BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer

Autores
Koenig, Theodore K.; Volkamer, Rainer; Baidar, Sunil; Dix, Barbara; Wang, Siyuan; Anderson, Daniel C.; Salawitch, Ross J.; Wales, Pamela A.; Cuevas, Carlos A.; Fernandez, Rafael Pedro; Saiz Lopez, Alfonso; Evans, Mathew J.; Sherwen, Tomás; Jacob, Daniel J.; Schmidt, Johan; Kinnison, Douglas; Lamarque, Jean François; Apel, Eric C.; Bresch, James C.; Campos, Teresa; Flocke, Frank M.; Hall, Samuel R.; Honomichl, Shawn B.; Hornbrook, Rebecca; Jensen, Jorgen B.; Lueb, Richard; Montzka, Denise D.; Pan, Laura L.; Reeves, J. Michael; Schauffle, Sue M.; Ullmann, Kirk; Weinheimer, Andrew J.; Atlas, Elliot L.; Donets, Valeria; Maria A. Navarro; Riemer, Daniel; Blake, Nicola J.; Chen, Dexien; Huey, L. Gregory; Tanner, David J.; Hanisco, Thomas F.; Wolfe, Glenn M.
Año de publicación
2017
Idioma
inglés
Tipo de recurso
artículo
Estado
versión publicada
Descripción
We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box-model to infer total gas phase inorganic bromine (Bry) over the tropical Western Pacific Ocean (tWPO) during the CONTRAST field 40 campaign (January – February 2014). The median tropospheric BrO Vertical Column Density (VCD) over the tWPO was measured as 1.6×1013 molec. cm˗2, compared to model predictions of 0.4×1013 in CAM-Chem, 0.9×1013 in GEOS-Chem, and 2.1×1013 in GEOS-Chem with a sea-salt aerosol (SSA) bromine source. The observed BrO and inferred Bry profiles is found to be C-shaped in the troposphere, with local maxima in the marine boundary layer (MBL) and in the upper free troposphere. Neither global model fully captures this profile shape. Between 6 and 13.5 km, the inferred Bry is highly sensitive to 5 assumptions about the rate of heterogeneous bromine recycling (depends on the surface area of ice/aerosols), and the inclusion of a SSA bromine source. A local Bry maximum of 3.6 ppt (2.3-11.1 ppt, 95% CI) is observed between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective TTL to the aged TTL, gas phase Bry decreases from the convective TTL to the aged TTL. Analysis of gas phase Bry against multiple tracers (CFC-11, H2O/O3 ratio, and θ) reveals a Bry minimum of 2.7 ppt (2.4-3.0 ppt, 95% CI) in the aged TTL, which is remarkably insensitive 10 to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.9-6.7 ppt, 95% CI) in the stratospheric middleworld, and 6.9 ppt (6.7-7.1 ppt, 95% CI) in the stratospheric overworld. The local Bry minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-chem, and suggests a more complex partitioning of gas phase and aerosol Bry species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA derived gas phase Bry) are needed to explain the gas phase Bry budget in the TTL. They are also consistent with observations of significant 15 bromide in UTLS aerosols. The total Bry budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas phase Bry species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. These simultaneous measurements are needed 1) to quantify SSA derived Bry aloft, 2) to test Bry partitioning, and explain the gas phase Bry minimum in the aged TTL, 3) to constrain heterogeneous reaction rates of bromine, and 4) to account for all of the sources of Bry to the lower stratosphere.
