Articles | Volume 17, issue 10
https://doi.org/10.5194/acp-17-6291-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-6291-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Evaporating brine from frost flowers with electron microscopy and implications for atmospheric chemistry and sea-salt aerosol formation
British Antarctic Survey, Natural Environment Research Council,
Cambridge, UK
Vilém Neděla
Environmental Electron Microscopy Group, Institute of Scientific
Instruments of the CAS, Brno, Czech Republic
Jiří Runštuk
Environmental Electron Microscopy Group, Institute of Scientific
Instruments of the CAS, Brno, Czech Republic
Gabriela Ondrušková
Department of Chemistry, Faculty of Science, Masaryk University,
Kamenice 5/A8, 625 00 Brno, Czech Republic
Research Centre for Toxic Compounds in the Environment (RECETOX),
Masaryk University, Kamenice 5/A29, 625 00 Brno, Czech Republic
Ján Krausko
Department of Chemistry, Faculty of Science, Masaryk University,
Kamenice 5/A8, 625 00 Brno, Czech Republic
Research Centre for Toxic Compounds in the Environment (RECETOX),
Masaryk University, Kamenice 5/A29, 625 00 Brno, Czech Republic
Ľubica Vetráková
Department of Chemistry, Faculty of Science, Masaryk University,
Kamenice 5/A8, 625 00 Brno, Czech Republic
Research Centre for Toxic Compounds in the Environment (RECETOX),
Masaryk University, Kamenice 5/A29, 625 00 Brno, Czech Republic
Department of Chemistry, Faculty of Science, Masaryk University,
Kamenice 5/A8, 625 00 Brno, Czech Republic
Research Centre for Toxic Compounds in the Environment (RECETOX),
Masaryk University, Kamenice 5/A29, 625 00 Brno, Czech Republic
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
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Salt aerosols are important to polar atmospheric chemistry and global climate. Therefore, we utilized a unique electron microscope to identify the most suitable conditions for formation of the small salt (CsCl) particles, proxies of the aerosols, from sublimating salty snow. Very low sublimation temperature and low salt concentration are needed for formation of such particles. These observations may help us to better understand polar spring ozone depletion and bromine explosion events.
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Preprint archived
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Snow pack in high Arctic plays a key role in polar atmospheric chemistry, especially in spring when photochemistry becomes active. By sampling surface snow from a Canadian high Arctic location at Eureka, Nunavut (80° N, 86° W), we demonstrate that surface snow is a net sink rather than a source of atmospheric reactive bromine and nitrate. This finding is new and opposite to previous conclusions that snowpack is a large and direct source of reactive bromine in polar spring.
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Manuscript not accepted for further review
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In polar regions, sea salt aerosols are important to polar atmospheric chemistry, yet their mechanism of formation is not well understood. We inspected the sublimation residues of salty ices in a unique electron microscope and sought for small salt particles, proxies of sea salt aerosols. Our experiments showed that aerosolizable salt particles are preferably generated from low-concentrated ices and at low temperatures. This condition favors salty snow as an efficient source of the aerosols.
Xin Yang, Anne-M. Blechschmidt, Kristof Bognar, Audra McClure-Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David W. Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
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This is a comprehensive model–data comparison aiming to evaluate the proposed mechanism of sea salt aerosol (SSA) production from blowing snow on sea ice. Some key parameters such as snow salinity and blowing-snow size distribution were constrained by data collected in the Weddell Sea. The good agreement between modelled SSA and the cruise data strongly indicates that sea ice surface is a large SSA source in polar regions, a process which has not been considered in current climate models.
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Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
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Sea salt aerosol comes from the open ocean or the sea ice surface. In the polar regions, this opens up the possibility of reconstructing sea ice history using sea salt recorded in ice cores. We use a chemical transport model to demonstrate that the sea ice source of aerosol is important in the Arctic. For the first time, we simulate realistic Greenland ice core sea salt in a process-based model. The importance of the sea ice source increases from south to north across the Greenland ice sheet.
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Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
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This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
S. Tegtmeier, F. Ziska, I. Pisso, B. Quack, G. J. M. Velders, X. Yang, and K. Krüger
Atmos. Chem. Phys., 15, 13647–13663, https://doi.org/10.5194/acp-15-13647-2015, https://doi.org/10.5194/acp-15-13647-2015, 2015
Short summary
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At present, man-made halogens and natural oceanic substances both contribute to the observed ozone depletion. Emissions of the anthropogenic halogens have been reduced, whereas emissions of the natural substances are expected to increase in future climate due to anthropogenic activities affecting oceanic processes. We assess the impact of these oceanic substances on ozone by weighting their emissions with their potential to destroy ozone for current conditions and future projections.
