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1. Measurement report: Sources, sinks, and lifetime of NOx in a suburban temperate forest at night.

Author

Andersen, Simone T., McGillen, Max R., Xue, Chaoyang, Seubert, Tobias, Dewald, Patrick, Türk, Gunther N. T. E., Schuladen, Jan, Denjean, Cyrielle, Etienne, Jean-Claude, Garrouste, Olivier, Jamar, Marina, Harb, Sergio, Cirtog, Manuela, Michoud, Vincent, Cazaunau, Mathieu, Bergé, Antonin, Cantrell, Christopher, Dusanter, Sebastien, Picquet-Varrault, Bénédicte, and Kukui, Alexandre

Subjects
TEMPERATE forests, TEMPERATURE inversions, ATMOSPHERIC chemistry, REACTIVE nitrogen species, BOUNDARY layer (Aerodynamics)
Abstract

The budget of reactive nitrogen species, which play a central role in atmospheric chemistry (e.g. in photochemical O3 production), is poorly understood in forested regions. In this study, through observations of NO, NO2 , NOy , and O3 in the Rambouillet Forest near Paris, France, we have examined nighttime processes controlling NOx in an anthropogenically impacted forest environment. The O3 mixing ratios displayed a strong diel profile at the site that was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity and temperature inversion. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long) were sustained NO peaks observed above the instrumental detection limit, enabling the derivation of average NO emission rates of ∼1.4 ppbvh-1 from the soil. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3 , enabled an effective lifetime of NO2 of ∼0.5 –3 h to be derived. As the loss of NO2 was not compensated for by the formation of gas- or particle-phase reactive nitrogen species, it was presumably either driven by deposition to soil and foliar surfaces or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 d. Our results indicate that the nighttime deposition of NO2 is a major sink of boundary layer NOx in this temperate forest environment. [ABSTRACT FROM AUTHOR]

Published
2024
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2. NO3 reactivity during a summer period in a temperate forest below and above the canopy.

Author

Dewald, Patrick, Seubert, Tobias, Andersen, Simone T., Türk, Gunther N. T. E., Schuladen, Jan, McGillen, Max R., Denjean, Cyrielle, Etienne, Jean-Claude, Garrouste, Olivier, Jamar, Marina, Harb, Sergio, Cirtog, Manuela, Michoud, Vincent, Cazaunau, Mathieu, Bergé, Antonin, Cantrell, Christopher, Dusanter, Sebastien, Picquet-Varrault, Bénédicte, Kukui, Alexandre, and Xue, Chaoyang

Subjects
ATMOSPHERIC chemistry, TEMPERATE forests, TEMPERATURE inversions, HYDROXYL group, NITRIC oxide
Abstract

We present direct measurements of biogenic volatile organic compound (BVOC)-induced nitrate radical (NO3) reactivity (kVOC) through the diel cycle in the suburban, temperate forest of Rambouillet near Paris (France). The data were obtained in a 6-week summer period in 2022 as part of the Atmospheric ChemistRy Of the Suburban foreSt (ACROSS) campaign. kVOC was measured in a small (700 m2) clearing mainly at a height of 5.5 m above ground level but also at 40 m (for 5 d and nights). At nighttime, mean values (and 25th–75th percentile ranges) of knightVOC(5.5m) = (0.24-0.06+0.32) s-1 and knightVOC(40m) = (0.016-0.007+0.018) s-1 indicate a significant vertical gradient and low NO3 reactivity above the canopy, whereas knightVOC (5.5 m) showed peak values of up to 2 s-1 close to the ground. The strong vertical gradient in NO3 reactivity could be confirmed by measurements between 0 and 24 m on one particular night characterized by a strong temperature inversion and is a result of the decoupling of air masses aloft from the ground- and canopy-level sources of BVOCs (and nitric oxide, NO). No strong vertical gradient was observed in the mean daytime NO3 reactivity, with kdayVOC(5.5m) = (0.12±0.04) s-1 for the entire campaign and kdayVOC(40m) = (0.07±0.02) s-1 during the 5 d period. Within the clearing, the fractional contribution of VOCs to the total NO3 loss rate coefficient (ktot , determined by photolysis, reaction with NO and VOCs) was 80 %–90 % during the night and ∼ 50 % during the day. In terms of chemical losses of α -pinene below canopy height in the clearing, we find that at nighttime hydroxyl radicals (OH) and ozone (O3) dominate, with NO3 contributing "only" 17 %, which decreases further to 8.5 % during the day. Based on measured OH, measured O3 , and calculated NO3 concentrations, the chemical lifetime of BVOCs at noon is about 1 h and is likely to be longer than timescales of transport out of the canopy (typically of the order of minutes), thus significantly reducing the importance of daytime in-canopy processing. Clearly, in forested regions where sufficient nitric oxide and nitrogen dioxide (NOx) is available, the role of NO3 and OH as initiators of BVOC oxidation is not strictly limited to nighttime and daytime, respectively, as often implied in e.g. atmospheric chemistry textbooks. [ABSTRACT FROM AUTHOR]

Published
2024
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3. NO3 reactivity during a summer period in a temperate forest below and above the canopy.