Fil: Koenig, Theodore K.. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados Unidos
Fil: Volkamer, Rainer. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados Unidos
Fil: Baidar, Sunil. Cooperative Institute for Research in Environmental Sciences; Estados Unidos. State University of Colorado at Boulder; Estados Unidos
Fil: Dix, Barbara. State University of Colorado at Boulder; Estados Unidos
Fil: Wang, Siyuan. State University of Colorado at Boulder; Estados Unidos. University of Michigan; Estados Unidos
Fil: Anderson, Daniel C.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Salawitch, Ross J.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Wales, Pamela A.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Cuevas, Carlos A.. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Fernandez, Rafael Pedro. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Evans, Mathew J.. University of York; Reino Unido
Fil: Sherwen, Tomás. University of York; Reino Unido
Fil: Jacob, Daniel J.. Harvard University; Estados Unidos
Fil: Schmidt, Johan. Universidad de Copenhagen; Dinamarca
Fil: Kinnison, Douglas. National Center for Atmospheric Research; Estados Unidos
Fil: Lamarque, Jean François. National Center for Atmospheric Research; Estados Unidos
Fil: Apel, Eric C.. National Center for Atmospheric Research; Estados Unidos
Fil: Bresch, James C.. National Center for Atmospheric Research; Estados Unidos
Fil: Campos, Teresa. National Center for Atmospheric Research; Estados Unidos
Fil: Flocke, Frank M.. National Center for Atmospheric Research; Estados Unidos
Fil: Hall, Samuel R.. National Center for Atmospheric Research; Estados Unidos
Fil: Honomichl, Shawn B.. National Center for Atmospheric Research; Estados Unidos
Fil: Hornbrook, Rebecca. National Center for Atmospheric Research; Estados Unidos
Fil: Jensen, Jorgen B.. National Center for Atmospheric Research; Estados Unidos
Fil: Lueb, Richard. National Center for Atmospheric Research; Estados Unidos
Fil: Montzka, Denise D.. National Center for Atmospheric Research; Estados Unidos
Fil: Pan, Laura L.. National Center for Atmospheric Research; Estados Unidos
Fil: Reeves, J. Michael. National Center for Atmospheric Research; Estados Unidos
Fil: Schauffle, Sue M.. National Center for Atmospheric Research; Estados Unidos
Fil: Ullmann, Kirk. National Center for Atmospheric Research; Estados Unidos
Fil: Weinheimer, Andrew J.. National Center for Atmospheric Research; Estados Unidos
Fil: Atlas, Elliot L.. University of Miami; Estados Unidos
Fil: Donets, Valeria. University of Miami; Estados Unidos
Fil: Maria A. Navarro. University of Miami; Estados Unidos
Fil: Riemer, Daniel. University of Miami; Estados Unidos
Fil: Blake, Nicola J.. University of California; Estados Unidos
Fil: Chen, Dexien. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Huey, L. Gregory. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Tanner, David J.. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Hanisco, Thomas F.. National Aeronautics and Space Administration; Estados Unidos
Fil: Wolfe, Glenn M.. University of Maryland; Estados Unidos. National Aeronautics and Space Administration; Estados Unidos
Materia
CONTRAST
VSL Chemistry
Stratospheric Injection
BrO and Bry
Nivel de accesibilidad
acceso abierto
Condiciones de uso
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
Repositorio
CONICET Digital (CONICET)
Institución
Consejo Nacional de Investigaciones Científicas y Técnicas
OAI Identificador
oai:ri.conicet.gov.ar:11336/78255
Acceder
id CONICETDig_621b6048b9e045386ab94379e8e3da84
oai_identifier_str oai:ri.conicet.gov.ar:11336/78255
network_acronym_str CONICETDig
repository_id_str 3498
network_name_str CONICET Digital (CONICET)
