A global stratospheric bromine monoxide climatology based on the BASCOE chemical transport model

Theys, Nicolas; Roozendaël, Michel Van; Errera, Quentin; Hendrick, F.; Daerden, Frank; Chabrillat, Simon; Dorf, M.; Pfeilsticker, Klaus; Rozanov, A.; Lotz, W.; Burrows, John P.; Lambert, J. C.; Goutail, Florence; Roscoe, H. K.; Mazière, Martine De

doi:10.5194/acp-9-831-2009

Cited by 72 publications

(94 citation statements)

References 72 publications

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“…Recently it has been shown by Theys et al (2009) that some enhancement in total BrO column can be caused by increases in stratospheric BrO due to a decrease in tropopause height coincident with low surface pressure. For the cases we have discussed here, tropospheric BrO columns (derived using climatological data validated using ground-based balloon and satellite limb stratospheric BrO observations) indicate the same structure of BrO enhancements that are evident in the total column, with tropospheric column amounts up to 8×10 13 molec/cm 2 (N. Theys personal communication, 2010).…”

Section: Expanding the Low Pressure System/bro Linkmentioning

confidence: 99%

“…For the cases we have discussed here, tropospheric BrO columns (derived using climatological data validated using ground-based balloon and satellite limb stratospheric BrO observations) indicate the same structure of BrO enhancements that are evident in the total column, with tropospheric column amounts up to 8×10 13 molec/cm 2 (N. Theys personal communication, 2010). Given that calculated stratospheric columns at southern high latitudes range from 2.5 to 4.5×10 13 molec/cm 2 (Theys et al, 2009), the BrO hotspots shown in the BrO total column cannot be attributed to the stratosphere and must arise from a tropospheric source.…”

Section: Expanding the Low Pressure System/bro Linkmentioning

confidence: 99%

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Vertical structure of Antarctic tropospheric ozone depletion events: characteristics and broader implications

et al. 2010

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Abstract. The majority of tropospheric ozone depletion event (ODE) studies have focussed on time-series measurements, with comparatively few studies of the vertical component. Those that exist have almost exclusively used freeflying balloon-borne ozonesondes and almost all have been conducted in the Arctic. Here we use measurements from two separate Antarctic field experiments to examine the vertical profile of ozone during Antarctic ODEs. We use tethersonde data to probe details in the lowest few hundred meters and find considerable structure in the profiles associated with complex atmospheric layering. The profiles were all measured at wind speeds less than 7 ms −1 , and on each occasion the lowest inversion height lay between 10 m and 40 m. We also use data from a free-flying ozonesonde study to select events where ozone depletion was recorded at altitudes >1 km above ground level. Using ERA-40 meteorological charts, we find that on every occasion the high altitude depletion was preceded by an atmospheric low pressure system. An examination of limited published ozonesonde data from other Antarctic stations shows this to be a consistent feature. Given the link between BrO and ODEs, we also examine ground-based and satellite BrO measurements and find a strong association between atmospheric low pressure systems and enhanced BrO that must arise in the troposphere. The results suggest that, in Antarctica, such depressions are responsible for driving high altitude ODEs and for generating the large-scale BrO clouds observed from satellites. In the Arctic, the prevailing meteorology differs from Correspondence to: A. E. Jones (aejo@bas.ac.uk) that in Antarctica, but, while a less common effect, major low pressure systems in the Arctic can also generate BrO clouds. Such depressions thus appear to be fundamental when considering the broader influence of ODEs, certainly in Antarctica, such as halogen export and the radiative influence of ozone-depleted air masses.

