The contribution of natural and anthropogenic very short-lived species to stratospheric bromine

Hossaini, Ryan; Chipperfield, Martyn P.; Feng, Wuhu; Breider, T. J.; Atlas, Elliot L.; Montzka, S. A.; Miller, Ben; Moore, F. L.; Elkins, James W.

doi:10.5194/acp-12-371-2012

Cited by 73 publications

(117 citation statements)

References 25 publications

(49 reference statements)

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“…Elevated BrO concentrations are measured within the LS (range 3-9 ppt), and lower BrO concentrations are measured in the TTL (range 0.5-5 ppt), with the smallest BrO concentrations (0.5-1 ppt) occurring near the bottom of the TTL. Overall, this behavior is expected from arguments based on the amount and composition of the brominated organic and inorganic source gases, their lifetimes, atmospheric transport, and photochemistry (e.g., Fueglistaler et al, 2009;Aschmann et al, 2009;Hossaini et al, 2012b;Ashfold et al, 2012;WMO, 2014;Fernandez et al, 2014;Saiz-Lopez and Fernandez, 2016). In particular, for our daytime measurements, it is observed that (a) BrO increases with O 3 and available Br inorg y and thus altitude and (b) the predicted BrO / Br inorg y ratio decreases towards the bottom of the TTL, where (c) HBr and/or Br atoms may become comparable to BrO, but HOBr does not play a major role in the Br inorg y partitioning.…”

Section: Comparisons Of Measured Bro With Previous Studiesmentioning

confidence: 99%

“…In the present context the most important were measurements performed within the TTL (for the definition of TTL, see Fueglistaler et al, 2009) over the Pacific from where most of the stratospheric air is predicted to originate (e.g., Fueglistaler et al, 2009;Aschmann et al, 2009;Hossaini et al, 2012b;Ashfold et al, 2012;WMO, 2014;Orbe et al, 2015). These include the measurements (a) by Schauffler et al (1993Schauffler et al ( , 1998Schauffler et al ( , 1999, who found [VSLS] = 1.3 ppt (contribution 3) at the tropical tropopause over the central Pacific (Hawaii) in 1996, (b) by Laube et al (2008) and Brinckmann et al (2012) Supporting information on brominated VSLS concentrations typical of the boundary layer of the western Pacific came from measurements performed during the TransBrom ship cruise in October 2009 (median 2.23 ppt and range from 1.45-4.14 ppt; Brinckmann et al, 2012) and the VSLS measurements made around Borneo during the SHIVA (Stratospheric Ozone: Halogen Impacts in a Varying Atmosphere) project (median 5.7 ppt and range from 3.9 to 10.7 ppt; Sala et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

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Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

et al. 2017

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Abstract. We report measurements of CH 4 (measured in situ by the Harvard University Picarro Cavity Ringdown Spectrometer (HUPCRS) and NOAA Unmanned Aircraft System Chromatograph for Atmospheric Trace Species (UCATS) instruments), O 3 (measured in situ by the NOAA dual-beam ultraviolet (UV) photometer), NO 2 , BrO (remotely detected by spectroscopic UV-visible (UV-vis) limb observations; see the companion paper of Stutz et al., 2016), and of some key brominated source gases in whole-air samples of the Global Hawk Whole Air Sampler (GWAS) instrument within the subtropical lowermost stratosphere (LS) and the tropical upper troposphere (UT) and tropopause layer (TTL). The measurements were performed within the framework of the NASA-ATTREX (National Aeronautics and Space Administration -Airborne Tropical Tropopause Experiment) project from aboard the Global Hawk (GH) during six deployments over the eastern Pacific in early 2013. These measurements are compared with TOMCAT/SLIMCAT (Toulouse Off-line Model of Chemistry And Transport/Single Layer Isentropic Model of Chemistry And Transport) 3-D model simulations, aiming at improvements of our understanding of the bromine budget and photochemistry in the LS, UT, and TTL.Changes in local O 3 (and NO 2 and BrO) due to transport processes are separated from photochemical processes in intercomparisons of measured and modeled CH 4 and O 3 . After excellent agreement is achieved among measured and simulated CH 4 and O 3 , measured and modeled [NO 2 ] are found to closely agree with ≤ 15 ppt in the TTL (which is the detection limit) and within a typical range of 70 to 170 ppt in the subtropical LS during the daytime. Measured [BrO] ranges between 3 and 9 ppt in the subtropical LS. In the TTL, [BrO] ] is found to increase from a mean of 2.63 ± 1.04 ppt for potential temperatures (θ ) in the range of 350-360 K to 5.11 ± 1.57 ppt for θ = 390 − 400 K, whereas in the subtropical LS (i.e., when [CH 4 ] ≤ 1790 ppb), it reaches 7.66 ± 2.95 ppt for θ in the range of 390-400 K. Finally, for the eastern Pacific (170-90 • W), the TOMCAT/SLIMCAT simulations indicate a net loss of ozone of −0.3 ppbv day −1 at the base of the TTL (θ = 355 K) and a net production of +1.8 ppbv day −1 in the upper part (θ = 383 K).