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
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Atmos. Chem. Phys., 23, 4463–4488, https://doi.org/10.5194/acp-23-4463-2023, https://doi.org/10.5194/acp-23-4463-2023, 2023
Short summary
Short summary
Salt aerosols are important to polar atmospheric chemistry and global climate. Therefore, we utilized a unique electron microscope to identify the most suitable conditions for formation of the small salt (CsCl) particles, proxies of the aerosols, from sublimating salty snow. Very low sublimation temperature and low salt concentration are needed for formation of such particles. These observations may help us to better understand polar spring ozone depletion and bromine explosion events.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
EGUsphere, https://doi.org/10.5194/egusphere-2022-696, https://doi.org/10.5194/egusphere-2022-696, 2022
Preprint archived
Short summary
Short summary
Snow pack in high Arctic plays a key role in polar atmospheric chemistry, especially in spring when photochemistry becomes active. By sampling surface snow from a Canadian high Arctic location at Eureka, Nunavut (80° N, 86° W), we demonstrate that surface snow is a net sink rather than a source of atmospheric reactive bromine and nitrate. This finding is new and opposite to previous conclusions that snowpack is a large and direct source of reactive bromine in polar spring.
Ľubica Vetráková, Vilém Neděla, Jiří Runštuk, Xin Yang, and Dominik Heger
The Cryosphere Discuss., https://doi.org/10.5194/tc-2021-376, https://doi.org/10.5194/tc-2021-376, 2022
Manuscript not accepted for further review
Short summary
Short summary
In polar regions, sea salt aerosols are important to polar atmospheric chemistry, yet their mechanism of formation is not well understood. We inspected the sublimation residues of salty ices in a unique electron microscope and sought for small salt particles, proxies of sea salt aerosols. Our experiments showed that aerosolizable salt particles are preferably generated from low-concentrated ices and at low temperatures. This condition favors salty snow as an efficient source of the aerosols.
Xin Yang, Anne-M. Blechschmidt, Kristof Bognar, Audra McClure-Begley, Sara Morris, Irina Petropavlovskikh, Andreas Richter, Henrik Skov, Kimberly Strong, David W. Tarasick, Taneil Uttal, Mika Vestenius, and Xiaoyi Zhao
Atmos. Chem. Phys., 20, 15937–15967, https://doi.org/10.5194/acp-20-15937-2020, https://doi.org/10.5194/acp-20-15937-2020, 2020
Short summary
Short summary
This is a modelling-based study on Arctic surface ozone, with a particular focus on spring ozone depletion events (i.e. with concentrations < 10 ppbv). Model experiments show that model runs with blowing-snow-sourced sea salt aerosols implemented as a source of reactive bromine can reproduce well large-scale ozone depletion events observed in the Arctic. This study supplies modelling evidence of the proposed mechanism of reactive-bromine release from blowing snow on sea ice (Yang et al., 2008).
V. Holly L. Winton, Alison Ming, Nicolas Caillon, Lisa Hauge, Anna E. Jones, Joel Savarino, Xin Yang, and Markus M. Frey
Atmos. Chem. Phys., 20, 5861–5885, https://doi.org/10.5194/acp-20-5861-2020, https://doi.org/10.5194/acp-20-5861-2020, 2020
Short summary
Short summary
The transfer of the nitrogen stable isotopic composition in nitrate between the air and snow at low accumulation sites in Antarctica leaves an UV imprint in the snow. Quantifying how nitrate isotope values change allows us to interpret longer ice core records. Based on nitrate observations and modelling at Kohnen, East Antarctica, the dominant factors controlling the nitrate isotope signature in deep snow layers are the depth of light penetration into the snowpack and the snow accumulation rate.
Markus M. Frey, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Xin Yang, Anna E. Jones, Michelle G. Nerentorp Mastromonaco, David H. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 20, 2549–2578, https://doi.org/10.5194/acp-20-2549-2020, https://doi.org/10.5194/acp-20-2549-2020, 2020
Short summary
Short summary
A winter sea ice expedition to Antarctica provided the first direct observations of sea salt aerosol (SSA) production during snow storms above sea ice, thereby validating a model hypothesis to account for winter time SSA maxima in Antarctica not explained otherwise. Defining SSA sources is important given the critical roles that aerosol plays for climate, for air quality and as a potential ice core proxy for sea ice conditions in the past.
Ľubica Vetráková, Vilém Neděla, Jiří Runštuk, and Dominik Heger
The Cryosphere, 13, 2385–2405, https://doi.org/10.5194/tc-13-2385-2019, https://doi.org/10.5194/tc-13-2385-2019, 2019
Short summary
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We froze salty solutions to examine where and how the brine is distributed within the ice by using an environmental scanning electron microscope. The structures are highly heterogeneous, consisting of almost pure ice intertwined with brine, which can form lamellae, veins, or pools on the surface. Considering various concentrations and methods for laboratory ice preparation, we determined how the freezing technique influences the microstructure of the brine on and in the ice.
