scholarly journals Chlorine activation on stratospheric aerosols: uncertainties in parameterizations and surface area

2012 ◽  
Vol 12 (8) ◽  
pp. 20561-20591 ◽  
Author(s):  
T. Wegner ◽  
J.-U. Grooß ◽  
M. von Hobe ◽  
F. Stroh ◽  
O. Sumińska-Ebersoldt ◽  
...  

Abstract. Chlorine activation in the Arctic is evaluated by examining the different parameterizations for uptake coefficients on stratospheric aerosols, high-resolution in-situ measurements and vortex-wide satellite observations. The parameterizations for heterogeneous chemistry on liquid aerosols are most sensitive to temperature with the reaction rates doubling for each Kelvin increase in temperature. However, differences between the parameterizations are negligible. For Nitric Acid Trihydrate particles (NAT) the major factors of uncertainty are the number density of nucleated particles and different parameterization choices. These two factors induce an uncertainty that covers several orders of magnitude on the reaction rate. But as predicted reaction rates on liquid aerosols always exceed those on NAT the overall uncertainty is small. In-situ observations of ClOx from Arctic winters in 2005 and 2010 are used to validate the heterogeneous chemistry parameterizations. The ambient conditions for these measurements proved to be very different between those two winters with HCl being the limiting reacting partner for the 2005 measurements and ClONO2 for the 2010 measurements. Modeled levels of chlorine activation are in very good agreement with the in-situ observations and the surface area provided by Polar Stratospheric Clouds (PSCs) has only a limited impact on modeled chlorine activation. This indicates that the parameterizations give a good representation of the processes in the atmosphere. Back-trajectories started on the location of the observations in 2005 indicate temperatures on the threshold for PSC formation, hence the surface area is mainly provided by the background aerosol. Still, the model shows additional chlorine activation during this time-frame, providing cautionary evidence for chlorine activation even in the absence of PSCs. Vortex-averaged satellite observations also show no definite connection between chlorine activation and PSC formation. The inter- and intra-annual variability of vortex-average HCl and HNO3 based on MLS observations is examined for the Arctic winters 2004/2005 to 2010/2011. These observations show that removal of HCl and HNO3 from the gas-phase are not correlated. HNO3 loss exhibits great inter-annual variability depending on prevailing temperatures while HCl loss is continuous through December without considerable inter- or intra-annual variability. Only the recovery of HCl in late in winter depends on the level of denitrification. Hence, the occurrence of HNO3 containing PSC particles does not seem to have a significant effect on the speed of initial chlorine activation on a vortex-wide scale.

2012 ◽  
Vol 12 (22) ◽  
pp. 11095-11106 ◽  
Author(s):  
T. Wegner ◽  
J.-U. Grooß ◽  
M. von Hobe ◽  
F. Stroh ◽  
O. Sumińska-Ebersoldt ◽  
...  

Abstract. Chlorine activation in the Arctic is investigated by examining different parameterizations for uptake coefficients on stratospheric aerosols, high-resolution in-situ measurements and vortex-wide satellite observations. The parameterizations for heterogeneous chemistry on liquid aerosols are most sensitive to temperature with the reaction rates doubling for every 1 K increase in temperature. However, differences between the currently available parameterizations are negligible. For Nitric Acid Trihydrate particles (NAT) the major factors of uncertainty are the number density of nucleated particles and different parameterizations for heterogeneous chemistry. These two factors induce an uncertainty that covers several orders of magnitude on the reaction rate. Nonetheless, since predicted reaction rates on liquid aerosols always exceed those on NAT, the overall uncertainty for chlorine activation is small. In-situ observations of ClOx from Arctic winters in 2005 and 2010 are used to evaluate the heterogeneous chemistry parameterizations. The conditions for these measurements proved to be very different between those two winters with HCl being the limiting reacting partner for the 2005 measurements and ClONO2 for the 2010 measurements. Modeled levels of chlorine activation are in very good agreement with the in-situ observations and the surface area provided by Polar Stratospheric Clouds (PSCs) has only a limited impact on modeled chlorine activation. This indicates that the parameterizations give a good representation of the processes in the atmosphere. Back-trajectories started on the location of the observations in 2005 indicate temperatures on the threshold for PSC formation, hence the surface area is mainly provided by the background aerosol. Still, the model shows additional chlorine activation during this time-frame, providing cautionary evidence for chlorine activation even in the absence of PSCs. Vortex-averaged satellite observations by the MLS instrument also show no definite connection between chlorine activation and PSC formation. The inter -and intra-annual variability of vortex-average HCl and HNO3 based on MLS observations is examined for the Arctic winters 2004/2005 to 2010/2011. These observations show that removal of HCl and HNO3 from the gas-phase are not correlated. HNO3 loss exhibits great inter-annual variability depending on prevailing temperatures while HCl loss is continuous through December without considerable inter- or intra-annual variability. Only the recovery of HCl in late winter depends on the level of denitrification. Hence, the occurrence of HNO3 containing PSC particles does not seem to have a significant effect on the speed of initial chlorine activation on a vortex-wide scale.


