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1. Shedding light on tropospheric H2SO4 production from Criegee intermediates + SO2: a comprehensive laboratory chamber study using the highly instrumented HELIOS platform

Author

Max R. McGillen, Abdelwahid Mellouki, Alexandre Kukui, Véronique Daële, Yangang Ren, Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut des Sciences de l'Ingénierie et des Systèmes (INSIS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National d’Études Spatiales [Paris] (CNES), interaction Clouds Aerosols Radiations - ICARE/AERIS Data and Services Center - UMS 2877 (ICARE), Centre National de la Recherche Scientifique (CNRS)-Centre National d'Études Spatiales [Toulouse] (CNES)-Université de Lille, ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), and Centre National d'Études Spatiales [Toulouse] (CNES)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)

Subjects
[SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, Troposphere, 13. Climate action, Environmental science, HeliOS, Laboratory chamber, Atmospheric sciences, 7. Clean energy, ComputingMilieux_MISCELLANEOUS
Abstract

Although the dominant source of H2SO4 in the atmosphere is generally considered to be the reaction of SO2 with OH, it is probable that the rapid reactions of Criegee intermediates (CIs) with SO2 can contribute significantly to the tropospheric H2SO4 budget under certain conditions. CIs are produced from alkene ozonolysis, and the vast quantities of unsaturated biogenic and anthropogenic volatile organic compounds emitted could provide a large and diverse flux of CIs to the atmosphere. There remain several key uncertainties regarding the global importance of CIs towards SO2 oxidation, which are principally related to the ambient concentrations of CIs and the competition between CI reaction with SO2 against the many other bimolecular and unimolecular loss processes. This is especially true of the larger, more complex CIs that are produced from terpene ozonolysis.We present experimental studies of the ozonolysis of tetramethylethylene, α-pinene and limonene, using the HELIOS chamber. HELIOS is a highly instrumented large-scale outdoor atmospheric simulation chamber and consists of a hemispheric 90 m3 Teflon-foil reactor, which is interfaced to a variety of on-line measurements including FTIR, PTR-ToF-MS, FIGAERO-ToF-CIMS, OH/H2SO4-CIMS, Aerolaser HCHO, LOPAP and SMPS, together with several GC-MS/FID and LC-MS instruments and a suite of monitors (NO, NO2, O3). Equipped with this range of instrumentation we are able to conduct alkene ozonolysis under near-ambient conditions, whilst we also have a high coverage of key reactive species in the systems of interest.From our results, we are able to provide new information regarding kinetic and mechanistic behaviour of several atmospherically important CIs and their reactive intermediates, providing new constraints on the role of CIs on the tropospheric H2SO4 budget.Keywords: ozonolysis, Criegee Intermediate, sulfur dioxide, sulfuric acid, kinetics

Published
2021
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2. Evidence of atmospheric nanoparticle formation from emissions of marine microorganisms

Author

David Parin, Nicolas Marchand, Karine Sellegri, A.N. Schwier, Sébastien Mas, Jorge Pey, A. Culot, Barbara D'Anna, Bruno Charrière, Clémence Rose, Alexandre Kukui, Brice Temime-Roussel, Richard Sempéré, Alfonso Saiz-Lopez, Anoop S. Mahajan, and H. L. Dewitt

Subjects
010504 meteorology & atmospheric sciences, Microorganism, Nucleation, Nanoparticle, Climate change, Pelagic zone, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Aerosol, Atmosphere, Geophysics, 13. Climate action, General Earth and Planetary Sciences, Particle, Environmental science, 14. Life underwater, 0105 earth and related environmental sciences
Abstract

Earth, as a whole, can be considered as a living organism emitting gases and particles into its atmosphere, in order to regulate its own temperature. In particular, oceans may respond to climate change by emitting particles that ultimately will influence cloud coverage. At the global scale, a large fraction of the aerosol number concentration is formed by nucleation of gas-phase species, but this process has never been directly observed above oceans. Here we present, using semicontrolled seawater-air enclosures, evidence that nucleation may occur from marine biological emissions in the atmosphere of the open ocean. We identify iodine-containing species as major precursors for new particle clusters’ formation, while questioning the role of the commonly accepted dimethyl sulfide oxidation products, in forming new particle clusters in the region investigated and within a time scale on the order of an hour. We further show that amines would sustain the new particle formation process by growing the new clusters to larger sizes. Our results suggest that iodine-containing species and amines are correlated to different biological tracers. These observations, if generalized, would call for a substantial change of modeling approaches of the sea-to-air interactions.

