Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer
A modelling study of radical chemistry in the coastal Antarctic boundary layer, based upon observations performed in the course of the CHABLIS (Chemistry of the Antarctic Boundary Layer and the Interface with Snow) campaign at Halley Research Station in coastal Antarctica during the austral summer 2...
Published in: | Atmospheric Chemistry and Physics |
---|---|
Main Authors: | , , , , , , , , |
Format: | Article in Journal/Newspaper |
Language: | English |
Published: |
Copernicus Publications
2010
|
Subjects: | |
Online Access: | http://nora.nerc.ac.uk/id/eprint/12755/ https://nora.nerc.ac.uk/id/eprint/12755/1/acp-10-10187-2010.pdf http://www.atmos-chem-phys.org/10/10187/2010/acp-10-10187-2010.pdf |
id |
ftnerc:oai:nora.nerc.ac.uk:12755 |
---|---|
record_format |
openpolar |
spelling |
ftnerc:oai:nora.nerc.ac.uk:12755 2023-05-15T13:45:11+02:00 Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer Bloss, W.J. Camredon, M. Lee, J.D. Heard, D.E. Plane, J.M.C. Saiz-Lopez, A. Bauguitte, Stephane J.-B Salmon, Rhian Anya Jones, Anna E. 2010 text http://nora.nerc.ac.uk/id/eprint/12755/ https://nora.nerc.ac.uk/id/eprint/12755/1/acp-10-10187-2010.pdf http://www.atmos-chem-phys.org/10/10187/2010/acp-10-10187-2010.pdf en eng Copernicus Publications https://nora.nerc.ac.uk/id/eprint/12755/1/acp-10-10187-2010.pdf Bloss, W.J.; Camredon, M.; Lee, J.D.; Heard, D.E.; Plane, J.M.C.; Saiz-Lopez, A.; Bauguitte, Stephane J.-B; Salmon, Rhian Anya; Jones, Anna E. orcid:0000-0002-2040-4841 . 2010 Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer. Atmospheric Chemistry and Physics, 10 (21). 10187-10209. https://doi.org/10.5194/acp-10-10187-2010 <https://doi.org/10.5194/acp-10-10187-2010> Glaciology Chemistry Atmospheric Sciences Publication - Article PeerReviewed 2010 ftnerc https://doi.org/10.5194/acp-10-10187-2010 2023-02-04T19:28:13Z A modelling study of radical chemistry in the coastal Antarctic boundary layer, based upon observations performed in the course of the CHABLIS (Chemistry of the Antarctic Boundary Layer and the Interface with Snow) campaign at Halley Research Station in coastal Antarctica during the austral summer 2004/2005, is described: a detailed zero-dimensional photochemical box model was used, employing inorganic and organic reaction schemes drawn from the Master Chemical Mechanism, with additional halogen (iodine and bromine) reactions added. The model was constrained to observations of long-lived chemical species, measured photolysis frequencies and meteorological parameters, and the simulated levels of HOx, NOx and XO compared with those observed. The model was able to replicate the mean levels and diurnal variation in the halogen oxides IO and BrO, and to reproduce NOx levels and speciation very well. The NOx source term implemented compared well with that directly measured in the course of the CHABLIS experiments. The model systematically overestimated OH and HO2 levels, likely a consequence of the combined effects of (a) estimated physical parameters and (b) uncertainties within the halogen, particularly iodine, chemical scheme. The principal sources of HOx radicals were the photolysis and bromine-initiated oxidation of HCHO, together with O(1D) + H2O. The main sinks for HOx were peroxy radical self- and cross-reactions, with the sum of all halogen-mediated HOx loss processes accounting for 40% of the total sink. Reactions with the halogen monoxides dominated CH3O2-HO2-OH interconversion, with associated local chemical ozone destruction in place of the ozone production which is associated with radical cycling driven by the analogous NO reactions. The analysis highlights the need for observations of physical parameters such as aerosol surface area and boundary layer structure to constrain such calculations, and the dependence of simulated radical levels and ozone loss rates upon a number of uncertain kinetic and ... Article in Journal/Newspaper Antarc* Antarctic Antarctica Natural Environment Research Council: NERC Open Research Archive Antarctic Austral Halley Research Station ENVELOPE(-26.209,-26.209,-75.605,-75.605) The Antarctic Atmospheric Chemistry and Physics 10 21 10187 10209 |
institution |
Open Polar |
collection |
Natural Environment Research Council: NERC Open Research Archive |
op_collection_id |
ftnerc |
language |
English |
topic |
Glaciology Chemistry Atmospheric Sciences |