2016 ◽  
Vol 97 (6) ◽  
pp. 1033-1056 ◽  
Author(s):  
Taneil Uttal ◽  
Sandra Starkweather ◽  
James R. Drummond ◽  
Timo Vihma ◽  
Alexander P. Makshtas ◽  
...  

Abstract International Arctic Systems for Observing the Atmosphere (IASOA) activities and partnerships were initiated as a part of the 2007–09 International Polar Year (IPY) and are expected to continue for many decades as a legacy program. The IASOA focus is on coordinating intensive measurements of the Arctic atmosphere collected in the United States, Canada, Russia, Norway, Finland, and Greenland to create synthesis science that leads to an understanding of why and not just how the Arctic atmosphere is evolving. The IASOA premise is that there are limitations with Arctic modeling and satellite observations that can only be addressed with boots-on-the-ground, in situ observations and that the potential of combining individual station and network measurements into an integrated observing system is tremendous. The IASOA vision is that by further integrating with other network observing programs focusing on hydrology, glaciology, oceanography, terrestrial, and biological systems it will be possible to understand the mechanisms of the entire Arctic system, perhaps well enough for humans to mitigate undesirable variations and adapt to inevitable change.


2021 ◽  
Author(s):  
Pia Nielsen-Englyst ◽  
Jacob L. Høyer ◽  
Kristine S. Madsen ◽  
Rasmus T. Tonboe ◽  
Gorm Dybkjær ◽  
...  

Abstract. The Arctic region is responding heavily to climate change, and yet, the air temperature of ice covered areas in the Arctic is heavily under-sampled when it comes to in situ measurements, resulting in large uncertainties in existing weather- and reanalysis products. This paper presents a method for estimating daily mean clear sky 2 meter air temperatures (T2m) in the Arctic from satellite observations of skin temperature, using the Arctic and Antarctic ice Surface Temperatures from thermal Infrared (AASTI) satellite dataset, providing spatially detailed observations of the Arctic. The method is based on a linear regression model, which has been tuned against in situ observations to estimate daily mean T2m based on clear sky satellite ice surface skin temperatures. The daily satellite derived T2m product includes estimated uncertainties and covers clear sky snow and ice surfaces in the Arctic region during the period 2000–2009, provided on a 0.25 degree regular latitude-longitude grid. Comparisons with independent in situ measured T2m show average biases of 0.30 °C and 0.35 °C and average root mean square errors of 3.47 °C and 3.20 °C for land ice and sea ice, respectively. The associated uncertainties are verified to be very realistic for both land ice and sea ice, using in situ observations. The reconstruction provides a much better spatial coverage than the sparse in situ observations of T2m in the Arctic, is independent of numerical weather prediction model input and it therefore provides an important supplement to simulated air temperatures to be used for assimilation or global surface temperature reconstructions. A comparison between in situ T2m versus T2m derived from satellite and ERA-Interim/ERA5 estimates shows that the T2m derived from satellite observations validate similar or better than ERA-Interim/ERA5 in the Arctic.


