrate, Ice core, lcsh:QD1-999, 13. Climate action, NOx, lcsh:Physics, Isotope analysis, 0105 earth and related environmental sciences
Abstract: Variations in the stable oxygen isotope composition of atmospheric nitrate act as novel tools for studying oxidative processes taking place in the troposphere. They provide both qualitative and quantitative constraints on the pathways determining the fate of atmospheric nitrogen oxides (NO + NO2 = NOx). The unique and distinctive 17O excess (Δ17O = δ17O − 0.52 × δ18O) of ozone, which is transferred to NOx via oxidation, is a particularly useful isotopic fingerprint in studies of NOx transformations. Constraining the propagation of 17O excess within the NOx cycle is critical in polar areas, where there exists the possibility of extending atmospheric investigations to the glacial–interglacial timescale using deep ice core records of nitrate. Here we present measurements of the comprehensive isotopic composition of atmospheric nitrate collected at Dome C (East Antarctic Plateau) during the austral summer of 2011/2012. Nitrate isotope analysis has been here combined for the first time with key precursors involved in nitrate production (NOx, O3, OH, HO2, RO2, etc.) and direct observations of the transferrable Δ17O of surface ozone, which was measured at Dome C throughout 2012 using our recently developed analytical approach. Assuming that nitrate is mainly produced in Antarctica in summer through the OH + NO2 pathway and using concurrent measurements of OH and NO2, we calculated a Δ17O signature for nitrate on the order of (21–22 ± 3) ‰. These values are lower than the measured values that ranged between 27 and 31 ‰. This discrepancy between expected and observed Δ17O(NO3−) values suggests the existence of an unknown process that contributes significantly to the atmospheric nitrate budget over this East Antarctic region. However, systematic errors or false isotopic balance transfer functions are not totally excluded.
Published: 2016
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20. Orbitrap-based mass analyser for in-situ characterization of asteroids: ILMA, Ion Laser Mass Analyser

Author: Christelle Briois, Hervé Cottin, Laurent Thirkell, Kenzi Aradj, Abdel Bouabdellah, Amirouche Boukrara, Nathalie Carrasco, Gilles Chalumeau, Olivier Chapelon, Fabrice Colin, Patrice Coll, Cécile Engrand, Noël Grand, Alexandre Kukui, Jean-Pierre Lebreton, Cyril Pennanech, Cyril Szopa, Roland Thissen, Véronique Vuitton, Pascal Zapf, Alexander Makarov, Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National d’Études Spatiales [Paris] (CNES), Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), PLANETO - LATMOS, Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut Universitaire de France (IUF), Ministère de l'Education nationale, de l’Enseignement supérieur et de la Recherche (M.E.N.E.S.R.), Centre de Sciences Nucléaires et de Sciences de la Matière (CSNSM), Université Paris-Sud - Paris 11 (UP11)-Institut National de Physique Nucléaire et de Physique des Particules du CNRS (IN2P3)-Centre National de la Recherche Scientifique (CNRS), Institut de Planétologie et d'Astrophysique de Grenoble (IPAG ), Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Thermo Fisher Scientific Inc., Karri Muinonen, Antti Penttilä, Mikael Granvik, Anne Virkki, Grigori Fedorets, Olli Wilkman, and Tomas Kohout (eds.), Cardon, Catherine, Karri Muinonen, Antti Penttilä, Mikael Granvik, Anne Virkki, Grigori Fedorets, Olli Wilkman, and Tomas Kohout (eds.), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), PSL Research University (PSL)-PSL Research University (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Centre National de la Recherche Scientifique (CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS), IMPEC - LATMOS, Institut de Planétologie et d'Astrophysique de Grenoble (IPAG), Centre National d'Études Spatiales [Toulouse] (CNES)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS), Thermo Fisher Scientific, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), and Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [PHYS.PHYS.PHYS-AO-PH] Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph]
Abstract: International audience; Since about a decade the boundaries between comets and carbonaceous asteroids are fading [1,2]. No doubt that the Rosetta mission should bring a new wealth of data on the composition of comets. But as promising as it may look, the mass resolving power of the mass spectrometers onboard (so far the best on a space mission) will only be able to partially account for the diversity of chemical structures present.ILMA (Ion-Laser Mass Analyser) is a new generation high mass resolution LDI-MS (Laser Desorption-Ionization Mass Spectrometer) instrument concept using the Orbitrap technique, which has been developed in the frame of the two Marco Polo & Marco Polo-R proposals to the ESA Cosmic Vision program. Flagged by ESA as an instrument concept of interest for the mission in 2012, it has been under study for a few years in the frame of a Research and Technology (R&T) development programme between 5 French laboratories (LPC2E, IPAG, LATMOS, LISA, CSNSM) [3,4], partly funded by the French Space Agency (CNES). The work is undertaken in close collaboration with the Thermo Fisher Scientific Company, which commercialises Orbitrap-based laboratory instruments.The R&T activities are currently concentrating on the core elements of the Orbitrap analyser that are required to reach a sufficient maturity level for allowing design studies of future space instruments. A prototype is under development at LPC2E and a mass resolution (m/Δm FWHM) of 100,000 as been obtained at m/z = 150 for a background pressure of 10-8mbar.ILMA would be a key instrument to measure the molecular, elemental and isotopic composition of objects such as carbonaceous asteroids, comets, or other bodies devoid of atmosphere such as the surface of an icy satellite, the Moon, or Mercury.
Published: 2014

