Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide

F. Ziska, B. Quack, K. Abrahamsson, S. D. Archer, Elliot L Atlas, T. Bell, J. H. Butler, L. J. Carpenter, C. E. Jones, N. R P Harris, H. Hepach, K. G. Heumann, C. Hughes, J. Kuss, K. Krüger, P. Liss, R. M. Moore, A. Orlikowska, S. Raimund, C. E. ReevesW. Reifenhäuser, A. D. Robinson, C. Schall, T. Tanhua, S. Tegtmeier, S. Turner, L. Wang, D. Wallace, J. Williams, H. Yamamoto, S. Yvon-Lewis, Y. Yokouchi

Research output: Contribution to journalArticle

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Abstract

Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (<a hrefCombining double low line"https://halocat. geomar.de/"targetCombining double low line" blank">https:// halocat.geomar.de/</a>). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1 &times;1 grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr-1 for CHBr3, 0.78/0.98 Gmol Br yr-1 for CH2Br2 and 1.24/1.45 Gmol Br yr-1 for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

Original languageEnglish (US)
Pages (from-to)8915-8934
Number of pages20
JournalAtmospheric Chemistry and Physics
Volume13
Issue number17
DOIs
StatePublished - 2013

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iodide
climatology
atmosphere
air
top-down approach
halogen
ocean
open ocean
stratosphere
halocarbon
bromine
ozone depletion
emission inventory
extreme event
iodine
gyre
annual variation
organic compound
troposphere
seasonal variation

ASJC Scopus subject areas

  • Atmospheric Science

Cite this

Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide. / Ziska, F.; Quack, B.; Abrahamsson, K.; Archer, S. D.; Atlas, Elliot L; Bell, T.; Butler, J. H.; Carpenter, L. J.; Jones, C. E.; Harris, N. R P; Hepach, H.; Heumann, K. G.; Hughes, C.; Kuss, J.; Krüger, K.; Liss, P.; Moore, R. M.; Orlikowska, A.; Raimund, S.; Reeves, C. E.; Reifenhäuser, W.; Robinson, A. D.; Schall, C.; Tanhua, T.; Tegtmeier, S.; Turner, S.; Wang, L.; Wallace, D.; Williams, J.; Yamamoto, H.; Yvon-Lewis, S.; Yokouchi, Y.

In: Atmospheric Chemistry and Physics, Vol. 13, No. 17, 2013, p. 8915-8934.

Research output: Contribution to journalArticle

Ziska, F, Quack, B, Abrahamsson, K, Archer, SD, Atlas, EL, Bell, T, Butler, JH, Carpenter, LJ, Jones, CE, Harris, NRP, Hepach, H, Heumann, KG, Hughes, C, Kuss, J, Krüger, K, Liss, P, Moore, RM, Orlikowska, A, Raimund, S, Reeves, CE, Reifenhäuser, W, Robinson, AD, Schall, C, Tanhua, T, Tegtmeier, S, Turner, S, Wang, L, Wallace, D, Williams, J, Yamamoto, H, Yvon-Lewis, S & Yokouchi, Y 2013, 'Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide', Atmospheric Chemistry and Physics, vol. 13, no. 17, pp. 8915-8934. https://doi.org/10.5194/acp-13-8915-2013
Ziska, F. ; Quack, B. ; Abrahamsson, K. ; Archer, S. D. ; Atlas, Elliot L ; Bell, T. ; Butler, J. H. ; Carpenter, L. J. ; Jones, C. E. ; Harris, N. R P ; Hepach, H. ; Heumann, K. G. ; Hughes, C. ; Kuss, J. ; Krüger, K. ; Liss, P. ; Moore, R. M. ; Orlikowska, A. ; Raimund, S. ; Reeves, C. E. ; Reifenhäuser, W. ; Robinson, A. D. ; Schall, C. ; Tanhua, T. ; Tegtmeier, S. ; Turner, S. ; Wang, L. ; Wallace, D. ; Williams, J. ; Yamamoto, H. ; Yvon-Lewis, S. ; Yokouchi, Y. / Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide. In: Atmospheric Chemistry and Physics. 2013 ; Vol. 13, No. 17. pp. 8915-8934.
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abstract = "Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (https:// halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1 &times;1 grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr-1 for CHBr3, 0.78/0.98 Gmol Br yr-1 for CH2Br2 and 1.24/1.45 Gmol Br yr-1 for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. {"}Hot spots{"} for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.",
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T1 - Global sea-to-air flux climatology for bromoform, dibromomethane and methyl iodide