Author

Dewald, Patrick, Seubert, Tobias, Andersen, Simone T., Türk, Gunther N. T. E., Schuladen, Jan, McGillen, Max R., Denjean, Cyrielle, Etienne, Jean-Claude, Garrouste, Olivier, Jamar, Marina, Harb, Sergio, Cirtog, Manuela, Michoud, Vincent, Cazaunau, Mathieu, Bergé, Antonin, Cantrell, Christopher, Dusanter, Sebastien, Picquet-Varrault, Bénédicte, Kukui, Alexandre, and Chaoyang Xue

Abstract

We present direct measurements of BVOC-induced nitrate radical (NO3) reactivity (kVOC) through the diel cycle in the suburban, temperate forest of Rambouillet near Paris (France). The data were obtained in a six-week summer period in 2022 as part of the ACROSS campaign (Atmospheric ChemistRy Of the Suburban foreSt). kVOC was measured in a small (700 m²) clearing mainly at a height of 5.5 m above ground level, but also at 40 m (for 5 days/nights). At nighttime, mean values of kVOCnight (5.5 m) = (0.24 ± 0.27) s-1 and kVOCnight (40 m) = (0.016 ± 0.007) s-1 indicate a significant vertical gradient and low NO3 reactivity above the canopy, whereas kVOCnight (5.5 m) showed peak values of up to 2 s-1 close to the ground. The strong vertical gradient in NO3 reactivity could be confirmed by measurements between 0 and 24 m on one particular night characterised by a strong temperature inversion, and is a result of the decoupling of air masses aloft from the ground- and canopy-level sources of BVOCs (and NO). No strong vertical gradient was observed in the mean daytime NO3 reactivity with kVOCnight(5.5 m) = (0.12 ± 0.04) s-1 for the entire campaign and kVOCnight(40 m) = (0.07 ± 0.02) s-1 during the 5-day period. Within the clearing, the fractional contribution of VOCs to the total NO3 loss rate (LNO3, determined by photolysis, reaction with NO and VOCs) was 80-90 % during the night and ~50 % during the day. In terms of chemical losses of α-pinene below canopy height in the clearing, we find that at nighttime OH and O3 dominate with NO3 contributing "only" 17 %, which decreases further to 8.5 % during the day. Based on OH, O3 and NO3 concentrations, the chemical lifetime of BVOCs at noon is about one hour and is likely to be longer than timescales of transport out of the canopy (typically in the order of minutes), thus significantly reducing the importance of daytime, in-canopy processing. Clearly, in forested regions where sufficient NOX is available, the role of NO3 and OH as initiators of BVOC oxidation are not strictly limited to the night and to the day, respectively, as often implied in e.g. atmospheric chemistry text-books. [ABSTRACT FROM AUTHOR]

Published
2024
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4. Measurement report: Sources, sinks and lifetime of NOX in a sub-urban temperate forest at night.

Author

Andersen, Simone T., McGillen, Max R., Chaoyang Xue, Seubert, Tobias, Dewald, Patrick, Türk, Gunther N. T. E., Schuladen, Jan, Denjean, Cyrielle, Etienne, Jean-Claude, Garrouste, Olivier, Jamar, Marina, Harb, Sergio, Cirtog, Manuela, Michoud, Vincent, Cazaunau, Mathieu, Bergé, Antonin, Cantrell, Christopher, Dusanter, Sebastien, Varrault, Bénédicte Picquet, and Kukui, Alexandre

Abstract

Through observations of NO, NO2, NOY and O3 in the Rambouillet forest near Paris, France, (as part of the ACROSS campaign, 2022) we have gained insight into nighttime processes controlling NOX in an anthropogenically impacted forest environment. O3 mixing ratios displayed a strong diel profile at the site, which was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity, which impacted the surface resistance to uptake, and temperature inversion, which influenced the rate of entrainment of O3 from above the canopy. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long), were sustained NO peaks observed above the instrumental detection limit, enabling derivation of average NO emission rates from the soil of -1.4 ppbv h-1. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3, enabled an effective lifetime of NO2 of -0.5-3 h to be derived. As the loss of NO2 was not compensated by the formation of gas- or particle-phase reactive nitrogen species it was presumably driven by deposition to soil and foliar surfaces, or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 day. We conclude that the nighttime deposition of NO2 is a major sink of boundary layer NOX in this temperate forest environment. [ABSTRACT FROM AUTHOR]

Published
2024
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5. Measurement report: Sources, sinks and lifetime of NOX in a sub-urban temperate forest at night.

Author

Andersen, Simone T., McGillen, Max R., Xue, Chaoyang, Seubert, Tobias, Dewald, Patrick, Türk, Gunther N. T. E., Schuladen, Jan, Denjean, Cyrielle, Etienne, Jean-Claude, Garrouste, Olivier, Jamar, Marina, Harb, Sergio, Cirtog, Manuela, Michoud, Vincent, Cazaunau, Mathieu, Bergé, Antonin, Cantrell, Christopher, Dusanter, Sebastien, Picquet-Varrault, Bénédicte, and Kukui, Alexandre

Subjects
TEMPERATURE inversions, SURFACE resistance, BOUNDARY layer (Aerodynamics), REACTIVE nitrogen species, TEMPERATE forests, HUMIDITY
Abstract

Through observations of NO, NO2, NOY and O3 in the Rambouillet forest near Paris, France, (as part of the ACROSS campaign, 2022) we have gained insight into nighttime processes controlling NOX in an anthropogenically impacted forest environment. O3 mixing ratios displayed a strong diel profile at the site, which was driven by a variable but generally rapid deposition to soil and foliar surfaces. The O3 diel profile was strongly influenced by relative humidity, which impacted the surface resistance to uptake, and temperature inversion, which influenced the rate of entrainment of O3 from above the canopy. Only when the O3 mixing ratio was sufficiently low (and thus the NO lifetime sufficiently long), were sustained NO peaks observed above the instrumental detection limit, enabling derivation of average NO emission rates from the soil of ~1.4 ppbv h‑1. Observations of the lack of increase in NO2 at night, despite a significant production rate from the reaction of NO with O3, enabled an effective lifetime of NO2 of ⁓0.5–3 h to be derived. As the loss of NO2 was not compensated by the formation of gas- or particle-phase reactive nitrogen species it was presumably driven by deposition to soil and foliar surfaces, or any products formed were themselves short-lived with respect to deposition. By comparison, the daytime lifetime of NO2 with respect to loss by reaction with OH is about 1 day. We conclude that the nighttime deposition of NO2 is a major sink of boundary layer NOX in this temperate forest environment. [ABSTRACT FROM AUTHOR]