21. Measurements of OH and RO2 radicals at Dome C, East Antarctica

Author: S. Preunkert, Alexandre Kukui, Rodrigue Loisil, J. Gil Roca, Michel Legrand, Bruno Jourdain, Gérard Ancellet, Markus M. Frey, and Martin D. King
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Chemistry, Stereochemistry, Radical, Photodissociation, East antarctica, 010501 environmental sciences, Photochemistry, 01 natural sciences, Dome (geology), 13. Climate action, Molecule, Oxidative capacity, 0105 earth and related environmental sciences, Antarctic plateau
Abstract: Concentrations of OH radicals and the sum of peroxy radicals, RO2, were measured in the boundary layer for the first time on the East Antarctic Plateau at the Concordia Station (Dome C, 75.10° S, 123.31° E) during the austral summer 2011/2012. The median concentrations of OH and RO2 radicals were 3.1 × 106 molecule cm−3 and 9.9 × 106 molecule cm−3, respectively. These values are comparable to those observed at the South Pole, confirming that the elevated oxidative capacity of the Antarctic atmospheric boundary layer found at the South Pole is not restricted to the South Pole but common over the high Antarctic plateau. At Concordia, the concentration of radicals showed distinct diurnal profiles with the median maximum of 5.2 × 106 molecule cm−3 at 11:00 and the median minimum of 1.1 × 106 molecule cm−3 at 01:00 for OH radicals and 1.7 × 108 molecule cm−3 and 2.5 × 107 molecule cm−3 for RO2 radicals at 13:00 and 23:00, respectively (all times are local times). Concurrent measurements of O3, HONO, NO, NO2, HCHO and H2O2 demonstrated that the major primary source of OH and RO2 radicals at Dome C was the photolysis of HONO, HCHO and H2O2, with the photolysis of HONO contributing ~75% of total primary radical production. However, photochemical modelling with accounting for all these radical sources overestimates the concentrations of OH and RO2 radicals by a factor of 2 compared to field observations. Neglecting the net OH production from HONO in the photochemical modelling results in an underestimation of the concentrations of OH and RO2 radicals by a factor of 2. To explain the observations of radicals in this case an additional source of OH equivalent to about (25–35)% of measured photolysis of HONO is required. Even with a factor of 5 reduction in the concentrations of HONO, the photolysis of HONO represents the major primary radical source at Dome C. To account for a possibility of an overestimation of NO2 observed at Dome C the calculations were also performed with NO2 concentrations estimated by assuming steady-state NO2 / NO ratios. In this case the net radical production from the photolysis of HONO should be reduced by a factor of 5 or completely removed based on the photochemical budget of OH or 0-D modelling, respectively. Another major factor leading to the large concentration of OH radicals measured at Dome C was large concentrations of NO molecules and fast recycling of peroxy radicals to OH radicals.
Published: 2014
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22. Large mixing ratios of atmospheric nitrous acid (HONO) at Concordia (East Antarctic Plateau) in summer: a strong source from surface snow?

