Articles | Volume 15, issue 4
https://doi.org/10.5194/tc-15-2001-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/tc-15-2001-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
23 Apr 2021
Research article |
| 23 Apr 2021
| 23 Apr 2021
Interfacial supercooling and the precipitation of hydrohalite in frozen NaCl solutions as seen by X-ray absorption spectroscopy
Thorsten Bartels-Rausch
CORRESPONDING AUTHOR
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
Xiangrui Kong
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
now at: Department of Chemistry and Molecular Biology, Atmospheric
Science, University of Gothenburg, Gothenburg, Sweden
Fabrizio Orlando
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
now at: Omya International AG, Oftringen, Switzerland
Luca Artiglia
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
Astrid Waldner
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
Thomas Huthwelker
Swiss Light Source (SLS), Paul Scherrer Institut, Villigen PSI,
Switzerland
Markus Ammann
Laboratory of Environmental Chemistry, Paul Scherrer Institut,
Villigen PSI, Switzerland
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Guo Li, Hang Su, Uwe Kuhn, Hannah Meusel, Markus Ammann, Min Shao, Ulrich Pöschl, and Yafang Cheng
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Coated-wall flow tube reactors are frequently used to investigate gas uptake and heterogeneous or multiphase reaction kinetics under laminar flow conditions. In previous applications, the effects of coating surface roughness on flow conditions were not well quantified. In this study, a criterion is proposed to eliminate/minimize the potential effects of coating surface roughness on laminar flow in coated-wall flow tube experiments and validate the applications of diffusion correction methods.
Hannah Meusel, Yasin Elshorbany, Uwe Kuhn, Thorsten Bartels-Rausch, Kathrin Reinmuth-Selzle, Christopher J. Kampf, Guo Li, Xiaoxiang Wang, Jos Lelieveld, Ulrich Pöschl, Thorsten Hoffmann, Hang Su, Markus Ammann, and Yafang Cheng
Atmos. Chem. Phys., 17, 11819–11833, https://doi.org/10.5194/acp-17-11819-2017, https://doi.org/10.5194/acp-17-11819-2017, 2017
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In this study we investigated protein nitration and decomposition by light in the presence of NO2 via flow tube measurements. Nitrated proteins have an enhanced allergenic potential but so far nitration was only studied in dark conditions. Under irradiated conditions we found that proteins predominantly decompose while forming nitrous acid (HONO) an important precursor of the OH radical. Unlike other studies on heterogeneous NO2 conversion we found a stable HONO formation over a long period.
Thomas Berkemeier, Markus Ammann, Ulrich K. Krieger, Thomas Peter, Peter Spichtinger, Ulrich Pöschl, Manabu Shiraiwa, and Andrew J. Huisman
Atmos. Chem. Phys., 17, 8021–8029, https://doi.org/10.5194/acp-17-8021-2017, https://doi.org/10.5194/acp-17-8021-2017, 2017
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Goran Gržinić, Thorsten Bartels-Rausch, Andreas Türler, and Markus Ammann
Atmos. Chem. Phys., 17, 6493–6502, https://doi.org/10.5194/acp-17-6493-2017, https://doi.org/10.5194/acp-17-6493-2017, 2017
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Nitrogen oxides (NOx) largely control the ozone budget in the troposphere globally. Dinitrogen pentoxide (N2O5) is an important species as a nighttime reservoir for nitrogen oxides. Loss of N2O5 to aerosol particles is therefore important for the budget of NOx and the oxidation capacity. Here we provide direct evidence for its efficient accommodation into aqueous aerosol particles and its fast dissociation, which has not been elucidated as directly in previous studies.
Pascale S. J. Lakey, Thomas Berkemeier, Manuel Krapf, Josef Dommen, Sarah S. Steimer, Lisa K. Whalley, Trevor Ingham, Maria T. Baeza-Romero, Ulrich Pöschl, Manabu Shiraiwa, Markus Ammann, and Dwayne E. Heard
Atmos. Chem. Phys., 16, 13035–13047, https://doi.org/10.5194/acp-16-13035-2016, https://doi.org/10.5194/acp-16-13035-2016, 2016
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Chemical oxidation in the atmosphere removes pollutants and greenhouse gases but generates undesirable products such as secondary organic aerosol. Radicals are key intermediates in oxidation, but how they interact with aerosols is still not well understood. Here we use a laser to measure the loss of radicals onto oxidised aerosols generated in a smog chamber. The loss of radicals was controlled by the thickness or viscosity of the aerosols, confirmed by using sugar aerosols of known thickness.
Laura González Palacios, Pablo Corral Arroyo, Kifle Z. Aregahegn, Sarah S. Steimer, Thorsten Bartels-Rausch, Barbara Nozière, Christian George, Markus Ammann, and Rainer Volkamer
Atmos. Chem. Phys., 16, 11823–11836, https://doi.org/10.5194/acp-16-11823-2016, https://doi.org/10.5194/acp-16-11823-2016, 2016
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The sources of radicals at aerosol surfaces are highly uncertain. Here we investigate the HO2 radical production from the UV irradiation of imidazole-2-carboxaldehyde (IC) in bulk aqueous films containing IC and citric acid, as well as IC in ammonium sulfate aerosols. We find that IC is an efficient photosensitizer that forms HO2 radicals from H-donor chemistry. IC is a proxy species for brown carbon in atmospheric aerosols.
Guo Li, Hang Su, Xin Li, Uwe Kuhn, Hannah Meusel, Thorsten Hoffmann, Markus Ammann, Ulrich Pöschl, Min Shao, and Yafang Cheng
Atmos. Chem. Phys., 16, 10299–10311, https://doi.org/10.5194/acp-16-10299-2016, https://doi.org/10.5194/acp-16-10299-2016, 2016
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Indoor and outdoor formaldehyde (HCHO) are both of considerable concern because of its health effects and its role in atmospheric chemistry. The heterogeneous reactions between gaseous HCHO with soils can pose important impact on both HCHO budget and soil ecosystem. Our results confirms that HCHO uptake by soil is a complex process involving both adsorption/desorption and chemical reactions. Soil and soil-derived airborne particles can either act as a source or a sink for HCHO.
G. Gržinić, T. Bartels-Rausch, T. Berkemeier, A. Türler, and M. Ammann
Atmos. Chem. Phys., 15, 13615–13625, https://doi.org/10.5194/acp-15-13615-2015, https://doi.org/10.5194/acp-15-13615-2015, 2015
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The heterogeneous loss of dinitrogen pentoxide (N2O5) to citric acid aerosol, a proxy for highly oxygenated secondary organic aerosol, is shown to be substantially lower than to other aqueous organic aerosol proxies investigated previously. This is attributed to the widely changing viscosity within the atmospherically relevant humidity range. It may explain some of the unexpectedly low loss rates of N2O5 to aerosol particles derived from field studies.
