scholarly journals Observation of HClO3 and HClO4 in the Arctic atmosphere

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

<p>Atmospheric halogens chemistry like the catalytic reaction of bromine and chlorine radicals with ozone (O<sub>3</sub>) 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 final oxidation steps leading to the formation of chlorate (ClO<sub>3</sub><sup>-</sup>) and perchlorate (ClO<sub>4</sub><sup>-</sup>) 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 HClO<sub>3</sub> (chloric acid) and HClO<sub>4</sub> (perchlorate acid) obtained from the field measurement at the Villum Research Station, Station Nord, in high arctic North Greenland (81°36’ N, 16°40’ 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 HClO<sub>3</sub> and HClO<sub>4</sub>. We measured significant level of HClO<sub>3</sub> and HClO<sub>4</sub> only during the springtime ozone depletion events in the Greenland, with concentration up to 9x10<sup>5</sup> molecule cm<sup>-3</sup>. Air mass trajectory analysis shows that the air during the ozone depletion event was confined to near-surface, indicating that the O<sub>3</sub> and surface of sea-ice/snowpack may play important roles in the formation of HClO<sub>3</sub> and HClO<sub>4</sub>. We used high-level quantum-chemical methods to calculate the ultraviolet-visible absorption spectra and cross-section of HClO<sub>3</sub> and HClO<sub>4</sub> in the gas-phase to assess their fates in the atmosphere. Overall, our results reveal the presence of HClO<sub>3</sub> and HClO<sub>4</sub> during ozone depletion events, which could affect the chlorine chemistry in the Arctic atmosphere.</p>

scholarly journals Cyclone-induced surface ozone and HDO depletion in the Arctic

2017 ◽  
Vol 17 (24) ◽  
pp. 14955-14974 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Dan Weaver ◽  
Kristof Bognar ◽  
Gloria Manney ◽  
Luis Millán ◽  
...  
Keyword(s):  
Ozone Depletion ◽  
Deuterium Oxide ◽  
Surface Ozone ◽  
Weddell Sea ◽  
Cloud Layer ◽  
The Arctic ◽  
Blowing Snow ◽  
Near Surface ◽  
Air Masses ◽  
Ice Cloud

Abstract. Ground-based, satellite, and reanalysis datasets were used to identify two similar cyclone-induced surface ozone depletion events at Eureka, Canada (80.1° 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.

scholarly journals Surface ozone depletion episodes in the Arctic and Antarctic from historical ozonesonde records

2002 ◽  
Vol 2 (3) ◽  
pp. 197-205 ◽  
Author(s):  
D. W. Tarasick ◽  
J. W. Bottenheim
Keyword(s):  
Ozone Depletion ◽  
Surface Ozone ◽  
Catalytic Reactions ◽  
The Arctic ◽  
Confidence Limits ◽  
Apparent Increase ◽  
Surface Temperatures ◽  
High Concentrations ◽  
Arctic Atmosphere ◽  
Arctic Biota

Abstract. Episodes of ozone depletion in the lowermost Arctic atmosphere (0--2 km) at polar sunrise have been intensively studied at Alert, Canada, and are thought to result from catalytic reactions involving bromine. Recent observations of high concentrations of tropospheric BrO over large areas of the Arctic and Antarctic suggest that such depletion events should also be seen by ozonesondes at other polar stations. An examination of historical ozonesonde records shows that such events occur frequently at Alert, Eureka and Resolute, but much less frequently at Churchill and at other stations. The differences appear to be related to differences in average springtime surface temperatures. The long record at Resolute shows depletions since 1966, but with an increase in their frequency over the period 1966--2000 of 0.66 ± 0.59% per year (95% confidence limits), explaining the apparent increase of Hg in Arctic biota in recent times.

scholarly journals Surface ozone depletion episodes in the Arctic and Antarctic from historical ozonesonde records