Author: Bruno Jourdain, Joel Savarino, Alexandre Kukui, S. Preunkert, Michel Kerbrat, Th Bartels-Rausch, Michel Legrand, Martin D. King, Markus M. Frey, Université Joseph Fourier - Grenoble 1 (UJF), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Laboratory of Radio- and Environmental Chemistry [Villigen], Paul Scherrer Institute (PSI), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), School of Earth Sciences [Bristol], University of Bristol [Bristol], NERC NE/F0004796/1 and NE/F010788, and NERC FSF grants 555.0608 and 584.0609, Institut Polaire Français-Paul Emile Victor (IPEV), Italian colleagues from Meteo- Climatological Observatory of PNRA for the meteorological data collected at Concordia., ANR-09-BLAN-0226,OPALE(2009), ANR-11-JS56-0005,MONISNOW,Suivi temporel de la neige dans un climat changeant(2011), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), ANR-09-BLAN-0226,OPALE, and ANR-11- JS56-005-01,MONISNOW
Subjects: Atmospheric Science, Nitrous acid, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Atmospheric sciences, Snow, 01 natural sciences, lcsh:QC1-999, Atmosphere, lcsh:Chemistry, chemistry.chemical_compound, chemistry, lcsh:QD1-999, 13. Climate action, [SDU]Sciences of the Universe [physics], Mixing ratio, Absorption (electromagnetic radiation), [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, NOx, Mixing (physics), lcsh:Physics, Antarctic plateau, 0105 earth and related environmental sciences
Abstract: During the austral summer 2011/2012 atmospheric nitrous acid (HONO) was investigated for the second time at the Concordia site (75°06' S, 123°33' E), located on the East Antarctic Plateau, by deploying a long-path absorption photometer (LOPAP). Hourly mixing ratios of HONO measured in December 2011/January 2012 (35 ± 5.0 pptv) were similar to those measured in December 2010/January 2011 (30.4 ± 3.5 pptv). The large value of the HONO mixing ratio at the remote Concordia site suggests a local source of HONO in addition to weak production from oxidation of NO by the OH radical. Laboratory experiments demonstrate that surface snow removed from Concordia can produce gas-phase HONO at mixing ratios half that of the NOx mixing ratio produced in the same experiment at typical temperatures encountered at Concordia in summer. Using these lab data and the emission flux of NOx from snow estimated from the vertical gradient of atmospheric concentrations measured during the campaign, a mean diurnal HONO snow emission ranging between 0.5 and 0.8 × 109 molecules cm−2 s−1 is calculated. Model calculations indicate that, in addition to around 1.2 pptv of HONO produced by the NO oxidation, these HONO snow emissions can only explain 6.5 to 10.5 pptv of HONO in the atmosphere at Concordia. To explain the difference between observed and simulated HONO mixing ratios, tests were done both in the field and at lab to explore the possibility that the presence of HNO4 had biased the measurements of HONO.
Published: 2014
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23. Formaldehyde (HCHO) in air, snow and interstitial air at Concordia (East Antarctic plateau) in summer

Author: Alexandre Kukui, Detlev Helmig, Hubert Gallée, Markus M. Frey, Joel Savarino, Martin D. King, Bruno Jourdain, William Vicars, Susanne Preunkert, Michel Legrand, Université Joseph Fourier - Grenoble 1 (UJF), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), British Antarctic Survey (BAS), Natural Environment Research Council (NERC), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), Department of Physics [Egham], Royal Holloway [University of London] (RHUL), Institute of Arctic and Alpine Research (INSTAAR), University of Colorado [Boulder], ANR-10-LABX-100-01/10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Birmingham City University (BCU), Agence Nationale de la Recherche (ANR), Institut Polaire Français- Paul Emile Victor (IPEV), ANR-09-BLAN-0226,OPALE,Oxidant Production over Antarctica Land and its Export(2009), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), ANR-09-BLAN-0226,OPALE(2009), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institute of Arctic Alpine Research [University of Colorado Boulder] (INSTAAR), and ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010)
Subjects: [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, 010504 meteorology & atmospheric sciences, Formaldehyde, 010501 environmental sciences, Snowpack, Noon, Snow, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, lcsh:Chemistry, chemistry.chemical_compound, Flux (metallurgy), lcsh:QD1-999, chemistry, 13. Climate action, Diurnal cycle, [SDU]Sciences of the Universe [physics], Climatology, Anaerobic oxidation of methane, [SDE]Environmental Sciences, Mixing ratio, lcsh:Physics, 0105 earth and related environmental sciences
Abstract: International audience; During the 2011/12 and 2012/13 austral summers , HCHO was investigated for the first time in ambient air, snow, and interstitial air at the Concordia site, located near Dome C on the East Antarctic Plateau, by deploying an Aerolaser AL-4021 analyzer. Snow emission fluxes were estimated from vertical gradients of mixing ratios observed at 1 cm and 1 m above the snow surface as well as in interstitial air a few centimeters below the surface and in air just above the snowpack. Typical flux values range between 1 and 2 × 1012 molecules m-2 s-1 at night and 3 and 5 × 1012 molecules m-2 s-1 at noon. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible compared to temperature-driven air–snow exchanges. At 1 m above the snow surface, the observed mean mixing ratio of 130 pptv and its diurnal cycle characterized by a slight decrease around noon are quite well reproduced by 1-D simulations that include snow emissions and gas-phase methane oxidation chemistry. Simulations indicate that the gas-phase production from CH4 oxidation largely contributes (66 %) to the observed HCHO mixing ratios. In addition, HCHO snow emissions account for ∼ 30 % at night and ∼ 10 % at noon to the observed HCHO levels.
Published: 2014
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24. The impact of the chemical production of methyl nitrate from the NO + CH3O2 reaction on the global distributions of alkyl nitrates, nitrogen oxides and tropospheric ozone: a global modeling study