Published
2016
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3. Atmospheric nitrogen oxides (NO and NO2) at Dome C, East Antarctica, during the OPALE campaign

Author

Joel Savarino, Martin D. King, S. Preunkert, Markus M. Frey, Michel Legrand, Howard K. Roscoe, and Alexandre Kukui

Subjects
Atmospheric Science, Ozone, Reactive nitrogen, Planetary boundary layer, Firn, Snow, Atmospheric sciences, Troposphere, chemistry.chemical_compound, chemistry, 13. Climate action, Atmospheric chemistry, Environmental science, NOx
Abstract

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

Published
2015
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4. Study of the unknown HONO daytime source at a European suburban site during the MEGAPOLI summer and winter field campaigns

Author

Sébastien Perrier, Charbel Afif, Matthias Beekmann, K. Miet, Markus Furger, Aurélie Colomb, Jean-Charles Dupont, Guillaume Siour, Martial Haeffelin, Alexandre Kukui, P. Zapf, Bernard Aumont, Jean-François Doussin, Vincent Michoud, Marie Camredon, Agnès Borbon, W. Ait-Helal, Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA (UMR_7583)), Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de météorologie physique (LaMP), Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Analytiques (ISA), Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), École des Mines de Douai (Mines Douai EMD), Institut Mines-Télécom [Paris] (IMT), Université Lille Nord (France), Centre d’Analyses et de Recherche, Centre d’Analyses et de Recherche - Lebanon, TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), Paul Scherrer Institute (PSI), Institut Pierre-Simon-Laplace (IPSL), École normale supérieure - Paris (ENS-PSL), Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-École polytechnique (X)-Centre National d'Études Spatiales [Toulouse] (CNES)-Centre National de la Recherche Scientifique (CNRS), ANR-09-BLAN-0356,MEGAPOLI-PARIS,MEGAPOLI - PARIS : Pollution des AéRosols: Impact sur la qualité de l'air et quantification des Sources(2009), ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), European Project: 212520,EC:FP7:ENV,FP7-ENV-2007-1,MEGAPOLI(2008), European Project: 228335,EC:FP7:INFRA,FP7-INFRASTRUCTURES-2008-1,EUROCHAMP-2(2009), Université Paris-Est Créteil Val-de-Marne - Paris 12 (UPEC UP12)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris Diderot - Paris 7 (UPD7)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP), Centre National de la Recherche Scientifique (CNRS)-Université de Lyon-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-École normale supérieure - Lyon (ENS Lyon), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), École normale supérieure - Paris (ENS Paris)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National d'Études Spatiales [Toulouse] (CNES)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-École polytechnique (X), ANR-10-LABX-100-01/10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Centre National de la Recherche Scientifique (CNRS)-Université Blaise Pascal - Clermont-Ferrand 2 (UBP)-Institut national des sciences de l'Univers (INSU - CNRS), Institut de Chimie du CNRS (INC)-Université Claude Bernard Lyon 1 (UCBL), Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), and École normale supérieure - Paris (ENS Paris)

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, Daytime, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Wind direction, Noon, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, Wind speed, Aerosol, lcsh:Chemistry, lcsh:QD1-999, [SDU]Sciences of the Universe [physics], 13. Climate action, Photostationary state, [SDE]Environmental Sciences, Environmental science, Relative humidity, [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, Water content, lcsh:Physics, 0105 earth and related environmental sciences
Abstract

Nitrous acid measurements were carried out during the MEGAPOLI summer and winter field campaigns at SIRTA observatory in Paris surroundings. Highly variable HONO levels were observed during the campaigns, ranging from 10 ppt to 500 ppt in summer and from 10 ppt to 1.7 ppb in winter. Significant HONO mixing ratios have also been measured during daytime hours, comprised between some tenth of ppt and 200 ppt for the summer campaign and between few ppt and 1 ppb for the winter campaign. Ancillary measurements, such as NOx, O3, photolysis frequencies, meteorological parameters (pressure, temperature, relative humidity, wind speed and wind direction), black carbon concentration, total aerosol surface area, boundary layer height and soil moisture, were conducted during both campaigns. In addition, for the summer period, OH radical measurements were made with a CIMS (Chemical Ionisation Mass Spectrometer). This large dataset has been used to investigate the HONO budget in a suburban environment. To do so, calculations of HONO concentrations using PhotoStationary State (PSS) approach have been performed, for daytime hours. The comparison of these calculations with measured HONO concentrations revealed an underestimation of the calculations making evident a missing source term for both campaigns. This unknown HONO source exhibits a bell-shaped like average diurnal profile with a maximum around noon of approximately 0.7 ppb h−1 and 0.25 ppb h−1, during summer and winter respectively. This source is the main HONO source during daytime hours for both campaigns. In both cases, this source shows a slight positive correlation with J(NO2) and the product between J(NO2) and soil moisture. This original approach had, thus, indicated that this missing source is photolytic and might be heterogeneous occurring at ground surface and involving water content available on the ground., Atmospheric Chemistry and Physics, 14 (6), ISSN:1680-7375, ISSN:1680-7367