spelling BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause LayerKoenig, Theodore K.Volkamer, RainerBaidar, SunilDix, BarbaraWang, SiyuanAnderson, Daniel C.Salawitch, Ross J.Wales, Pamela A.Cuevas, Carlos A.Fernandez, Rafael PedroSaiz Lopez, AlfonsoEvans, Mathew J.Sherwen, TomásJacob, Daniel J.Schmidt, JohanKinnison, DouglasLamarque, Jean FrançoisApel, Eric C.Bresch, James C.Campos, TeresaFlocke, Frank M.Hall, Samuel R.Honomichl, Shawn B.Hornbrook, RebeccaJensen, Jorgen B.Lueb, RichardMontzka, Denise D.Pan, Laura L.Reeves, J. MichaelSchauffle, Sue M.Ullmann, KirkWeinheimer, Andrew J.Atlas, Elliot L.Donets, ValeriaMaria A. NavarroRiemer, DanielBlake, Nicola J.Chen, DexienHuey, L. GregoryTanner, David J.Hanisco, Thomas F.Wolfe, Glenn M.CONTRASTVSL ChemistryStratospheric InjectionBrO and Bryhttps://purl.org/becyt/ford/1.5https://purl.org/becyt/ford/1We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box-model to infer total gas phase inorganic bromine (Bry) over the tropical Western Pacific Ocean (tWPO) during the CONTRAST field 40 campaign (January – February 2014). The median tropospheric BrO Vertical Column Density (VCD) over the tWPO was measured as 1.6×1013 molec. cm˗2, compared to model predictions of 0.4×1013 in CAM-Chem, 0.9×1013 in GEOS-Chem, and 2.1×1013 in GEOS-Chem with a sea-salt aerosol (SSA) bromine source. The observed BrO and inferred Bry profiles is found to be C-shaped in the troposphere, with local maxima in the marine boundary layer (MBL) and in the upper free troposphere. Neither global model fully captures this profile shape. Between 6 and 13.5 km, the inferred Bry is highly sensitive to 5 assumptions about the rate of heterogeneous bromine recycling (depends on the surface area of ice/aerosols), and the inclusion of a SSA bromine source. A local Bry maximum of 3.6 ppt (2.3-11.1 ppt, 95% CI) is observed between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective TTL to the aged TTL, gas phase Bry decreases from the convective TTL to the aged TTL. Analysis of gas phase Bry against multiple tracers (CFC-11, H2O/O3 ratio, and θ) reveals a Bry minimum of 2.7 ppt (2.4-3.0 ppt, 95% CI) in the aged TTL, which is remarkably insensitive 10 to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.9-6.7 ppt, 95% CI) in the stratospheric middleworld, and 6.9 ppt (6.7-7.1 ppt, 95% CI) in the stratospheric overworld. The local Bry minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-chem, and suggests a more complex partitioning of gas phase and aerosol Bry species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA derived gas phase Bry) are needed to explain the gas phase Bry budget in the TTL. They are also consistent with observations of significant 15 bromide in UTLS aerosols. The total Bry budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas phase Bry species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. These simultaneous measurements are needed 1) to quantify SSA derived Bry aloft, 2) to test Bry partitioning, and explain the gas phase Bry minimum in the aged TTL, 3) to constrain heterogeneous reaction rates of bromine, and 4) to account for all of the sources of Bry to the lower stratosphere.Fil: Koenig, Theodore K.. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados UnidosFil: Volkamer, Rainer. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados UnidosFil: Baidar, Sunil. Cooperative Institute for Research in Environmental Sciences; Estados Unidos. State University of Colorado at Boulder; Estados UnidosFil: Dix, Barbara. State University of Colorado at Boulder; Estados UnidosFil: Wang, Siyuan. State University of Colorado at Boulder; Estados Unidos. University of Michigan; Estados UnidosFil: Anderson, Daniel C.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados UnidosFil: Salawitch, Ross J.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados UnidosFil: Wales, Pamela A.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados UnidosFil: Cuevas, Carlos A.. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Fernandez, Rafael Pedro. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; ArgentinaFil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; EspañaFil: Evans, Mathew J.. University of York; Reino UnidoFil: Sherwen, Tomás. University of York; Reino UnidoFil: Jacob, Daniel J.. Harvard University; Estados UnidosFil: Schmidt, Johan. Universidad de Copenhagen; DinamarcaFil: Kinnison, Douglas. National Center for Atmospheric Research; Estados UnidosFil: Lamarque, Jean François. National Center for Atmospheric Research; Estados UnidosFil: Apel, Eric C.. National Center for Atmospheric Research; Estados UnidosFil: Bresch, James C.. National Center for Atmospheric Research; Estados UnidosFil: Campos, Teresa. National Center for Atmospheric Research; Estados