Author: Helmut Ziereis, G. Le Bras, Alexandre Kukui, Carl A. M. Brenninkmeijer, and J. E. Williams
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Reactive nitrogen, Chemistry, 15. Life on land, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Troposphere, chemistry.chemical_compound, Deposition (aerosol physics), Nitrate, 13. Climate action, Climatology, Nitrogen oxide, Tropospheric ozone, Methyl nitrate, NOx, 0105 earth and related environmental sciences
Abstract: The formation, abundance and distribution of organic nitrates are relevant for determining the production efficiency and resident mixing ratios of tropospheric ozone (O3) on both regional and global scales. Here we investigate the effect of applying the recently measured direct chemical production of methyl nitrate (CH3ONO2) during NOx recycling involving the methyl-peroxy radical on the global tropospheric distribution of CH3ONO2 and the perturbations introduced towards tropospheric NOx and O3 using the TM5 global chemistry transport model. By comparisons against numerous observations, we show that the global surface distribution of CH3ONO2 can be largely explained by introducing the chemical production mechanism using a branching ratio of 0.3%, when assuming a direct oceanic emission source of ~0.15 Tg N yr−1. On a global scale, the chemical production of CH3ONO2 converts 1 Tg N yr−1 from nitrogen oxide for this branching ratio. The resident mixing ratios of CH3ONO2 are found to be highly sensitive to the dry deposition velocity that is prescribed, where more than 50% of the direct oceanic emission is lost near the source regions, thereby mitigating the subsequent effects due to long-range and convective transport out of the source region. For the higher alkyl nitrates (RONO2) we find improvements in the simulated distribution near the surface in the tropics (10° S–10° N) when introducing direct oceanic emissions equal to ~0.17 Tg N yr−1 . In terms of the vertical profile of CH3ONO2, there are persistent overestimations in the free troposphere and underestimations in the upper troposphere across a wide range of latitudes and longitudes when compared against data from measurement campaigns. This suggests either a missing transport pathway or source/sink term, although measurements show significant variability in resident mixing ratios at high altitudes at global scale. For the vertical profile of RONO2, TM5 performs better at tropical latitudes than at mid-latitudes, with similar features in the comparisons to those for CH3ONO2. Comparisons of CH3ONO2 with a wide range of surface measurements shows that further constraints are necessary regarding the variability in the deposition terms for different land surfaces in order to improve on the comparisons presented here. For total reactive nitrogen (NOy) ~20% originates from alkyl nitrates in the tropics and subtropics, where the introduction of both direct oceanic emissions and the chemical formation mechanism of CH3ONO2 only makes a ~5% contribution to the total alkyl nitrate content in the upper troposphere when compared with aircraft observations. We find that the increases in tropospheric O3 that occur due oxidation of CH3ONO2 originating from direct oceanic emission is negated when accounting for the chemical formation of CH3ONO2, meaning that the impact of such oceanic emissions on atmospheric lifetimes becomes marginal when a branching ratio of 0.3% is adopted.
Published: 2013
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25. Oxidant Production over Antarctic Land and its Export (OPALE) project: An overview of the 2010-2011 summer campaign

Author: Gérard Ancellet, Valérie Gros, Michel Legrand, Alexandre Kukui, Bruno Jourdain, Michael Kerbrat, Susanne Preunkert, and Roland Sarda-Esteve
Subjects: Atmospheric Science, Marine boundary layer, 010504 meteorology & atmospheric sciences, Planetary boundary layer, Soil Science, 010501 environmental sciences, Aquatic Science, Oceanography, Atmospheric sciences, High ozone, 01 natural sciences, Geochemistry and Petrology, Earth and Planetary Sciences (miscellaneous), 14. Life underwater, Air mass, 0105 earth and related environmental sciences, Earth-Surface Processes, Water Science and Technology, Ecology, Chemical measurement, Paleontology, Forestry, East antarctica, Geophysics, 13. Climate action, Space and Planetary Science
Abstract: [1] This paper summarizes the objectives and setting of the OPALE (Oxidant Production over Antarctic Land and its Export) project during summer 2010/2011 at Dumont d'Urville. The primary goal of the campaign is to characterize the oxidizing environment of the atmospheric boundary layer along the coast of East Antarctica. A summary of the relevant field chemical measurements is presented including the carbon monoxide and ammonia records that are used here to identify local influences due to station activities and penguin emissions. An overview of the basic meteorological conditions experienced by the site is presented including the results from the trajectory/dispersion model FLEXPART to highlight which types of air mass were sampled (marine boundary layer versus continental Antarctic air). The results of the FLEXPART analysis demonstrate that high ozone levels and related changes in the OH concentrations are associated with the transport of continental air to DDU. Finally, three companion papers are introduced. A first paper is dedicated to the impact of local penguin emissions on the atmospheric budget of several oxygenated volatile organic compounds. The second paper reports on HONO levels that were measured for the first time in Antarctica by using the long path absorption photometer (LOPAP) technique. Finally, in a third paper, major findings on the HOx levels are detailed, leading to the overall conclusion that the photochemistry at coastal East Antarctica is strongly driven by an efficient HOx chemistry compared to the situation at other coastal Antarctic regions.
Published: 2012
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26. Measurements of OH and RO2radicals at the coastal Antarctic site of Dumont d'Urville (East Antarctica) in summer 2010-2011