Xin Yang, Markus M. Frey, Rachael H. Rhodes, Sarah J. Norris, Ian M. Brooks, Philip S. Anderson, Kouichi Nishimura, Anna E. Jones, and Eric W. Wolff
Atmos. Chem. Phys., 19, 8407–8424, https://doi.org/10.5194/acp-19-8407-2019, https://doi.org/10.5194/acp-19-8407-2019, 2019
Short summary
Short summary
This is a comprehensive model–data comparison aiming to evaluate the proposed mechanism of sea salt aerosol (SSA) production from blowing snow on sea ice. Some key parameters such as snow salinity and blowing-snow size distribution were constrained by data collected in the Weddell Sea. The good agreement between modelled SSA and the cruise data strongly indicates that sea ice surface is a large SSA source in polar regions, a process which has not been considered in current climate models.
Fraser Dennison, James Keeble, Olaf Morgenstern, Guang Zeng, N. Luke Abraham, and Xin Yang
Geosci. Model Dev., 12, 1227–1239, https://doi.org/10.5194/gmd-12-1227-2019, https://doi.org/10.5194/gmd-12-1227-2019, 2019
Short summary
Short summary
Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
Xiaoyi Zhao, Dan Weaver, Kristof Bognar, Gloria Manney, Luis Millán, Xin Yang, Edwin Eloranta, Matthias Schneider, and Kimberly Strong
Atmos. Chem. Phys., 17, 14955–14974, https://doi.org/10.5194/acp-17-14955-2017, https://doi.org/10.5194/acp-17-14955-2017, 2017
Short summary
Short summary
Few scientific questions about surface ozone depletion have been addressed, using a variety of measurements and atmospheric models. The lifetime of reactive bromine is only a few hours in the absence of recycling. Evidence of this recycling over aerosol or blowing-snow/ice particles was found at Eureka. The blowing snow sublimation process is a key step in producing bromine-enriched sea-salt aerosol. Ground-based FTIR isotopologue measurements at Eureka provided evidence of this key step.
Rachael H. Rhodes, Xin Yang, Eric W. Wolff, Joseph R. McConnell, and Markus M. Frey
Atmos. Chem. Phys., 17, 9417–9433, https://doi.org/10.5194/acp-17-9417-2017, https://doi.org/10.5194/acp-17-9417-2017, 2017
Short summary
Short summary
Sea salt aerosol comes from the open ocean or the sea ice surface. In the polar regions, this opens up the possibility of reconstructing sea ice history using sea salt recorded in ice cores. We use a chemical transport model to demonstrate that the sea ice source of aerosol is important in the Arctic. For the first time, we simulate realistic Greenland ice core sea salt in a process-based model. The importance of the sea ice source increases from south to north across the Greenland ice sheet.
Oleg Travnikov, Hélène Angot, Paulo Artaxo, Mariantonia Bencardino, Johannes Bieser, Francesco D'Amore, Ashu Dastoor, Francesco De Simone, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Christian N. Gencarelli, Ian M. Hedgecock, Olivier Magand, Lynwill Martin, Volker Matthias, Nikolay Mashyanov, Nicola Pirrone, Ramesh Ramachandran, Katie Alana Read, Andrei Ryjkov, Noelle E. Selin, Fabrizio Sena, Shaojie Song, Francesca Sprovieri, Dennis Wip, Ingvar Wängberg, and Xin Yang
Atmos. Chem. Phys., 17, 5271–5295, https://doi.org/10.5194/acp-17-5271-2017, https://doi.org/10.5194/acp-17-5271-2017, 2017
Short summary
Short summary
The study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measurement data and simulation results of chemical transport models. Evaluation of the model simulations and numerical experiments against observations allows explaining spatial and temporal variations of Hg concentration in the near-surface atmospheric layer and shows possibility of multiple pathways of Hg oxidation occurring concurrently in various parts of the atmosphere.
Christian N. Gencarelli, Johannes Bieser, Francesco Carbone, Francesco De Simone, Ian M. Hedgecock, Volker Matthias, Oleg Travnikov, Xin Yang, and Nicola Pirrone
Atmos. Chem. Phys., 17, 627–643, https://doi.org/10.5194/acp-17-627-2017, https://doi.org/10.5194/acp-17-627-2017, 2017
Short summary
Short summary
Atmospheric deposition is an important pathway by which Hg reaches marine ecosystems, where it can be methylated and enter the base of food chain. High resolution numerical experiments has been performed in order to investigate the contributions (sensitivity) of the Hg anthtropogenic emissions, speciation and atmospherical chemical reactions on Hg depositions over Europe. The comparison of wet deposition fluxes and concentrations measured on 28 monitioring sites were used to support the analysis.
