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

2003 ◽  
Vol 30 (24) ◽  
Author(s):  
Tao Zeng ◽  
Yuhang Wang ◽  
Kelly Chance ◽  
Edward V. Browell ◽  
Brian A. Ridley ◽  
...  
2020 ◽  
Author(s):  
Yee Jun Tham ◽  
Nina Sarnela ◽  
Carlos A. Cuevas ◽  
Iyer Siddharth ◽  
Lisa Beck ◽  
...  

<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>


Elem Sci Anth ◽  
2016 ◽  
Vol 4 ◽  
Author(s):  
Peter K. Peterson ◽  
Kerri A. Pratt ◽  
William R. Simpson ◽  
Son V. Nghiem ◽  
Lemuel X. Pérez Pérez ◽  
...  

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.


2017 ◽  
Vol 17 (24) ◽  
pp. 14955-14974 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Dan Weaver ◽  
Kristof Bognar ◽  
Gloria Manney ◽  
Luis Millán ◽  
...  

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.


2014 ◽  
Vol 41 (7) ◽  
pp. 2582-2589 ◽  
Author(s):  
Ja-Ho Koo ◽  
Yuhang Wang ◽  
Tianyu Jiang ◽  
Yi Deng ◽  
Samuel J. Oltmans ◽  
...  

2017 ◽  
Author(s):  
Xiaoyi Zhao ◽  
Dan Weaver ◽  
Kristof Bognar ◽  
Gloria Manney ◽  
Luis Millán ◽  
...  

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.


2009 ◽  
Vol 9 (2) ◽  
pp. 8561-8586
Author(s):  
J. W. Bottenheim ◽  
S. Netcheva ◽  
S. Morin ◽  
S. V. Nghiem

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.


2011 ◽  
Vol 11 (4) ◽  
pp. 10875-10933 ◽  
Author(s):  
I. Cionni ◽  
V. Eyring ◽  
J. F. Lamarque ◽  
W. J. Randel ◽  
D. S. Stevenson ◽  
...  

Abstract. A continuous tropospheric and stratospheric vertically resolved ozone time series, from 1850 to 2099, has been generated to be used as forcing in global climate models that do not include interactive chemistry. A multiple linear regression analysis of SAGE I+II satellite observations and polar ozonesonde measurements is used for the stratospheric zonal mean dataset during the well-observed period from 1979 to 2009. In addition to terms describing the mean annual cycle, the regression includes terms representing equivalent effective stratospheric chlorine (EESC) and the 11-yr solar cycle variability. The EESC regression fit coefficients, together with pre-1979 EESC values, are used to extrapolate the stratospheric ozone time series backward to 1850. While a similar procedure could be used to extrapolate into the future, coupled chemistry climate model (CCM) simulations indicate that future stratospheric ozone abundances are likely to be significantly affected by climate change, and capturing such effects through a regression model approach is not feasible. Therefore, the stratospheric ozone dataset is extended into the future (merged in 2009) with multi-model mean projections from 13 CCMs that performed a simulation until 2099 under the SRES (Special Report on Emission Scenarios) A1B greenhouse gas scenario and the A1 adjusted halogen scenario in the second round of the Chemistry-Climate Model Validation (CCMVal-2) Activity. The stratospheric zonal mean ozone time series is merged with a three-dimensional tropospheric data set extracted from simulations of the past by two CCMs (CAM3.5 and PUCCINI) and of the future by one CCM (CAM3.5). The future tropospheric ozone time series continues the historical CAM3.5 simulation until 2099 following the four different Representative Concentration Pathways (RCPs). Generally good agreement is found between the historical segment of the ozone database and satellite observations, although it should be noted that total column ozone is overestimated in the southern polar latitudes during spring and tropospheric column ozone is slightly underestimated. Vertical profiles of tropospheric ozone are broadly consistent with ozonesondes and in-situ measurements, with some deviations in regions of biomass burning. The tropospheric ozone radiative forcing (RF) from the 1850s to the 2000s is 0.23 W m−2, lower than previous results. The lower value is mainly due to (i) a smaller increase in biomass burning emissions; (ii) a larger influence of stratospheric ozone depletion on upper tropospheric ozone at high southern latitudes; and possibly (iii) a larger influence of clouds (which act to reduce the net forcing) compared to previous radiative forcing calculations. Over the same period, decreases in stratospheric ozone, mainly at high latitudes, produce a RF of −0.08 W m−2, which is more negative than the central Intergovernmental Panel on Climate Change (IPCC) Fourth Assessment Report (AR4) value of −0.05 W m−2, but which is within the stated range of −0.15 to +0.05 W m−2. The more negative value is explained by the fact that the regression model simulates significant ozone depletion prior to 1979, in line with the increase in EESC and as confirmed by CCMs, while the AR4 assumed no change in stratospheric RF prior to 1979. A negative RF of similar magnitude persists into the future, although its location shifts from high latitudes to the tropics. This shift is due to increases in polar stratospheric ozone, but decreases in tropical lower stratospheric ozone, related to a strengthening of the Brewer-Dobson circulation, particularly through the latter half of the 21st century. Differences in trends in tropospheric ozone among the four RCPs are mainly driven by different methane concentrations, resulting in a range of tropospheric ozone RFs between 0.4 and 0.1 W m−2 by 2100. The ozone dataset described here has been released for the Coupled Model Intercomparison Project (CMIP5) model simulations in netCDF Climate and Forecast (CF) Metadata Convention at the PCMDI website (http://cmip-pcmdi.llnl.gov/).


