Cyclone-induced surface ozone and HDO depletion in the Arctic

Abstract. Ground-based, satellite, and reanalysis datasets were used to identify two similar cyclone-induced surface ozone depletion events at Eureka, Canada (80.1° N, 86.4° W), in March 2007 and April 2011. These two events were coincident with observations of hydrogen deuterium oxide (HDO) depletion, indicating that condensation and sublimation occurred during the transport of the ozone-depleted air masses. Ice clouds (vapour and crystals) and aerosols were detected by lidar and radar when the ozone- and HDO-depleted air masses arrived over Eureka. For the 2007 event, an ice cloud layer was coincident with an aloft ozone depletion layer at 870 m altitude on 2–3 March, indicating this ice cloud layer contained bromine-enriched blowing-snow particles. Over the following 3 days, a shallow surface ozone depletion event (ODE) was observed at Eureka after the precipitation of bromine-enriched particles onto the local snowpack. A chemistry–climate model (UKCA) and a chemical transport model (pTOMCAT) were used to simulate the surface ozone depletion events. Incorporating the latest surface snow salinity data obtained for the Weddell Sea into the models resulted in improved agreement between the modelled and measured BrO concentrations above Eureka. MERRA-2 global reanalysis data and the FLEXPART particle dispersion model were used to study the link between the ozone and HDO depletion. In general, the modelled ozone and BrO showed good agreement with the ground-based observations; however, the modelled BrO and ozone in the near-surface layer are quite sensitive to the snow salinity. HDO depletion observed during these two blowing-snow ODEs was found to be weaker than pure Rayleigh fractionation. This work provides evidence of a blowing-snow sublimation process, which is a key step in producing bromine-enriched sea-salt aerosol.

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Cyclone-Induced Surface Ozone and HDO Depletion in the Arctic

10.5194/acp-2017-427 ◽

2017 ◽

Author(s):

Xiaoyi Zhao ◽

Dan Weaver ◽

Kristof Bognar ◽

Gloria Manney ◽

Luis Millán ◽

...

Keyword(s):

Ozone Depletion ◽

Transport Model ◽

Surface Ozone ◽

Particle Dispersion ◽

Weddell Sea ◽

Cloud Layer ◽

The Arctic ◽

Blowing Snow ◽

Near Surface ◽

Ice Cloud

Abstract. Ground-based, satellite, and reanalysis datasets were used to identify two similar cyclone-induced surface ozone depletion events at Eureka, Canada (80.1º N, 86.4º W), in March 2007 and April 2011. These two events were coincident with observations of HDO depletion, indicating that condensation and sublimation occurred during the transport of the ozone-depleted airmasses. Ice clouds (vapour and crystals) and aerosols were detected by lidar and radar when the ozone- and HDO-depleted airmasses arrived over Eureka. For the 2007 event, an ice cloud layer was coincident with an aloft ozone depletion layer at 870 m altitude on 2–3 March, indicating this ice cloud layer contained bromine-enriched blowing snow particles. Over the following three days, a shallow surface ozone depletion event (ODE) was observed at Eureka after the precipitation of bromine-enriched particles onto the local snow pack. A chemistry climate model (UKCA) and a chemical transport model (pTOMCAT) were used to simulate the surface ozone depletion events. Incorporating the latest surface snow salinity data obtained for the Weddell Sea into the models resulted in improved agreement between the modelled and measured BrO concentrations above Eureka. MERRA-2 global reanalysis data and the FLEXPART particle dispersion model were used to study the link between the ozone and HDO depletion. In general, the modelled ozone and BrO showed good agreement with the ground-based observations, however the modelled BrO and ozone in the near surface layer are quite sensitive to the snow salinity. HDO depletion observed during these two blowing-snow ODEs was found to be weaker than pure Rayleigh fractionation. This work provides evidence of a blowing-snow sublimation process, which is a key step in producing bromine-enriched sea-salt aerosol.

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Observation of HClO3 and HClO4 in the Arctic atmosphere

10.5194/egusphere-egu2020-16908 ◽

2020 ◽

Author(s):

Yee Jun Tham ◽

Nina Sarnela ◽

Carlos A. Cuevas ◽

Iyer Siddharth ◽

Lisa Beck ◽

...