Hélène Angot, Ashu Dastoor, Francesco De Simone, Katarina Gårdfeldt, Christian N. Gencarelli, Ian M. Hedgecock, Sarka Langer, Olivier Magand, Michelle N. Mastromonaco, Claus Nordstrøm, Katrine A. Pfaffhuber, Nicola Pirrone, Andrei Ryjkov, Noelle E. Selin, Henrik Skov, Shaojie Song, Francesca Sprovieri, Alexandra Steffen, Kenjiro Toyota, Oleg Travnikov, Xin Yang, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 10735–10763, https://doi.org/10.5194/acp-16-10735-2016, https://doi.org/10.5194/acp-16-10735-2016, 2016
Short summary
Short summary
This is a synthesis of the atmospheric mercury (Hg) monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. Based on this comparison, we discuss whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models, and identify remaining research gaps.
S. Tegtmeier, F. Ziska, I. Pisso, B. Quack, G. J. M. Velders, X. Yang, and K. Krüger
Atmos. Chem. Phys., 15, 13647–13663, https://doi.org/10.5194/acp-15-13647-2015, https://doi.org/10.5194/acp-15-13647-2015, 2015
Short summary
Short summary
At present, man-made halogens and natural oceanic substances both contribute to the observed ozone depletion. Emissions of the anthropogenic halogens have been reduced, whereas emissions of the natural substances are expected to increase in future climate due to anthropogenic activities affecting oceanic processes. We assess the impact of these oceanic substances on ozone by weighting their emissions with their potential to destroy ozone for current conditions and future projections.
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
A. Banerjee, A. T. Archibald, A. C. Maycock, P. Telford, N. L. Abraham, X. Yang, P. Braesicke, and J. A. Pyle
Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, https://doi.org/10.5194/acp-14-9871-2014, 2014
Related subject area
Subject: Hydrosphere Interactions | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Short summary
Short summary
Chemicals are commonly found in snowpacks throughout the world and may be degraded by sunlight; some previous research has reported faster decay rates for chemicals on the surface of snow and ice compared to in water. We found photodegradation on snow can be as much as 30 times faster than in solution for the three dimethoxybenzene isomers. Our computational modeling found light absorbance by dimethoxybenzenes increases on the snow surface, but this only partially explains the decay rate.
Dimitri Osmont, Isabel A. Wendl, Loïc Schmidely, Michael Sigl, Carmen P. Vega, Elisabeth Isaksson, and Margit Schwikowski
Atmos. Chem. Phys., 18, 12777–12795, https://doi.org/10.5194/acp-18-12777-2018, https://doi.org/10.5194/acp-18-12777-2018, 2018
Short summary
Short summary
This study presents the first long-term and high-resolution refractory black carbon (rBC) ice core record from Svalbard, spanning the last 800 years. Our results show that rBC has had a predominant anthropogenic origin since the beginning of the Industrial Revolution in Europe and that rBC concentrations have been declining in the last 40 years. We discuss the impact of 20th century snowmelt on our record. We reconstruct biomass burning trends prior to 1800 by using a multi-proxy approach.
T. Bartels-Rausch, H.-W. Jacobi, T. F. Kahan, J. L. Thomas, E. S. Thomson, J. P. D. Abbatt, M. Ammann, J. R. Blackford, H. Bluhm, C. Boxe, F. Domine, M. M. Frey, I. Gladich, M. I. Guzmán, D. Heger, Th. Huthwelker, P. Klán, W. F. Kuhs, M. H. Kuo, S. Maus, S. G. Moussa, V. F. McNeill, J. T. Newberg, J. B. C. Pettersson, M. Roeselová, and J. R. Sodeau
Atmos. Chem. Phys., 14, 1587–1633, https://doi.org/10.5194/acp-14-1587-2014, https://doi.org/10.5194/acp-14-1587-2014, 2014
S. Zhou, L. Gonzalez, A. Leithead, Z. Finewax, R. Thalman, A. Vlasenko, S. Vagle, L.A. Miller, S.-M. Li, S. Bureekul, H. Furutani, M. Uematsu, R. Volkamer, and J. Abbatt
Atmos. Chem. Phys., 14, 1371–1384, https://doi.org/10.5194/acp-14-1371-2014, https://doi.org/10.5194/acp-14-1371-2014, 2014
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Short summary
A unique environmental electron microscope was used for monitoring the evaporation of salty frost flowers. We observe a cohesive villous brine surface layer facilitating the formation of NaCl microcrystals at temperatures below −10°C as the brine oversaturation is achieved. This finding confirms the increased surface area and thus also the enhanced heterogeneous reactivity; however, no support for the easiness of fragmentation to produce aerosols can be provided.
A unique environmental electron microscope was used for monitoring the evaporation of salty...
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