2002 ◽  
Vol 2 (2) ◽  
pp. 339-356 ◽  
Author(s):  
D. W. Tarasick ◽  
J. W. Bottenheim
Keyword(s):  
Ozone Depletion ◽  
Surface Ozone ◽  
Catalytic Reactions ◽  
The Arctic ◽  
Apparent Increase ◽  
Natural Origin ◽  
High Concentrations ◽  
Arctic Atmosphere

Abstract. Episodes of ozone depletion in the lowermost Arctic atmosphere (0--2 km) at polar sunrise have been intensively studied at Alert, Canada, and are thought to result from catalytic reactions involving bromine. Recent observations of high concentrations of tropospheric BrO over large areas of the Arctic and Antarctic suggest that such depletion events should also be seen by ozonesondes at other polar stations. An examination of historical ozonesonde records shows that such events occur frequently at Alert, Eureka and Resolute, but much less frequently at Churchill and at other stations. The differences appear to be attributable to differences in surface meteorology. The long record at Resolute shows depletions since 1966, but with an apparent increase in their frequency since about 1985. This is surprising, since the Br involved in the depletion mechanism is believed to be entirely of natural origin.

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

2014 ◽  
Vol 41 (7) ◽  
pp. 2582-2589 ◽  
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

scholarly journals Cyclone-Induced Surface Ozone and HDO Depletion in the Arctic

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.

scholarly journals Reproducing springtime Arctic tropospheric ozone depletion events in an outdoor mesocosm sea-ice facility

2021 ◽  
Author(s):  
Zhiyuan Gao ◽  
Nicolas-Xavier Geilfus ◽  
Alfonso Saiz-Lopez ◽  
Feiyue Wang
Keyword(s):  
Boundary Layer ◽  
Sea Ice ◽  
Gas Phase ◽  
Ozone Depletion ◽  
Surface Ozone ◽  
Environmental Research ◽  
The Arctic ◽  
Ozone Loss ◽  
Ozone Concentrations ◽  
Air Temperatures

Abstract. The episodic build-up of gas-phase reactive bromine species over sea ice and snowpack in the springtime Arctic plays an important role in the boundary layer, causing annual concurrent depletion of ozone and gaseous elemental mercury during polar sunrise. Extensive studies have shown that these phenomena, known as bromine explosion events (BEEs), ozone depletion events (ODEs) and mercury depletion events (MDEs), respectively, are all triggered by gas-phase reactive bromine species that are photochemically activated from bromide via multi-phase reactions under freezing air temperatures. However, major knowledge gaps exist in both fundamental cryo-photochemical processes causing these events and meteorological conditions that may affect their timing and magnitude. Here, we report an outdoor mesocosm-scale study in which we successfully reproduced ODEs at the Sea-ice Environmental Research Facility (SERF) in Winnipeg, Canada. By monitoring ozone concentrations inside large, acrylic tubes over bromide-enriched artificial seawater during entire sea ice freeze-and-melt cycles, we observed mid-day photochemical ozone loss in winter in the boundary layer air immediately above the sea ice surface in a pattern that is characteristic of BEE-induced ODEs in the Arctic. The importance of UV radiation and the presence of a condensed phase (experimental sea ice or snow) in causing such surface ozone loss was demonstrated by comparing ozone concentrations between UV-transmitting and UV-blocking acrylic tubes under different air temperatures. The ability of reproducing BEE-induced ODEs at a mesocosm scale in a non-polar region provides a new approach to systematically studying the cryo-photochemical and meteorological processes leading to BEEs, ODEs, and MDEs in the Arctic, their role in biogeochemical cycles across the ocean-sea ice-atmosphere interfaces, and their sensitivities to climate change.

scholarly journals Polyfluoroalkyl compounds in the Canadian Arctic atmosphere

2011 ◽  
Vol 8 (4) ◽  
pp. 399 ◽  
Author(s):  
Lutz Ahrens ◽  
Mahiba Shoeib ◽  
Sabino Del Vento ◽  
Garry Codling ◽  
Crispin Halsall
Keyword(s):  
Gas Phase ◽  
Environmental Concern ◽  
Canadian Arctic ◽  
High Volume ◽  
Ambient Air ◽  
Coast Guard ◽  
The Arctic ◽  
Particle Phase ◽  
Method Performance ◽  
Arctic Atmosphere

