Measurements of OH and RO 2 radicals at Dome C, East Antarctica

Concentrations of OH radicals and the sum of peroxy radicals, RO 2 , were measured in the boundary layer for the first time on the East Antarctic Plateau at the Concordia Station (Dome C, 75.10° S, 123.31° E) during the austral summer 2011/2012. The median concentrations of OH and RO 2 radicals were...

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Published in:Atmospheric Chemistry and Physics
Main Authors: Kukui, Alexandre, Legrand, Michel, Preunkert, S., Frey, M. M., Loisil, R., Gil Roca, Jaime, Jourdain, Benjamin, King, M. D., France, J. L., Ancellet, Gérard
Other Authors: TROPO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Laboratoire de Physique et Chimie de l'Environnement et de l'Espace (LPC2E), Observatoire des Sciences de l'Univers en région Centre (OSUC), Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire de Paris, Université Paris sciences et lettres (PSL)-Université Paris sciences et lettres (PSL)-Université d'Orléans (UO)-Centre National de la Recherche Scientifique (CNRS)-Centre National d’Études Spatiales Paris (CNES), Laboratoire de 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), British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Division technique INSU/SDU (DTI), 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), Department of Earth Sciences Egham, Royal Holloway University of London (RHUL), Institut Polaire Français-Paul EmileVictor (IPEV) within programs No. 414 and 903. M. D. Kingand J. L. France wish to thank NERC (NE/F0004796/1 andNE/F0104788) and NERC FSF (555.0608 and 584.0609)., ANR-09-BLAN-0226,OPALE(2009), ANR-10-LABX-0100,VOLTAIRE,Geofluids and Volatil elements – Earth, Atmosphere, Interfaces – Resources and Environment(2010)
Format: Article in Journal/Newspaper
Language:English
Published: HAL CCSD 2014
Subjects:
Online Access:https://hal.science/hal-01002612
https://hal.science/hal-01002612/document
https://hal.science/hal-01002612/file/acp-14-12373-2014.pdf
https://doi.org/10.5194/acp-14-12373-2014
Description
Summary:Concentrations of OH radicals and the sum of peroxy radicals, RO 2 , were measured in the boundary layer for the first time on the East Antarctic Plateau at the Concordia Station (Dome C, 75.10° S, 123.31° E) during the austral summer 2011/2012. The median concentrations of OH and RO 2 radicals were 3.1 × 106 molecule cm −3 and 9.9 × 107 molecule cm −3 , respectively. These values are comparable to those observed at the South Pole, confirming that the elevated oxidative capacity of the Antarctic atmospheric boundary layer found at the South Pole is not restricted to the South Pole but common over the high Antarctic plateau. At Concordia, the concentration of radicals showed distinct diurnal profiles with the median maximum of 5.2 × 106 molecule cm −3 at 11:00 and the median minimum of 1.1 × 106 molecule cm −3 at 01:00 for OH radicals and 1.7 × 108 molecule cm −3 and 2.5 × 107 molecule cm −3 for RO 2 radicals at 13:00 and 23:00, respectively (all times are local times). Concurrent measurements of O 3 , HONO, NO, NO 2 , HCHO and H 2 O 2 demonstrated that the major primary source of OH and RO 2 radicals at Dome C was the photolysis of HONO, HCHO and H 2 O 2 , with the photolysis of HONO contributing ∼75% of total primary radical production. However, photochemical modelling with accounting for all these radical sources overestimates the concentrations of OH and RO 2 radicals by a factor of 2 compared to field observations. Neglecting the OH production from HONO in the photochemical modelling results in an underestimation of the concentrations of OH and RO 2 radicals by a factor of 2. To explain the observations of radicals in this case an additional source of OH equivalent to about 25% of measured photolysis of HONO is required. Even with a factor of 4 reduction in the concentrations of HONO, the photolysis of HONO represents the major primary radical source at Dome C. Another major factor leading to the large concentration of OH radicals measured at Dome C was large concentrations of NO molecules and fast recycling ...