Published
2024
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6. Investigation of ROx radical chemistry during the ChArMEx field campaign

Author

Dusanter, Sébastien, Shahin, Marwa, Lahib, Ahmad, Kukui, Alexandre, Zannoni, Nora, Gros, Valérie, Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), 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 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), and KUKUI, Alexandre

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
2021

8. Mechanism of the OH-initiated oxidation of glycoaldehyde over the temperature range 233-296 K

Author

Butkovskaya, Nadezhda I., Pouvesle, Nicolas, Kukui, Alexandre, and Le Bras, Georges

Subjects
Aldehydes -- Chemical properties, Hydroxides -- Chemical properties, Oxidation-reduction reaction, Chemicals, plastics and rubber industries
Abstract

A study of the mechanism of the gas-phase OH initiated oxidation of glycoaldehyde in the 233-296 K temperature range using a turbulent flow reactor coupled with a chemical ionization mass spectrometer is presented. Formaldehyde, C[O.sub.2], formic acid and glyoxal were observed at RT with the yields of 80, 34, 18 and 14% respectively, in the presence of oxygen and decrease of temperature to 233K led to significant change in the yields of stable products.

Published
2006

9. The influence of organic and inorganic gases during New Particle Formation (NPF) events at the Mediterranean remote site of ERSA in Cape-Corsica during the summer of 2013

Author

Waked, Antoine, Sauvage, Stephane, Michoud, Vincent, Sellegri, Karine, Berland, Kevin, Kukui, Alexandre, Hallemans, Elise, Zannoni, Nora, Kalogridis, Cerise, Gros, Valerie, Dusanter, Sebastien, Locoge, Nadine, Doussin, Jean-Francois, Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), 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), and KUKUI, Alexandre

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere
Abstract

International audience; As part of the CHARMEX (Chemistry Aerosol Mediterranean Experiments) project, more than one hundred organic and inorganic gaseous compounds were measured in the summer of 2013 at the Mediterranean remote site of ERSA in Cape-Corsica. During this period, New Particle formation (NPF) events were identified from July 31th to august 2nd when air masses originated from the North-eastern sector (Southern Europe). The results were compared to a non-NPF event from July 21th to July 23rd for which the same wind sectors were identified. They showed that the particles number [10-20 nm] measured by SMPS (Scanning Mobility Particle Sizer) were more correlated with carbon monoxide (CO) during non-NPF events indicating an influence of more polluted and more aged air masses (residence time of CO of 60 days). Sulfuric acid (H2SO4) and sulfur dioxide do not show a significant influence in the formation of nucleation events. On the other hand, biogenic Volatile Organic Compounds (BVOCs) such as isoprene, and mono-terpenes as well as their oxidation products (e.g. MACR+MVK, MTOP) showed good correlation during NPF-events in the range of (r from 0.45 to 0.59) higher than the ones reported during non-NPF events (0.11-0.34) highlighting the importance of these BVOCs on NPF days. The comparison of measured vs calculated reactivity (Zannoni et al, 2016) showed that during NPF-events, the missing part of OH reactivity was higher. It indicates that unmeasured species like sesquiterpenes, organo-nitrates, or oxygenated compounds may play a significant role in such events.

Published
2017

10. Role of Criegee intermediates in the formation of sulfuric acid at a Mediterranean (Cape Corsica) site under influence of biogenic emissions.

Author

Kukui, Alexandre, Chartier, Michel, Wang, Jinhe, Chen, Hui, Dusanter, Sébastien, Sauvage, Stéphane, Michoud, Vincent, Locoge, Nadine, Gros, Valérie, Bourrianne, Thierry, Sellegri, Karine, and Pichon, Jean-Marc

Subjects
SULFURIC acid, VOLATILE organic compounds, STRUCTURE-activity relationships
Abstract

Reaction of stabilized Criegee intermediates (SCIs) with SO 2 was proposed as an additional pathway of gaseous sulfuric acid (H 2 SO 4) formation in the atmosphere, supplementary to the conventional mechanism of H 2 SO 4 production by oxidation of SO 2 in reaction with OH radicals. However, because of a large uncertainty in mechanism and rate coefficients for the atmospheric formation and loss reactions of different SCIs, the importance of this additional source is not well established. In this work, we present an estimation of the role of SCIs in H 2 SO 4 formation at a western Mediterranean (Cape Corsica) remote site, where comprehensive field observations including gas-phase H 2 SO 4 , OH radicals, SO 2 , volatile organic compounds (VOCs) and aerosol size distribution measurements were performed in July–August 2013 as a part of the project ChArMEx (Chemistry-Aerosols Mediterranean Experiment). The measurement site was under strong influence of local emissions of biogenic volatile organic compounds, including monoterpenes and isoprene generating SCIs in reactions with ozone, and, hence, presenting an additional source of H 2 SO 4 via SO 2 oxidation by the SCIs. Assuming the validity of a steady state between H 2 SO 4 production and its loss by condensation on existing aerosol particles with a unity accommodation coefficient, about 90 % of the H 2 SO 4 formation during the day could be explained by the reaction of SO 2 with OH. During the night the oxidation of SO 2 by OH radicals was found to contribute only about 10 % to the H 2 SO 4 formation. The accuracy of the derived values for the contribution of OH + SO 2 reaction to the H 2 SO 4 formation is limited mostly by a large, at present factor of 2, uncertainty in the OH + SO 2 reaction rate coefficient. The contribution of the SO 2 oxidation by SCIs to the H 2 SO 4 formation was evaluated using available measurements of unsaturated VOCs and steady-state SCI concentrations estimated by adopting rate coefficients for SCI reactions based on structure–activity relationships (SARs). The estimated concentration of the sum of SCIs was in the range of (1–3) × 10 3 molec. cm -3. During the day the reaction of SCIs with SO 2 was found to account for about 10 % and during the night for about 40 % of the H 2 SO 4 production, closing the H 2 SO 4 budget during the day but leaving unexplained about 50 % of the H 2 SO 4 formation during the night. Despite large uncertainties in used kinetic parameters, these results indicate that the SO 2 oxidation by SCIs may represent an important H 2 SO 4 source in VOC-rich environments, especially during nighttime. [ABSTRACT FROM AUTHOR]