S. S. Steimer, U. K. Krieger, Y.-F. Te, D. M. Lienhard, A. J. Huisman, B. P. Luo, M. Ammann, and T. Peter
Atmos. Meas. Tech., 8, 2397–2408, https://doi.org/10.5194/amt-8-2397-2015, https://doi.org/10.5194/amt-8-2397-2015, 2015
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Atmospheric aerosol is often subject to supersaturated or supercooled conditions where bulk measurements are not possible. Here we demonstrate how measurements using single particle electrodynamic levitation combined with light scattering spectroscopy allow the retrieval of thermodynamic data, optical properties and water diffusivity of such metastable particles even when auxiliary bulk data are not available due to lack of sufficient amounts of sample.
E. S. Thomson, X. Kong, P. Papagiannakopoulos, and J. B. C. Pettersson
Atmos. Chem. Phys., 15, 1621–1632, https://doi.org/10.5194/acp-15-1621-2015, https://doi.org/10.5194/acp-15-1621-2015, 2015
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We present new observations of ice nucleation on substrate surfaces that affirm the ``puzzle'' of very high supersaturations required for nucleation from the vapor phase. To explain the observations, the kinetics and thermodynamics of nucleation theory are explored. The results explicitly connect the nucleation to the substrate material's surface binding energy and demonstrate that an improved fundamental understanding must include a strict understanding of the relevant microphysics.
S. S. Steimer, M. Lampimäki, E. Coz, G. Grzinic, and M. Ammann
Atmos. Chem. Phys., 14, 10761–10772, https://doi.org/10.5194/acp-14-10761-2014, https://doi.org/10.5194/acp-14-10761-2014, 2014
M. Legrand, S. Preunkert, M. Frey, Th. Bartels-Rausch, A. Kukui, M. D. King, J. Savarino, M. Kerbrat, and B. Jourdain
Atmos. Chem. Phys., 14, 9963–9976, https://doi.org/10.5194/acp-14-9963-2014, https://doi.org/10.5194/acp-14-9963-2014, 2014
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
M. Ammann, R. A. Cox, J. N. Crowley, M. E. Jenkin, A. Mellouki, M. J. Rossi, J. Troe, and T. J. Wallington
Atmos. Chem. Phys., 13, 8045–8228, https://doi.org/10.5194/acp-13-8045-2013, https://doi.org/10.5194/acp-13-8045-2013, 2013
T. Bartels-Rausch, S. N. Wren, S. Schreiber, F. Riche, M. Schneebeli, and M. Ammann
Atmos. Chem. Phys., 13, 6727–6739, https://doi.org/10.5194/acp-13-6727-2013, https://doi.org/10.5194/acp-13-6727-2013, 2013
T. Berkemeier, A. J. Huisman, M. Ammann, M. Shiraiwa, T. Koop, and U. Pöschl
Atmos. Chem. Phys., 13, 6663–6686, https://doi.org/10.5194/acp-13-6663-2013, https://doi.org/10.5194/acp-13-6663-2013, 2013
E. S. Thomson, X. Kong, N. Marković, P. Papagiannakopoulos, and J. B. C. Pettersson
Atmos. Chem. Phys., 13, 2223–2233, https://doi.org/10.5194/acp-13-2223-2013, https://doi.org/10.5194/acp-13-2223-2013, 2013
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From atmospheric water isotopes measurement to firn core interpretation in Adélie Land: a case study for isotope-enabled atmospheric models in Antarctica
Black carbon concentrations and modeled smoke deposition fluxes to the bare-ice dark zone of the Greenland Ice Sheet
Dynamics of the snow grain size in a windy coastal area of Antarctica from continuous in situ spectral-albedo measurements
Forcing and impact of the Northern Hemisphere continental snow cover in 1979–2014
On the energy budget of a low-Arctic snowpack
The role of sublimation as a driver of climate signals in the water isotope content of surface snow: laboratory and field experimental results
Synoptic control on snow avalanche activity in central Spitsbergen
Tracing devastating fires in Portugal to a snow archive in the Swiss Alps: a case study
Systematic bias of Tibetan Plateau snow cover in subseasonal-to-seasonal models
Warm-air entrainment and advection during alpine blowing snow events
Quantifying the impact of synoptic weather types and patterns on energy fluxes of a marginal snowpack
Radar measurements of blowing snow off a mountain ridge
Brief communication: Rare ambient saturation during drifting snow occurrences at a coastal location of East Antarctica
Understanding snow bedform formation by adding sintering to a cellular automata model
Evaluation of snow depth and snow cover over the Tibetan Plateau in global reanalyses using in situ and satellite remote sensing observations
Brief communication: Analysis of organic matter in surface snow by PTR-MS – implications for dry deposition dynamics in the Alps
Evaluation of the CloudSat surface snowfall product over Antarctica using ground-based precipitation radars
Sonja Wahl, Benjamin Walter, Franziska Aemisegger, Luca Bianchi, and Michael Lehning
The Cryosphere, 18, 4493–4515, https://doi.org/10.5194/tc-18-4493-2024, https://doi.org/10.5194/tc-18-4493-2024, 2024
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Wind-driven airborne transport of snow is a frequent phenomenon in snow-covered regions and a process difficult to study in the field as it is unfolding over large distances. Thus, we use a ring wind tunnel with infinite fetch positioned in a cold laboratory to study the evolution of the shape and size of airborne snow. With the help of stable water isotope analyses, we identify the hitherto unobserved process of airborne snow metamorphism that leads to snow particle rounding and growth.
Dylan Reynolds, Louis Quéno, Michael Lehning, Mahdi Jafari, Justine Berg, Tobias Jonas, Michael Haugeneder, and Rebecca Mott
The Cryosphere, 18, 4315–4333, https://doi.org/10.5194/tc-18-4315-2024, https://doi.org/10.5194/tc-18-4315-2024, 2024
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Information about atmospheric variables is needed to produce simulations of mountain snowpacks. We present a model that can represent processes that shape mountain snowpack, focusing on the accumulation of snow. Simulations show that this model can simulate the complex path that a snowflake takes towards the ground and that this leads to differences in the distribution of snow by the end of winter. Overall, this model shows promise with regard to improving forecasts of snow in mountains.
Lara Foth, Wolfgang Dorn, Annette Rinke, Evelyn Jäkel, and Hannah Niehaus
The Cryosphere, 18, 4053–4064, https://doi.org/10.5194/tc-18-4053-2024, https://doi.org/10.5194/tc-18-4053-2024, 2024
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It is demonstrated that the explicit consideration of the cloud dependence of the snow surface albedo in a climate model results in a more realistic simulation of the surface albedo during the snowmelt period in late May and June. Although this improvement appears to be relatively insubstantial, it has significant impact on the simulated sea-ice volume and extent in the model due to an amplification of the snow/sea-ice albedo feedback, one of the main contributors to Arctic amplification.
