The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions
Atmospheric nitrogen oxides (NO and NO2) were observed at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), for a total of 50 days, from 10 December 2009 to 28 January 2010. Average (±1σ) mixing ratios at 1.0 m of NO and NO2, the latter measured for the first time on the East Antarctic Plateau, w...
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Online Access: | http://eprints.esc.cam.ac.uk/2810/ http://eprints.esc.cam.ac.uk/2810/1/acp-13-3045-2013.pdf http://www.atmos-chem-phys.net/13/3045/2013/acp-13-3045-2013.html https://doi.org/10.5194/acp-13-3045-2013 |
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ftucambridgeesc:oai:eprints.esc.cam.ac.uk:2810 2023-05-15T13:55:44+02:00 The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions Frey, M.M. Brough, N. France, J. L. Traulle, O. Anderson, P.S. King, M.D. Jones, A.E. Wolff, E. W. Savarino, J. 2013-03 application/pdf http://eprints.esc.cam.ac.uk/2810/ http://eprints.esc.cam.ac.uk/2810/1/acp-13-3045-2013.pdf http://www.atmos-chem-phys.net/13/3045/2013/acp-13-3045-2013.html https://doi.org/10.5194/acp-13-3045-2013 en eng Copernicus Publications http://eprints.esc.cam.ac.uk/2810/1/acp-13-3045-2013.pdf Frey, M.M. and Brough, N. and France, J. L. and Traulle, O. and Anderson, P.S. and King, M.D. and Jones, A.E. and Wolff, E. W. and Savarino, J. (2013) The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions. Atmospheric Chemistry and Physics, 13 (6). pp. 3045-3062. ISSN 1680-7316 eISSN 1680-7324 DOI https://doi.org/10.5194/acp-13-3045-2013 <https://doi.org/10.5194/acp-13-3045-2013> cc_by CC-BY 01 - Climate Change and Earth-Ocean Atmosphere Systems Article PeerReviewed 2013 ftucambridgeesc https://doi.org/10.5194/acp-13-3045-2013 2020-08-27T18:09:24Z Atmospheric nitrogen oxides (NO and NO2) were observed at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), for a total of 50 days, from 10 December 2009 to 28 January 2010. Average (±1σ) mixing ratios at 1.0 m of NO and NO2, the latter measured for the first time on the East Antarctic Plateau, were 111 (±89) and 98 (±89) pptv, respectively. Atmospheric mixing ratios are on average comparable to those observed previously at South Pole, but in contrast show strong diurnal variability: a minimum around local noon and a maximum in the early evening coincide with the development and collapse of a convective boundary layer. The asymmetric diurnal cycle of NOx concentrations and likely any other chemical tracer with a photolytic surface source is driven by the turbulent diffusivity and height of the atmospheric boundary layer, with the former controlling the magnitude of the vertical flux and the latter the size of the volume into which snow emissions are transported. In particular, the average (±1σ) NOx emission flux from 22 December 2009 to 28 January 2010, estimated from atmospheric concentration gradients, was 8.2 (±7.4) × 1012 molecule m−2 s−1 belongs to the largest values measured so far in the polar regions and explains the 3-fold increase in mixing ratios in the early evening when the boundary layer becomes very shallow. Dome C is likely not representative for the entire East Antarctic Plateau but illustrates the need of an accurate description of the boundary layer above snow in atmospheric chemistry models. A simple nitrate photolysis model matches the observed median diurnal NOx flux during the day but has significant low bias during the night. The difference is significant taking into account the total random error in flux observations and model uncertainties due to the variability of NO3− concentrations in snow and potential contributions from NO2− photolysis. This highlights uncertainties in the parameterization of the photolytic NOx source in natural snowpacks, such as the poorly constrained quantum yield of nitrate photolysis. A steady-state analysis of the NO2 : NO ratios indicates that peroxy (HO2 + RO2) or other radical concentrations in the boundary layer of Dome C are either higher than measured elsewhere in the polar regions or other processes leading to enhanced NO2 have to be invoked. These results confirm the existence of a strongly oxidising canopy enveloping the East Antarctic Plateau in summer. Article in Journal/Newspaper Antarc* Antarctic Antarctica East Antarctica South pole South pole University of Cambridge, Department of Earth Sciences: ESC Publications Antarctic The Antarctic East Antarctica South Pole Atmospheric Chemistry and Physics 13 6 3045 3062 |
institution |
Open Polar |
collection |
University of Cambridge, Department of Earth Sciences: ESC Publications |
op_collection_id |
ftucambridgeesc |
language |
English |
topic |
01 - Climate Change and Earth-Ocean Atmosphere Systems |
spellingShingle |
01 - Climate Change and Earth-Ocean Atmosphere Systems Frey, M.M. Brough, N. France, J. L. Traulle, O. Anderson, P.S. King, M.D. Jones, A.E. Wolff, E. W. Savarino, J. The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
