Oxidation of mercury by bromine in the subtropical Pacific free troposphere

L. E. Gratz; J. L. Ambrose; D. A. Jaffe; V. Shah; L. Jaeglé; J. Stutz; J. Festa; M. Spolaor; C. Tsai; N. E. Selin; S. Song; X. Zhou; A. J. Weinheimer; D. J. Knapp; D. D. Montzka; F. M. Flocke; T. L. Campos; E. Apel; R. Hornbrook; N. J. Blake; S. Hall; G. S. Tyndall; M. Reeves; D. Stechman; M. Stell

doi:10.1002/2015GL066645

Oxidation of mercury by bromine in the subtropical Pacific free troposphere

L. E. Gratz
, J. L. Ambrose
, D. A. Jaffe
, V. Shah
, L. Jaeglé
, J. Stutz
, J. Festa
, M. Spolaor
, C. Tsai
, N. E. Selin
, S. Song
, X. Zhou
, A. J. Weinheimer
, D. J. Knapp
, D. D. Montzka
, F. M. Flocke
, T. L. Campos
, E. Apel
, R. Hornbrook
, N. J. Blake

S. Hall, G. S. Tyndall, M. Reeves, D. Stechman, M. Stell

Experimental Science Section

Colorado College
University of New Hampshire
University of Washington
University of California at Los Angeles
Massachusetts Institute of Technology
Wadsworth Center for Laboratories and Research
SUNY Albany
National Center for Atmospheric Research
University of California at Irvine

Research output: Contribution to journal › Article › peer-review

69 Scopus citations

Abstract

Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

Original language	English
Pages (from-to)	10494-10502
Number of pages	9
Journal	Geophysical Research Letters
Volume	42
Issue number	23
DOIs	https://doi.org/10.1002/2015GL066645
State	Published - Dec 16 2015

Keywords

NOMADSS
airborne measurements
bromine radicals
free troposphere
oxidized mercury

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10.1002/2015GL066645

Cite this

Gratz, L. E., Ambrose, J. L., Jaffe, D. A., Shah, V., Jaeglé, L., Stutz, J., Festa, J., Spolaor, M., Tsai, C., Selin, N. E., Song, S., Zhou, X., Weinheimer, A. J., Knapp, D. J., Montzka, D. D., Flocke, F. M., Campos, T. L., Apel, E., Hornbrook, R., ... Stell, M. (2015). Oxidation of mercury by bromine in the subtropical Pacific free troposphere. Geophysical Research Letters, 42(23), 10494-10502. https://doi.org/10.1002/2015GL066645

@article{ba97c31097cb43bfbb6370d767075690,

title = "Oxidation of mercury by bromine in the subtropical Pacific free troposphere",

abstract = "Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.",

keywords = "NOMADSS, airborne measurements, bromine radicals, free troposphere, oxidized mercury",

author = "Gratz, \{L. E.\} and Ambrose, \{J. L.\} and Jaffe, \{D. A.\} and V. Shah and L. Jaegl{\'e} and J. Stutz and J. Festa and M. Spolaor and C. Tsai and Selin, \{N. E.\} and S. Song and X. Zhou and Weinheimer, \{A. J.\} and Knapp, \{D. J.\} and Montzka, \{D. D.\} and Flocke, \{F. M.\} and Campos, \{T. L.\} and E. Apel and R. Hornbrook and Blake, \{N. J.\} and S. Hall and Tyndall, \{G. S.\} and M. Reeves and D. Stechman and M. Stell",

year = "2015",

month = dec,

day = "16",

doi = "10.1002/2015GL066645",

language = "English",

volume = "42",

pages = "10494--10502",

journal = "Geophysical Research Letters",

issn = "0094-8276",

publisher = "John Wiley and Sons Inc.",

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Gratz, LE, Ambrose, JL, Jaffe, DA, Shah, V, Jaeglé, L, Stutz, J, Festa, J, Spolaor, M, Tsai, C, Selin, NE, Song, S, Zhou, X, Weinheimer, AJ, Knapp, DJ, Montzka, DD, Flocke, FM, Campos, TL , Apel, E , Hornbrook, R, Blake, NJ, Hall, S, Tyndall, GS, Reeves, M, Stechman, D & Stell, M 2015, 'Oxidation of mercury by bromine in the subtropical Pacific free troposphere', Geophysical Research Letters, vol. 42, no. 23, pp. 10494-10502. https://doi.org/10.1002/2015GL066645

TY - JOUR

T1 - Oxidation of mercury by bromine in the subtropical Pacific free troposphere

AU - Gratz, L. E.

AU - Ambrose, J. L.

AU - Jaffe, D. A.

AU - Shah, V.

AU - Jaeglé, L.

AU - Stutz, J.

AU - Festa, J.

AU - Spolaor, M.

AU - Tsai, C.

AU - Selin, N. E.

AU - Song, S.

AU - Zhou, X.

AU - Weinheimer, A. J.

AU - Knapp, D. J.

AU - Montzka, D. D.

AU - Flocke, F. M.

AU - Campos, T. L.

AU - Apel, E.

AU - Hornbrook, R.

AU - Blake, N. J.

AU - Hall, S.

AU - Tyndall, G. S.

AU - Reeves, M.

AU - Stechman, D.

AU - Stell, M.

PY - 2015/12/16

Y1 - 2015/12/16

N2 - Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

AB - Mercury is a global toxin that can be introduced to ecosystems through atmospheric deposition. Mercury oxidation is thought to occur in the free troposphere by bromine radicals, but direct observational evidence for this process is currently unavailable. During the 2013 Nitrogen, Oxidants, Mercury and Aerosol Distributions, Sources and Sinks campaign, we measured enhanced oxidized mercury and bromine monoxide in a free tropospheric air mass over Texas. We use trace gas measurements, air mass back trajectories, and a chemical box model to confirm the origin and chemical history of the sampled air mass. We find the presence of elevated oxidized mercury to be consistent with oxidation of elemental mercury by bromine atoms in this subsiding upper tropospheric air mass within the subtropical Pacific High, where dry atmospheric conditions are conducive to oxidized mercury accumulation. Our results support the role of bromine as the dominant oxidant of mercury in the upper troposphere.

KW - NOMADSS

KW - airborne measurements

KW - bromine radicals

KW - free troposphere

KW - oxidized mercury

UR - https://www.scopus.com/pages/publications/84953637753

U2 - 10.1002/2015GL066645

DO - 10.1002/2015GL066645

M3 - Article

AN - SCOPUS:84953637753

SN - 0094-8276

VL - 42

SP - 10494

EP - 10502

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 23

ER -

Oxidation of mercury by bromine in the subtropical Pacific free troposphere

Abstract

Keywords

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