Keyword(s):

Gas Phase ◽

Ozone Depletion ◽

Surface Ozone ◽

Negative Ion ◽

The Arctic ◽

Research Station ◽

Visible Absorption ◽

Data Set ◽

Near Surface ◽

Arctic Atmosphere

Atmospheric halogens chemistry like the catalytic reaction of bromine and chlorine radicals with ozone (O3) has been known to cause the springtime surface-ozone destruction in the polar region. Although the initial atmospheric reactions of chlorine with ozone are well understood, the &#64257;nal oxidation steps leading to the formation of chlorate (ClO3-) and perchlorate (ClO4-) remain unclear due to the lack of direct evidence of their presence and fate in the atmosphere. In this study, we present the first high-resolution ambient data set of gas-phase HClO3 (chloric acid) and HClO4 (perchlorate acid) obtained from the field measurement at the Villum Research Station, Station Nord, in high arctic North Greenland (81&#176;36&#8217; N, 16&#176;40&#8217; W) during the spring of 2015. A state-of-the-art chemical ionization atmospheric pressure interface time-of-flight mass spectrometer (CI-APi-TOF) was used in negative ion mode with nitrate ion as the reagent ion to detect the gas-phase HClO3 and HClO4. We measured significant level of HClO3 and HClO4 only during the springtime ozone depletion events in the Greenland, with concentration up to 9x105 molecule cm-3. Air mass trajectory analysis shows that the air during the ozone depletion event was confined to near-surface, indicating that the O3 and surface of sea-ice/snowpack may play important roles in the formation of HClO3 and HClO4. We used high-level quantum-chemical methods to calculate the ultraviolet-visible absorption spectra and cross-section of HClO3 and HClO4 in the gas-phase to assess their fates in the atmosphere. Overall, our results reveal the presence of HClO3 and HClO4 during ozone depletion events, which could affect the chlorine chemistry in the Arctic atmosphere.

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The role of open lead interactions in atmospheric ozone variability between Arctic coastal and inland sites

Elem Sci Anth ◽

10.12952/journal.elementa.000109 ◽

2016 ◽

Vol 4 ◽

Cited By ~ 2

Author(s):

Peter K. Peterson ◽

Kerri A. Pratt ◽

William R. Simpson ◽

Son V. Nghiem ◽

Lemuel X. Pérez Pérez ◽

...

Keyword(s):

Boundary Layer ◽

Sea Ice ◽

Ozone Depletion ◽

Surface Ozone ◽

Optical Absorption Spectroscopy ◽

Atmospheric Ozone ◽

Vertical Profiles ◽

Large Spatial Scale ◽

Near Surface ◽

Air Masses

Abstract Boundary layer atmospheric ozone depletion events (ODEs) are commonly observed across polar sea ice regions following polar sunrise. During March-April 2005 in Alaska, the coastal site of Barrow and inland site of Atqasuk experienced ODEs (O3< 10 nmol mol-1) concurrently for 31% of the observations, consistent with large spatial scale ozone depletion. However, 7% of the time ODEs were exclusively observed inland at Atqasuk. This phenomenon also occurred during one of nine flights during the BRomine, Ozone, and Mercury EXperiment (BROMEX), when atmospheric vertical profiles at both sites showed near-surface ozone depletion only at Atqasuk on 28 March 2012. Concurrent in-flight BrO measurements made using nadir scanning differential optical absorption spectroscopy (DOAS) showed the differences in ozone vertical profiles at these two sites could not be attributed to differences in locally occurring halogen chemistry. During both studies, backward air mass trajectories showed that the Barrow air masses observed had interacted with open sea ice leads, causing increased vertical mixing and recovery of ozone at Barrow and not Atqasuk, where the air masses only interacted with tundra and consolidated sea ice. These observations suggest that, while it is typical for coastal and inland sites to have similar ozone conditions, open leads may cause heterogeneity in the chemical composition of the springtime Arctic boundary layer over coastal and inland areas adjacent to sea ice regions.