UnidosFil: Flocke, Frank M.. National Center for Atmospheric Research; Estados UnidosFil: Hall, Samuel R.. National Center for Atmospheric Research; Estados UnidosFil: Honomichl, Shawn B.. National Center for Atmospheric Research; Estados UnidosFil: Hornbrook, Rebecca. National Center for Atmospheric Research; Estados UnidosFil: Jensen, Jorgen B.. National Center for Atmospheric Research; Estados UnidosFil: Lueb, Richard. National Center for Atmospheric Research; Estados UnidosFil: Montzka, Denise D.. National Center for Atmospheric Research; Estados UnidosFil: Pan, Laura L.. National Center for Atmospheric Research; Estados UnidosFil: Reeves, J. Michael. National Center for Atmospheric Research; Estados UnidosFil: Schauffle, Sue M.. National Center for Atmospheric Research; Estados UnidosFil: Ullmann, Kirk. National Center for Atmospheric Research; Estados UnidosFil: Weinheimer, Andrew J.. National Center for Atmospheric Research; Estados UnidosFil: Atlas, Elliot L.. University of Miami; Estados UnidosFil: Donets, Valeria. University of Miami; Estados UnidosFil: Maria A. Navarro. University of Miami; Estados UnidosFil: Riemer, Daniel. University of Miami; Estados UnidosFil: Blake, Nicola J.. University of California; Estados UnidosFil: Chen, Dexien. School of Earth & Atmospheric Sciences; Estados UnidosFil: Huey, L. Gregory. School of Earth & Atmospheric Sciences; Estados UnidosFil: Tanner, David J.. School of Earth & Atmospheric Sciences; Estados UnidosFil: Hanisco, Thomas F.. National Aeronautics and Space Administration; Estados UnidosFil: Wolfe, Glenn M.. University of Maryland; Estados Unidos. National Aeronautics and Space Administration; Estados UnidosCopernicus Publication2017-07info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/78255Koenig, Theodore K.; Volkamer, Rainer; Baidar, Sunil; Dix, Barbara; Wang, Siyuan; et al.; BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer; Copernicus Publication; Atmospheric Chemistry and Physics Discussions; 17; 24; 7-2017; 1-461680-7375CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/url/https://www.atmos-chem-phys-discuss.net/acp-2017-572/info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-2017-572info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-sa/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-03T09:56:48Zoai:ri.conicet.gov.ar:11336/78255instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-03 09:56:48.645CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse
dc.title.none.fl_str_mv BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
title BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
spellingShingle BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
Koenig, Theodore K.
CONTRAST
VSL Chemistry
Stratospheric Injection
BrO and Bry
title_short BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
title_full BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
title_fullStr BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
title_full_unstemmed BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
title_sort BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer
dc.creator.none.fl_str_mv Koenig, Theodore K.
Volkamer, Rainer
Baidar, Sunil
Dix, Barbara
Wang, Siyuan
Anderson, Daniel C.
Salawitch, Ross J.
Wales, Pamela A.
Cuevas, Carlos A.
Fernandez, Rafael Pedro
Saiz Lopez, Alfonso
Evans, Mathew J.
Sherwen, Tomás
Jacob, Daniel J.
Schmidt, Johan
Kinnison, Douglas
Lamarque, Jean François
Apel, Eric C.
Bresch, James C.
Campos, Teresa
Flocke, Frank M.
Hall, Samuel R.
Honomichl, Shawn B.
Hornbrook, Rebecca
Jensen, Jorgen B.
Lueb, Richard
Montzka, Denise D.
Pan, Laura L.
Reeves, J. Michael
Schauffle, Sue M.
Ullmann, Kirk
Weinheimer, Andrew J.
Atlas, Elliot L.
Donets, Valeria
Maria A. Navarro
Riemer, Daniel
Blake, Nicola J.
Chen, Dexien
Huey, L. Gregory
Tanner, David J.
Hanisco, Thomas F.
Wolfe, Glenn M.
author Koenig, Theodore K.
author_facet Koenig, Theodore K.
Volkamer, Rainer
Baidar, Sunil
Dix, Barbara
Wang, Siyuan
Anderson, Daniel C.
Salawitch, Ross J.
Wales, Pamela A.
Cuevas, Carlos A.
Fernandez, Rafael Pedro
Saiz Lopez, Alfonso
Evans, Mathew J.
Sherwen, Tomás
Jacob, Daniel J.
Schmidt, Johan
Kinnison, Douglas
Lamarque, Jean François
Apel, Eric C.
Bresch, James C.
Campos, Teresa
Flocke, Frank M.
