Observations of bromine monoxide transport in the Arctic sustained on aerosol particles

Peterson, Peter K.; Pöhler, Denis; Sihler, Holger; Zielcke, Johannes; General, Stephan; Frieß, Udo; Platt, U.; Simpson, W. R.; Nghiem, S. V.; Shepson, P. B.; Stirm, B. H.; Dhaniyala, Suresh; Wagner, Thomas; Caulton, D.; Fuentes, José D.; Pratt, Kerri A.

doi:10.5194/acp-17-7567-2017

Cited by 60 publications

(70 citation statements)

References 44 publications

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“…The BrO vmr ranges reported herein (Fig. 10) are comparable to previous tropospheric Artic studies (e.g., Tuckermann et al, 1997;Hönninger and Platt, 2002;Prados-Roman et al, 2011;Liao et al, 2012;Peterson et al, 2017;Simpson et al, 2017) and 35 consistent with the few existing Antarctic measurements (e.g., Table 1). By adding the BrO measurements provided in the frame of this work to the few previous ground-based observations performed at Antarctica from different sites, Fig.…”

Section: Vertical Profiles Of Bro In the Antarctic Tropospheresupporting

confidence: 91%

“…Note that, although the definition of the height of the boundary layer over ice and snow surfaces (e.g., Anderson and Neff, 2008) is out of the scope of this work, the BrO detection limit here provided may be regarded as an upper limit of BrO in the free troposphere since former studies place the top of the boundary layer in Antarctica between 100 m and 2 km, depending on the boundary layer parametrization and time of the year (e.g., King et al , 2006;Nygård et al, 2013). This upper limit of BrO in the free 5 troposphere of Antarctica is consistent with the few previous studies of the vertical distribution of this trace gas in the Arctic and Antarctic regions that set upper limits of BrO in the polar free troposphere of 1.5 and 2 pmol mol -1 , respectively (e.g., Frieß et al, 2011;Prados-Roman et al, 2011;Peterson et al, 2017;Hüneke et al, 2017).…”

Section: Vertical Profiles Of Bro In the Antarctic Tropospheresupporting

confidence: 89%

“…Either with active set-ups (e.g., Long path-DOAS) or with passive 10 ones (e.g., zenith-DOAS, MAX-DOAS, satellite observations), the DOAS technique has been used broadly to research the troposphere in remote environments (e.g., Wagner and Platt, 1998;Bobrowsky et al 2003;Wagner et al, 2007;Saiz-Lopez et al, 2007a,b;Puentedura, et al 2012, Prados-Roman et al, 2015Peterson et al, 2017). In particular, the MAX-DOAS instrumental set-up referred to in this work consists in a telescope scanning the atmosphere at different elevation angles inferring with it vertically-resolved information of the status of the atmosphere regarding aerosols and trace gases (e.g., 15 Hönninger et al, 2004;Wagner et al, 2004).…”

Section: Max-doas Instrumentsmentioning

confidence: 99%

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Reactive bromine in the low troposphere of Antarctica. Estimations at two research sites

Prados-Román¹,

Gómez²,

Puentedura³

et al. 2018

Preprint

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Abstract.For decades, reactive halogen species (RHS) have been subject of detailed scientific research due to their influence on the 20 oxidizing capacity of the atmosphere and on the climate. From the RHS, those containing bromine are of particular interest in the polar troposphere as a result of their link to ozone depletion events (ODEs) and to the perturbation of the cycle of e.g. the toxic mercury. Given its remoteness and related limited accessibility compared to the Arctic region, the RHS in the Antarctic troposphere are still poorly characterized. This work presents ground-based observations of tropospheric BrO from two different Antarctic locations: Marambio (64º 13' S, 56º 37' W) and Belgrano II (77º 52' S, 34º 37' W) during the sunlit period 25 of 2015. By means of MAX-DOAS (Multi-axis Differential Optical Absorption Spectroscopy) measurements of BrO performed from the two research sites, the seasonal variation of this reactive trace gas is described along with its vertical and geographical distribution in the Antarctic environment. Results show an overall vertical profile of BrO mixing ratio decreasing with altitude, with a median value of 1.6 pmol mol -1 in the lowest layers of the troposphere and undetectable values above 2 km at both sites. Additionally, observations show that the polar sunrise triggers a heterogeneous increase of bromine content 30 in the Antarctic troposphere yielding a maximum BrO at Marambio (26 pmol mol -1 ), amounting threefold the values observed at Belgrano at dawn. Data presented herein are combined with previous studies and ancillary data to update and expand our knowledge of the geographical and vertical distribution of BrO in the Antarctic troposphere, revealing Marambio as one of the locations with highest BrO reported so far in Antarctica. Furthermore, the observations gathered during 2015 serve as a proxy to investigate the budget of reactive bromine (BrOx = Br + BrO) and the bromine-mediated ozone loss rate in the Antarctic 35 troposphere.