2019 ◽  
Author(s):  
Pia Nielsen-Englyst ◽  
Jacob L. Høyer ◽  
Kristine S. Madsen ◽  
Rasmus T. Tonboe ◽  
Gorm Dybkjær

Abstract. The Arctic region is responding heavily to climate change, and yet, the air temperature of Arctic, ice covered areas is heavily under-sampled when it comes to in situ measurements, and large uncertainties exist in weather- and reanalysis products. This paper presents a method for estimating daily mean 2 meter air temperatures (T2m) in the Arctic from satellite observations of skin temperature, using the Arctic and Antarctic ice Surface Temperatures from thermal Infrared (AASTI) satellite dataset, providing spatially detailed observations of the Arctic. The method is based on a linear regression model which has been developed using in situ observations and daily mean satellite ice surface skin temperatures combined with a seasonal variation to estimate daily T2m. The satellite derived T2m product including estimated uncertainties covers clear sky snow and ice surfaces in the Arctic region during the period 2000–2009. Comparison with independent in situ measured T2m gives average correlations of 95.5 % and 96.5 % and average root mean square errors of 3.47 °C and 3.19 °C for land ice and sea ice, respectively. The reconstruction provides a much better spatial coverage than the sparse in situ observations of T2m in the Arctic, is independent of numerical weather prediction model input and it therefore provides an important alternative to simulated air temperatures to be used for assimilation or global surface temperature reconstructions. A comparison between in situ T2m versus T2m from satellite and ERA-Interim shows that the T2m derived from satellite observations validate similar or better than ERA-Interim estimates in the Arctic.


2013 ◽  
Vol 13 (9) ◽  
pp. 24171-24222 ◽  
Author(s):  
L. Cao ◽  
H. Sihler ◽  
U. Platt ◽  
E. Gutheil

Abstract. In recent years, the role of halogen species (e.g. Br, Cl) in the troposphere of polar regions is investigated after the discovery of their importance for boundary layer ozone destruction in the polar spring. Halogen species take part in an auto-catalytic chemical cycle including key self reactions. In this study, several chemical reaction schemes are investigated, and the importance of specific reactions and their rate constants is identified by a sensitivity analysis. A category of heterogeneous reactions related to HOBr activate halogen ions from sea salt aerosols, fresh sea ice or snow pack, driving the "bromine explosion". In the Arctic, a small amount of NOx may exist, which comes from nitrate contained in the snow, and this NOx may have a strong impact on ozone depletion. The heterogeneous reaction rates are parameterized by considering the aerodynamic resistance, a reactive surface ratio, β, i.e. ratio of reactive surface area to total ground surface area, and the boundary layer height, Lmix. It is found that for β = 1, the ozone depletion process starts after five days and lasts for 40 h for Lmix = 200 m. Ozone depletion duration becomes independent of the height of the boundary layer for about β≥20, and it approaches a value of two days for β=100. The role of nitrogen and chlorine containing species on the ozone depletion rate is studied. The calculation of the time integrated bromine and chlorine atom concentrations suggests a value in the order of 103 for the [Br] / [Cl] ratio, which reveals that atomic chlorine radicals have minor direct influence on the ozone depletion. The NOx concentrations are influenced by different chemical cycles over different time periods. During ozone depletion, the reaction cycle involving the BrONO2 hydrolysis is dominant. A critical value of 0.002 of the uptake coefficient of the BrONO2 hydrolysis reaction at the aerosol and saline surfaces is identified, beyond which the existence of NOx species accelerate the ozone depletion event – for lower values, deceleration occurs.


2020 ◽  
Author(s):  
Tuukka Petäjä ◽  
Ella-Maria Duplissy ◽  
Ksenia Tabakova ◽  
Julia Schmale ◽  
Barbara Altstädter ◽  
...  

Abstract. The role of polar regions increases in terms of megatrends such as globalization, new transport routes, demography and use of natural resources consequent effects of regional and transported pollutant concentrations. We set up the ERA-PLANET Strand 4 project iCUPE – integrative and Comprehensive Understanding on Polar Environments to provide novel insights and observational data on global grand challenges with an Arctic focus. We utilize an integrated approach combining in situ observations, satellite remote sensing Earth Observations (EO) and multi-scale modeling to synthesize data from comprehensive long-term measurements, intensive campaigns and satellites to deliver data products, metrics and indicators to the stakeholders concerning the environmental status, availability and extraction of natural resources in the polar areas. The iCUPE work consists of thematic state-of-the-art research and provision of novel data in atmospheric pollution, local sources and transboundary transport, characterization of arctic surfaces and their changes, assessment of concentrations and impacts of heavy metals and persistent organic pollutants and their cycling, quantification of emissions from natural resource extraction and validation and optimization of satellite Earth Observation (EO) data streams. In this paper we introduce the iCUPE project and summarize initial results arising out of integration of comprehensive in situ observations, satellite remote sensing and multiscale modeling in the Arctic context.


