Dataset Information

Direct detection of atmospheric atomic bromine leading to mercury and ozone depletion.

ABSTRACT: Bromine atoms play a central role in atmospheric reactive halogen chemistry, depleting ozone and elemental mercury, thereby enhancing deposition of toxic mercury, particularly in the Arctic near-surface troposphere. However, direct bromine atom measurements have been missing to date, due to the lack of analytical capability with sufficient sensitivity for ambient measurements. Here we present direct atmospheric bromine atom measurements, conducted in the springtime Arctic. Measured bromine atom levels reached 14 parts per trillion (ppt, pmol mol-1; 4.2 × 108 atoms per cm-3) and were up to 3-10 times higher than estimates using previous indirect measurements not considering the critical role of molecular bromine. Observed ozone and elemental mercury depletion rates are quantitatively explained by the measured bromine atoms, providing field validation of highly uncertain mercury chemistry. Following complete ozone depletion, elevated bromine concentrations are sustained by photochemical snowpack emissions of molecular bromine and nitrogen oxides, resulting in continued atmospheric mercury depletion. This study provides a breakthrough in quantitatively constraining bromine chemistry in the polar atmosphere, where this chemistry connects the rapidly changing surface to pollutant fate.

SUBMITTER: Wang S

PROVIDER: S-EPMC6642345 | biostudies-literature | 2019 Jul

REPOSITORIES: biostudies-literature

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Direct detection of atmospheric atomic bromine leading to mercury and ozone depletion.

Wang Siyuan S McNamara Stephen M SM Moore Christopher W CW Obrist Daniel D Steffen Alexandra A Shepson Paul B PB Staebler Ralf M RM Raso Angela R W ARW Pratt Kerri A KA

Proceedings of the National Academy of Sciences of the United States of America 20190628 29

Bromine atoms play a central role in atmospheric reactive halogen chemistry, depleting ozone and elemental mercury, thereby enhancing deposition of toxic mercury, particularly in the Arctic near-surface troposphere. However, direct bromine atom measurements have been missing to date, due to the lack of analytical capability with sufficient sensitivity for ambient measurements. Here we present direct atmospheric bromine atom measurements, conducted in the springtime Arctic. Measured bromine atom ...[more]

PMID: 31253702

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Project description:Recent studies have focused on the chemistry of tropospheric halogen species which are able to deplete tropospheric ozone (O3). In this study, the effect of bromine and iodine chemistry on tropospheric O3 within the annual cycle in Asia-Pacific is investigated using the CMAQ model with the newly embedded bromine and iodine chemistry and a blended and customized emission inventory considering marine halogen emission. Results indicate that the vertical profiles of bromine and iodine species show distinct features over land/ocean and daytime/nighttime, related to natural and anthropogenic emission distributions and photochemical reactions. The halogen-mediated O3 loss has a strong seasonal cycle, and reaches a maximum of -15.9 ppbv (-44.3%) over the ocean and -13.4 ppbv (-38.9%) over continental Asia among the four seasons. Changes in solar radiation, dominant wind direction, and nearshore chlorophyll-a accumulation all contribute to these seasonal differences. Based on the distances to the nearest coastline, the onshore and offshore features of tropospheric O3 loss caused by bromine and iodine chemistry are studied. Across a coastline-centric 400-km-wide belt from onshore to offshore, averaged maximum gradient of O3 loss reaches 1.1 ppbv/100 km at surface level, while planetary boundary layer (PBL) column mean of O3 loss is more moderate, being approximately 0.7 ppbv/100 km. Relative high halogen can be found over Tibetan Plateau (TP) and the largest O3 loss (approximately 4-5 ppbv) in the PBL can be found between the western boundary of the domain and the TP. Halogens originating from marine sources can potentially affect O3 concentration transported from the stratosphere over the TP region. As part of efforts to improve our understanding of the effect of bromine and iodine chemistry on tropospheric O3, we call for more models and monitoring studies on halogen chemistry and be considered further in air pollution prevention and control policy.

Dataset Information

Direct detection of atmospheric atomic bromine leading to mercury and ozone depletion.

Publications

Direct detection of atmospheric atomic bromine leading to mercury and ozone depletion.

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