Snow-sourced bromine and its implications for polar tropospheric ozone

Yang, Xin; Pyle, J. A.; Cox, R. A.; Theys, Nicolas; Roozendaël, Michel Van

doi:10.5194/acp-10-7763-2010

Cited by 152 publications

(218 citation statements)

References 49 publications

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“…The general tendency of elevated tropospheric BrO columns linked to low tropopause heights being well captured by the p-TOMCAT model. It should be noted that the model definitely fails to reproduce the observed features when the blowing snow-sourced bromine is omitted (in line with the findings of Yang et al, 2010). The results of Fig.…”

Section: Polar Tropospheric Brosupporting

confidence: 76%

“…p-TOMCAT (parallelTropospheric Off-Line Model of Chemistry and Transport) is an off-line three-dimensional tropospheric chemical transport model with a detailed bromine chemistry scheme that contains gas-phase reactions and heterogeneous reactions on cloud particles and aerosols, as well as bromine removal from dry and wet deposition (Yang et al, 2005(Yang et al, , 2008(Yang et al, and 2010. It includes bromine emissions from sea salt, bromocarbon photo-oxidation and also a parameterization for sea salt aerosol production through blowing snow events (in the latest version of p-TOMCAT; see Yang et al, 2010). For the present study, the model was run for the 2007-2008 period at a horizontal resolution of 2.8 • × 2.8 • and an output frequency of 2 h using winds and temperature derived from the ECMWF operational analysis.…”

Section: Polar Tropospheric Bromentioning

confidence: 99%

“…Observations from space (e.g., Richter et al, 2002;Van Roozendael et al, 2002), ground-based Theys et al, 2007) and balloon-borne (Harder et al, 1998;Fitzenberger et al, 2000) instruments have shown that inorganic bromine may be produced and sustained in the free troposphere at the global scale. Elaborating on these observations, modelling results (von Glasow et al, 2004;Lary, 2005;Yang et al, 2005Yang et al, , 2010 have shown that freetropospheric bromine might have a significant impact on the tropospheric ozone budget (and on tropospheric chemistry in general), leading to a reduction in the O 3 mixing ratio of up to 40% locally.…”

Section: Introductionmentioning

confidence: 99%

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Global observations of tropospheric BrO columns using GOME-2 satellite data

et al. 2011

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Abstract.Measurements from the GOME-2 satellite instrument have been analyzed for tropospheric BrO using a residual technique that combines measured BrO columns and estimates of the stratospheric BrO content from a climatological approach driven by O 3 and NO 2 observations. Comparisons between the GOME-2 results and BrO vertical columns derived from correlative ground-based and SCIAMACHY nadir observations, present a good level of consistency. We show that the adopted technique enables separation of stratospheric and tropospheric fractions of the measured total BrO columns and allows quantitative study of the BrO plumes in polar regions. While some satellite observed plumes of enhanced BrO can be explained by stratospheric descending air, we show that most BrO hotspots are of tropospheric origin, although they are often associated to regions with low tropopause heights as well. Elaborating on simulations using the p-TOMCAT tropospheric chemical transport model, this result is found to be consistent with the mechanism of bromine release through sea salt aerosols production during blowing snow events. No definitive conclusion can be drawn however on the importance of blowing snow sources in comparison to other bromine release mechanisms. Outside polar regions, evidence is provided for a global tropospheric BrO background with column of 1-3 × 10 13 molec cm −2 , consistent with previous estimates.

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Section: Polar Tropospheric Brosupporting

confidence: 76%

Section: Polar Tropospheric Bromentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Global observations of tropospheric BrO columns using GOME-2 satellite data

et al. 2011

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“…The detailed chemistry scheme for the troposphere and stratosphere, CheST, combines the schemes described by Morgenstern et al (2009) andO'Connor et al (2014), and was further updated with tropospheric bromine chemistry based on our work in the pTOMCAT chemistry transport model (Yang et al, 2005(Yang et al, , 2010. The stratospheric halogen scheme is improved by introducing a number of heterogeneous reactions to stratospheric particles (polar stratospheric clouds (PSCs) and sulfate aerosol) to account for inter-halogen (chlorine and bromine) reactivation, as in our recent study (Braesicke et al, 2013).…”