2020 ◽  
Author(s):  
Roberta Pirazzini ◽  
Michael Tjernström ◽  
Stein Sandven ◽  
Hanne Sagen ◽  
Torill Hamre ◽  
...  

<p>A comprehensive assessment of a substantial subset of Arctic observing systems, data collections and satellite products across scientific disciplines was carried out in INTAROS, also including data repositories and a brief scientific gap analysis. The assessments cover a multitude of aspects such as sustainability, technical maturity and data handling for the entire chain from observation to users, including metadata procedures and availability to data. Community based environment monitoring programs were surveyed and assessed separately; they do not form part of the present assessment.</p><p>The assessed observing systems were first ranked according to general sustainability and other aspects, were analyzed subsequently. While the range of sustainability is large, it was found that high scores on all other aspects, such as for data handling and technical maturity, are more likely for systems with high sustainability. Moreover, many systems with high sustainability, as well as advanced systems for data handling and availability in place, resulted from national commitments to international monitoring or infrastructure programs, several of which are not necessarily particular to the Arctic.</p><p>Traditionally, terrestrial and atmospheric observation network assessments build on the network concept with a “comprehensive” level including all observations, a “baseline” level of an agreed subset of sustained observations, and a “reference” level, with observations adhering to specific calibrations and traceability criteria. Examples from atmospheric observations are the “comprehensive” global GCOS radiosounding network, the “baseline” GUAN (GCOS Upper Air Network) and “reference” GRUAN (GCOS Reference Upper Air Network) networks. With the lack of in-situ observations especially from the Arctic Ocean and the logistical difficulties to deploy new stations, it was concluded that this concept does not work well in the Arctic.</p><p>In summary, we recommend that:</p><ul><li>advancement in Arctic observing should be done in international global or regional programs with well-established routines and procedures, rather than to invest in new Arctic-specific programs</li> <li>investments in new instruments and techniques be done at already established sites, to benefit interdisciplinary studies and optimize infrastructure costs</li> <li>more observations be based on ships of opportunity and that a subset of ocean, sea-ice and atmosphere observations always be made on all research expeditions, regardless of their scientific aim</li> <li>the funding structures for science expeditions is reviewed to maintain, and preferably increase, the number of expeditions and to safeguard funding for appropriate data handling and storage</li> <li>observing-network concept for the atmosphere over the Arctic Ocean is revised, so that coupled reanalyses represent the “comprehensive level”, satellite observations complemented with available in-situ data is the “baseline level”, while scientific expeditions is the “reference level”. This requires substantial improvements in reanalysis, better numerical models and data assimilation, better satellite observations and improved data handling and accessibility for scientific expeditions.</li> </ul>


2012 ◽  
Vol 25 (1) ◽  
pp. 5-24 ◽  
Author(s):  
Richard I. Cullather ◽  
Michael G. Bosilovich

Abstract Components of the atmospheric energy budget from the Modern-Era Retrospective Analysis for Research and Applications (MERRA) are evaluated in polar regions for the period 1979–2005 and compared with previous estimates, in situ observations, and contemporary reanalyses. Closure of the budget is reflected by the analysis increments term, which indicates an energy surplus of 11 W m−2 over the North Polar cap (70°–90°N) and 22 W m−2 over the South Polar cap (70°–90°S). Total atmospheric energy convergence from MERRA compares favorably with previous studies for northern high latitudes but exceeds the available previous estimate for the South Polar cap by 46%. Discrepancies with the Southern Hemisphere energy transport are largest in autumn and may be related to differences in topography with earlier reanalyses. For the Arctic, differences between MERRA and other sources in top of atmosphere (TOA) and surface radiative fluxes are largest in May. These differences are concurrent with the largest discrepancies between MERRA parameterized and observed surface albedo. For May, in situ observations of the upwelling shortwave flux in the Arctic are 80 W m−2 larger than MERRA, while the MERRA downwelling longwave flux is underestimated by 12 W m−2 throughout the year. Over grounded ice sheets, the annual mean net surface energy flux in MERRA is erroneously nonzero. Contemporary reanalyses from the Climate Forecast Center (CFSR) and the Interim Re-Analyses of the European Centre for Medium-Range Weather Forecasts (ERA-I) are found to have better surface parameterizations; however, these reanalyses also disagree with observed surface and TOA energy fluxes. Discrepancies among available reanalyses underscore the challenge of reproducing credible estimates of the atmospheric energy budget in polar regions.


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