Published
2014
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5. First investigations of IO, BrO, and NO2summer atmospheric levels at a coastal East Antarctic site using mode-locked cavity enhanced absorption spectroscopy

Author

Daniele Romanini, G. Méjean, Alexandre Kukui, Suzanne Preunkert, Michel Legrand, and Roberto Grilli

Subjects
Detection limit, Marine boundary layer, 010504 meteorology & atmospheric sciences, Absorption spectroscopy, Planetary boundary layer, East antarctica, Atmospheric sciences, 01 natural sciences, 010309 optics, Geophysics, 13. Climate action, 0103 physical sciences, General Earth and Planetary Sciences, Oxidative capacity, 14. Life underwater, Spectroscopy, Enhanced absorption, 0105 earth and related environmental sciences
Abstract

[1] IO, BrO, and NO2 were measured for the first time at Dumont d'Urville (East Antarctic coast) during summer 2011/2012 by using a near-UV-Visible laser spectrometer based on mode-locked cavity-enhanced absorption spectroscopy. IO mixing ratios ranged from the 2σ detection limit (0.04 pptv) up to 0.15 pptv. BrO remained close or below the detection limit (2 pptv) of the instrument. Daily averaged NO2 values ranged between the detection limit (10 pptv) and 60 pptv being far higher than levels of a few pptv commonly observed in the remote marine boundary layer. Data are discussed and compared with those available for another coastal Antarctic station (Halley, West Antarctica). It is shown that the oxidative capacity of the atmospheric boundary layer at coastal Antarctic sites is quite different in nature from West to East Antarctica, with the halogen chemistry being promoted at West and the OH chemistry at East.

Published
2013
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6. Oxygen isotope mass balance of atmospheric nitrate at Dome C, East Antarctica, during the OPALE campaign

Author

Jaime Gil Roca, Alexandre Kukui, Joel Savarino, Nicolas Caillon, S. Preunkert, William Vicars, Bruno Jourdain, Michel Legrand, Markus M. Frey, Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG ), Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Université Grenoble Alpes [2016-2019] (UGA [2016-2019]), Colorado Department of Public Health and Environment, University of Colorado [Denver], Institute of Arctic and Alpine Research (INSTAAR), University of Colorado [Boulder], British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), European Community's Seventh Framework Programme (FP7/2007-2013), INSU (LEFE Programme), Agence Nationale de la Recherche (ANR), IPEV (programme SUNITEDC n° 1011), ANR-05-PGCU-0004,OPALE,Risque d'inondation en ville et évaluation de scénarios(2005), ANR-10-LABX-0056,OSUG@2020,Innovative strategies for observing and modelling natural systems(2010), European Project: 237890,EC:FP7:PEOPLE,FP7-PEOPLE-ITN-2008,INTRAMIF(2009), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), CNRS-INSU : LEFE programThe Institute Polaire Paul-Emile Victor (IPEV)the program SUNITEDC No. 1011, Université Grenoble Alpes (UGA), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), ANR: OPALE,NT09-451281, ANR-10-LABX-0056/10-LABX-0056,OSUG@2020,Innovative strategies for observing and modelling natural systems(2010), ANR10 LABX56,ANR10 LABX56, and Institute of Arctic Alpine Research [University of Colorado Boulder] (INSTAAR)

Subjects
Hydrology, [PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, Ozone, 010504 meteorology & atmospheric sciences, δ18O, 010401 analytical chemistry, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Isotopes of oxygen, lcsh:QC1-999, 0104 chemical sciences, lcsh:Chemistry, chemistry.chemical_compound, Isotopic signature, chemistry, Nitrate, Ice core, lcsh:QD1-999, 13. Climate action, NOx, lcsh:Physics, Isotope analysis, 0105 earth and related environmental sciences
Abstract