AU - Ziska, F.

AU - Quack, B.

AU - Abrahamsson, K.

AU - Archer, S. D.

AU - Atlas, Elliot L

AU - Bell, T.

AU - Butler, J. H.

AU - Carpenter, L. J.

AU - Jones, C. E.

AU - Harris, N. R P

AU - Hepach, H.

AU - Heumann, K. G.

AU - Hughes, C.

AU - Kuss, J.

AU - Krüger, K.

AU - Liss, P.

AU - Moore, R. M.

AU - Orlikowska, A.

AU - Raimund, S.

AU - Reeves, C. E.

AU - Reifenhäuser, W.

AU - Robinson, A. D.

AU - Schall, C.

AU - Tanhua, T.

AU - Tegtmeier, S.

AU - Turner, S.

AU - Wang, L.

AU - Wallace, D.

AU - Williams, J.

AU - Yamamoto, H.

AU - Yvon-Lewis, S.

AU - Yokouchi, Y.

PY - 2013

Y1 - 2013

N2 - Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (https:// halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1 &times;1 grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr-1 for CHBr3, 0.78/0.98 Gmol Br yr-1 for CH2Br2 and 1.24/1.45 Gmol Br yr-1 for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

AB - Volatile halogenated organic compounds containing bromine and iodine, which are naturally produced in the ocean, are involved in ozone depletion in both the troposphere and stratosphere. Three prominent compounds transporting large amounts of marine halogens into the atmosphere are bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I). The input of marine halogens to the stratosphere has been estimated from observations and modelling studies using low-resolution oceanic emission scenarios derived from top-down approaches. In order to improve emission inventory estimates, we calculate data-based high resolution global sea-to-air flux estimates of these compounds from surface observations within the HalOcAt (Halocarbons in the Ocean and Atmosphere) database (https:// halocat.geomar.de/). Global maps of marine and atmospheric surface concentrations are derived from the data which are divided into coastal, shelf and open ocean regions. Considering physical and biogeochemical characteristics of ocean and atmosphere, the open ocean water and atmosphere data are classified into 21 regions. The available data are interpolated onto a 1 &times;1 grid while missing grid values are interpolated with latitudinal and longitudinal dependent regression techniques reflecting the compounds' distributions. With the generated surface concentration climatologies for the ocean and atmosphere, global sea-to-air concentration gradients and sea-to-air fluxes are calculated. Based on these calculations we estimate a total global flux of 1.5/2.5 Gmol Br yr-1 for CHBr3, 0.78/0.98 Gmol Br yr-1 for CH2Br2 and 1.24/1.45 Gmol Br yr-1 for CH3I (robust fit/ordinary least squares regression techniques). Contrary to recent studies, negative fluxes occur in each sea-to-air flux climatology, mainly in the Arctic and Antarctic regions. "Hot spots" for global polybromomethane emissions are located in the equatorial region, whereas methyl iodide emissions are enhanced in the subtropical gyre regions. Inter-annual and seasonal variation is contained within our flux calculations for all three compounds. Compared to earlier studies, our global fluxes are at the lower end of estimates, especially for bromoform. An under-representation of coastal emissions and of extreme events in our estimate might explain the mismatch between our bottom-up emission estimate and top-down approaches.

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