Hall, Samuel R.
Honomichl, Shawn B.
Hornbrook, Rebecca
Jensen, Jorgen B.
Lueb, Richard
Montzka, Denise D.
Pan, Laura L.
Reeves, J. Michael
Schauffle, Sue M.
Ullmann, Kirk
Weinheimer, Andrew J.
Atlas, Elliot L.
Donets, Valeria
Maria A. Navarro
Riemer, Daniel
Blake, Nicola J.
Chen, Dexien
Huey, L. Gregory
Tanner, David J.
Hanisco, Thomas F.
Wolfe, Glenn M.
author_role author
author2 Volkamer, Rainer
Baidar, Sunil
Dix, Barbara
Wang, Siyuan
Anderson, Daniel C.
Salawitch, Ross J.
Wales, Pamela A.
Cuevas, Carlos A.
Fernandez, Rafael Pedro
Saiz Lopez, Alfonso
Evans, Mathew J.
Sherwen, Tomás
Jacob, Daniel J.
Schmidt, Johan
Kinnison, Douglas
Lamarque, Jean François
Apel, Eric C.
Bresch, James C.
Campos, Teresa
Flocke, Frank M.
Hall, Samuel R.
Honomichl, Shawn B.
Hornbrook, Rebecca
Jensen, Jorgen B.
Lueb, Richard
Montzka, Denise D.
Pan, Laura L.
Reeves, J. Michael
Schauffle, Sue M.
Ullmann, Kirk
Weinheimer, Andrew J.
Atlas, Elliot L.
Donets, Valeria
Maria A. Navarro
Riemer, Daniel
Blake, Nicola J.
Chen, Dexien
Huey, L. Gregory
Tanner, David J.
Hanisco, Thomas F.
Wolfe, Glenn M.
author2_role author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
author
dc.subject.none.fl_str_mv CONTRAST
VSL Chemistry
Stratospheric Injection
BrO and Bry
topic CONTRAST
VSL Chemistry
Stratospheric Injection
BrO and Bry
purl_subject.fl_str_mv https://purl.org/becyt/ford/1.5
https://purl.org/becyt/ford/1
dc.description.none.fl_txt_mv We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box-model to infer total gas phase inorganic bromine (Bry) over the tropical Western Pacific Ocean (tWPO) during the CONTRAST field 40 campaign (January – February 2014). The median tropospheric BrO Vertical Column Density (VCD) over the tWPO was measured as 1.6×1013 molec. cm˗2, compared to model predictions of 0.4×1013 in CAM-Chem, 0.9×1013 in GEOS-Chem, and 2.1×1013 in GEOS-Chem with a sea-salt aerosol (SSA) bromine source. The observed BrO and inferred Bry profiles is found to be C-shaped in the troposphere, with local maxima in the marine boundary layer (MBL) and in the upper free troposphere. Neither global model fully captures this profile shape. Between 6 and 13.5 km, the inferred Bry is highly sensitive to 5 assumptions about the rate of heterogeneous bromine recycling (depends on the surface area of ice/aerosols), and the inclusion of a SSA bromine source. A local Bry maximum of 3.6 ppt (2.3-11.1 ppt, 95% CI) is observed between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective TTL to the aged TTL, gas phase Bry decreases from the convective TTL to the aged TTL. Analysis of gas phase Bry against multiple tracers (CFC-11, H2O/O3 ratio, and θ) reveals a Bry minimum of 2.7 ppt (2.4-3.0 ppt, 95% CI) in the aged TTL, which is remarkably insensitive 10 to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.9-6.7 ppt, 95% CI) in the stratospheric middleworld, and 6.9 ppt (6.7-7.1 ppt, 95% CI) in the stratospheric overworld. The local Bry minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-chem, and suggests a more complex partitioning of gas phase and aerosol Bry species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA derived gas phase Bry) are needed to explain the gas phase Bry budget in the TTL. They are also consistent with observations of significant 15 bromide in UTLS aerosols. The total Bry budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas phase Bry species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. These simultaneous measurements are needed 1) to quantify SSA derived Bry aloft, 2) to test Bry partitioning, and explain the gas phase Bry minimum in the aged TTL, 3) to constrain heterogeneous reaction rates of bromine, and 4) to account for all of the sources of Bry to the lower stratosphere.