Daniela Brito Melo, Armin Sigmund, and Michael Lehning
The Cryosphere, 18, 1287–1313, https://doi.org/10.5194/tc-18-1287-2024, https://doi.org/10.5194/tc-18-1287-2024, 2024
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Snow saltation – the transport of snow close to the surface – occurs when the wind blows over a snow-covered surface with sufficient strength. This phenomenon is represented in some climate models; however, with limited accuracy. By performing numerical simulations and a detailed analysis of previous works, we show that snow saltation is characterized by two regimes. This is not represented in climate models in a consistent way, which hinders the quantification of snow transport and sublimation.
Annelies Voordendag, Brigitta Goger, Rainer Prinz, Tobias Sauter, Thomas Mölg, Manuel Saigger, and Georg Kaser
The Cryosphere, 18, 849–868, https://doi.org/10.5194/tc-18-849-2024, https://doi.org/10.5194/tc-18-849-2024, 2024
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Wind-driven snow redistribution affects glacier mass balance. A case study of Hintereisferner glacier in Austria used high-resolution observations and simulations to model snow redistribution. Simulations matched observations, showing the potential of the model for studying snow redistribution on other mountain glaciers.
Christophe Leroy-Dos Santos, Elise Fourré, Cécile Agosta, Mathieu Casado, Alexandre Cauquoin, Martin Werner, Benedicte Minster, Frédéric Prié, Olivier Jossoud, Leila Petit, and Amaëlle Landais
The Cryosphere, 17, 5241–5254, https://doi.org/10.5194/tc-17-5241-2023, https://doi.org/10.5194/tc-17-5241-2023, 2023
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In the face of global warming, understanding the changing water cycle and temperatures in polar regions is crucial. These factors directly impact the balance of ice sheets in the Arctic and Antarctic. By studying the composition of water vapor, we gain insights into climate variations. Our 2-year study at Dumont d’Urville station, Adélie Land, offers valuable data to refine models. Additionally, we demonstrate how modeling aids in interpreting signals from ice core samples in the region.
Alia L. Khan, Peng Xian, and Joshua P. Schwarz
The Cryosphere, 17, 2909–2918, https://doi.org/10.5194/tc-17-2909-2023, https://doi.org/10.5194/tc-17-2909-2023, 2023
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Ice–albedo feedbacks in the ablation region of the Greenland Ice Sheet are difficult to constrain and model. Surface samples were collected across the 2014 summer melt season from different ice surface colors. On average, concentrations were higher in patches that were visibly dark, compared to medium patches and light patches, suggesting that black carbon aggregation contributed to snow aging, and vice versa. High concentrations are likely due to smoke transport from high-latitude wildfires.
Sara Arioli, Ghislain Picard, Laurent Arnaud, and Vincent Favier
The Cryosphere, 17, 2323–2342, https://doi.org/10.5194/tc-17-2323-2023, https://doi.org/10.5194/tc-17-2323-2023, 2023
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To assess the drivers of the snow grain size evolution during snow drift, we exploit a 5-year time series of the snow grain size retrieved from spectral-albedo observations made with a new, autonomous, multi-band radiometer and compare it to observations of snow drift, snowfall and snowmelt at a windy location of coastal Antarctica. Our results highlight the complexity of the grain size evolution in the presence of snow drift and show an overall tendency of snow drift to limit its variations.
Guillaume Gastineau, Claude Frankignoul, Yongqi Gao, Yu-Chiao Liang, Young-Oh Kwon, Annalisa Cherchi, Rohit Ghosh, Elisa Manzini, Daniela Matei, Jennifer Mecking, Lingling Suo, Tian Tian, Shuting Yang, and Ying Zhang
The Cryosphere, 17, 2157–2184, https://doi.org/10.5194/tc-17-2157-2023, https://doi.org/10.5194/tc-17-2157-2023, 2023
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Snow cover variability is important for many human activities. This study aims to understand the main drivers of snow cover in observations and models in order to better understand it and guide the improvement of climate models and forecasting systems. Analyses reveal a dominant role for sea surface temperature in the Pacific. Winter snow cover is also found to have important two-way interactions with the troposphere and stratosphere. No robust influence of the sea ice concentration is found.
Georg Lackner, Florent Domine, Daniel F. Nadeau, Annie-Claude Parent, François Anctil, Matthieu Lafaysse, and Marie Dumont
The Cryosphere, 16, 127–142, https://doi.org/10.5194/tc-16-127-2022, https://doi.org/10.5194/tc-16-127-2022, 2022
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The surface energy budget is the sum of all incoming and outgoing energy fluxes at the Earth's surface and has a key role in the climate. We measured all these fluxes for an Arctic snowpack and found that most incoming energy from radiation is counterbalanced by thermal radiation and heat convection while sublimation was negligible. Overall, the snow model Crocus was able to simulate the observed energy fluxes well.
Abigail G. Hughes, Sonja Wahl, Tyler R. Jones, Alexandra Zuhr, Maria Hörhold, James W. C. White, and Hans Christian Steen-Larsen
The Cryosphere, 15, 4949–4974, https://doi.org/10.5194/tc-15-4949-2021, https://doi.org/10.5194/tc-15-4949-2021, 2021
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Water isotope records in Greenland and Antarctic ice cores are a valuable proxy for paleoclimate reconstruction and are traditionally thought to primarily reflect precipitation input. However,
post-depositional processes are hypothesized to contribute to the isotope climate signal. In this study we use laboratory experiments, field experiments, and modeling to show that sublimation and vapor–snow isotope exchange can rapidly influence the isotopic composition of the snowpack.
Holt Hancock, Jordy Hendrikx, Markus Eckerstorfer, and Siiri Wickström
The Cryosphere, 15, 3813–3837, https://doi.org/10.5194/tc-15-3813-2021, https://doi.org/10.5194/tc-15-3813-2021, 2021
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We investigate how snow avalanche activity in central Spitsbergen, Svalbard, is broadly controlled by atmospheric circulation. Avalanche activity in this region is generally associated with atmospheric circulation conducive to increased precipitation, wind speeds, and air temperatures near Svalbard during winter storms. Our results help place avalanche activity on Spitsbergen in the wider context of Arctic environmental change and provide a foundation for improved avalanche forecasting here.