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Section: Comparisons Of Measured Bro With Previous Studiesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

et al. 2017

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“…Being short lived, there are large uncertainties in using atmospheric concentration measurements to estimate their global fluxes and their net contribution to the stratospheric bromine (Warwick et al, 2006;Liang et al, 2010;Pyle et al, 2011;Ordóñez et al, 2012;Ziska et al, 2013;Hossaini et al, 2013). A large range of contributions to stratospheric inorganic bromine of 110 ppt can be found in the literature (Dorf et al, 2008;Salawich et al, 2010;Schofield et al, 2011;Aschmann et al, 2011;Tegtmeier et al, 2012;Stachnik et al, 2013;Hossaini et al, 2012a). The UNEP/WMO ozone assessment of 2011 reports the value as 6(3-8) ppt (Montzka, Reimann et al, 2011).…”

Section: Introductionmentioning

confidence: 98%

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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“…They may be the dominant source of Br y in the upper troposphere and lowermost stratosphere (Dvortsov et al, 1999;Salawitch et al, 2005). Bromoform (CHBr 3 ) and dibromomethane (CH 2 Br 2 ) have received most attention, and appear to account for the bulk of bromine bound within VSLS (Hossaini et al, 2012). A further organic source of bromine is…”

Section: Introductionmentioning

confidence: 99%

Estimates of tropical bromoform emissions using an inversion method

et al. 2014

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Abstract. Bromine plays an important role in ozone chemistry in both the troposphere and stratosphere. When measured by mass, bromoform (CHBr 3 ) is thought to be the largest organic source of bromine to the atmosphere. While seaweed and phytoplankton are known to be dominant sources, the size and the geographical distribution of CHBr 3 emissions remains uncertain. Particularly little is known about emissions from the Maritime Continent, which have usually been assumed to be large, and which appear to be especially likely to reach the stratosphere. In this study we aim to reduce this uncertainty by combining the first multiannual set of CHBr 3 measurements from this region, and an inversion process, to investigate systematically the distribution and magnitude of CHBr 3 emissions. The novelty of our approach lies in the application of the inversion method to CHBr 3 . We find that local measurements of a short-lived gas like CHBr 3 can be used to constrain emissions from only a relatively small, sub-regional domain. We then obtain detailed estimates of CHBr 3 emissions within this area, which appear to be relatively insensitive to the assumptions inherent in the inversion process. We extrapolate this information to produce estimated emissions for the entire tropics (defined as 20 • S-20 • N) of 225 Gg CHBr 3 yr −1 . The ocean in the area we base our extrapolations upon is typically somewhat shallower, and more biologically productive, than the tropical average. Despite this, our tropical estimate is lower than most other recent studies, and suggests that CHBr 3 emissions in the coastline-rich Maritime Continent may not be stronger than emissions in other parts of the tropics.

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The contribution of natural and anthropogenic very short-lived species to stratospheric bromine

Cited by 73 publications

References 25 publications

Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

Probing the subtropical lowermost stratosphere and the tropical upper troposphere and tropopause layer for inorganic bromine

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

Estimates of tropical bromoform emissions using an inversion method

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