topic_facet |
01 - Climate Change and Earth-Ocean Atmosphere Systems |
description |
Atmospheric nitrogen oxides (NO and NO2) were observed at Dome C, East Antarctica (75.1° S, 123.3° E, 3233 m), for a total of 50 days, from 10 December 2009 to 28 January 2010. Average (±1σ) mixing ratios at 1.0 m of NO and NO2, the latter measured for the first time on the East Antarctic Plateau, were 111 (±89) and 98 (±89) pptv, respectively. Atmospheric mixing ratios are on average comparable to those observed previously at South Pole, but in contrast show strong diurnal variability: a minimum around local noon and a maximum in the early evening coincide with the development and collapse of a convective boundary layer. The asymmetric diurnal cycle of NOx concentrations and likely any other chemical tracer with a photolytic surface source is driven by the turbulent diffusivity and height of the atmospheric boundary layer, with the former controlling the magnitude of the vertical flux and the latter the size of the volume into which snow emissions are transported. In particular, the average (±1σ) NOx emission flux from 22 December 2009 to 28 January 2010, estimated from atmospheric concentration gradients, was 8.2 (±7.4) × 1012 molecule m−2 s−1 belongs to the largest values measured so far in the polar regions and explains the 3-fold increase in mixing ratios in the early evening when the boundary layer becomes very shallow. Dome C is likely not representative for the entire East Antarctic Plateau but illustrates the need of an accurate description of the boundary layer above snow in atmospheric chemistry models. A simple nitrate photolysis model matches the observed median diurnal NOx flux during the day but has significant low bias during the night. The difference is significant taking into account the total random error in flux observations and model uncertainties due to the variability of NO3− concentrations in snow and potential contributions from NO2− photolysis. This highlights uncertainties in the parameterization of the photolytic NOx source in natural snowpacks, such as the poorly constrained quantum yield of nitrate photolysis. A steady-state analysis of the NO2 : NO ratios indicates that peroxy (HO2 + RO2) or other radical concentrations in the boundary layer of Dome C are either higher than measured elsewhere in the polar regions or other processes leading to enhanced NO2 have to be invoked. These results confirm the existence of a strongly oxidising canopy enveloping the East Antarctic Plateau in summer. |
format |
Article in Journal/Newspaper |
author |
Frey, M.M. Brough, N. France, J. L. Traulle, O. Anderson, P.S. King, M.D. Jones, A.E. Wolff, E. W. Savarino, J. |
author_facet |
Frey, M.M. Brough, N. France, J. L. Traulle, O. Anderson, P.S. King, M.D. Jones, A.E. Wolff, E. W. Savarino, J. |
author_sort |
Frey, M.M. |
title |
The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
title_short |
The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
title_full |
The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
title_fullStr |
The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
title_full_unstemmed |
The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions |
title_sort |
diurnal variability of atmospheric nitrogen oxides (no & no2) above the antarctic plateau deiven by atmospheric stability and snow emissions |
publisher |
Copernicus Publications |
publishDate |
2013 |
url |
http://eprints.esc.cam.ac.uk/2810/ http://eprints.esc.cam.ac.uk/2810/1/acp-13-3045-2013.pdf http://www.atmos-chem-phys.net/13/3045/2013/acp-13-3045-2013.html https://doi.org/10.5194/acp-13-3045-2013 |
geographic |
Antarctic The Antarctic East Antarctica South Pole |
geographic_facet |
Antarctic The Antarctic East Antarctica South Pole |
genre |
Antarc* Antarctic Antarctica East Antarctica South pole South pole |
genre_facet |
Antarc* Antarctic Antarctica East Antarctica South pole South pole |
op_relation |
http://eprints.esc.cam.ac.uk/2810/1/acp-13-3045-2013.pdf Frey, M.M. and Brough, N. and France, J. L. and Traulle, O. and Anderson, P.S. and King, M.D. and Jones, A.E. and Wolff, E. W. and Savarino, J. (2013) The diurnal variability of atmospheric nitrogen oxides (NO & NO2) above the Antarctic plateau deiven by atmospheric stability and snow emissions. Atmospheric Chemistry and Physics, 13 (6). pp. 3045-3062. ISSN 1680-7316 eISSN 1680-7324 DOI https://doi.org/10.5194/acp-13-3045-2013 <https://doi.org/10.5194/acp-13-3045-2013> |
op_rights |
cc_by |
op_rightsnorm |
CC-BY |
op_doi |
https://doi.org/10.5194/acp-13-3045-2013 |
container_title |
Atmospheric Chemistry and Physics |
container_volume |
13 |
container_issue |
6 |
container_start_page |
3045 |
op_container_end_page |
3062 |
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1766262566465568768 |