Dimitri Osmont, Sandra Brugger, Anina Gilgen, Helga Weber, Michael Sigl, Robin L. Modini, Christoph Schwörer, Willy Tinner, Stefan Wunderle, and Margit Schwikowski
The Cryosphere, 14, 3731–3745, https://doi.org/10.5194/tc-14-3731-2020, https://doi.org/10.5194/tc-14-3731-2020, 2020
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In this interdisciplinary case study, we were able to link biomass burning emissions from the June 2017 wildfires in Portugal to their deposition in the snowpack at Jungfraujoch, Swiss Alps. We analysed black carbon and charcoal in the snowpack, calculated backward trajectories, and monitored the fire evolution by remote sensing. Such case studies help to understand the representativity of biomass burning records in ice cores and how biomass burning tracers are archived in the snowpack.
Wenkai Li, Shuzhen Hu, Pang-Chi Hsu, Weidong Guo, and Jiangfeng Wei
The Cryosphere, 14, 3565–3579, https://doi.org/10.5194/tc-14-3565-2020, https://doi.org/10.5194/tc-14-3565-2020, 2020
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Understanding the forecasting skills of the subseasonal-to-seasonal (S2S) model on Tibetan Plateau snow cover (TPSC) is the first step to applying the S2S model to hydrological forecasts over the Tibetan Plateau. This study conducted a multimodel comparison of the TPSC prediction skill to learn about their performance in capturing TPSC variability. S2S models can skillfully forecast TPSC within a lead time of 2 weeks but show limited skill beyond 3 weeks. Systematic biases of TPSC were found.
Nikolas O. Aksamit and John W. Pomeroy
The Cryosphere, 14, 2795–2807, https://doi.org/10.5194/tc-14-2795-2020, https://doi.org/10.5194/tc-14-2795-2020, 2020
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In cold regions, it is increasingly important to quantify the amount of water stored as snow at the end of winter. Current models are inconsistent in their estimates of snow sublimation due to atmospheric turbulence. Specific wind structures have been identified that amplify potential rates of surface and blowing snow sublimation during blowing snow storms. The recurrence of these motions has been modeled by a simple scaling argument that has its foundation in turbulent boundary layer theory.
Andrew J. Schwartz, Hamish A. McGowan, Alison Theobald, and Nik Callow
The Cryosphere, 14, 2755–2774, https://doi.org/10.5194/tc-14-2755-2020, https://doi.org/10.5194/tc-14-2755-2020, 2020
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This study measured energy available for snowmelt during the 2016 and 2017 snow seasons in Kosciuszko National Park, NSW, Australia, and identified common traits for days with similar weather characteristics. The analysis showed that energy available for snowmelt was highest in the days before cold fronts passed through the region due to higher air temperatures. Regardless of differences in daily weather characteristics, solar radiation contributed the highest amount of energy to snowpack melt.
Benjamin Walter, Hendrik Huwald, Josué Gehring, Yves Bühler, and Michael Lehning
The Cryosphere, 14, 1779–1794, https://doi.org/10.5194/tc-14-1779-2020, https://doi.org/10.5194/tc-14-1779-2020, 2020
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We applied a horizontally mounted low-cost precipitation radar to measure velocities, frequency of occurrence, travel distances and turbulence characteristics of blowing snow off a mountain ridge. Our analysis provides a first insight into the potential of radar measurements for determining blowing snow characteristics, improves our understanding of mountain ridge blowing snow events and serves as a valuable data basis for validating coupled numerical weather and snowpack simulations.
Charles Amory and Christoph Kittel
The Cryosphere, 13, 3405–3412, https://doi.org/10.5194/tc-13-3405-2019, https://doi.org/10.5194/tc-13-3405-2019, 2019
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Snow mass fluxes and vertical profiles of relative humidity are used to document concurrent occurrences of drifting snow and near-surface air saturation at a site dominated by katabatic winds in East Antarctica. Despite a high prevalence of drifting snow conditions, we demonstrate that saturation is reached only in the most extreme wind and transport conditions and discuss implications for the understanding of surface mass and atmospheric moisture budgets of the Antarctic ice sheet.
Varun Sharma, Louise Braud, and Michael Lehning
The Cryosphere, 13, 3239–3260, https://doi.org/10.5194/tc-13-3239-2019, https://doi.org/10.5194/tc-13-3239-2019, 2019
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Snow surfaces, under the action of wind, form beautiful shapes such as waves and dunes. This study is the first ever study to simulate these shapes using a state-of-the-art numerical modelling tool. While these beautiful and ephemeral shapes on snow surfaces are fascinating from a purely aesthetic point of view, they are also critical in regulating the transfer of heat and mass between the atmosphere and snowpacks, thus being of huge importance to the Earth system.
Yvan Orsolini, Martin Wegmann, Emanuel Dutra, Boqi Liu, Gianpaolo Balsamo, Kun Yang, Patricia de Rosnay, Congwen Zhu, Wenli Wang, Retish Senan, and Gabriele Arduini
The Cryosphere, 13, 2221–2239, https://doi.org/10.5194/tc-13-2221-2019, https://doi.org/10.5194/tc-13-2221-2019, 2019
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The Tibetan Plateau region exerts a considerable influence on regional climate, yet the snowpack over that region is poorly represented in both climate and forecast models due a large precipitation and snowfall bias. We evaluate the snowpack in state-of-the-art atmospheric reanalyses against in situ observations and satellite remote sensing products. Improved snow initialisation through better use of snow observations in reanalyses may improve medium-range to seasonal weather forecasts.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Niels Souverijns, Alexandra Gossart, Stef Lhermitte, Irina V. Gorodetskaya, Jacopo Grazioli, Alexis Berne, Claudio Duran-Alarcon, Brice Boudevillain, Christophe Genthon, Claudio Scarchilli, and Nicole P. M. van Lipzig
The Cryosphere, 12, 3775–3789, https://doi.org/10.5194/tc-12-3775-2018, https://doi.org/10.5194/tc-12-3775-2018, 2018
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Snowfall observations over Antarctica are scarce and currently limited to information from the CloudSat satellite. Here, a first evaluation of the CloudSat snowfall record is performed using observations of ground-based precipitation radars. Results indicate an accurate representation of the snowfall climatology over Antarctica, despite the low overpass frequency of the satellite, outperforming state-of-the-art model estimates. Individual snowfall events are however not well represented.
Cited articles
Abbatt, J. P. D., Thomas, J. L., Abrahamsson, K., Boxe, C., Granfors, A., Jones, A. E., King, M. D., Saiz-Lopez, A., Shepson, P. B., Sodeau, J., Toohey, D. W., Toubin, C., von Glasow, R., Wren, S. N., and Yang, X.: Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions, Atmos. Chem. Phys., 12, 6237–6271, https://doi.org/10.5194/acp-12-6237-2012, 2012.
Alpert, P. A. and Knopf, D. A.: Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model, Atmos. Chem. Phys., 16, 2083–2107, https://doi.org/10.5194/acp-16-2083-2016, 2016.