Published
2021
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11. Chamber study of the Oxalyl Chloride Photodissociation in Sunlight

Author

Kukui, Alexandre, Ren, Yangang, Catoire, Valéry, Daële, Véronique, Mellouki, Wahid, Ravishankara, A. R., and Daele, Veronique

Subjects
Chamber, Kinetics, [CHIM.THEO] Chemical Sciences/Theoretical and/or physical chemistry, Photolysis, CIMS, Oxalyl Chloride, Peroxy Radicals
Abstract

Oxalyl chloride, (ClCO)2, has been used as a photolytic Cl atoms precursor for kinetic and photochemical studies. Previous studies of the (ClCO)2 photodynamic at 193, 248, and 351 nm suggest that UV photodissociation proceeds via a two-step mechanism including formation of an excited ClCO* radical (1) and dissociation of a fraction of the ClCO* depending on the photolysis wavelength into Cl + CO (2):(ClCO)2 + hv → ClCO* + CO + Cl (1)ClCO*→ Cl + CO (2)The ClCO radical formed with the energy lower than its dissociation barrier has been found to undergo unimolecular dissociation (3) on the time scale of several microseconds at room temperature and atmospheric pressure: ClCO + M → Cl + CO + M (3)In this work the photodissociation of (COCl)2 by solar irradiation has been studied in the HELIOS environmental chamber. An effective (COCl)2 dissociation quantum yield of 0.34±0.03 has been derived from the measured actinic flux in the chamber and the observed (COCl)2 decay rate. Thisresult is in agreement with previous studies. The relative yields of CO and Cl atoms were derived by comparing the (COCl)2 loss rate with the production rates of CO and Cl atoms. The Cl production rate was derived from the measured by CIMS steady state HO2 or CH3O2 radicalconcentrations generated by scavenging of Cl by H2 or CH4, respectively. The obtained relative CO yield of 2.2±0.1 is in agreement with previous studies. The relative yield of Cl has been found to be 2 times lower, 1.01±0.03, in disagreement with previous studies and suggesting anothermechanism of the (COCl)2 photodissociation at wavelengths longer than 300 nm.

Published
2019

12. Atmospheric nitrogen oxides (NO and NO2) at Dome C, East Antarctica, during the OPALE campaign

Author

Frey, N. M., Roscoe, H. K., Kukui, Alexandre, Savarino, Joël A., France, J. L., King, M.D., Legrand, Michel, Preunkert, Susanne, 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)-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), 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 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), School of Environmental Sciences [Norwich], University of East Anglia [Norwich] (UEA), School of Earth Sciences [Bristol], University of Bristol [Bristol], Université Joseph Fourier - Grenoble 1 (UJF), 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), 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), 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), and 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)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, lcsh:Chemistry, lcsh:QD1-999, [SDE]Environmental Sciences, lcsh:Physics, lcsh:QC1-999
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. Influence of Water on the H2SO4 Yield from the Ozonolysis of 2,3-dimethyl-butene (TME) in Presence of SO2

Author

Kukui, Alexandre, Chen, Hui, Daële, Véronique, Mellouki, Wahid, 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), and KUKUI, Alexandre

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, ATMOSPHERIC COMPOSITION AND STRUCTUREDE: 0365 Troposphere: composition and chemistry, 0317 Chemical kinetic and photochemical properties, ATMOSPHERIC COMPOSITION AND STRUCTUREDE: 0394 Instruments and techniques, ATMOSPHERIC COMPOSITION AND STRUCTUREDE: 0340 Middle atmosphere: composition and chemistry, ATMOSPHERIC COMPOSITION AND STRUCTURE
Abstract

International audience; The influence of the water vapor content on the yield of H2SO4 from the ozonolysis of 2,3-dimethyl-butene (TME) in presence of SO2 was studied using laminar flow reactor coupled with Chemical Ionisation Mass Spectrometer (CIMS) for the H2SO4 monitoring within the range of H2O from 10 ppmv to 3×104 ppmv at different concentrations of TME, O3, SO2. The observed dependences of the H2SO4 yield on H2O concentration can be interpreted by assuming two different paths of the H2SO4 formation: 1) via the formation of SO3 in the reaction of Stabilized Criegee Intermediate (SCI) with SO2 (2a) followed by the reaction of SO3 with H2O (3) and 2) via the formation of stabilized secondary ozonide (SOZ) (2b) producing H2SO4 in the reaction with H2O (4a) in competition with the SOZ decomposition to other products (5): O3+TME => (CH3)2COO (1) (CH3)2COO + SO2 => SO3 (2a) => SOZ (2b) SO3 + H2O => H2SO4 (3) SOZ + H2O => H2SO4 (or SO3) (4a) SOZ + M => products (5) The yield of the SCI, SOZ and the rates of the SCI and SOZ decomposition relative to their reactions with SO2 and H2O, respectively, were estimated from the dependencies of the H2SO4 yield on the concentrations of the reactants.