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Br2, BrCl, BrO and surface ozone in coastal Antarctica: a meteorological and chemical analysis

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-11035-2012 ◽

2012 ◽

Vol 12 (4) ◽

pp. 11035-11077 ◽

Cited By ~ 8

Author(s):

Z. Buys ◽

N. Brough ◽

G. Huey ◽

D. Tanner ◽

R. von Glasow ◽

...

Keyword(s):

Ozone Depletion ◽

Surface Ozone ◽

Source Region ◽

The Arctic ◽

High Temporal Resolution ◽

Blowing Snow ◽

Model Calculations ◽

Air Mass ◽

Unusual Event ◽

Mixing Ratios

Abstract. There is much debate over the source of bromine radicals in the atmosphere that drives polar boundary layer ozone depletion events (ODEs), but there is strong evidence to suggest a source associated with the sea ice zone. Here we report the first high temporal resolution measurements of Br2, BrCl and BrO in coastal Antarctica, made using a Chemical Ionisation Mass Spectrometer (CIMS). Mixing ratios ranged from instrumental detection limits to 13 pptv for BrO, 45 pptv for Br2, and 6 pptv for BrCl. We find evidence for blowing snow as a source of reactive bromine both directly during a storm and subsequently from recycling of bromide deposited on the continental snowpack. An unusual event of trans-continental air mass transport might have been responsible for severe surface ozone depletion observed at Halley. The halogen source region was the Bellingshausen Sea, to the west of the Antarctic Peninsula, the air mass having spent 3 1/2 days in complete darkness prior to arrival at Halley. We, further, identify an artefact in daytime BrCl measurements arising from conversion of HOBr, similar to that already identified for CIMS observations of Br2. Model calculations using the MISTRA 0-D model suggest a 50–60% conversion of HOBr to Br2, and 5–10% conversion to BrCl. Careful data filtering enabled us to use the halogen observations, in conjunction with the MISTRA model, to explore the temperature dependence of the Br2:BrCl ratio. We find evidence of a ratio shift towards Br2 at temperatures below ~−21 °C, suggesting a relationship with hydrohalite (NaCl.2H2O) precipitation. This suite of Antarctic data provides the first analogue to similar measurements made in the Arctic.

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Influence of climate variability on near-surface ozone depletion events in the Arctic spring

Geophysical Research Letters ◽

10.1002/2014gl059275 ◽

2014 ◽

Vol 41 (7) ◽

pp. 2582-2589 ◽

Cited By ~ 3

Author(s):

Ja-Ho Koo ◽

Yuhang Wang ◽

Tianyu Jiang ◽

Yi Deng ◽

Samuel J. Oltmans ◽

...

Keyword(s):

Climate Variability ◽

Ozone Depletion ◽

Surface Ozone ◽

The Arctic ◽

Near Surface

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Ozone in the Boundary Layer air over the Arctic Ocean – measurements during the TARA expedition

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-9-8561-2009 ◽

2009 ◽

Vol 9 (2) ◽

pp. 8561-8586

Author(s):

J. W. Bottenheim ◽

S. Netcheva ◽

S. Morin ◽

S. V. Nghiem

Keyword(s):

Boundary Layer ◽

Arctic Ocean ◽

Ozone Depletion ◽

Surface Ozone ◽

The Arctic ◽

Total Absence ◽

Trajectory Calculations ◽

The Arctic Ocean ◽

Ocean Measurements ◽

Siberian Coast

Abstract. A full year of measurements of surface ozone over the Arctic Ocean far removed from land is presented (81° N – 88° N latitude). The data were obtained during the drift of the French schooner TARA between September 2006 and January 2008, while frozen in the Arctic Ocean. The data confirm that long periods of virtually total absence of ozone occur in the spring (mid March to mid June) after Polar sunrise. At other times of the year ozone concentrations are comparable to other oceanic observations with winter mole fractions of ca. 30–40 nmol mol−1 and summer minima of ca. 20 nmol mol−1. Contrary to earlier observations from ozone sonde data obtained at Arctic coastal observatories, the ambient temperature was well above −20°C during most ODEs (ozone depletion episodes). Backwards trajectory calculations suggest that during these ODEs the air had previously been in contact with the frozen ocean surface for several days and originated largely from the Siberian coast where several large open flaw leads developed in the spring of 2007.