Author: Rodrigue Loisil, Roland Sarda-Esteve, Valérie Gros, Gérard Ancellet, Suzanne Preunkert, Slimane Bekki, Michel Legrand, and Alexandre Kukui
Subjects: Atmospheric Science, 010504 meteorology & atmospheric sciences, Radical, Soil Science, Aquatic Science, Oceanography, 01 natural sciences, Geochemistry and Petrology, Earth and Planetary Sciences (miscellaneous), 0105 earth and related environmental sciences, Earth-Surface Processes, Water Science and Technology, High concentration, Ecology, Chemistry, 010401 analytical chemistry, Photodissociation, Paleontology, Forestry, East antarctica, 0104 chemical sciences, Geophysics, 13. Climate action, Space and Planetary Science, Environmental chemistry
Abstract: Measurements of OH and total proxy RO 2 (HO 2 plus organic peroxy) radicals were conducted in December 2010/January 2011 at the coastal East Antarctic site of Dumont d'Urville (DDU, 66°40'S 140°01'E) as part of the Oxidant Production over Antarctic Land and its Export (OPALE) project. Compared to measurements carried out at the West Antarctic coast, relatively high concentrations of radicals were found with 24 h average values of 2.1 × 10 6 and 3.3 × 10 8 molecule cm -3 for OH and peroxy radicals, respectively. On the basis of the steady-state calculations, the observed high concentration of peroxy radicals is in good agreement with the observed levels of O 3 and HCHO representing via their photolysis the major primary radical sources. The observed OH levels at DDU could be explained only assuming some RO 2 to OH conversion mechanism equivalent to the presence of NO in the range of 10 to 50 pptv. As neither NO nor halogen oxides were measured at DDU the mechanism of this recycling could not be explicitly identified. However, an examination of variability of radical levels as a function of the origin (oceanic versus continental) of sampled air masses suggests a more important OH production from RO 2 recycling in continental air masses.
Published: 2012
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27. Pressure and temperature dependence of methyl nitrate formation in the CH3O2 + NO reaction

Author: N. I. Butkovskaya, Alexandre Kukui, Georges Le Bras, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de combustion et systèmes reactifs (LCSR), Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS - CNRS), and Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)
Subjects: Chemical ionization, Nitrates, 010504 meteorology & atmospheric sciences, Chemistry, Branching fraction, Analytical chemistry, Temperature, 010402 general chemistry, Mass spectrometry, Nitric Oxide, 01 natural sciences, 0104 chemical sciences, Peroxides, Troposphere, [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, chemistry.chemical_compound, 13. Climate action, Torr, Yield (chemistry), Pressure, Physical and Theoretical Chemistry, Methyl nitrate, Stratosphere, ComputingMilieux_MISCELLANEOUS, 0105 earth and related environmental sciences
Abstract: The branching ratio β = k(1b)/k(1a) for the formation of methyl nitrate, CH(3)ONO(2), in the gas-phase CH(3)O(2) + NO reaction, CH(3)O(2) + NO → CH(3)O + NO(2) (1a), CH(3)O(2) + NO → CH(3)ONO(2) (1b), has been determined over the pressure and temperature ranges 50-500 Torr and 223-300 K, respectively, using a turbulent flow reactor coupled with a chemical ionization mass spectrometer. At 298 K, the CH(3)ONO(2) yield has been found to increase linearly with pressure from 0.33 ± 0.16% at 50 Torr to 0.80 ± 0.54% at 500 Torr (errors are 2σ). Decrease of temperature from 300 to 220 K leads to an increase of β by a factor of about 3 in the 100-200 Torr range. These data correspond to a value of β ≈ 1.0 ± 0.7% over the pressure and temperature ranges of the whole troposphere. Atmospheric concentrations of CH(3)ONO(2) roughly estimated using results of this work are in reasonable agreement with those observed in polluted environments and significantly higher compared with measurements in upper troposphere and lower stratosphere.
Published: 2012
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28. Impact of the new HNO3-forming channel of the HO2+NO reaction on tropospheric HNO3, NOx, HOx and ozone

