Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo
Autor: | P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, G. Krysztofiak, F. Ziska, A. Engel, S. Sala, T. Keber, H. Bönisch, E. Atlas, K. Krüger, M. Chipperfield, V. Catoire, A. A. Samah, M. Dorf, P. Siew Moi, H. Schlager, K. Pfeilsticker |
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Přispěvatelé: | Norwegian Institute for Air Research (NILU), Centre national de recherches météorologiques (CNRM), Météo France-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Lancaster Environment Centre, Lancaster University, 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), Helmholtz Centre for Ocean Research [Kiel] (GEOMAR), Institute for Atmospheric and Environmental Sciences [Frankfurt/Main] (IAU), Goethe-University Frankfurt am Main, European Project: 226224,EC:FP7:ENV,FP7-ENV-2008-1,SHIVA(2009), Institut national des sciences de l'Univers (INSU - CNRS)-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)-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 -Centre National de la Recherche Scientifique (CNRS) |
Jazyk: | angličtina |
Rok vydání: | 2021 |
Předmět: |
Convection
Atmospheric Science 010504 meteorology & atmospheric sciences QC1-999 Context (language use) 010501 environmental sciences Atmospheric sciences 01 natural sciences Troposphere chemistry.chemical_compound Washout (aeronautics) tropical convection ozone destruction Tropospheric ozone Scavenging QD1-999 0105 earth and related environmental sciences halogene compounds Physics Boundary layer Chemistry chemistry 13. Climate action [SDU]Sciences of the Universe [physics] Environmental science Outflow |
Zdroj: | Atmospheric Chemistry and Physics Atmospheric Chemistry and Physics, European Geosciences Union, 2021, 21 (22), pp.16955-16984. ⟨10.5194/acp-21-16955-2021⟩ Atmospheric Chemistry and Physics, 2021, 21 (22), pp.16955-16984. ⟨10.5194/acp-21-16955-2021⟩ 16955-16984 Atmospheric Chemistry and Physics (ACP) Atmospheric Chemistry and Physics, Vol 21, Pp 16955-16984 (2021) |
ISSN: | 1680-7316 1680-7324 |
DOI: | 10.5194/acp-21-16955-2021⟩ |
Popis: | This paper presents a modelling study on the fate of CHBr3 and its product gases in the troposphere within the context of tropical deep convection. A cloud-scale case study was conducted along the west coast of Borneo, where several deep convective systems were triggered on the afternoon and early evening of 19 November 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project and analysed using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2×2 km resolution that represents the emissions, transport by large-scale flow, convection, photochemistry, and washout of CHBr3 and its product gases (PGs). We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source at the regional scale. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that >85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e. HBr, HOBr, and BrONO2, and, consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. We find that HBr is the most abundant PG in background lower-tropospheric air and that this prevalence of HBr is a result of the relatively low background tropospheric ozone levels at the regional scale. Contrary to a previous study in a different environment, for the conditions in the simulation, the insoluble Br2 species is hardly formed within the convective systems and therefore plays no significant role in the vertical transport of bromine. This likely results from the relatively small quantities of simulated inorganic bromine involved, the presence of HBr in large excess compared to HOBr and BrO, and the relatively efficient removal of soluble compounds within the convective column. |
Databáze: | OpenAIRE |
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