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Pan-Arctic surface ozone seasonality modified by sea-ice-sourced bromine: modelling vs measurements

10.5194/egusphere-egu21-1262 ◽

2021 ◽

Author(s):

Xin Yang ◽

Anne-M Blechschmidt2 ◽

Kristof Bognar ◽

Audra McClure–Begley ◽

Sara Morris ◽

...

Keyword(s):

Boundary Layer ◽

Sea Ice ◽

Surface Ozone ◽

Open Ocean ◽

Arctic Sea Ice ◽

The Arctic ◽

Sea Spray ◽

Research Station ◽

Blowing Snow ◽

Model Control

Within the framework of the International Arctic Systems for Observing the Atmosphere (IASOA), we report a modelling-based study on surface ozone across the Arctic. We use surface ozone from six sites: Summit (Greenland), Pallas (Finland), Barrow (USA), Alert (Canada), Tiksi (Russia), and Villum Research Station (VRS) at Station Nord (North Greenland, Danish Realm), and ozonesonde data from three Canadian sites: Resolute, Eureka, and Alert. Two global chemistry models: a global chemistry transport model (p-TOMCAT) and a global chemistry climate model (UKCA), are used for model-data comparisons. Remotely sensed data of BrO from the GOME-2 satellite instrument at Eureka, Canada are used for model validation.The observed climatology data show that spring surface ozone at coastal Arctic is heavily depleted, making ozone seasonality at Arctic coastal sites distinctly different from that at inland sites. Model simulations show that surface ozone can be greatly reduced by bromine chemistry. In April, bromine chemistry can cause a net ozone loss (monthly mean) of 10-20 ppbv, with almost half attributable to open-ocean-sourced bromine and the rest to sea-ice-sourced bromine. However, the open-ocean-sourced bromine, via sea spray bromide depletion, cannot by itself produce ozone depletion events (ODEs) (defined as ozone volume mixing ratios VMRs < 10 ppbv). In contrast, sea-ice-sourced bromine, via sea salt aerosol (SSA) production from blowing snow, can produce ODEs even without bromine from sea spray, highlighting the importance of sea ice surface in polar boundary layer chemistry.Modelled total inorganic bromine (BrY) over the Arctic sea ice &#160;is sensitive to model configuration, e.g., under the same bromine loading, BrY in the Arctic spring boundary layer in the p-TOMCAT control run (i.e., with all bromine emissions) can be 2 times that in the UKCA control run. Despite the model differences, both model control runs can successfully reproduce large bromine explosion events (BEEs) and ODEs in polar spring. Model-integrated tropospheric column BrO generally matches GOME-2 tropospheric columns within ~50% in UKCA and a factor of 2 in p-TOMCAT. The success of the models in reproducing both ODEs and BEEs in the Arctic indicates that the relevant parameterizations implemented in the models work reasonably well, which supports the proposed mechanism of SSA production and bromide release on sea ice. Given that sea ice is a large source of SSA and halogens, changes in sea ice type and extent in a warming climate will influence Arctic boundary layer chemistry, including the oxidation of atmospheric elemental mercury. Note that this work dose not necessary rule out other possibilities that may act as a source of reactive bromine from sea ice zone.

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Regional responses of surface ozone in Europe to the location of high-latitude blocks and subtropical ridges

10.5194/acp-2016-832 ◽

2016 ◽

Author(s):

Carlos Ordóñez ◽

David Barriopedro ◽

Ricardo García-Herrera ◽

Pedro M. Sousa ◽

Jordan L. Schnell

Keyword(s):