Ammann, M., Artiglia, L., and Bartels-Rausch, T.: X-ray excited electron
spectroscopy to study gas–liquid interfaces of atmospheric relevance, in:
Physical chemistry of gas-liquid interfaces, Elsevier, 135–166, 2018.
Antalek, M., Pace, E., Hedman, B., Hodgson, K. O., Chillemi, G., Benfatto,
M., Sarangi, R., and Frank, P.: Solvation structure of the halides from
x-ray absorption spectroscopy, J. Chem. Phys., 145, 044318, https://doi.org/10.1063/1.4959589, 2016.
Aristov, Y. I., Di Marco, G., Tokarev, M. M., and Parmon, V. N.: Selective
water sorbents for multiple applications, 3. CaCl2 solution confined in
micro- and mesoporous silica gels: Pore size effect on the
“solidification-melting” diagram, React. Kinet. Catal. Lett., 61, 147–154, https://doi.org/10.1007/BF02477527, 1997.
Artiglia, L., Edebeli, J., Orlando, F., Chen, S., Lee, M.-T., Corral Arroyo,
P., Gilgen, A., Bartels-Rausch, T., Kleibert, A., Vazdar, M., Carignano, M.
A., Francisco, J. S., Shepson, P. B., Gladich, I., and Ammann, M.: A
surface-stabilized ozonide triggers bromide oxidation at the aqueous
solution-vapour interface, Nat. Commun., 8, 700, https://doi.org/10.1038/s41467-017-00823-x,
2017.
Bartels-Rausch, T.: Data set on interfacial supercooling and
the precipitation of hydrohalite in frozen NaCl solutions by X-ray
absorption spectroscopy, EnviDat, https://doi.org/10.16904/envidat.164, 2020.
Bartels-Rausch, T., Jacobi, H.-W., Kahan, T. F., Thomas, J. L., Thomson, E. S., Abbatt, J. P. D., Ammann, M., Blackford, J. R., Bluhm, H., Boxe, C., Domine, F., Frey, M. M., Gladich, I., Guzmán, M. I., Heger, D., Huthwelker, Th., Klán, P., Kuhs, W. F., Kuo, M. H., Maus, S., Moussa, S. G., McNeill, V. F., Newberg, J. T., Pettersson, J. B. C., Roeselová, M., and Sodeau, J. R.: A review of air–ice chemical and physical interactions (AICI): liquids, quasi-liquids, and solids in snow, Atmos. Chem. Phys., 14, 1587–1633, https://doi.org/10.5194/acp-14-1587-2014, 2014.
Bartels-Rausch, T., Orlando, F., Kong, X., Artiglia, L., and Ammann, M.:
Experimental evidence for the formation of solvation shells by soluble
species at a nonuniform air-ice interface, ACS Earth Space Chem., 1,
572–579, https://doi.org/10.1021/acsearthspacechem.7b00077, 2017.
Blackford, J. R.: Sintering and microstructure of ice: A review, J. Phys. D, 40, R355–R385, https://doi.org/10.1088/0022-3727/40/21/R02, 2007.
Blackford, J. R., Jeffree, C. E., Noake, D. F. J., and Marmo, B. A.:
Microstructural evolution in sintered ice particles containing NaCl observed
by low-temperature scanning electron microscope, Proc. Inst. Mech. Eng, 221,
151–156, https://doi.org/10.1243/14644207JMDA134, 2007.
Bluhm, H., Ogletree, D. F., Fadley, C. S., Hussain, Z., and Salmeron, N.:
The premelting of ice studied with photoelectron spectroscopy, J. Phys.:
Condens. Matter, 14, L227-L233, https://doi.org/10.1088/0953-8984/14/8/108, 2002.
Bluhm, H.: Photoelectron spectroscopy of surfaces under humid conditions,
J. Electron Spectrosc., 177, 71–84, https://doi.org/10.1016/j.elspec.2009.08.006, 2010.
Chakraborty, S. and Kahan, T. F.: Physical characterization of frozen
aqueous solutions containing sodium chloride and humic acid at
environmentally relevant temperatures, ACS Earth Space Chem., 4, 305–310, https://doi.org/10.1021/acsearthspacechem.9b00319, 2020.
Cho, H., Shepson, P. B., Barrie, L. A., Cowin, J. P., and Zaveri, R.: NMR
investigation of the quasi-brine layer in ice/brine mixtures, J. Phys. Chem.
B, 106, 11226–11232, https://doi.org/10.1021/jp020449+, 2002.
Christenson, H. K.: Confinement effects on freezing and melting, J. Phys., 13, R95–R133, https://doi.org/10.1088/0953-8984/13/11/201, 2001.
Cleff, B. and Mehlhorn, W.: Das KLL- Auger-Spektrum von Chlor, Z. Phys. A, 219, 311–324, https://doi.org/10.1007/BF01395528, 1969.
Craig, J. R., Light, J. F., Parker, B. C., and Mudrey, M. G.: Identification
of hydrohalite, Antarct. J. US, 10, 178–179, 1975.
Custard, K. D., Raso, A. R. W., Shepson, P. B., Staebler, R. M., and Pratt,
K. A.: Production and release of molecular bromine and chlorine from the
arctic coastal snowpack, ACS Earth Space Chem., 1, 142–151, https://doi.org/10.1021/acsearthspacechem.7b00014, 2017.
Dominé, F. and Shepson, P. B.: Air-snow interactions and atmospheric
chemistry, Science, 297, 1506–1510, https://doi.org/10.1126/science.1074610, 2002.
Dominé, F., Sparapani, R., Ianniello, A., and Beine, H. J.: The origin of sea salt in snow on Arctic sea ice and in coastal regions, Atmos. Chem. Phys., 4, 2259–2271, https://doi.org/10.5194/acp-4-2259-2004, 2004.
Edebeli, J., Ammann, M., and Bartels-Rausch, T.: Microphysics of the aqueous
bulk counters the water activity driven rate acceleration of bromide
oxidation by ozone from 289–245 K, Environ. Sci. Process. Impacts, 21, 63–73, https://doi.org/10.1039/c8em00417j, 2019.
Evans, K. A., Mavrogenes, J. A., O'Neill, H. S., Keller, N. S., and Jang, L.
Y.: A preliminary investigation of chlorine XANES in silicate glasses,
Geochem. Geophys. Geosy., 9, Q10003, https://doi.org/10.1029/2008gc002157, 2008.
Ewing, G. E.: H2O on NaCl: From single molecule, to clusters, to monolayer,
to thin film, to deliquescence, chap. 12, Springer-Verlag,
Berlin/Heidelberg, 1–25, 2005.
Finlayson-Pitts, B. J.: The tropospheric chemistry of sea salt: A
molecular-level view of the chemistry of NaCl and NaBr, Chem. Rev., 103,
4801–4822, https://doi.org/10.1021/cr020653t, 2003.