Author: Cariolle, D., Evans, M. J., Chipperfield, M. P., Butkovskaya, N., Alexandre Kukui, Le Bras, G., Centre Européen de Recherche et de Formation Avancée en Calcul Scientifique (CERFACS), Météo-France, Institute for Atmospheric Science [Leeds], School of Earth and Environment [Leeds] (SEE), University of Leeds-University of Leeds, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS - CNRS), Service d'aéronomie (SA), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), CERFACS, Météo-France [Paris], Météo France, and Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere
Abstract: International audience; We have studied the impact of the recently established reaction NO+HO2?HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2?NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM). Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT). Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and southern hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. Mean global decreases in OH are around 13% which leads to a increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and southern hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.
Published: 2008

29. Chemical ionisation mass spectrometer for measurements of OH and Peroxy radical concentrations in moderately polluted atmospheres

Author: Georges Le Bras, Gérard Ancellet, Alexandre Kukui, TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), and Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS - CNRS)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Atmospheric Science, Chemical ionization, 010504 meteorology & atmospheric sciences, Atmospheric pressure, 010401 analytical chemistry, Analytical chemistry, Mass spectrometry, 01 natural sciences, Atmospheric measurements, Ion source, 0104 chemical sciences, Ion, chemistry.chemical_compound, chemistry, 13. Climate action, Ionization, Atmospheric chemistry, Chemical ionisation mass spectrometer, [SDE]Environmental Sciences, Peroxy radical, Environmental Chemistry, Hydroxyl radical, 0105 earth and related environmental sciences
Abstract: International audience; A new version of an atmospheric pressure chemical ionisation mass spectrometer has been developed for ground based in situ atmospheric measurements of OH and total peroxy (HO2 + organic peroxy) radicals. Based on the previously developed principle of chemical conversion of OH radicals to H2SO4 in reaction with SO2 and detection of H2SO4 using an ion molecule reaction with NO3--, the new instrument is equipped with a turbulent chemical conversion reactor allowing for measurements in moderately polluted atmosphere at NO concentrations up to several ppb. Unlike other similar devices, where the primary NO3-- ions are produced using radioactive ion sources, the new instrument is equipped with a specially developed corona discharge ion source. According to laboratory measurements, the overall accuracy and detection limits are estimated to be, respectively, 25% and 2 × 105 molecule cm-3 for OH and 30% and 1 × 105 molecule cm-3 for HO2 at 10 min integration times. The detection limit for measurements of OH radicals under polluted conditions is 5 × 105 molecules cm-3 at 10 min integration times. Examples of ambient air measurements during a field campaign near Paris in July 2007 are presented demonstrating the capability of the new instrument, although with reduced performance due to the employment of non isotopic SO2.
Published: 2008
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30. Les conditions climatiques de la dispersion des Grands Singes hors d'Afrique

Author: Michel Legrand, Slimane Bekki, Noémie Hamon, Alexandre Kukui, Véronique Ducrocq, Olivier Bousquet, Gérard Ancellet, Jean-Charles Dupont, Morgane Daudier, S. Preunkert, and Pierre Tabary
Abstract: Les conditions climatiques de la dispersion des Grands Singes hors d'Afrique. Le surprenant pouvoir oxydant de l'atmosphere en Antarctique de l'Est. Fin de mission pour le satellite europeen ENVISAT. Le SIRTA : 10 ans d'observation. Le prix Prud'homme 2012 attribue a Laure Raynaud. La conference ERAD2012 : la communaute radar meteo rassemblee a Toulouse. HyMeX : la premiere periode d'observations intensives.
Published: 2012
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31. Mass spectrometric determination of the rate constants for the reactions of H atoms with fluorine molecules, xenon and krypton fluorides at 298-505 K. 1. Reactions H+F2, H+XeF2, XeF4, XeF6

Author: Zelenov, V. V., Alexandre Kukui, Dodonov, A. F., Aleinikov, N. N., Kashtanov, S. A., Turchin, A. V., KUKUI, Alexandre, N. N. Semenov Institute of Chemical Physics, and Russian Academy of Sciences [Moscow] (RAS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 1991

32. Mass spectrometric determination of the rate constants for the reactions of H atoms with fluorine molecules, xenon and krypton fluorides at 298-505 K. 2. Reaction H+KrF2

Author: Zelenov, V. V., Alexandre Kukui, Dodonov, A. F., Aleinikov, N. N., Kashtanov, S. A., Turchin, A. V., N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: International audience
Published: 1991

33. Mass spectrometric studies of oxygen atom reaction with tetrafluoroethylene and CF2, CF3 and FCO radicals

Author: Dodonov, A. F., Zelenov, V. V., Alexandre Kukui, N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1987), 6(12), 1713Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience
Published: 1990

34. Mass spectrometric study of reactions in the system F+C2F4

Author: Dodonov, A. F., Zelenov, V. V., Alexandre Kukui, N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1987), 6(11), 1562Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience
Published: 1990

35. Water Vapor Effect on the HNO3Yield in the HO2+ NO Reaction: Experimental and Theoretical Evidence.

Author: Nadezhda Butkovskaya, Marie-Thérèse Rayez, Jean-Claude Rayez, Alexandre Kukui, and Georges Le Bras
Published: 2009
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36. HNO3Forming Channel of the HO2NO Reaction as a Function of Pressure and Temperature in the Ranges of 72−600 Torr and 223−323 K.