Environmental contextPerfluoroalkyl compounds are of rising environmental concern because of their ubiquitous distribution in remote regions like the Arctic. The present study quantifies these contaminants in the gas and particle phases of the Canadian Arctic atmosphere. The results demonstrate the important role played by gas–particle partitioning in the transport and fate of perfluoroalkyl compounds in the atmosphere. AbstractPolyfluoroalkyl compounds (PFCs) were determined in high-volume air samples during a ship cruise onboard the Canadian Coast Guard Ship Amundsen crossing the Labrador Sea, Hudson Bay and the Beaufort Sea of the Canadian Arctic. Five PFC classes (i.e. perfluoroalkyl carboxylates (PFCAs), polyfluoroalkyl sulfonates (PFSAs), fluorotelomer alcohols (FTOHs), fluorinated sulfonamides (FOSAs), and sulfonamidoethanols (FOSEs)) were analysed separately in the gas phase collected on PUF/XAD-2 sandwiches and in the particle phase on glass-fibre filters (GFFs). The method performance of sampling, extraction and instrumental analysis were compared between two research groups. The FTOHs were the dominant PFCs in the gas phase (20–138 pg m–3), followed by the FOSEs (0.4–23 pg m–3) and FOSAs (0.5–4.7 pg m–3). The PFCAs could only be quantified in the particle phase with low levels (<0.04–0.18 pg m–3). In the particle phase, the dominant PFC class was the FOSEs (0.3–8.6 pg m–3). The particle-associated fraction followed the general trend of: FOSEs (~25 %) > FOSAs (~9 %) > FTOHs (~1 %). Significant positive correlation between ∑FOSA concentrations in the gas phase and ambient air temperature indicate that cold Arctic surfaces, such as the sea-ice snowpack and surface seawater could be influencing FOSAs in the atmosphere.

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

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.

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

Elem Sci Anth ◽  
2016 ◽  
Vol 4 ◽  
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&lt; 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.

scholarly journals Seasonal and interannual variations in the propagation of photosynthetically available radiation through the Arctic atmosphere

Elem Sci Anth ◽  
2021 ◽  
Vol 9 (1) ◽  
Author(s):  
J. Laliberté ◽  
S. Bélanger ◽  
M. Babin
Keyword(s):  
Large Data ◽  
The Arctic ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
The Sun ◽  
Photosynthetically Available Radiation ◽  
Data Set ◽  
Melt Ponds ◽  
Arctic Atmosphere ◽  
Marine Productivity

The Arctic atmosphere–surface system transmits visible light from the Sun to the ocean, determining the annual cycle of light available to microalgae. This light is referred to as photosynthetically available radiation (PAR). A known consequence of Arctic warming is the change at the atmosphere–ocean interface (longer ice-free season, younger ice), implying an increase in the percentage of PAR being transferred to the water. However, much less is known about the recent changes in how much PAR is being transferred by the overlaying atmosphere. We studied the transfer of PAR through the atmosphere between May 21 and July 23 at a pan-Arctic scale for the period ranging from 2000 to 2016. By combining a large data set of atmospheric and surface conditions into a radiative transfer model, we computed the percentage of PAR transferred to the surface. We found that typical Arctic atmospheres convey between 60% and 70% of the incident PAR received from the Sun, meaning the Arctic atmosphere typically transmits more light than most sea ice surfaces, with the exception of mature melt ponds. We also found that the transfer of PAR through the atmosphere decreased at a rate of 2.3% per decade over the studied period, due to the increase in cloudiness and the weaker radiative interaction between the atmosphere and the surface. Further investigation is required to address how, in the warmer Arctic climate, this negative trend would compensate for the increased surface transmittance and its consequences on marine productivity.

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