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Section: Vertical Profiles Of Bro In the Antarctic Tropospheresupporting

confidence: 91%

Section: Vertical Profiles Of Bro In the Antarctic Tropospheresupporting

confidence: 89%

Section: Max-doas Instrumentsmentioning

confidence: 99%

See 1 more Smart Citation

Reactive bromine in the low troposphere of Antarctica. Estimations at two research sites

Prados-Román¹,

Gómez²,

Puentedura³

et al. 2018

Preprint

View full text Add to dashboard Cite

show abstract

“…These gradient observations complement Peterson et al (2017), who used airborne DOAS to study an episode of reactive halogen transport. Here, we use these observations to study BrO spatial structures and the effects of sea-ice-lead-induced vertical mixing on reactive bromine.…”

Section: Introductionmentioning

confidence: 54%

“…4 shows time-staggered changes in BrO LT-VCD and f 200 . Peterson et al (2017) used airborne DOAS to study the 13 March case and observed a very steep BrO gradient that transports with the wind, clearly indicating that features on the edges of air masses are < 30 km. Therefore, we interpret the BrO distribution as being large regions of relatively consistent BrO on > 30 km length scales with sharp contrasts at their edges that are much smaller than satellite length scales.…”

Section: Bro Measurements Were Highly Correlated On ∼ 30 Km Length Scmentioning

confidence: 99%

Horizontal and vertical structure of reactive bromine events probed by bromine monoxide MAX-DOAS

et al. 2017

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Abstract. Heterogeneous photochemistry converts bromide (Br − ) to reactive bromine species (Br atoms and bromine monoxide, BrO) that dominate Arctic springtime chemistry. This phenomenon has many impacts such as boundarylayer ozone depletion, mercury oxidation and deposition, and modification of the fate of hydrocarbon species. To study environmental controls on reactive bromine events, the BRomine, Ozone, and Mercury EXperiment (BROMEX) was carried out from early March to mid-April 2012 near Barrow (Utqiaġvik), Alaska. We measured horizontal and vertical gradients in BrO with multiple-axis differential optical absorption spectroscopy (MAX-DOAS) instrumentation at three sites, two mobile and one fixed. During the campaign, a large crack in the sea ice (an open lead) formed pushing one instrument package ∼ 250 km downwind from Barrow (Utqiaġvik). Convection associated with the open lead converted the BrO vertical structure from a surfacebased event to a lofted event downwind of the lead influence. The column abundance of BrO downwind of the refreezing lead was comparable to upwind amounts, indicating direct reactions on frost flowers or open seawater was not a major reactive bromine source. When these three sites were separated by ∼ 30 km length scales of unbroken sea ice, the BrO amount and vertical distributions were highly correlated for most of the time, indicating the horizontal length scales of BrO events were typically larger than ∼ 30 km in the absence of sea ice features. Although BrO amount and vertical distribution were similar between sites most of the time, rapid changes in BrO with edges significantly smaller than this ∼ 30 km length scale episodically transported between the sites, indicating BrO events were large but with sharp edge contrasts. BrO was often found in shallow layers that recycled reactive bromine via heterogeneous reactions on snowpack. Episodically, these surface-based events propagated aloft when aerosol extinction was higher (> 0.1 km −1 ); however, the presence of aerosol particles aloft was not sufficient to produce BrO aloft. Highly depleted ozone (< 1 nmol mol −1 ) repartitioned reactive bromine away from BrO and drove BrO events aloft in cases. This work demonstrates the interplay between atmospheric mixing and heterogeneous chemistry that affects the vertical structure and horizontal extent of reactive bromine events.

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Trace Gases in the Arctic Atmosphere

Strong

Simpson

Bognar

et al. 2020

Physics and Chemistry of the Arctic Atmosphere

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Observations of bromine monoxide transport in the Arctic sustained on aerosol particles

Cited by 60 publications

References 44 publications

Reactive bromine in the low troposphere of Antarctica. Estimations at two research sites

Reactive bromine in the low troposphere of Antarctica. Estimations at two research sites

Horizontal and vertical structure of reactive bromine events probed by bromine monoxide MAX-DOAS

Trace Gases in the Arctic Atmosphere

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