Author: Nadezhda Butkovskaya, Alexandre Kukui, and Georges Le Bras
Subjects: *TURBULENCE, *CHEMICAL ionization mass spectrometry, *SCISSION (Chemistry), *CHEMICAL reactions
Abstract: A high-pressure turbulent flow reactor coupled with a chemical ionization mass-spectrometer was used to determine the branching ratio of the HO2NO reaction: HO2NO → OH NO2(1a), HO2NO → HNO3(1b). The branching ratio, k1b/k1a, was derived from the measurements of “chemically amplified” concentrations of the NO2and HNO3products in the presence of O2and CO. The pressure and temperature dependence of was determined in the pressure range of 72−600 Torr of N2carrier gas between 323 and 223 K. At each pressure, the branching ratio was found to increase with the decrease of temperature, the increase becoming less pronounced with the increase of pressure. In the 298−223 K range, the data could be fitted by the expression: (T,P) (530 ± 10)/T(K) (6.4 ± 1.3) × 10-4P(Torr) − (1.73 ± 0.07), giving 0.5% near the Earth's surface (298 K, 760 Torr) and 0.8% in the tropopause region (220 K, 200 Torr). The atmospheric implication of these results is briefly discussed. [ABSTRACT FROM AUTHOR]
Published: 2007
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37. Mass spectrometric investigation of the elementary gas phase reactions in the H+O2+O3 system. The H+O3 => OH(v)+O2 and H+O3 => HO2+O reaction channels

Author: Dodonov, A. F., Zelenov, V. V., Alexandre Kukui, Ponomarev, E. A., Tal Roze, V. L., KUKUI, Alexandre, N. N. Semenov Institute of Chemical Physics, and Russian Academy of Sciences [Moscow] (RAS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1985), 4(10), 1335Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience
Published: 1989

38. Mass spectrometric investigation of the elementary gas phase reactions in the H+O2+O3 system. The reactions H+OH(v>6) => H2(v=5)+O and H+H2(v=5) => H2(v<4)+H

Author: Dodonov, A. F., Zelenov, V. V., Alexandre Kukui, Ponomarev, E. A., Tal Roze, V. L., KUKUI, Alexandre, N. N. Semenov Institute of Chemical Physics, and Russian Academy of Sciences [Moscow] (RAS)
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1985), 4(10), 1344Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience
Published: 1989

39. Mass spectrometric investigation of the elementary gas phase reactions in the H+O2+O3 system. Singlet oxygen formation in the reactions of ozone

Author: Zelenov, V. V., Alexandre Kukui, Dodonov, A. F., Tal Roze, V. L., N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, ComputingMilieux_MISCELLANEOUS
Abstract: International audience

40. New Measurements of Methyl Ethyl Ketone (MEK) Photolysis Rates and Their Relevance to Global Oxidative Capacity

Author: Brewer, J., Ravishankara, A. R., Wahid Mellouki, Fischer, E. V., Alexandre Kukui, Véronique DAËLE, Ait-Helal, W., Leglise, J., Ren, Y., KUKUI, Alexandre, Colorado State University [Fort Collins] (CSU), Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), École des Mines de Douai (Mines Douai EMD), and Institut Mines-Télécom [Paris] (IMT)
Subjects: [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere
Abstract: International audience; Methyl ethyl ketone (MEK) is one of the most abundant ketones in the atmosphere. MEK can be emitted directly into the atmosphere from both anthropogenic and natural sources, and it is also formed during the gas-phase oxidation of volatile organic compounds (VOCs). MEK is lost via reaction with OH, photolysis and deposition to the surface. Similar to the other atmospheric ketones, the photolysis of MEK may represent a source of HOx (OH + HO2) radicals in the upper troposphere. The degradation of MEK also leads to the atmospheric formation of acetaldehyde and formaldehyde. This work presents a new analysis of the temperature dependence of MEK photolysis cross-sections and a quantification of MEK photolysis rates under surface pressures using the CNRS HELIOS outdoor atmospheric chamber (Chambre de simulation atmosphérique à irradiation naturelle d'Orléans; http://www.era-orleans.org/ERA-TOOLS/helios-project.html). Additionally, we use the GEOS-Chem 3-D CTM (version 10-01, www.geos-chem.org) to investigate the impact of these newly measured rates and cross-sections on the global distribution and seasonality of MEK, as well as its importance to the tropospheric oxidative capacity.