Published
2016

14. Field measurements of methylglyoxal using proton transfer reaction time-of-flight mass spectrometry and comparison to the DNPH–HPLC–UV method

Author

Michoud, Vincent, Sauvage, Stéphane, Léonardis, Thierry, Fronval, Isabelle, Kukui, Alexandre, Locoge, Nadine, Dusanter, Sébastien, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), 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), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), 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), 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 Ecologie Fonctionnelle et Environnement (ECOLAB), Université Toulouse III - Paul Sabatier (UT3), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut Ecologie et Environnement (INEE), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-Météo France-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche pour le Développement (IRD)-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), Centre for Energy and Environment (CERI EE), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Regional Council Nord-Pas de Calais and the 'Eu-ropean Funds for Regional Economic Development' (FEDER)Région Hauts-de-France, the Ministère de l’Enseignement Supérieur et de la Recherche and the European Fund for Regional Economic Development through the CLIMIBIO project., ANR-11-LABX-0005,Cappa,Physiques et Chimie de l'Environnement Atmosphérique(2011), European Project: 293897,EC:FP7:PEOPLE,FP7-PEOPLE-2011-CIG,DEFI-VOC(2011), Laboratoire Ecologie Fonctionnelle et Environnement (LEFE), Institut Ecologie et Environnement (INEE), Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Observatoire Midi-Pyrénées (OMP), Institut de Recherche pour le Développement (IRD)-Université Toulouse III - Paul Sabatier (UT3), Université de Toulouse (UT)-Université de Toulouse (UT)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université de Toulouse (UT), Centre for Energy and Environment (CERI EE - IMT Nord Europe), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Nord Europe), 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), Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Observatoire Midi-Pyrénées (OMP), Université Fédérale Toulouse Midi-Pyrénées-Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP), Université Fédérale Toulouse Midi-Pyrénées, Département S.A.G.E (SAGE), ANR-11-LABX-0005/11-LABX-0005,Cappa,Physiques et Chimie de l’Environnement Atmosphérique(2011), and Université Fédérale Toulouse Midi-Pyrénées-Université Fédérale Toulouse Midi-Pyrénées-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Institut de Recherche pour le Développement (IRD)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS)-Météo-France -Centre National de la Recherche Scientifique (CNRS)-Institut National Polytechnique (Toulouse) (Toulouse INP)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, ChArMEx, [SDE]Environmental Sciences, [CHIM.OTHE]Chemical Sciences/Other
Abstract

Methylglyoxal (MGLY) is an important atmospheric α-dicarbonyl species for which 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 presents the first field measurements of MGLY by proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS) 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 liquid chromatography (HPLC) with UV detection. PTR-ToF-MS 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 to 365 pptv, with a clear diurnal cycle due to elevated concentrations of primary biogenic species during the daytime, and its oxidation led to large production rates of MGLY. A scatter plot of the PTR-ToF-MS 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 or methyl ethyl ketone (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 artifacts 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-ToF-MS. 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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17. The Atmospheric Reactivity studies Plateform of Orléans-France

Author

Daële, Véronique, Mellouki, A., Catoire, Valéry, Kukui, Alexandre, and MELLOUKI, ABDELWAHID

Subjects
[SDE] Environmental Sciences, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, [CHIM] Chemical Sciences
Published
2018

20. HN[O.sub.3] Forming channel of the H[O.sub.2] + NO reaction as a function of pressure and temperature in the ranges of 72-600 Torr and 223-323 K

Author

Butkovskaya, Nadezhda, Kukui, Alexandre, and Le Bras, Georges

Subjects
Nitric oxide -- Spectra, Chemical reactions -- Analysis, Hydrogen -- Spectra, Chemicals, plastics and rubber industries
Abstract

A high-pressure turbulent flow reactor coupled with a chemical ionization mass-spectrometer is used for determining the branching ratio of the H[O.sub.2] + NO reaction. The pressure and temperature dependence of the branching ratio ([beta]) is determined in the pressure range of 72-600 Torr of [N.sub.2] carrier gas between 323 and 223 K.

Published
2007

21. The Atmospheric Reactivity studies Plateform of Orléans -France

Author

Daële, Véronique, Catoire, Valéry, Kukui, Alexandre, Mellouki, Wahid, Daele, Veronique, and Laboratoires d'excellence - Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment - - VOLTAIRE2010 - ANR-10-LABX-0100 - LABX - VALID

Subjects
[SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere
Published
2016

22. The impact of the chemical production of methyl nitrate from the NO + CH 3 O 2 reaction on the global distributions of alkyl nitrates, nitrogen oxides and tropospheric ozone: a global modelling study

Author

Williams, J.E., Le Bras, G, Kukui, Alexandre, Ziereis, H, Brenninkmeijer, C. A. M., Royal Netherlands Meteorological Institute (KNMI), 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), Deutsches Zentrum für Luft- und Raumfahrt (DLR), Atmospheric Chemistry Department [MPIC], Max Planck Institute for Chemistry (MPIC), Max-Planck-Gesellschaft-Max-Planck-Gesellschaft, and ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, [SDU]Sciences of the Universe [physics]
Abstract