Variations in the stable oxygen isotope composition of atmospheric nitrate act as novel tools for studying oxidative processes taking place in the troposphere. They provide both qualitative and quantitative constraints on the pathways determining the fate of atmospheric nitrogen oxides (NO + NO2 = NOx). The unique and distinctive 17O excess (Δ17O = δ17O − 0.52 × δ18O) of ozone, which is transferred to NOx via oxidation, is a particularly useful isotopic fingerprint in studies of NOx transformations. Constraining the propagation of 17O excess within the NOx cycle is critical in polar areas, where there exists the possibility of extending atmospheric investigations to the glacial–interglacial timescale using deep ice core records of nitrate. Here we present measurements of the comprehensive isotopic composition of atmospheric nitrate collected at Dome C (East Antarctic Plateau) during the austral summer of 2011/2012. Nitrate isotope analysis has been here combined for the first time with key precursors involved in nitrate production (NOx, O3, OH, HO2, RO2, etc.) and direct observations of the transferrable Δ17O of surface ozone, which was measured at Dome C throughout 2012 using our recently developed analytical approach. Assuming that nitrate is mainly produced in Antarctica in summer through the OH + NO2 pathway and using concurrent measurements of OH and NO2, we calculated a Δ17O signature for nitrate on the order of (21–22 ± 3) ‰. These values are lower than the measured values that ranged between 27 and 31 ‰. This discrepancy between expected and observed Δ17O(NO3−) values suggests the existence of an unknown process that contributes significantly to the atmospheric nitrate budget over this East Antarctic region. However, systematic errors or false isotopic balance transfer functions are not totally excluded.

Published
2016
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7. Large mixing ratios of atmospheric nitrous acid (HONO) at Concordia (East Antarctic Plateau) in summer: a strong source from surface snow?

Author

Bruno Jourdain, Joel Savarino, Alexandre Kukui, S. Preunkert, Michel Kerbrat, Th Bartels-Rausch, Michel Legrand, Martin D. King, Markus M. Frey, Université Joseph Fourier - Grenoble 1 (UJF), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Laboratory of Radio- and Environmental Chemistry [Villigen], Paul Scherrer Institute (PSI), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), School of Earth Sciences [Bristol], University of Bristol [Bristol], NERC NE/F0004796/1 and NE/F010788, and NERC FSF grants 555.0608 and 584.0609, Institut Polaire Français-Paul Emile Victor (IPEV), Italian colleagues from Meteo- Climatological Observatory of PNRA for the meteorological data collected at Concordia., ANR-09-BLAN-0226,OPALE(2009), ANR-11-JS56-0005,MONISNOW,Suivi temporel de la neige dans un climat changeant(2011), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), ANR-09-BLAN-0226,OPALE, and ANR-11- JS56-005-01,MONISNOW

Subjects
Atmospheric Science, Nitrous acid, 010504 meteorology & atmospheric sciences, 010501 environmental sciences, Atmospheric sciences, Snow, 01 natural sciences, lcsh:QC1-999, Atmosphere, lcsh:Chemistry, chemistry.chemical_compound, chemistry, lcsh:QD1-999, 13. Climate action, [SDU]Sciences of the Universe [physics], Mixing ratio, Absorption (electromagnetic radiation), [SDU.ENVI]Sciences of the Universe [physics]/Continental interfaces, environment, NOx, Mixing (physics), lcsh:Physics, Antarctic plateau, 0105 earth and related environmental sciences
Abstract

During the austral summer 2011/2012 atmospheric nitrous acid (HONO) was investigated for the second time at the Concordia site (75°06' S, 123°33' E), located on the East Antarctic Plateau, by deploying a long-path absorption photometer (LOPAP). Hourly mixing ratios of HONO measured in December 2011/January 2012 (35 ± 5.0 pptv) were similar to those measured in December 2010/January 2011 (30.4 ± 3.5 pptv). The large value of the HONO mixing ratio at the remote Concordia site suggests a local source of HONO in addition to weak production from oxidation of NO by the OH radical. Laboratory experiments demonstrate that surface snow removed from Concordia can produce gas-phase HONO at mixing ratios half that of the NOx mixing ratio produced in the same experiment at typical temperatures encountered at Concordia in summer. Using these lab data and the emission flux of NOx from snow estimated from the vertical gradient of atmospheric concentrations measured during the campaign, a mean diurnal HONO snow emission ranging between 0.5 and 0.8 × 109 molecules cm−2 s−1 is calculated. Model calculations indicate that, in addition to around 1.2 pptv of HONO produced by the NO oxidation, these HONO snow emissions can only explain 6.5 to 10.5 pptv of HONO in the atmosphere at Concordia. To explain the difference between observed and simulated HONO mixing ratios, tests were done both in the field and at lab to explore the possibility that the presence of HNO4 had biased the measurements of HONO.