Atmosphere ◽  
2021 ◽  
Vol 12 (11) ◽  
pp. 1494
Author(s):  
Fernanda Casagrande ◽  
Francisco A. B. Neto ◽  
Ronald B. de Souza ◽  
Paulo Nobre

One of the most visible signs of global warming is the fast change in the polar regions. The increase in Arctic temperatures, for instance, is almost twice as large as the global average in recent decades. This phenomenon is known as the Arctic Amplification and reflects several mutually supporting processes. An equivalent albeit less studied phenomenon occurs in Antarctica. Here, we used numerical climate simulations obtained from CMIP5 and CMIP6 to investigate the effects of +1.5, 2 and 3 °C warming thresholds for sea ice changes and polar amplification. Our results show robust patterns of near-surface air-temperature response to global warming at high latitudes. The year in which the average air temperatures brought from CMIP5 and CMIP6 models rises by 1.5 °C is 2024. An average rise of 2 °C (3 °C) global warming occurs in 2042 (2063). The equivalent warming at northern (southern) high latitudes under scenarios of 1.5 °C global warming is about 3 °C (1.8 °C). In scenarios of 3 °C global warming, the equivalent warming in the Arctic (Antarctica) is close to 7 °C (3.5 °C). Ice-free conditions are found in all warming thresholds for both the Arctic and Antarctica, especially from the year 2030 onwards.


Atmosphere ◽  
2019 ◽  
Vol 10 (12) ◽  
pp. 760 ◽  
Author(s):  
Wanyi Qiu ◽  
Shule Li ◽  
Yuhan Liu ◽  
Keding Lu

Due to the development of industrialization and urbanization, secondary pollution is becoming increasingly serious in the Yangtze River Delta. Volatile organic compounds (VOCs) are key precursors of the near-surface ozone, secondary organic aerosol (SOA), and other secondary pollutants. In this study, we chose a serious ozone pollution period (01 May–31 July 2017) in Jinshan, which is a petrochemical and industrial area in Shanghai. We explored the VOCs distribution characteristics and contribution to secondary pollutants via constructing a regional network based on wind patterns. We determined that dense pollutants were accumulated at adjacent sites under local circulation (LC), and pollution from petrochemical discharge was more serious than industry for all sites under southeast (SE) wind. We also found that cyclopentane, o-xylene, m/p-xylene, 1-3-butadiene, and 1-hexene were priority-controlled species as they were most vital to form secondary pollutants. This study proves that regional network analysis can be successfully applied to explore pollution characteristics and regional secondary pollutants formation.


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