Finlayson-Pitts, B. J.: Halogens in the troposphere, Anal. Chem., 82,
770–776, https://doi.org/10.1021/ac901478p, 2010.
Fujimori, T., Takaoka, M., and Morisawa, S.: Chlorinated aromatic compounds
in a thermal process promoted by oxychlorination of ferric chloride,
Environ. Sci. Technol., 44, 1974–1979, https://doi.org/10.1021/es903337d, 2010.
Gladich, I., Chen, S., Vazdar, M., Boucly, A., Yang, H., Ammann, M., and
Artiglia, L.: Surface propensity of aqueous atmospheric bromine at the
liquid-gas interface, J. Phys. Chem. Lett., 11, 3422–3429, https://doi.org/10.1021/acs.jpclett.0c00633, 2020.
Grannas, A. M., Bausch, A. R., and Mahanna, K. M.: Enhanced aqueous
photochemical reaction rates after freezing, J. Phys. Chem. A, 111,
11043–11049, https://doi.org/10.1021/jp073802q, 2007.
Halfacre, J. W., Shepson, P. B., and Pratt, K. A.: pH-dependent production of molecular chlorine, bromine, and iodine from frozen saline surfaces, Atmos. Chem. Phys., 19, 4917–4931, https://doi.org/10.5194/acp-19-4917-2019, 2019.
Harada, M., Tasaki, Y., Tasaki, Y., Qu, H., and Okada, T.: Hydration of ions
and salt crystallization in liquid phase coexistent with ice at temperature
below eutectic point, RSC Advances, 2, 461–466, https://doi.org/10.1039/c1ra00801c, 2011.
Huggins, F. E. and Huffman, G. P.: Chlorine in coal – an XAFS spectroscopic
investigation, Fuel, 74, 556–569, https://doi.org/10.1016/0016-2361(95)98359-m, 1995.
Hullar, T. and Anastasio, C.: Direct visualization of solute locations in laboratory ice samples, The Cryosphere, 10, 2057–2068, https://doi.org/10.5194/tc-10-2057-2016, 2016.
Kahan, T. F., Wren, S. N., and Donaldson, D. J.: A pinch of salt is all it
takes: Chemistry at the frozen water surface, Acc. Chem. Res., 47,
1587–1594, https://doi.org/10.1021/ar5000715, 2014.
Kirpes, R. M., Bonanno, D., May, N. W., Fraund, M., Barget, A. J., Moffet,
R. C., Ault, A. P., and Pratt, K. A.: Wintertime arctic sea spray aerosol
composition controlled by sea ice lead microbiology, ACS Cent. Sci., 5,
1760–1767, https://doi.org/10.1021/acscentsci.9b00541, 2019.
Klewe, B., Pedersen, B., and Iucr: The crystal structure of sodium chloride
dihydrate, Acta Crystallogr., 30, 2363–2371, https://doi.org/10.1107/S0567740874007138, 1974.
Knipping, E. M., Lakin, M. J., Foster, K. L., Jungwirth, P., Tobias, D. J.,
Gerber, R. B., Dabdub, D., and Finlayson-Pitts, B. J.: Experiments and
simulations of ion-enhanced interfacial chemistry on aqueous NaCl aerosols,
Science, 288, 301–306, https://doi.org/10.1126/science.288.5464.301, 2000.
Kong, X., Waldner, A., Orlando, F., Artiglia, L., Huthwelker, T., Ammann,
M., and Bartels-Rausch, T.: Coexistence of physisorbed and solvated HCl at
warm ice surfaces, J. Phys. Chem. Lett., 8, 4757–4762, https://doi.org/10.1021/acs.jpclett.7b01573, 2017.
Kong, X., Castarède, D., Boucly, A., Artiglia, L., Ammann, M.,
Bartels-Rausch, T., Thomson, E. S., and Pettersson, J. B. C.: Reversibly
physisorbed and chemisorbed water on carboxylic salt surfaces under
atmospheric conditions, J. Phys. Chem. C, 124, 5263–5269, https://doi.org/10.1021/acs.jpcc.0c00319, 2020.
Koop, T., Kapilashrami, A., Molina, L. T., and Molina, M. J.: Phase
transitions of sea-salt/water mixtures at low temperatures: Implications for
ozone chemistry in the polar marine boundary layer, J. Geophys. Res., 105,
26393–26402, https://doi.org/10.1029/2000JD900413, 2000a.
Koop, T., Luo, B. P., Tsias, A., and Peter, T.: Water activity as the
determinant for homogeneous ice nucleation in aqueous solutions, Nature,
406, 611–614, https://doi.org/10.1038/35020537, 2000b.
Krausko, J., Runštuk, J., Neděla, V., Klan, P., and Heger, D.:
Observation of a brine layer on an ice surface with an environmental
scanning electron microscope at higher pressures and temperatures, Langmuir,
30, 5441–5447, https://doi.org/10.1021/la500334e, 2014.
Krepelova, A., Huthwelker, T., Bluhm, H., and Ammann, M.: Surface chemical
properties of eutectic and frozen NaCl solutions probed by XPS and NEXAFS,
Chem. Phys. Chem., 11, 3859–3866, https://doi.org/10.1002/cphc.201000461, 2010a.
Krepelova, A., Newberg, J. T., Huthwelker, T., Bluhm, H., and Ammann, M.:
The nature of nitrate at the ice surface studied by XPS and NEXAFS, Phys.
Chem. Chem. Phys., 12, 8870–8880, https://doi.org/10.1039/c0cp00359j, 2010b.
Krepelova, A., Bartels-Rausch, T., Brown, M. A., Bluhm, H., and Ammann, M.:
Adsorption of acetic acid on ice studied by ambient-pressure XPS and
partial-electron-yield NEXAFS spectroscopy at 230–240 K, J. Phys. Chem. A,
117, 401–409, https://doi.org/10.1021/jp3102332, 2013.
Laskin, A., Wang, H., Robertson, W. H., Cowin, J. P., Ezell, M. J., and
Finlayson-Pitts, B. J.: A new approach to determining gas-particle reaction
probabilities and application to the heterogeneous reaction of deliquesced
sodium chloride particles with gas-phase hydroxyl radicals, J. Phys. Chem.
A, 110, 10619–10627, https://doi.org/10.1021/jp063263+, 2006.
Lieb-Lappen, R. M., Golden, E. J., and Obbard, R. W.: Metrics for
interpreting the microstructure of sea ice using X-ray micro-computed
tomography, Cold Reg. Sci. Technol., 138, 24–35, https://doi.org/10.1016/j.coldregions.2017.03.001, 2017.