41. Reactions of acetone oxide stabilized Criegee intermediate with SO2, NO2, H2O and O3

Author: Alexandre Kukui, Hui Chen, Shan Xiao, Wahid Mellouki, Véronique DAËLE, Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Department of Environmental Science and Engineering [Shanghai], Fudan University [Shanghai], COPERNICUS, and POTHIER, Nathalie
Subjects: [SDU] Sciences of the Universe [physics], [SDU]Sciences of the Universe [physics]
Abstract: International audience; Atmospheric aerosol particles represent a critical component of the atmosphere, impacting global climate, regionalair pollution, and human health. The formation of new atmospheric particles and their subsequent growth to largersizes are the key processes for understanding of the aerosol effects. Sulphuric acid, H2SO4, has been identified toplay the major role in formation of new atmospheric particles and in subsequent particle growth. Until recently thereaction of OH with SO2 has been considered as the only important source of H2SO4 in the atmosphere. However,recently it has been suggested that the oxidation of SO2 by Criegee biradicals can be a significant additionalatmospheric source of H2SO4 comparable with the reaction of SO2 with OH.Here we present some results about the reactions of the acetone oxide stabilized Criegee intermediate, (CH3)2=OO,produced in the reaction of 2,3-dimethyl-butene (TME) with O3.The formation of the H2SO4 in the reaction of acetone oxide with SO2 was investigated in the speciallyconstructed atmospheric pressure laminar flow reactor. The Criegee intermediate was generated by ozonolysisof TME. The H2SO4, generated by addition of SO2, was directly monitored with Chemical Ionization MassSpectrometer (SAMU, LPC2E). Relative rates of reactions of acetone oxide with SO2, NO2, H2O and ozone weredetermined from the dependencies of the H2SO4 yield at different concentrations of the reactants.Atmospheric applications of the obtained results are discussed in relation to the importance of this additionalH2SO4 formation pathway compared to the reaction of OH with SO2.

42. OH and RO2 radicals at Dome C (East Antarctica): first observations and assessment of photochemical budget

Author: Alexandre Kukui, Rodrigue Loisil, Michael Kerbrat, Markus Frey, Jaime Gil, Bruno Jourdain, Gérard Ancellet, Slimane Bekki, Michel Legrand, Susanne Preunkert, Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Division technique INSU/SDU (DTI), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS), Centre Alpin de Recherche sur les Réseaux Trophiques et Ecosystèmes Limniques (CARRTEL), Institut National de la Recherche Agronomique (INRA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]), Centre d'Enseignement et de Recherche en Mathématiques et Calcul Scientifique (CERMICS), École des Ponts ParisTech (ENPC), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), STRATO - LATMOS, Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Centre National d’Études Spatiales [Paris] (CNES), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Université de Strasbourg (UNISTRA)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace (FMNGE), and Institut de Chimie du CNRS (INC)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Centre National de la Recherche Scientifique (CNRS)
Subjects: [SDU]Sciences of the Universe [physics]
Abstract: International audience; Measurements of OH and total peroxy RO 2 (HO 2 + organic peroxy) radicals were performed in December 2011/January 2012 at the Dome C Concordia station (East Antarctica, 75.1˚S / 123.3˚E) in the frame of the Oxi-dant Production over Antarctic Land and its Export (OPALE) project. The goal of these first on the East Antarctica plateau radical measurements was to estimate the oxidative capacity and assess the role of snow emissions on the radical budget in this part of Antarctica. The OH concentration levels were found to be in general similar to those observed at South Pole. However, based on the analysis of the OH sources and sinks derived from the available measurements of NO x , HONO, HCHO, H 2 O 2 and others, it has been concluded that, in contrast to South Pole, the photolysis of HONO is the major OH source at Dome C site. The role of HONO as the major source of OH is also supported by an excellent correlation of OH with the production rate of OH from the HONO photolysis. The observed diurnal profiles of OH and RO 2 are discussed in relation with boundary dynamics and the variability of photolysis and snow emissions rates.

43. Study of reactions between O( 3P) oxygen atoms and CF2(1A1) and CF2(3B1) radicals

Author: Dodonov, A. F., Zelenov, V. V., Alexandre Kukui, N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1988), 7(5), 658Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience

44. Mass spectrometric determination of the diffusion coefficients of hydrogen, oxygen and nitrogen atoms and H2 and O2 molecules in helium at temperatures 205-490 K

Author: Zelenov, V. V., Alexandre Kukui, Dodonov, A. F., N. N. Semenov Institute of Chemical Physics, Russian Academy of Sciences [Moscow] (RAS), and KUKUI, Alexandre
Subjects: [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry
Abstract: First published in Khimicheskaya Fizika (1986), 5(5), 702Sov. J Chem. Phys is a cover-to-cover translation of Khimicheskaya Fizika; International audience

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