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Section: Expanding the Low Pressure System/bro Linkmentioning

confidence: 99%

Section: Expanding the Low Pressure System/bro Linkmentioning

confidence: 99%

Vertical structure of Antarctic tropospheric ozone depletion events: characteristics and broader implications

et al. 2010

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“…Theys et al (2011) fitted total slant columns of BrO to the solar backscattered radiation spectra. They then removed the stratospheric contribution by using correlations of stratospheric BrO with ozone and NO 2 from the BASCOE 3D-CTM (Theys et al, 2009) and applying these correlations to the local GOME-2 observations of ozone and stratospheric NO 2 columns. They converted the tropospheric slant columns to vertical columns with an air mass factor assuming a Gaussian-shaped vertical distribution of BrO peaking at 6 km altitude.…”

Section: Comparison To Satellite Observations Of Tropospheric Bromentioning

confidence: 99%

Tropospheric bromine chemistry: implications for present and pre-industrial ozone and mercury

et al. 2012

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Abstract. We present a new model for the global tropospheric chemistry of inorganic bromine (Br y ) coupled to oxidant-aerosol chemistry in the GEOS-Chem chemical transport model (CTM). Sources of tropospheric Br y include debromination of sea-salt aerosol, photolysis and oxidation of short-lived bromocarbons, and transport from the stratosphere. Comparison to a GOME-2 satellite climatology of tropospheric BrO columns shows that the model can reproduce the observed increase of BrO with latitude, the northern mid-latitudes maximum in winter, and the Arctic maximum in spring. This successful simulation is contingent on the HOBr + HBr reaction taking place in aqueous aerosols and ice clouds. Bromine chemistry in the model decreases tropospheric ozone mixing ratios by < 1-8 nmol mol −1 (6.5 % globally), with the largest effects in the northern extratropics in spring. The global mean tropospheric OH concentration decreases by 4 %. Inclusion of bromine chemistry improves the ability of global models (GEOS-Chem and p-TOMCAT) to simulate observed 19th-century ozone and its seasonality. Bromine effects on tropospheric ozone are comparable in the present-day and pre-industrial atmospheres so that estimates of anthropogenic radiative forcing are minimally affected. Br atom concentrations are 40 % higher in the pre-industrial atmosphere due to lower ozone, which would decrease by a factor of 2 the atmospheric lifetime of elemental mercury against oxidation by Br. This suggests that historical anthropogenic mercury emissions may have mostly deposited to northern mid-latitudes, enriching the corresponding surface reservoirs. The persistent rise in background surface ozone at northern mid-latitudes during the past decades could possibly contribute to the observations of elevated mercury in subsurface waters of the North Atlantic.

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“…In a second step, the stratospheric component of the signal is removed by subtracting the stratospheric BrO column, calculated using a stratospheric BrO climatology. The stratospheric BrO correction is based on a dynamical climatology generated from the BASCOE 3D chemical transport model (Theys et al, 2009). This climatology explicitly accounts for the impact of atmospheric dynamics and photochemistry on the stratospheric BrO distribution.…”

Section: Satellite Tropospheric Bro Retrievalmentioning

confidence: 99%

Snow-sourced bromine and its implications for polar tropospheric ozone

et al. 2010

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Abstract. In the last two decades, significant depletion of boundary layer ozone (ozone depletion events, ODEs) has been observed in both Arctic and Antarctic spring. ODEs are attributed to catalytic destruction by bromine radicals (Br plus BrO), especially during bromine explosion events (BEs), when high concentrations of BrO periodically occur. However, neither the exact source of bromine nor the mechanism for sustaining the observed high BrO concentrations is completely understood. Here, by considering the production of sea salt aerosol from snow lying on sea ice during blowing snow events and the subsequent release of bromine, we successfully simulate the BEs using a global chemistry transport model. We find that heterogeneous reactions play an important role in sustaining a high fraction of the total inorganic bromine as BrO. We also find that emissions of bromine associated with blowing snow contribute significantly to BrO at mid-latitudes. Modeled tropospheric BrO columns generally compare well with the tropospheric BrO columns retrieved from the GOME satellite instrument (Global Ozone Monitoring Experiment). The additional blowing snow bromine source, identified here, reduces modeled high latitude lower tropospheric ozone amounts by up to an average 8% in polar spring.

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A global stratospheric bromine monoxide climatology based on the BASCOE chemical transport model

Cited by 72 publications

References 72 publications

Vertical structure of Antarctic tropospheric ozone depletion events: characteristics and broader implications

Vertical structure of Antarctic tropospheric ozone depletion events: characteristics and broader implications

Tropospheric bromine chemistry: implications for present and pre-industrial ozone and mercury

Snow-sourced bromine and its implications for polar tropospheric ozone

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