Fil: Koenig, Theodore K.. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados Unidos
Fil: Volkamer, Rainer. State University of Colorado at Boulder; Estados Unidos. Cooperative Institute for Research in Environmental Sciences; Estados Unidos
Fil: Baidar, Sunil. Cooperative Institute for Research in Environmental Sciences; Estados Unidos. State University of Colorado at Boulder; Estados Unidos
Fil: Dix, Barbara. State University of Colorado at Boulder; Estados Unidos
Fil: Wang, Siyuan. State University of Colorado at Boulder; Estados Unidos. University of Michigan; Estados Unidos
Fil: Anderson, Daniel C.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Salawitch, Ross J.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Wales, Pamela A.. University of Maryland. Department of Atmospheric and Oceanic Science; Estados Unidos
Fil: Cuevas, Carlos A.. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Fernandez, Rafael Pedro. Universidad Nacional de Cuyo. Facultad de Ciencias Exactas y Naturales; Argentina. Universidad Tecnologica Nacional. Facultad Regional Mendoza. Secretaría de Ciencia, Tecnología y Postgrado; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Mendoza; Argentina
Fil: Saiz Lopez, Alfonso. Consejo Superior de Investigaciones Científicas. Instituto de Química Física; España
Fil: Evans, Mathew J.. University of York; Reino Unido
Fil: Sherwen, Tomás. University of York; Reino Unido
Fil: Jacob, Daniel J.. Harvard University; Estados Unidos
Fil: Schmidt, Johan. Universidad de Copenhagen; Dinamarca
Fil: Kinnison, Douglas. National Center for Atmospheric Research; Estados Unidos
Fil: Lamarque, Jean François. National Center for Atmospheric Research; Estados Unidos
Fil: Apel, Eric C.. National Center for Atmospheric Research; Estados Unidos
Fil: Bresch, James C.. National Center for Atmospheric Research; Estados Unidos
Fil: Campos, Teresa. National Center for Atmospheric Research; Estados Unidos
Fil: Flocke, Frank M.. National Center for Atmospheric Research; Estados Unidos
Fil: Hall, Samuel R.. National Center for Atmospheric Research; Estados Unidos
Fil: Honomichl, Shawn B.. National Center for Atmospheric Research; Estados Unidos
Fil: Hornbrook, Rebecca. National Center for Atmospheric Research; Estados Unidos
Fil: Jensen, Jorgen B.. National Center for Atmospheric Research; Estados Unidos
Fil: Lueb, Richard. National Center for Atmospheric Research; Estados Unidos
Fil: Montzka, Denise D.. National Center for Atmospheric Research; Estados Unidos
Fil: Pan, Laura L.. National Center for Atmospheric Research; Estados Unidos
Fil: Reeves, J. Michael. National Center for Atmospheric Research; Estados Unidos
Fil: Schauffle, Sue M.. National Center for Atmospheric Research; Estados Unidos
Fil: Ullmann, Kirk. National Center for Atmospheric Research; Estados Unidos
Fil: Weinheimer, Andrew J.. National Center for Atmospheric Research; Estados Unidos
Fil: Atlas, Elliot L.. University of Miami; Estados Unidos
Fil: Donets, Valeria. University of Miami; Estados Unidos
Fil: Maria A. Navarro. University of Miami; Estados Unidos
Fil: Riemer, Daniel. University of Miami; Estados Unidos
Fil: Blake, Nicola J.. University of California; Estados Unidos
Fil: Chen, Dexien. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Huey, L. Gregory. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Tanner, David J.. School of Earth & Atmospheric Sciences; Estados Unidos
Fil: Hanisco, Thomas F.. National Aeronautics and Space Administration; Estados Unidos
Fil: Wolfe, Glenn M.. University of Maryland; Estados Unidos. National Aeronautics and Space Administration; Estados Unidos
