A new interpretation of total column BrO during Arctic spring

Salawitch, R. J.; Canty, T. P.; Kurosu, Thomas P.; Chance, K.; Liang, Qing; Silva, A. da; Pawson, Steven; Nielsen, J. E.; Rodríguez, José M.; Bhartia, P. K.; Liu, Xueliang; Huey, L. G.; Liao, J.; Stickel, R. E.; Tanner, David J.; Dibb, Jack E.; Simpson, W. R.; Donohoue, D.; Weinheimer, A. J.; Flocke, Frank; Knapp, D. J.; Montzka, D. D.; Neuman, J. Andrew; Nowak, John B.; Ryerson, T. B.; Oltmans, S. J.; Blake, Donald R.; Atlas, Elliot L.; Kinnison, Douglas E.; Tilmes, Simone; Pan, Laura L.; Hendrick, F.; Roozendaël, Michel Van; Kreher, K.; Johnston, P. V.; Gao, R. S.; Johnson, B. J.; Bui, T. P.; Chen, G.; Pierce, R. Bradley; Crawford, J. H.; Jacob, Daniel J.

doi:10.1029/2010gl043798

Cited by 125 publications

(180 citation statements)

References 35 publications

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“…However, these hypotheses are questionable because of the possible overall presence of BrO in the troposphere and the longitudinal and latitudinal inhomogeneity of stratospheric BrO. The latter point is crucial as it has recently been argued that the stratospheric BrO column variability could be larger than previously thought, being exacerbated by the supply of significant amounts of Br y in the lower stratosphere from short-lived bromocarbons (Salawitch et al, 2010). One possibility to estimate stratospheric BrO columns at the global scale is to use the BrO profiles measured by the SCIAMACHY instrument in its limb mode (see e.g.…”

Section: Introductionmentioning

confidence: 65%

“…The approach is similar in concept to the correction used for the retrieval of tropospheric NO 2 columns by Richter et al (2005). Here the correction is based on the fact that the variations in stratospheric Br y are controlled by atmospheric dynamics in a way that matches closely the O 3 fluctuations, as clearly established by Theys et al (2009b) and further demonstrated by Salawitch et al (2010) using measured O 3 and BrO vertical columns. We assume that in conditions described below the slope of a BrO versus O 3 regression plot is fully controlled by stratospheric BrO.…”

Section: Stratospheric Bro Correctionmentioning

confidence: 88%

“…The main sources of Br y in the stratosphere are long-lived organic bromine compounds (CH 3 Br, CBrClF 2 , CBrF 3 , CBrF 2 CBrF 2 ), mostly of anthropogenic origin, which contribute to the stratospheric Br y loading by about 16-17 parts per trillion volume (pptv) (Montzka et al, 2003). However, several measurements of stratospheric BrO using remote-sensing UV-visible techniques have inferred a total Br y loading of 18-25 pptv, suggesting that an additional contribution must be considered, possibly due to the bromine release from short-lived biogenic organic compounds (e.g., CHBr 3 , CH 2 Br 2 )or even through direct injection of tropospheric Br y into the lower stratosphere (WMO, 2007, and references therein; Salawitch et al, 2010).…”

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: Introductionmentioning

confidence: 65%

Section: Stratospheric Bro Correctionmentioning

confidence: 88%

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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“…Recently, novel observations of BrO (Liao et al, 2011) have shown that "BrO clouds" tend to be distributed homogeneously over scales of a few kilometres during ODEs, while Salawitch et al (2010) found that BrO columns are correlated with the height of the tropopause, although some "hotspots" are related to free-tropospheric or stratospheric intrusions.…”

Section: P S Monks Et Al: Tropospheric Ozone and Its Precursorsmentioning

confidence: 99%

Tropospheric ozone and its precursors from the urban to the global scale from air quality to short-lived climate forcer

et al. 2015

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Abstract. Ozone holds a certain fascination in atmospheric science. It is ubiquitous in the atmosphere, central to tropospheric oxidation chemistry, yet harmful to human and ecosystem health as well as being an important greenhouse gas. It is not emitted into the atmosphere but is a byproduct of the very oxidation chemistry it largely initiates. Much effort is focused on the reduction of surface levels of ozone owing to its health and vegetation impacts, but recent efforts to achieve reductions in exposure at a country scale have proved difficult to achieve owing to increases in background ozone at the zonal hemispheric scale. There is also a growing realisation that the role of ozone as a short-lived climate pollutant could be important in integrated air quality climate change mitigation. This review examines current understanding of the processes regulating tropospheric ozone at global to local scales from both measurements and models. It takes the view that knowledge across the scales is important for dealing with air quality and climate change in a synergistic manner. The review shows that there remain a number of clear challenges for ozone such as explaining surface trends, incorporating new chemical understanding, ozone-climate coupling, and a better assessment of impacts. There is a clear and present need to treat ozone across the range of scales, a transboundary issue, but with an emphasis on the hemispheric scales. New observational opportunities are offered both by satellites and small sensors that bridge the scales.

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“…The low chlorine level of 0.8 ppb represents both a pre-industrial chlorine value (when CH 3 Cl at 0.6 ppb was the major chlorine carrier), as well as a likely chlorine level towards the end of the century, on a Montreal Protocol trajectory towards "recovery", according to projected mitigation scenarios for 2100. For stratospheric inorganic bromine, we chose three levels of ∼ 10, ∼ 15 and ∼ 23 ppt to represent approximately a low (∼ pre-industrial era, when ice core data suggest a methyl bromide concentration of about 5 ppt; Saltzman et al, 2008), medium and high (∼ present-day) level, respectively. These values all include ∼ 5 ppt from VSLS (as described above), with the remaining Br y coming from long-lived halons and CH 3 Br.…”

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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A new interpretation of total column BrO during Arctic spring

Cited by 125 publications

References 35 publications

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

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

Tropospheric ozone and its precursors from the urban to the global scale from air quality to short-lived climate forcer

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

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