High Latitude ◽

Climate Models ◽

Surface Ozone ◽

Zonal Flow ◽

Near Surface ◽

Air Masses ◽

Anticyclonic Circulation ◽

The Uk ◽

The Impact ◽

First Time

Abstract. This paper analyses for the first time the impact of high-latitude blocks and subtropical ridges on near-surface ozone in Europe during a 15-year period. For this purpose, a catalogue of blocks and ridges over the Euro-Atlantic region is used together with a gridded dataset of maximum daily 8-hour running average ozone (MDA8 O3) covering the period 1998–2012. The response of ozone to the location of blocks and ridges with centres in three longitudinal sectors (Atlantic, ATL, 30º–0º W; European, EUR, 0º–30º E; Russian, RUS, 30º–60º E) is examined. The impact of blocks on ozone is regionally and seasonally dependent. In particular, blocks within the EUR sector yield positive ozone anomalies of ~ 5–10 ppb over large parts of central Europe in spring and northern Europe in summer. Over 20 % and 30 % of the days with blocks in that sector register exceedances of the 90th percentile of the seasonal ozone distribution at many European locations during spring and summer, respectively. The impacts of ridges during those seasons are subtle and more sensitive to their specific location, although they can trigger ozone anomalies of ~ 5–10 ppb in Italy and the surrounding countries in summer, eventually exceeding European air quality targets. During winter, surface ozone in the northwest of Europe presents completely opposite responses to blocks and ridges. The anticyclonic circulation associated with winter EUR blocking, and to a lesser extent with ATL blocking, yields negative ozone anomalies between −5 ppb and −10 ppb over the UK, Northern France and the Benelux. Conversely, the enhanced zonal flow around 50˚–60˚ N during the occurrence of ATL ridges favours the arrival of background air masses from the Atlantic and the ventilation of the boundary layer, producing positive ozone anomalies above 5 ppb in an area spanning from the British Isles to Germany. This work provides the first quantitative assessments of the remarkable but distinct impacts that the anticyclonic circulation and the diversion of the zonal flow associated with blocks and ridges exert on surface ozone in Europe. The findings reported here can be exploited in the future to evaluate the modelled responses of ozone to circulation changes within chemical transport models (CTMs) and chemistry-climate models (CCMs).

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Widespread persistent near-surface ozone depletion at northern high latitudes in spring

Geophysical Research Letters ◽

10.1029/2003gl018587 ◽

2003 ◽

Vol 30 (24) ◽

Cited By ~ 49

Author(s):

Tao Zeng ◽

Yuhang Wang ◽

Kelly Chance ◽

Edward V. Browell ◽

Brian A. Ridley ◽

...

Keyword(s):

Ozone Depletion ◽

Surface Ozone ◽

High Latitudes ◽

Near Surface

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Direct Detection of Atmospheric Atomic Bromine Leading to Mercury and Ozone Depletion

10.5194/egusphere-egu2020-9439 ◽

2020 ◽

Author(s):

Kerri Pratt ◽

Siyuan Wang ◽

Stephen McNamara ◽

Christopher Moore ◽

Daniel Obrist ◽

...

Keyword(s):

Ozone Depletion ◽

Direct Detection ◽

Bromine Atom ◽

Critical Role ◽

Elemental Mercury ◽

Atmospheric Mercury ◽

The Arctic ◽

Molecular Bromine ◽

Near Surface ◽

Halogen Chemistry

Bromine atoms play a central role in atmospheric reactive halogen chemistry, depleting ozone and elemental mercury, thereby enhancing deposition of toxic mercury, particularly in the Arctic near-surface troposphere. Yet, direct bromine atom measurements have been missing to date, due to the lack of analytical capability with sufficient sensitivity for ambient measurements. Here we present direct atmospheric bromine atom measurements, conducted in the springtime Arctic near Utqiagvik, Alaska in March 2012. Measured bromine atom levels reached up to 14 ppt (4.2&#215;108 atoms cm-3) and were up to 3-10 higher than estimates using previous indirect measurements not considering the critical role of molecular bromine. Observed ozone and elemental mercury depletion rates are quantitatively explained by the measured bromine atoms, providing field validation of highly uncertain mercury chemistry. Following complete ozone depletion, elevated bromine concentrations are sustained by photochemical snowpack emissions of molecular bromine and nitrogen oxides, resulting in continued atmospheric mercury depletion. This study shows that measured bromine atoms, resulting from photochemical snowpack production of molecular bromine, can quantitatively explain ozone and mercury loss in the near-surface polar atmosphere.

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Cyclone-induced surface ozone and HDO depletion in the Arctic