Global S&T Development Trend Analysis Platform of Resources and Environment
DOI | 10.5194/acp-17-15245-2017 |
BrO and inferred Br-y profiles over the western Pacific: relevance of inorganic bromine sources and a Br-y minimum in the aged tropical tropopause layer | |
Koenig, Theodore K.1,2; Volkamer, Rainer1,2; Baidar, Sunil1,2,19; Dix, Barbara1; Wang, Siyuan2,3; Anderson, Daniel C.4,13,20; Salawitch, Ross J.4,5,6; Wales, Pamela A.5; Cuevas, Carlos A.7; Fernandez, Rafael P.7,8; Saiz-Lopez, Alfonso7; Evans, Mathew J.9; Sherwen, Tomas9; Jacob, Daniel J.10,11; Schmidt, Johan12; Kinnison, Douglas13; Lamarque, Jean-Francois13; Apel, Eric C.13; Bresch, James C.13; Campos, Teresa13; Flocke, Frank M.13; Hall, Samuel R.13; Honomichl, Shawn B.13; Hornbrook, Rebecca13; Jensen, Jorgen B.13; Lueb, Richard13; Montzka, Denise D.13; Pan, Laura L.13; Reeves, J. Michael13; Schauffler, Sue M.13; Ullmann, Kirk13; Weinheimer, Andrew J.13; Atlas, Elliot L.14; Donets, Valeria14; Navarro, Maria A.14; Riemer, Daniel14; Blake, Nicola J.15; Chen, Dexian16,21; Huey, L. Gregory16; Tanner, David J.16; Hanisco, Thomas F.17; Wolfe, Glenn M.17,18 | |
2017-12-22 | |
发表期刊 | ATMOSPHERIC CHEMISTRY AND PHYSICS
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ISSN | 1680-7316 |
EISSN | 1680-7324 |
出版年 | 2017 |
卷号 | 17期号:24 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Spain; Argentina; England; Denmark |
英文摘要 | We report measurements of bromine monoxide (BrO) and use an observationally constrained chemical box model to infer total gas-phase inorganic bromine (Br-y) over the tropical western Pacific Ocean (tWPO) during the CONTRAST field campaign (January-February 2014). The observed BrO and inferred Bry profiles peak in the marine boundary layer (MBL), suggesting the need for a bromine source from sea-salt aerosol (SSA), in addition to organic bromine (CBry). Both profiles are found to be C-shaped with local maxima in the upper free troposphere (FT). The median tropospheric BrO vertical column density (VCD) was measured as 1 : 6 X 10(13) molec Cm-2, compared to model predictions of 0 : 9 X 10(13) molec cm(-2) in GEOS-Chem (CBry but no SSA source), 0 : 4 X 10(13) molec cm(-2) in CAM-Chem (CBry and SSA), and 2 : 1 X 10(13) molec cm(-2) in GEOS-Chem (CBry and SSA). Neither global model fully captures the C-shape of the Br-y profile. A local Br-y maximum of 3.6 ppt (2.9-4.4 ppt; 95% confidence interval, CI) is inferred between 9.5 and 13.5 km in air masses influenced by recent convective outflow. Unlike BrO, which increases from the convective tropical tropopause layer (TTL) to the aged TTL, gas-phase Br-y decreases from the convective TTL to the aged TTL. Analysis of gas-phase Br-y against multiple tracers (CFC-11, H2O = O-3 ratio, and potential temperature) reveals a Br-y minimum of 2.7 ppt (2.3-3.1 ppt; 95% CI) in the aged TTL, which agrees closely with a stratospheric injection of 2 : 6 X 0 : 6 ppt of inorganic Br-y (estimated from CFC-11 correlations), and is remarkably insensitive to assumptions about heterogeneous chemistry. Br-y increases to 6.3 ppt (5.6-7.0 ppt; 95% CI) in the stratospheric "middle-world" and 6.9 ppt (6.5-7.3 ppt; 95% CI) in the stratospheric "overworld". The local Br-y 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 Br-y species than previously recognized. Our data provide corroborating evidence that inorganic bromine sources (e.g., SSA-derived