Light, B., Brandt, R. E., and Warren, S. G.: Hydrohalite in cold sea ice:
Laboratory observations of single crystals, surface accumulations, and
migration rates under a temperature gradient, with application to “snowball
earth”, J. Geophys. Res., 114, C07018, https://doi.org/10.1029/2008JC005211, 2009.
Lopez-Hilfiker, F. D., Constantin, K., Kercher, J. P., and Thornton, J. A.: Temperature dependent halogen activation by N2O5 reactions on halide-doped ice surfaces, Atmos. Chem. Phys., 12, 5237–5247, https://doi.org/10.5194/acp-12-5237-2012, 2012.
Luna, M., Rieutord, F., Melman, N. A., Dai, Q., and Salmeron, M.: Adsorption
of water on alkali halide surfaces studied by scanning polarization force
microscopy, J. Phys. Chem. A, 102, 6793–6800, https://doi.org/10.1021/jp9820875, 1998.
Malley, P. P. A., Chakraborty, S., and Kahan, T. F.: Physical
characterization of frozen saltwater solutions using Raman microscopy, ACS
Earth Space Chem., 2, 702–710, https://doi.org/10.1021/acsearthspacechem.8b00045, 2018.
Marti, J. and Mauersberger, K.: A survey and new measurements of ice vapor
pressure at temperatures between 170 and 250 K, Geophys. Res. Lett., 20,
363–366, https://doi.org/10.1029/93GL00105, 1993.
Maus, S., Huthwelker, T., Enzmann, F., Miedaner, M. M., Stampanoni, M.,
Marone, F., Hutterli, M. A., Hintermüller, C., Hintermüller, C., and
Kersten, M.: Synchrotron-based X-ray micro-tomography: Insights into sea ice
microstructure, Sixth Workshop on Baltic Sea Ice Climate, Lammi Biological
Station, Finland, 2008.
Maus, S., Huthwelker, T., Schwikowski, M., and Enzmann, F.: Ion
fractionation in young sea ice from Kongsfjorden, svalbard, Ann.
Glaciol., 52, 301–310, https://doi.org/10.3189/172756411795931804, 2011.
Murphy, D. M., Froyd, K. D., Bian, H., Brock, C. A., Dibb, J. E., DiGangi, J. P., Diskin, G., Dollner, M., Kupc, A., Scheuer, E. M., Schill, G. P., Weinzierl, B., Williamson, C. J., and Yu, P.: The distribution of sea-salt aerosol in the global troposphere, Atmos. Chem. Phys., 19, 4093–4104, https://doi.org/10.5194/acp-19-4093-2019, 2019.
Newberg, J. T. and Bluhm, H.: Adsorption of 2-propanol on ice probed by
ambient pressure X-ray photoelectron spectroscopy, Phys. Chem. Chem. Phys.,
17, 23554–23558, https://doi.org/10.1039/C5CP03821A, 2015.
Nilsson, A., Nordlund, D., Waluyo, I., Huang, N., Ogasawara, H., Kaya, S.,
Bergmann, U., Näslund, L. A., Öström, H., Wernet, P., Andersson,
K. J., Schiros, T., and Pettersson, L. G. M.: X-ray absorption spectroscopy
and X-ray Raman scattering of water and ice; an experimental view, J. Electron Spectrosc., 177, 99–129, https://doi.org/10.1016/j.elspec.2010.02.005, 2010.
Nye, J. F.: Thermal behaviour of glacier and laboratory ice, J. Glaciol.,
37, 401–413, https://doi.org/10.3189/S0022143000005839, 1991.
O'Dowd, C. D., Facchini, M. C., Cavalli, F., Ceburnis, D., Mircea, M.,
Decesari, S., Fuzzi, S., Yoon, Y. J., and Putaud, J.-P.: Biogenically driven
organic contribution to marine aerosol, Nature, 431, 676–680, https://doi.org/10.1038/nature02959, 2004.
Obbard, R. W., Troderman, G., and Baker, I.: Imaging brine and air
inclusions in sea ice using micro-X-ray computed tomography, J. Glaciol.,
55, 1113–1115, https://doi.org/10.3189/002214309790794814, 2009.
Oldridge, N. W. and Abbatt, J. P. D.: Formation of gas-phase bromine from
interaction of ozone with frozen and liquid NaCl/NaBr solutions:
Quantitative separation of surficial chemistry from bulk-phase reaction, J.
Phys. Chem. A, 115, 2590–2598, https://doi.org/10.1021/jp200074u, 2011.
Orlando, F., Waldner, A., Bartels-Rausch, T., Birrer, M., Kato, S., Lee,
M.-T., Proff, C., Huthwelker, T., Kleibert, A., van Bokhoven, J. A., and
Ammann, M.: The environmental photochemistry of oxide surfaces and the
nature of frozen salt solutions: A new in situ XPS approach, Top. Catal.,
59, 591–604, https://doi.org/10.1007/s11244-015-0515-5, 2016.
Osthoff, H. D., Roberts, J. M., Ravishankara, A. R., Williams, E. J.,
Lerner, B. M., Sommariva, R., Bates, T. S., Coffman, D., Quinn, P. K., Dibb,
J. E., Stark, H., Burkholder, J. B., Talukdar, R. K., Meagher, J.,
Fehsenfeld, F. C., and Brown, S. S.: High levels of nitryl chloride in the
polluted subtropical marine boundary layer, Nat. Geosi., 1, 324–328, https://doi.org/10.1038/ngeo177, 2008.
Peckhaus, A., Kiselev, A., Wagner, R., Duft, D., and Leisner, T.:
Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea
salt aerosol particles, J. Chem. Phys., 145, 244503, https://doi.org/10.1063/1.4972589,
2016.
Petrich, C. and Eicken, H.: Growth, structure and properties of sea ice,
Sea Ice, 23–77, https://doi.org/10.1002/9781444317145.ch2, 2009.
Rumble, J.: CRC handbook of chemistry and physics, 100th Edn., CRC
Press/Taylor & Francis, Boca Raton, FL., 2019.
Saiz-Lopez, A. and von Glasow, R.: Reactive halogen chemistry in the
troposphere, Chem. Soc. Rev., 41, 6448–6472, https://doi.org/10.1039/C2CS35208G, 2012.
Simpson, W. R., von Glasow, R., Riedel, K., Anderson, P., Ariya, P., Bottenheim, J., Burrows, J., Carpenter, L. J., Frieß, U., Goodsite, M. E., Heard, D., Hutterli, M., Jacobi, H.-W., Kaleschke, L., Neff, B., Plane, J., Platt, U., Richter, A., Roscoe, H., Sander, R., Shepson, P., Sodeau, J., Steffen, A., Wagner, T., and Wolff, E.: Halogens and their role in polar boundary-layer ozone depletion, Atmos. Chem. Phys., 7, 4375–4418, https://doi.org/10.5194/acp-7-4375-2007, 2007.