International audience; The formation, abundance and distribution of organic nitrates are relevant for determining the production efficiency and resident mixing ratios of tropospheric ozone (O 3) on both regional and global scales. Here we investigate the effect of applying the recently measured direct chemical production of methyl nitrate (CH 3 ONO 2) during NO x recycling involving the methyl-peroxy radical on the global tropospheric distribution of CH 3 ONO 2 and the perturbations introduced towards tropospheric NO x and O 3 using the TM5 global chemistry transport model. By comparisons against numerous observations, we show that the global surface distribution of CH 3 ONO 2 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 CH 3 ONO 2 converts 1 Tg N yr −1 from nitrogen oxide for this branching ratio. The resident mixing ratios of CH 3 ONO 2 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 (RONO 2) 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 CH 3 ONO 2 , there are persistent overestima-tions 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 RONO 2 , TM5 performs better at tropical latitudes than at mid-latitudes, with similar features in the comparisons to those for CH 3 ONO 2. Comparisons of CH 3 ONO 2 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 (NO y) ∼ 20 % originates from alkyl nitrates in the tropics and subtropics, where the introduction of both direct oceanic emissions and the chemical formation mechanism of CH 3 ONO 2 only makes a ∼ 5 % contribution to the total alkyl nitrate content in the upper tro-posphere when compared with aircraft observations. We find that the increases in tropospheric O 3 that occur due oxidation of CH 3 ONO 2 originating from direct oceanic emission is negated when accounting for the chemical formation of CH 3 ONO 2 , meaning that the impact of such oceanic emissions on atmospheric lifetimes becomes marginal when a branching ratio of 0.3 % is adopted.

Published
2014
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23. OH and RO 2 radicals at Dome C (East Antarctica): first observations and assessment of photochemical budget

Author

Kukui, Alexandre, Loisil, Rodrigue, Kerbrat, Michael, Frey, Markus, Gil, Jaime, Jourdain, Bruno, Ancellet, Gérard, Bekki, Slimane, Legrand, Michel, Preunkert, Susanne, 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, 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), 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 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 de chimie et procédés pour l'énergie, l'environnement et la santé (ICPEES), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et nanosciences d'Alsace, 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), Centre Alpin de Recherche sur les Réseaux Trophiques et Ecosystèmes Limniques (CARRTEL), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut National de la Recherche Agronomique (INRA), 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), and STRATO - LATMOS

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.

Published
2013

24. First investigations of IO, BrO, and NO2 summer atmospheric levels at a coastal East Antarctic site using mode-locked cavity enhanced absorption spectroscopy

Author

Grilli, Roberto, Legrand, Michel, Kukui, Alexandre, Méjean, Guillaume, Preunkert, Suzanne, Romanini, Daniele, LIPhy-LAME, Université Joseph Fourier - Grenoble 1 (UJF)-Laboratoire Interdisciplinaire de Physique [Saint Martin d’Hères] (LIPhy), Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), 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), 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, 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), Laboratoire Interdisciplinaire de Physique [Saint Martin d’Hères] (LIPhy), Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA), National financial support and field logistic supplies for the summer campaign were provided by Institut Polaire Français-Paul Emile Victor (IPEV) within program 414, ANR-09-BLAN-0016,MoCaMAR, ANR-09-BLAN-0226,OPALE, Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Centre National de la Recherche Scientifique (CNRS), 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 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), Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF), ANR-09-BLAN-0016,MoCaMAR(2009), and ANR-09-BLAN-0226,OPALE(2009)

Subjects
[PHYS.PHYS.PHYS-OPTICS]Physics [physics]/Physics [physics]/Optics [physics.optics], Antarctica, Atmospheric oxidants, Radicals
Abstract

International audience; 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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25. Field measurements of methylglyoxal using Proton Transfer Reaction-Time of Flight Mass Spectrometry and comparison to the DNPH/HPLC-UV method.

Author

Michoud, Vincent, Sauvage, Stéphane, Léonardis, Thierry, Fronval, Isabelle, Kukui, Alexandre, Locoge, Nadine, and Dusanter, Sébastien

Subjects
PYRUVALDEHYDE, PROTON transfer reactions, HIGH performance liquid chromatography
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. [ABSTRACT FROM AUTHOR]

Published
2018
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26. Oxidant Production over Antarctic Land and its Export (OPALE) project: An overview of the 2010-2011 summer campaign

Author

Preunkert, Susanne, Ancellet, Gérard, Legrand, Michel R., Kukui, Alexandre, Kerbrat, Michael, Sarda-Estève, Roland, Gros, Valérie, Jourdain, Bruno, 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), 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 des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE), 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), Chimie Atmosphérique Expérimentale (CAE), 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), Agence Nationale de la Recherche (ANR), Institut Polaire Français-Paul Emile Victor (IPEV), Centre National de la Recherche Scientifique (CNRS/INSU), Commissariat à l'Energie Atomique (CEA), Région Ile de France, European Commission, ANR-09-BLAN-0226,OPALE(2009), European Project: 252086,EC:FP7:PEOPLE,FP7-PEOPLE-2009-IEF,ANTARCTIC HONO(2010), 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), 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), ANR-09-BLAN-0226,OPALE,Oxidant Production over Antarctica Land and its Export(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), 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), and 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)

Subjects
Hydroxyl radicals, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Antarctic photochemistry, Atmospheric oxidants, Nitrous acid
Abstract

International audience; 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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27. Measurements of OH and RO2 radicals at the coastal Antarctic site of Dumont d'Urville (East Antarctica) in summer 2010-2011

Author

Kukui, Alexandre, Legrand, Michel R., Ancellet, Gérard, Gros, Valérie, Bekki, Slimane, Sarda-Estève, Roland, Loisil, Rodrigue, Preunkert, Suzanne, 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 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), 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), STRATO - LATMOS, Division technique INSU/SDU (DTI), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Agence Nationale de la Recherche (ANR), Institut Polaire Français-Paul Emile Victor (IPEV), Centre National de la Recherche Scientifique (INSU), Centre Energie Atomique (CEA), Region Ile de France, ANR-09-BLAN-0226,OPALE(2009), 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), 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), 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), 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), and 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)

Subjects
Hydroxyl radicals, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Antarctic photochemistry, Atmospheric oxidants
Abstract

International audience; Measurements of OH and total proxy RO2 (HO2 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 × 106 and 3.3 × 108 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 O3 and HCHO representing via their photolysis the major primary radical sources. The observed OH levels at DDU could be explained only assuming some RO2 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 RO2 recycling in continental air masses.