Published
2014
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8. Formaldehyde (HCHO) in air, snow and interstitial air at Concordia (East Antarctic plateau) in summer

Author

Alexandre Kukui, Detlev Helmig, Hubert Gallée, Markus M. Frey, Joel Savarino, Martin D. King, Bruno Jourdain, William Vicars, Susanne Preunkert, Michel Legrand, Université Joseph Fourier - Grenoble 1 (UJF), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), British Antarctic Survey (BAS), Natural Environment Research Council (NERC), TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université d'Orléans (UO)-Observatoire de Paris, PSL Research University (PSL)-PSL Research University (PSL)-Centre National d’Études Spatiales [Paris] (CNES), Department of Physics [Egham], Royal Holloway [University of London] (RHUL), Institute of Arctic and Alpine Research (INSTAAR), University of Colorado [Boulder], ANR-10-LABX-100-01/10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010), Birmingham City University (BCU), Agence Nationale de la Recherche (ANR), Institut Polaire Français- Paul Emile Victor (IPEV), ANR-09-BLAN-0226,OPALE,Oxidant Production over Antarctica Land and its Export(2009), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales [Paris] (CNES), ANR-09-BLAN-0226,OPALE(2009), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS), Institute of Arctic Alpine Research [University of Colorado Boulder] (INSTAAR), and ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010)

Subjects
[PHYS.PHYS.PHYS-AO-PH]Physics [physics]/Physics [physics]/Atmospheric and Oceanic Physics [physics.ao-ph], Atmospheric Science, 010504 meteorology & atmospheric sciences, Formaldehyde, 010501 environmental sciences, Snowpack, Noon, Snow, Atmospheric sciences, 01 natural sciences, lcsh:QC1-999, lcsh:Chemistry, chemistry.chemical_compound, Flux (metallurgy), lcsh:QD1-999, chemistry, 13. Climate action, Diurnal cycle, [SDU]Sciences of the Universe [physics], Climatology, Anaerobic oxidation of methane, [SDE]Environmental Sciences, Mixing ratio, lcsh:Physics, 0105 earth and related environmental sciences
Abstract

International audience; During the 2011/12 and 2012/13 austral summers , HCHO was investigated for the first time in ambient air, snow, and interstitial air at the Concordia site, located near Dome C on the East Antarctic Plateau, by deploying an Aerolaser AL-4021 analyzer. Snow emission fluxes were estimated from vertical gradients of mixing ratios observed at 1 cm and 1 m above the snow surface as well as in interstitial air a few centimeters below the surface and in air just above the snowpack. Typical flux values range between 1 and 2 × 1012 molecules m-2 s-1 at night and 3 and 5 × 1012 molecules m-2 s-1 at noon. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible compared to temperature-driven air–snow exchanges. At 1 m above the snow surface, the observed mean mixing ratio of 130 pptv and its diurnal cycle characterized by a slight decrease around noon are quite well reproduced by 1-D simulations that include snow emissions and gas-phase methane oxidation chemistry. Simulations indicate that the gas-phase production from CH4 oxidation largely contributes (66 %) to the observed HCHO mixing ratios. In addition, HCHO snow emissions account for ∼ 30 % at night and ∼ 10 % at noon to the observed HCHO levels.

Published
2014
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9. The impact of the chemical production of methyl nitrate from the NO + CH3O2 reaction on the global distributions of alkyl nitrates, nitrogen oxides and tropospheric ozone: a global modeling study

Author

Helmut Ziereis, G. Le Bras, Alexandre Kukui, Carl A. M. Brenninkmeijer, and J. E. Williams

Subjects
Atmospheric Science, 010504 meteorology & atmospheric sciences, Reactive nitrogen, Chemistry, 15. Life on land, 010501 environmental sciences, Atmospheric sciences, 01 natural sciences, Troposphere, chemistry.chemical_compound, Deposition (aerosol physics), Nitrate, 13. Climate action, Climatology, Nitrogen oxide, Tropospheric ozone, Methyl nitrate, NOx, 0105 earth and related environmental sciences
Abstract