description We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box-model to infer total gas phase inorganic bromine (Bry) over the tropical Western Pacific Ocean (tWPO) during the CONTRAST field 40 campaign (January – February 2014). The median tropospheric BrO Vertical Column Density (VCD) over the tWPO was measured as 1.6×1013 molec. cm˗2, compared to model predictions of 0.4×1013 in CAM-Chem, 0.9×1013 in GEOS-Chem, and 2.1×1013 in GEOS-Chem with a sea-salt aerosol (SSA) bromine source. The observed BrO and inferred Bry profiles is found to be C-shaped in the troposphere, with local maxima in the marine boundary layer (MBL) and in the upper free troposphere. Neither global model fully captures this profile shape. Between 6 and 13.5 km, the inferred Bry is highly sensitive to 5 assumptions about the rate of heterogeneous bromine recycling (depends on the surface area of ice/aerosols), and the inclusion of a SSA bromine source. A local Bry maximum of 3.6 ppt (2.3-11.1 ppt, 95% CI) is observed between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective TTL to the aged TTL, gas phase Bry decreases from the convective TTL to the aged TTL. Analysis of gas phase Bry against multiple tracers (CFC-11, H2O/O3 ratio, and θ) reveals a Bry minimum of 2.7 ppt (2.4-3.0 ppt, 95% CI) in the aged TTL, which is remarkably insensitive 10 to assumptions about heterogeneous chemistry. Bry increases to 6.3 ppt (5.9-6.7 ppt, 95% CI) in the stratospheric middleworld, and 6.9 ppt (6.7-7.1 ppt, 95% CI) in the stratospheric overworld. The local Bry minimum in the aged TTL is qualitatively (but not quantitatively) captured by CAM-chem, and suggests a more complex partitioning of gas phase and aerosol Bry species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA derived gas phase Bry) are needed to explain the gas phase Bry budget in the TTL. They are also consistent with observations of significant 15 bromide in UTLS aerosols. The total Bry budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas phase Bry species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. These simultaneous measurements are needed 1) to quantify SSA derived Bry aloft, 2) to test Bry partitioning, and explain the gas phase Bry minimum in the aged TTL, 3) to constrain heterogeneous reaction rates of bromine, and 4) to account for all of the sources of Bry to the lower stratosphere.
publishDate 2017
dc.date.none.fl_str_mv 2017-07
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
http://purl.org/coar/resource_type/c_6501
info:ar-repo/semantics/articulo
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/11336/78255
Koenig, Theodore K.; Volkamer, Rainer; Baidar, Sunil; Dix, Barbara; Wang, Siyuan; et al.; BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer; Copernicus Publication; Atmospheric Chemistry and Physics Discussions; 17; 24; 7-2017; 1-46
1680-7375
CONICET Digital
CONICET
url http://hdl.handle.net/11336/78255
identifier_str_mv Koenig, Theodore K.; Volkamer, Rainer; Baidar, Sunil; Dix, Barbara; Wang, Siyuan; et al.; BrO and Bry profiles over the Western Pacific: Relevance of Inorganic Bromine Sources and a Bry Minimum in the Aged Tropical Tropopause Layer; Copernicus Publication; Atmospheric Chemistry and Physics Discussions; 17; 24; 7-2017; 1-46
1680-7375
CONICET Digital
CONICET
dc.language.none.fl_str_mv eng
language eng
dc.relation.none.fl_str_mv info:eu-repo/semantics/altIdentifier/url/https://www.atmos-chem-phys-discuss.net/acp-2017-572/
info:eu-repo/semantics/altIdentifier/doi/10.5194/acp-2017-572
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
eu_rights_str_mv openAccess
rights_invalid_str_mv https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.format.none.fl_str_mv application/pdf
application/pdf
dc.publisher.none.fl_str_mv Copernicus Publication
publisher.none.fl_str_mv Copernicus Publication
dc.source.none.fl_str_mv reponame:CONICET Digital (CONICET)
instname:Consejo Nacional de Investigaciones Científicas y Técnicas
reponame_str CONICET Digital (CONICET)
collection CONICET Digital (CONICET)
instname_str Consejo Nacional de Investigaciones Científicas y Técnicas
repository.name.fl_str_mv CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas
repository.mail.fl_str_mv dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar
_version_ 1842269424876257280
score 13.13397

Publicaciones similares