Section: Model and Experimentsmentioning

confidence: 99%

How sensitive is the recovery of stratospheric ozone to changes in concentrations of very short-lived bromocarbons?

et al. 2014

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Abstract. Naturally produced very short-lived substances (VSLS) account for almost a quarter of the current stratospheric inorganic bromine, Br y . Following VSLS oxidation, bromine radicals (Br and BrO) can catalytically destroy ozone. The extent to which possible increases in surface emissions or transport of these VSLS bromocarbons to the stratosphere could counteract the effect of halogen reductions under the Montreal Protocol is an important policy question. Here, by using a chemistry-climate model, UM-UKCA, we investigate the impact of a hypothetical doubling (an increase of 5 ppt Br y ) of VSLS bromocarbons on ozone and how the resulting ozone changes depend on the background concentrations of chlorine and bromine. Our model experiments indicate that for the 5 ppt increase in Br y from VSLS, the ozone decrease in the lowermost stratosphere of the Southern Hemisphere (SH) may reach up to 10 % in the annual mean; the ozone decrease in the Northern Hemisphere (NH) is smaller (4-6 %). The largest impact on the ozone column is found in the Antarctic spring. There is a significantly larger ozone decrease following the doubling of the VSLS burden under a high stratospheric chlorine background than under a low chlorine background, indicating the importance of the inter-halogen reactions. For example, the decline in the high-latitude, lower-stratospheric ozone concentration as a function of Br y is higher by about 30-40 % when stratospheric Cl y is ∼ 3 ppb (present day), compared with Cl y of ∼ 0.8 ppb (a pre-industrial or projected future situation). Bromine will play an important role in the future ozone layer. However, even if bromine levels from natural VSLS were to increase significantly later this century, changes in the concentration of ozone will likely be dominated by the decrease in anthropogenic chlorine. Our calculation suggests that for a 5 ppt increase in Br y from VSLS, the Antarctic ozone hole recovery date could be delayed by approximately 6-8 years, depending on Cl y levels.

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“…As there remains some uncertainty concerning atmospheric Hg oxidation process [35][36][37], simulations were also run including an oxidation mechanism based on bromine, with oxidant fields from the p-Tomcat model [38,39].…”

Section: Methodsmentioning

confidence: 99%

Estimating Uncertainty in Global Mercury Emission Source and Deposition Receptor Relationships

et al. 2017

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Establishing mercury (Hg) source-receptor (SR) relationship matrices provides a tool to improve the understanding of the geographic relationship between regions of Hg release and its eventual deposition. SR relationship matrices are therefore a useful starting point for the development of policies aimed at reducing the impact of Hg emissions from anthropogenic activities (Hg anthr ) on sensitive ecosystems and areas potentially at risk of Hg contamination. A global Chemical Transport Model (CTM) has been used to simulate the emission, transport and fate of Hg anthr from 12 source regions, considering a range of uncertainty in the modelled chemical and physical processes. This ensemble of simulations gives an estimate of the Hg deposition which derives from each source region, as well as an estimate of the uncertainty of the calculated deposition flux. The uncertainty has been calculated using the bootstrap method to estimate this uncertainty in terms of the normalised confidence interval amplitude of the mean (NCIAM). Within the calculated confidence ranges, for almost all regions the contribution to the Hg deposition flux from remote sources is greater than that from domestic sources. Europe and South Asia, where the contributions are statistically indistinguishable, are exceptions, as is East Asia, with local sources dominating the Hg deposition flux. East Asia is the single most important remote source region for most receptor regions. The results yield such high uncertainties in the deposition flux for many receptor regions that the results are unlikely to be taken into consideration by policy makers. This uncertainty is particularly relevant when considering the "domestic" contribution to regional deposition, highlighting the need for more studies to resolve remaining uncertainties in the atmospheric Hg cycle, and Hg anthr emission inventories.

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Snow-sourced bromine and its implications for polar tropospheric ozone

Cited by 152 publications

References 49 publications

Global observations of tropospheric BrO columns using GOME-2 satellite data

Global observations of tropospheric BrO columns using GOME-2 satellite data

How sensitive is the recovery of stratospheric ozone to changes in concentrations of very short-lived bromocarbons?

Estimating Uncertainty in Global Mercury Emission Source and Deposition Receptor Relationships

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