The formation, abundance and distribution of organic nitrates are relevant for determining the production efficiency and resident mixing ratios of tropospheric ozone (O3) on both regional and global scales. Here we investigate the effect of applying the recently measured direct chemical production of methyl nitrate (CH3ONO2) during NOx recycling involving the methyl-peroxy radical on the global tropospheric distribution of CH3ONO2 and the perturbations introduced towards tropospheric NOx and O3 using the TM5 global chemistry transport model. By comparisons against numerous observations, we show that the global surface distribution of CH3ONO2 can be largely explained by introducing the chemical production mechanism using a branching ratio of 0.3%, when assuming a direct oceanic emission source of ~0.15 Tg N yr−1. On a global scale, the chemical production of CH3ONO2 converts 1 Tg N yr−1 from nitrogen oxide for this branching ratio. The resident mixing ratios of CH3ONO2 are found to be highly sensitive to the dry deposition velocity that is prescribed, where more than 50% of the direct oceanic emission is lost near the source regions, thereby mitigating the subsequent effects due to long-range and convective transport out of the source region. For the higher alkyl nitrates (RONO2) we find improvements in the simulated distribution near the surface in the tropics (10° S–10° N) when introducing direct oceanic emissions equal to ~0.17 Tg N yr−1 . In terms of the vertical profile of CH3ONO2, there are persistent overestimations in the free troposphere and underestimations in the upper troposphere across a wide range of latitudes and longitudes when compared against data from measurement campaigns. This suggests either a missing transport pathway or source/sink term, although measurements show significant variability in resident mixing ratios at high altitudes at global scale. For the vertical profile of RONO2, TM5 performs better at tropical latitudes than at mid-latitudes, with similar features in the comparisons to those for CH3ONO2. Comparisons of CH3ONO2 with a wide range of surface measurements shows that further constraints are necessary regarding the variability in the deposition terms for different land surfaces in order to improve on the comparisons presented here. For total reactive nitrogen (NOy) ~20% originates from alkyl nitrates in the tropics and subtropics, where the introduction of both direct oceanic emissions and the chemical formation mechanism of CH3ONO2 only makes a ~5% contribution to the total alkyl nitrate content in the upper troposphere when compared with aircraft observations. We find that the increases in tropospheric O3 that occur due oxidation of CH3ONO2 originating from direct oceanic emission is negated when accounting for the chemical formation of CH3ONO2, meaning that the impact of such oceanic emissions on atmospheric lifetimes becomes marginal when a branching ratio of 0.3% is adopted.

Published
2013
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10. Oxidant Production over Antarctic Land and its Export (OPALE) project: An overview of the 2010-2011 summer campaign

Author

Gérard Ancellet, Valérie Gros, Michel Legrand, Alexandre Kukui, Bruno Jourdain, Michael Kerbrat, Susanne Preunkert, and Roland Sarda-Esteve

Subjects
Atmospheric Science, Marine boundary layer, 010504 meteorology & atmospheric sciences, Planetary boundary layer, Soil Science, 010501 environmental sciences, Aquatic Science, Oceanography, Atmospheric sciences, High ozone, 01 natural sciences, Geochemistry and Petrology, Earth and Planetary Sciences (miscellaneous), 14. Life underwater, Air mass, 0105 earth and related environmental sciences, Earth-Surface Processes, Water Science and Technology, Ecology, Chemical measurement, Paleontology, Forestry, East antarctica, Geophysics, 13. Climate action, Space and Planetary Science
Abstract

[1] This paper summarizes the objectives and setting of the OPALE (Oxidant Production over Antarctic Land and its Export) project during summer 2010/2011 at Dumont d'Urville. The primary goal of the campaign is to characterize the oxidizing environment of the atmospheric boundary layer along the coast of East Antarctica. A summary of the relevant field chemical measurements is presented including the carbon monoxide and ammonia records that are used here to identify local influences due to station activities and penguin emissions. An overview of the basic meteorological conditions experienced by the site is presented including the results from the trajectory/dispersion model FLEXPART to highlight which types of air mass were sampled (marine boundary layer versus continental Antarctic air). The results of the FLEXPART analysis demonstrate that high ozone levels and related changes in the OH concentrations are associated with the transport of continental air to DDU. Finally, three companion papers are introduced. A first paper is dedicated to the impact of local penguin emissions on the atmospheric budget of several oxygenated volatile organic compounds. The second paper reports on HONO levels that were measured for the first time in Antarctica by using the long path absorption photometer (LOPAP) technique. Finally, in a third paper, major findings on the HOx levels are detailed, leading to the overall conclusion that the photochemistry at coastal East Antarctica is strongly driven by an efficient HOx chemistry compared to the situation at other coastal Antarctic regions.

Published
2012
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