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, Daniel, Evans, M.J., Chipperfield, M.P., Butkovskaya, N., Kukui, Alexandre, Le Bras, Georges, Météo-France [Paris], Météo France, Centre Européen de Recherche et de Formation Avancée en Calcul Scientifique (CERFACS), CERFACS, Institute for Climate and Atmospheric Science [Leeds] (ICAS), 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), 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), Météo-France, and Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS - CNRS)

Subjects
lcsh:Chemistry, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], lcsh:QD1-999, lcsh:Physics, lcsh:QC1-999
Abstract

We have studied the impact of the recently observed 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. The mean global decrease in OH is around 13%, which is very large compared to the impact that typical photochemical revisions have on this modelled quantity. This OH decrease leads to an 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
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29. Inter-annual variability of surface ozone at coastal (Dumont d'Urville, 2004-2014) and inland (Concordia, 2007-2014) sites in East Antarctica.

Author

Legrand, Michel, Preunkert, Susanne, Savarino, Joël, Frey, Markus M., Kukui, Alexandre, Helmig, Detlev, Jourdain, Bruno, Jones, Anna E., Weller, Rolf, Brough, Neil, and Gallée, Hubert

Subjects
ATMOSPHERIC ozone, METEOROLOGICAL observations, ULTRAVIOLET radiation, SOLAR radiation, BROMINE
Abstract

Surface ozone has been measured since 2004 at the coastal East Antarctic site of Dumont d'Urville (DDU), and since 2007 at the Concordia station located on the high East Antarctic plateau. This paper discusses long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites. At Concordia, near-surface ozone data were complemented by balloon soundings and compared to similar measurements done at the South Pole. The DDU record is compared to those obtained at the coastal site of Syowa, also located in East Antarctica, as well as the coastal sites of Neumayer and Halley, both located on the coast of the Weddell Sea in West Antarctica. Surface ozone mixing ratios exhibit very similar seasonal cycles at Concordia and the South Pole. However, in summer the diurnal cycle of ozone is different at the two sites with a drop of ozone in the afternoon at Concordia but not at the South Pole. The vertical distribution of ozone above the snow surface also differs. When present, the ozone-rich layer located near the ground is better mixed and deeper at Concordia (up to 400 m) than at the South Pole during sunlight hours. These differences are related to different solar radiation and wind regimes encountered at these two inland sites. DDU appears to be the coastal site where the impact of the late winter/spring bromine chemistry is the weakest, but where the impact of elevated ozone levels caused by NOx snow emissions from the high Antarctic plateau is the highest. The highest impact of the bromine chemistry is seen at Halley and Neumayer, and to a lesser extent at Syowa. These three sites are only weakly impacted by the NOx chemistry and the net ozone production occurring on the high Antarctic plateau. The differences in late winter/spring are attributed to the abundance of sea ice offshore from the sites, whereas those in summer are related to the topography of East Antarctica that promotes the katabatic flow bringing oxidant-rich inland air masses to the site. There appears to be a decreasing change in summer surface ozone at the two East Antarctic sites of Concordia and DDU over the most recent period (2004-2014 and 2007-2014). Further research, including continued monitoring, is needed at these two sites to better separate the effect of synoptic transport from possible change of NOx snow emissions in response to recovery of the stratospheric ozone layer leading to penetration of more UV radiation to the surface. [ABSTRACT FROM AUTHOR]

Published
2016
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30. Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign.

Author

Savarino, Joël, Vicars, William C., Legrand, Michel, Preunkert, Suzanne, Jourdain, Bruno, Frey, Markus M., Kukui, Alexandre, Caillon, Nicolas, and Roca, Jaime Gil

Subjects
ATMOSPHERIC aerosols, OXYGEN isotopes, MASS budget (Geophysics), NITRATES & the environment, CHEMICAL precursors
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. [ABSTRACT FROM AUTHOR]

Published
2016
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31. Pressure and TemperatureDependence of Methyl NitrateFormation in the CH3O2+ NO Reaction.

Author

Butkovskaya, Nadezhda, Kukui, Alexandre, and Le Bras, Georges

Subjects
*PRESSURE, *TEMPERATURE effect, *METHYL nitrate, *NITRIC oxide, *TURBULENCE, *CHEMICAL ionization mass spectrometry, *STRATOSPHERE, *CHEMICAL reactions
Abstract

The branching ratio β = k1b/k1afor the formation of methylnitrate, CH3ONO2, in the gas-phase CH3O2+ NO reaction, CH3O2+ NO →CH3O + NO2(1a), CH3O2+ NO→ CH3ONO2(1b), has been determined overthe pressure and temperature ranges 50–500 Torr and 223–300K, respectively, using a turbulent flow reactor coupled with a chemicalionization mass spectrometer. At 298 K, the CH3ONO2yield has been found to increase linearly with pressure from0.33 ± 0.16% at 50 Torr to 0.80 ± 0.54% at 500 Torr (errorsare 2σ). Decrease of temperature from 300 to 220 K leads toan increase of β by a factor of about 3 in the 100–200Torr range. These data correspond to a value of β ≈ 1.0± 0.7% over the pressure and temperature ranges of the wholetroposphere. Atmospheric concentrations of CH3ONO2roughly estimated using results of this work are in reasonable agreementwith those observed in polluted environments and significantly highercompared with measurements in upper troposphere and lower stratosphere. [ABSTRACT FROM AUTHOR]

Published
2012
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32. Atmospheric chamber measurements of H2SO4: characterization of formation and loss rates during the ozonolysis and aerosol formation studies.