spellingShingle |
Glaciology Chemistry Atmospheric Sciences Bloss, W.J. Camredon, M. Lee, J.D. Heard, D.E. Plane, J.M.C. Saiz-Lopez, A. Bauguitte, Stephane J.-B Salmon, Rhian Anya Jones, Anna E. Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
topic_facet |
Glaciology Chemistry Atmospheric Sciences |
description |
A modelling study of radical chemistry in the coastal Antarctic boundary layer, based upon observations performed in the course of the CHABLIS (Chemistry of the Antarctic Boundary Layer and the Interface with Snow) campaign at Halley Research Station in coastal Antarctica during the austral summer 2004/2005, is described: a detailed zero-dimensional photochemical box model was used, employing inorganic and organic reaction schemes drawn from the Master Chemical Mechanism, with additional halogen (iodine and bromine) reactions added. The model was constrained to observations of long-lived chemical species, measured photolysis frequencies and meteorological parameters, and the simulated levels of HOx, NOx and XO compared with those observed. The model was able to replicate the mean levels and diurnal variation in the halogen oxides IO and BrO, and to reproduce NOx levels and speciation very well. The NOx source term implemented compared well with that directly measured in the course of the CHABLIS experiments. The model systematically overestimated OH and HO2 levels, likely a consequence of the combined effects of (a) estimated physical parameters and (b) uncertainties within the halogen, particularly iodine, chemical scheme. The principal sources of HOx radicals were the photolysis and bromine-initiated oxidation of HCHO, together with O(1D) + H2O. The main sinks for HOx were peroxy radical self- and cross-reactions, with the sum of all halogen-mediated HOx loss processes accounting for 40% of the total sink. Reactions with the halogen monoxides dominated CH3O2-HO2-OH interconversion, with associated local chemical ozone destruction in place of the ozone production which is associated with radical cycling driven by the analogous NO reactions. The analysis highlights the need for observations of physical parameters such as aerosol surface area and boundary layer structure to constrain such calculations, and the dependence of simulated radical levels and ozone loss rates upon a number of uncertain kinetic and ... |
format |
Article in Journal/Newspaper |
author |
Bloss, W.J. Camredon, M. Lee, J.D. Heard, D.E. Plane, J.M.C. Saiz-Lopez, A. Bauguitte, Stephane J.-B Salmon, Rhian Anya Jones, Anna E. |
author_facet |
Bloss, W.J. Camredon, M. Lee, J.D. Heard, D.E. Plane, J.M.C. Saiz-Lopez, A. Bauguitte, Stephane J.-B Salmon, Rhian Anya Jones, Anna E. |
author_sort |
Bloss, W.J. |
title |
Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
title_short |
Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
title_full |
Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
title_fullStr |
Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
title_full_unstemmed |
Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer |
title_sort |
coupling of hox, nox and halogen chemistry in the antarctic boundary layer |
publisher |
Copernicus Publications |
publishDate |
2010 |
url |
http://nora.nerc.ac.uk/id/eprint/12755/ https://nora.nerc.ac.uk/id/eprint/12755/1/acp-10-10187-2010.pdf http://www.atmos-chem-phys.org/10/10187/2010/acp-10-10187-2010.pdf |
long_lat |
ENVELOPE(-26.209,-26.209,-75.605,-75.605) |
geographic |
Antarctic Austral Halley Research Station The Antarctic |
geographic_facet |
Antarctic Austral Halley Research Station The Antarctic |
genre |
Antarc* Antarctic Antarctica |
genre_facet |
Antarc* Antarctic Antarctica |
op_relation |
https://nora.nerc.ac.uk/id/eprint/12755/1/acp-10-10187-2010.pdf Bloss, W.J.; Camredon, M.; Lee, J.D.; Heard, D.E.; Plane, J.M.C.; Saiz-Lopez, A.; Bauguitte, Stephane J.-B; Salmon, Rhian Anya; Jones, Anna E. orcid:0000-0002-2040-4841 . 2010 Coupling of HOx, NOx and halogen chemistry in the Antarctic boundary layer. Atmospheric Chemistry and Physics, 10 (21). 10187-10209. https://doi.org/10.5194/acp-10-10187-2010 <https://doi.org/10.5194/acp-10-10187-2010> |
op_doi |
https://doi.org/10.5194/acp-10-10187-2010 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
10 |
container_issue |
21 |
container_start_page |
10187 |
op_container_end_page |
10209 |
_version_ |
1766215241060843520 |