Simpson, W. R., Brown, S. S., Saiz-Lopez, A., Thornton, J. A., and von
Glasow, R.: Tropospheric halogen chemistry: Sources, cycling, and impacts,
Chem. Rev., 115, 4035–4062, https://doi.org/10.1021/cr5006638, 2015.
Sjostedt, S. J. and Abbatt, J. P. D.: Release of gas-phase halogens from
sodium halide substrates: Heterogeneous oxidation of frozen solutions and
desiccated salts by hydroxyl radicals, Environ. Res. Lett., 3, 045007, https://doi.org/10.1088/1748-9326/3/4/045007, 2008.
Tanuma, S., Powell, C. J., and Penn, D. R.: Calculations of electron
inelastic mean free paths: 3. Data for 15 inorganic-compounds over the
50–2000 eV range, Surf. Interface Anal., 17, 927–939, https://doi.org/10.1002/sia.740171305,
1991.
Tasaki, Y., Harada, M., and Okada, T.: Eutectic transition of local
structure for bromide ion in bulk and on surface of doped ice, J. Phys.
Chem. C, 114, 12573–12579, https://doi.org/10.1021/jp102246f, 2010.
Thomas, J. L., Stutz, J., Frey, M. M., Bartels-Rausch, T., Altieri, K.,
Baladima, F., Browse, J., Dall'Osto, M., Marelle, L., Mouginot, J.,
Jennifer, G. M., Nomura, D., Pratt, K. A., Willis, M. D., Zieger, P.,
Abbatt, J., Douglas, T. A., Facchini, M. C., France, J., Jones, A. E., Kim,
K., Matrai, P. A., McNeill, V. F., Saiz-Lopez, A., Shepson, P., Steiner, N.,
Law, K. S., Arnold, S. R., Delille, B., Schmale, J., Sonke, J. E.,
Dommergue, A., Voisin, D., Melamed, M. L., and Gier, J.: Fostering
multidisciplinary research on interactions between chemistry, biology, and
physics within the coupled cryosphere-atmosphere system, Elementa, 7, 58,
doi10.1525/elementa.396, 2019.
doi10.1525/elementa.396, 2019.
Thornton, J. A., Kercher, J. P., Riedel, T. P., Wagner, N. L., Cozic, J.,
Holloway, J. S., Dube, W. P., Wolfe, G. M., Quinn, P. K., Middlebrook, A.
M., Alexander, B., and Brown, S. S.: A large atomic chlorine source inferred
from mid-continental reactive nitrogen chemistry, Nature, 464, 271–274, https://doi.org/10.1038/nature08905, 2010.
Tokumasu, K., Harada, M., and Okada, T.: X-ray fluorescence imaging of
frozen aqueous NaCl solutions, Langmuir, 32, 527–533, https://doi.org/10.1021/acs.langmuir.5b04411, 2016.
Wagner, R., Möhler, O., Saathoff, H., Schnaiter, M., and Leisner, T.: New cloud chamber experiments on the heterogeneous ice nucleation ability of oxalic acid in the immersion mode, Atmos. Chem. Phys., 11, 2083–2110, https://doi.org/10.5194/acp-11-2083-2011, 2011.
Wagner, R., Mohler, O., and Schnaiter, M.: Infrared optical constants of
crystalline sodium chloride dihydrate: Application to study the
crystallization of aqueous sodium chloride solution droplets at low
temperatures, J. Phys. Chem. A, 116, 8557–8571, https://doi.org/10.1021/jp306240s, 2012.
Wagner, R., Höhler, K., Möhler, O., Saathoff, H., and Schnaiter, M.:
Crystallization and immersion freezing ability of oxalic and succinic acid
in multicomponent aqueous organic aerosol particles, Geophys. Res. Lett.,
42, 2464–2472, https://doi.org/10.1002/2015GL063075, 2015.
Waldner, A., Artiglia, L., Kong, X., Orlando, F., Huthwelker, T., Ammann,
M., and Bartels-Rausch, T.: Pre-melting and the adsorption of formic acid at
the air–ice interface at 253 K as seen by NEXAFS and XPS, Phys. Chem. Chem.
Phys., 20, 24408–24417, https://doi.org/10.1039/C8CP03621G, 2018.
Wang, S., Schmidt, J. A., Baidar, S., Coburn, S., Dix, B., Koenig, T. K.,
Apel, E. C., Bowdalo, D., Campos, T. L., Eloranta, E., Evans, M. J.,
DiGangi, J. P., Zondlo, M. A., Gao, R.-S., Haggerty, J. A., Hall, S. R.,
Hornbrook, R. S., Jacob, D., Morley, B., Pierce, B., Reeves, M., Romashkin,
P., ter Schure, A., and Volkamer, R.: Active and widespread halogen
chemistry in the tropical and subtropical free troposphere, P. Natl. Acad.
Sci. USA, 112, 201505142–201509286, https://doi.org/10.1073/pnas.1505142112, 2015.
Wise, M. E., Martin, S. T., Russell, L. M., and Buseck, P. R.: Water uptake
by NaCl particles prior to deliquescence and the phase rule, Aerosol Sci.
Technol., 42, 281–294, https://doi.org/10.1080/02786820802047115, 2008.
Wise, M. E., Baustian, K. J., Koop, T., Freedman, M. A., Jensen, E. J., and Tolbert, M. A.: Depositional ice nucleation onto crystalline hydrated NaCl particles: a new mechanism for ice formation in the troposphere, Atmos. Chem. Phys., 12, 1121–1134, https://doi.org/10.5194/acp-12-1121-2012, 2012.
Wren, S. N., Donaldson, D. J., and Abbatt, J. P. D.: Photochemical chlorine and bromine activation from artificial saline snow, Atmos. Chem. Phys., 13, 9789–9800, https://doi.org/10.5194/acp-13-9789-2013, 2013.
Yang, X., Neděla, V., Runštuk, J., Ondrušková, G., Krausko, J., Vetráková, Ľ., and Heger, D.: Evaporating brine from frost flowers with electron microscopy and implications for atmospheric chemistry and sea-salt aerosol formation, Atmos. Chem. Phys., 17, 6291–6303, https://doi.org/10.5194/acp-17-6291-2017, 2017.
Short summary
Chemical reactions in sea salt embedded in coastal polar snow impact the composition and air quality of the atmosphere. Here, we investigate the phase changes of sodium chloride. This is of importance as chemical reactions proceed faster in liquid solutions compared to in solid salt and the precise precipitation temperature of sodium chloride is still under debate. We focus on the upper nanometres of sodium chloride–ice samples because of their role as a reactive interface in the environment.
Chemical reactions in sea salt embedded in coastal polar snow impact the composition and air...