Author

Ren, Yangang, Kukui, Alexandre, Ahmad, Waed, Bernard, Francois, Leglise, Joris, Zhou, Li, Cai, Min, Coujou, Clara, Benoit, Roland, Catoire, Valéry, Daële, Veronique, and Mellouki, Abdelwahid

Subjects
*AEROSOLS, *PINENE, *SULFUR dioxide, *OZONOLYSIS, *HYDROXYL group, *VOLATILE organic compounds, *SULFURIC acid
Abstract

Sulphuric acid, H2SO4, has been identified to play major role in atmospheric new particleformation and in subsequent particle growth. The oxidation of sulfur dioxide (SO2) tosulfur trioxide (SO3) initiated by the reaction with the hydroxyl radicals (OH) isassumed to be the dominant formation pathway of sulfuric acid (H2SO4) in thetroposphere. It has been suggested in the recent years that the reactions of CriegeeIntermediates (CIs) with SO2 may also contribute to the H2SO4 formation, althoughthe significance of this pathway compared to the reaction of OH with SO2 is stillunder discussion. As the ozonolysis of anthropogenic and biogenic terpenes emittedinto the atmosphere may represent an important source of OH and CIs a betterunderstanding of the ozonolysis mechanism in relation to the H2SO4 formation isrequired. In this study, we present the results obtained during the investigation of the ozonolysis ofseveral unsaturated volatile organic compounds, including tetramethylethylene, α-pinene andlimonene, using a newly constructed large atmospheric simulation chamber, HELIOS(ICARE-CNRS, Orléans, France). The HELIOS facility consists of a large outdoorsimulation chamber (volume of 90 m3) equipped with a wide range of in-situ on-line andoff-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 andmechanistic studies of the reactions of different CIs with SO2 induced by the ozonolysis ofthe studied VOCs under different conditions will be presented. The H2SO4 loss on the Teflonchamber wall and by the aerosol uptake were characterized using direct H2SO4 and particlemeasurements. Keywords: ozonolysis, Criegee Intermediate, sulfur dioxide, sulfuric acid, HELIOS [ABSTRACT FROM AUTHOR]

Published
2019

34. 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

35. 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

36. 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

37. Intercomparison of peroxy radical instruments at the HELIOS atmospheric simulation chamber

Author

LAHIB, A., Duncianu, M., TOMAS, A., SCHOEMAECKER, C., Batut, S., KUKUI, A., Ren, Y., Zhou, L., Benoit, R., Grosselin, B., Daele, V., Mellouki, A., STEVENS, P., Dusanter, S., KUKUI, Alexandre, IMT Lille Douai, Institut Mines-Télécom, Univ. Lille, Centre for Materials and Processes, F-59000 Lille, France, 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), Ecole nationale supérieure Mines-Télécom Lille Douai (IMT Lille Douai), Institut Mines-Télécom [Paris] (IMT), Université des Sciences et Technologies (Lille 1) (USTL), Ford Motor Company, Research and Advanced Engineering, Mail Drop RIC-2122, Dearborn, Michigan 48121-2053, USA, INDIANA UNIVERSITY SCHOOL OF PUBLIC AND ENVIRONMENTAL AFFAIRS BLOOMINGTON USA, Partenaires IRSTEA, and Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, 0341 Middle atmosphere: constituent transport and chemistry, 0305 Aerosols and particles, 0317 Chemical kinetic and photochemical properties, [SDU.OCEAN] Sciences of the Universe [physics]/Ocean, Atmosphere, 0312 Air/sea constituent fluxes, [INFO]Computer Science [cs], ATMOSPHERIC COMPOSITION AND STRUCTURE, ComputingMilieux_MISCELLANEOUS
Abstract

International audience; Peroxy radicals (HO 2 and RO 2 ) are key species in atmospheric chemistry, which together with the hydroxyl radical (OH), are involved in oxidation processes leading to the formation of secondary pollutants such as ozone and organic aerosols. Monitoring these short-lived species during intensive field campaigns and comparing the measured concentrations to box model simulations allow assessing the reliability of chemical mechanisms implemented in atmospheric models. However, ambient measurements of peroxy radicals are still considered challenging and only a few techniques have been used for field measurements. Three complementary instruments capable of ambient measurements of pe roxy radicals have been deployed together at the HELIOS atmospheric simulation chamber (Orléans, France) in October 2018. These instruments rely on the PEroxy Radical Chemical Amplification (PERCA), Laser Induced Fluorescence-Fluorescent Assay by Gas Expansion (LIF-FAGE), and Chemical Ionisation Mass Spectrometry (CIMS) techniques. Several chamber experiments have been conducted under dark and irradiated conditions, including oxidation experiments of dihydrogen, methane, pentene, isoprene, and α-pinene. In this presentation, the agreement between the different instruments will be discussed in the light of supporting measurements of volatile organic compounds and inorganic species (O3, NO, NO2), photolysis frequencies, as well as box modelling of the chamber chemistry.

Published
2019

38. 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

39. 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

40. 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

41. 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

42. 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

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