gas-phase Br-y) are needed to explain the gas-phase Br-y budget in the upper free troposphere and TTL. They are also consistent with observations of significant bromide in Upper Troposphere-Lower Stratosphere aerosols. The total Br-y budget in the TTL is currently not closed, because of the lack of concurrent quantitative measurements of gas-phase Br-y species (i.e., BrO, HOBr, HBr, etc.) and aerosol bromide. Such simultaneous measurements are needed to (1) quantify SSA-derived Br-y in the upper FT, (2) test Br-y partitioning, and possibly explain the gas-phase Bry Br-y minimum in the aged TTL, (3) constrain heterogeneous reaction rates of bromine, and (4) account for all of the sources of Br-y to the lower stratosphere. |
领域 | 地球科学 |
收录类别 | SCI-E |
WOS记录号 | WOS:000418683300001 |
WOS关键词 | AIRBORNE MAX-DOAS ; ABSORPTION CROSS-SECTIONS ; HALOGEN CHEMISTRY ; FREE TROPOSPHERE ; BOUNDARY-LAYER ; OZONE LOSS ; TEMPERATURE-DEPENDENCE ; ATMOSPHERIC CHEMISTRY ; GENERAL-CIRCULATION ; AEROSOL EXTINCTION |
WOS类目 | Environmental Sciences ; Meteorology & Atmospheric Sciences |
WOS研究方向 | Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/29475 |
专题 | 地球科学 |
作者单位 | 1.Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA; 2.CIRES, Boulder, CO 80309 USA; 3.Univ Michigan, Dept Chem, Ann Arbor, MI 48109 USA; 4.Univ Maryland, Dept Atmospher & Ocean Sci, College Pk, MD 20742 USA; 5.Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA; 6.Univ Maryland, Earth Syst Sci Interdisciplinary Ctr, College Pk, MD 20742 USA; 7.CSIC, Dept Atmospher Chem & Climate, Inst Phys Chem Rocasolano, Spanish Natl Res Council, Madrid, Spain; 8.UNT FRM, CONICET, Argentine Natl Res Council, FCEN UNCuyo, Mendoza, Argentina; 9.Univ York, Dept Chem, WACL, York, N Yorkshire, England; 10.Harvard Univ, John A Paulson Sch Engn & Appl Sci, Cambridge, MA 02138 USA; 11.Harvard Univ, Dept Earth & Planetary Sci, Cambridge, MA 02138 USA; 12.Univ Copenhagen, Dept Chem, Copenhagen, Denmark; 13.NCAR, Boulder, CO USA; 14.Univ Miami, Dept Atmospher Sci, RSMAS, Miami, FL USA; 15.Univ Calif Irvine, Dept Chem, Irvine, CA 92717 USA; 16.Georgia Tech, Sch Earth & Atmospher Sci, Atlanta, GA USA; 17.NASA, Goddard Space Flight Ctr, Atmospher Chem & Dynam Lab, Greenbelt, MD USA; 18.Univ Maryland, Joint Ctr Earth Syst Technol, Baltimore, MD 21201 USA; 19.NOAA, Chem Sci Div, Boulder, CO USA; 20.Drexel Univ, Dept Chem, Philadelphia, PA 19104 USA; 21.Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA |
推荐引用方式 GB/T 7714 | Koenig, Theodore K.,Volkamer, Rainer,Baidar, Sunil,et al. BrO and inferred Br-y profiles over the western Pacific: relevance of inorganic bromine sources and a Br-y minimum in the aged tropical tropopause layer[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(24). |
APA | Koenig, Theodore K..,Volkamer, Rainer.,Baidar, Sunil.,Dix, Barbara.,Wang, Siyuan.,...&Wolfe, Glenn M..(2017).BrO and inferred Br-y profiles over the western Pacific: relevance of inorganic bromine sources and a Br-y minimum in the aged tropical tropopause layer.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(24). |
MLA | Koenig, Theodore K.,et al."BrO and inferred Br-y profiles over the western Pacific: relevance of inorganic bromine sources and a Br-y minimum in the aged tropical tropopause layer".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.24(2017). |
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